Abstract:
A metal coordination compound having a binuclear molecular structure represented by the following formula (1):                            
     wherein M1 and M2 independently denotes a metal atom selected from the group consisting of Ir, Pt, Rh, Pd, Ru and Os; P is a quadridentate ligand connected to M1 and M1; Q1 is a bidentate ligand connected to M1; Q2 is a bidentate ligand connected to M2; and n is 1 or 2.

Description:
FIELD OF THE INVENTION AND RELATED ART 
     The present invention relates to a metal coordination compound having a binuclear molecular structure and an organic luminescence device using the metal coordination compound, more particularly to an organic luminescence device exhibiting a long life and a high luminescence efficiency by using the metal coordination compound as a luminescence material. 
     An extensive study on an organic electroluminescence (EL) device for device formation as a luminescence device of a high-speed responsiveness and a high efficiency, has been conducted. 
     As described in detail in, e.g., Macromol. Symp. 125, 1-48 (1997), an organic EL device generally has a structure comprising upper and lower two electrodes and a plurality of organic film layers between the electrodes formed on a transparent substrate. Basic structures thereof are shown in FIGS. 1A-1D. 
     As shown in these figures, an organic EL device generally has a structure comprising a transparent electrode  14 , a metal electrode  11 , and a plurality of organic film layers therebetween on a transparent substrate  15 . 
     In the device of FIG. 1A, the organic layers comprise a luminescence layer  12  and a hole-transporting layer  13 . For the transparent electrode  14 , ITO, etc., having a large work function are used, for providing a good hole-injection characteristic from the transparent electrode  14  to the hole-transporting layer  13 . For the metal electrode  11 , a metal, such as aluminum, magnesium or an alloy of these, having a small work function is used for providing a good electron-injection characteristic to the organic film layers. These electrodes have a thickness of 50-200 nm. 
     For the luminescence layer  12 , aluminum quinolynol complexes (a representative example thereof is Alq3 shown hereinafter), etc., having an electron-transporting characteristic and luminescence characteristic are used. For the hole-transporting layer  13 , biphenyldiamine derivatives (a representative example thereof is α-NPD shown hereinafter), etc., having an electron-donative characteristic are used. 
     The above-structured device has a rectifying characteristic, and when an electric field is applied between the metal electrode  11  as a cathode and the transparent electrode  14  as an anode, electrons are injected from the metal electrode  11  into the luminescence layer  12  and holes are injected from the transparent electrode  15 . The injected holes and electrons are recombined within the luminescence layer  12  to form excitons and cause luminescence. At this time, the hole-transporting layer  13  functions as an electron-blocking layer to increase the recombination efficiency at a boundary between the luminescence layer  12  and hole-transporting layer  13 , thereby increasing the luminescence efficiency. 
     Further, in the structure of FIG. 1B, an electron-transporting layer  16  is disposed between the metal electrode  11  and the luminescence layer  12 . By separating the luminescence and the electron and hole-transportation to provide a more effective carrier blocking structure, effective luminescence can be performed. For the electron-transporting layer  16 , an electron-transporting material, such as an oxidiazole derivative, is used. 
     Further, in the structure of FIG. 1D, a luminescence layer  12  as a single organic layer is disposed between the metal electrode  12  and the transparent electrode  14 . This structure is advantageous in view of productivity of the resultant device, and applicable to production processes using vapor deposition and wet coating. The luminescence layer  12  used in this structure is required to exhibit electron and hole transfer performances in addition to a luminescence performance. 
     Known luminescence processes used heretofore in organic EL devices include one utilizing an excited singlet state and one utilizing an excited triplet state, and the transition from the former state to the ground state is called “fluorescence” and the transition from the latter state to the ground state is called “phosphorescence”. And the substances in these excited states are called a singlet exciton and a triplet exciton, respectively. 
     In most of the organic luminescence devices studied heretofore, fluorescence caused by the transition from the excited singlet state to the ground state, has been utilized. On the other hand, in recent years, devices utilizing phosphorescence via triplet excitons have been studied. 
     Representative published literature may include: 
     Article 1: Improved energy transfer in electrophosphorescent device (D. F. O&#39;Brien, et al., Applied Physics Letters, Vol. 74, No. 3, p. 422-(1999)); and 
     Article 2: Very high-efficiency green organic light-emitting devices based on electrophosphorescence (M. A. Baldo, et al., Applied Physics Letters, Vol. 75, No. 1, p. 4-(1999)). 
     In these articles, a structure including 4 organic layers devices as shown in FIG. 1C has been principally used, including, from the anode side, a hole-transporting layer  13 , a luminescence layer  12 , an exciton diffusion-prevention layer  17  and an electron-transporting layer  16 . Materials used therein include carrier-transporting materials and phosphorescent materials, of which the names and structures are shown below together with their abbreviations. 
     Alq3: aluminum quinolinol complex 
     α-NPD: N4,N4′-di-naphthalene-1-yl-N4,N4′-diphenyl-biphenyl-4,4′-diamine 
     CBP: 4,4′-N,N′-dicarbazole-biphenyl 
     BCP: 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline 
     PtOEP: platinum-octaethylporphyrin complex 
     Ir(ppy) 3 : iridium-phenylpyrimidine complex                         
                           
     Such a phosphorescent material is particularly noted at present because it is expected to provide a luminescence efficiency of 100% in principle being four times that of a fluorescent material. 
     However, such an organic luminescence device utilizing phosphorescence is generally required to be further improved regarding the deterioration of luminescence efficiency and device stability. 
     The reason of the deterioration has not been fully clarified, but the present inventors consider as follows based on the mechanism of phosphorescence. 
     Generally, in a phosphorescent material, a life of the triplet excitons is longer by three or more digits than the life of a-singlet exciton. More specifically, molecules are held in a high-energy excited state for a longer period to cause reaction with surrounding materials, polymer formation among the excitons, a change in fine molecular structure, and a change in structure of the surrounding materials. 
     For this reason, a luminescence center material for use in the phosphorescent-type luminescence device is desired to exhibit a high-efficiency luminescence and a high stability. Further, a phosphorescent material providing a high phosphorescence yield and allowing control of emission wavelength has not been proposed heretofore. Accordingly, such a phosphorescent material is desired to be provided. 
     SUMMARY OF THE INVENTION 
     In view of the above-mentioned circumstances, an object of the present invention is to provide a phosphorescent material allowing a high phosphorescence yield and control of emission wavelength. 
     Another object of the present invention is to provide an organic luminescence device using the phosphorescent material capable of producing high-efficiency luminescence and holding a high luminescence for a long period. 
     According to the present invention, there is provided a metal coordination compound represented by the following formula (1):                           
     wherein M1 and M2 independently denotes a metal atom selected from the group consisting of Ir, Pt, Rh, Pd, Ru and Os; P is a quadridentate ligand connected to M1 and M1; Q1 is a bidentate ligand connected to M1; Q2 is a bidentate ligand connected to M2; and n is 1 or 2. 
     In a preferred embodiment, the bidentate ligand Q1 is represented by formula (2) shown below and the bidentate ligand Q2 is represented by formula (3) shown below:                           
     wherein CyN1 and CyN2 are each cyclic group capable of having a substituent, including a nitrogen atom and bonded to the metal atom M1 or M2 via the nitrogen atom; CyC1 and CyC2 are each cyclic group capable of having a substituent, including a carbon atom and bonded to the metal atom M1 or M2 via the carbon atom with the proviso that the cyclic group CyN1 and the cyclic group CyC1 are bonded to each other via a covalent bond and the cyclic group CyN2 and the cyclic group CyC2 are bonded to each other via covalent bond; 
     the optional substituent of the cyclic groups is selected from a halogen atom; cyano group; a nitro group; a trialkylsilyl group of which the alkyl groups are independently a linear or branched alkyl group having 1 to 8 carbon atoms; a linear or branched alkyl group having 1 to 20 carbon atoms of which the alkyl group can include one or non-neighboring two or more methylene groups that can be replaced with —O—, —S—, —CO—, —CO—O—, —O—CO—, —CH═CH— or —C≡C—, and the alkyl group can include a hydrogen atom that can be optionally replaced with a fluorine atom; and an aromatic group capable of having a substituent (that is a halogen atom, a cyano atom, a nitro atom, a linear or branched alkyl group having 1 to 20 carbon atoms of which the alkyl group can include one or non-neighboring two or more methylene groups that can be replaced with —O—, —S—, —CO—, —CO—O—, —O—CO—, —CH═CH— or —C≡C—, and the alkyl group can include a hydrogen atom that can be optionally replaced with a fluorine atom). 
     In the above-mentioned formula (1), the quadridentate ligand P may preferably be connected to the metal atoms M1 and M2 each via a carbon atom, an oxygen atom or a nitrogen atom. The metal atom M1 is identical in species to the metal atom M2. The bidentate ligand Q1 may preferably be identical to the bidentate ligand Q2. The bidentate ligands Q1 and Q2 may preferably be respectively a carrier-transporting ligand or an energy-trapping ligand and the quadridentate ligand P may preferably be a luminescent ligand. 
     According to the present invention, there is also provided an organic luminescence device, comprising: a pair of electrodes disposed on a substrate, and a luminescence layer comprising at least one organic compound disposed between the electrodes, said organic compound comprising at least one species of a metal coordination compound of the formula (1) described above. 
     These and other objects, features and advantages of the present invention will become more apparent upon a consideration of the following description of the preferred embodiments of the present invention taken in conjunction with the accompanying drawings. 
    
    
     BRIEF DESCRIPTION OF THE DRAWINGS 
     FIGS. 1A-1D respectively illustratively an embodiment of a film layer structure of the organic luminescence device according to the present invention. 
     FIG. 2 illustrates a simple matrix-type organic EL device according to Example 3. 
     FIG. 3 illustrates drive signals used in Example 3. 
     FIG. 4 is an emission spectrum diagram of a metal coordination compound of the present invention in a solution state used in Example 5. 
     FIG. 5 is an emission spectrum diagram of a metal coordination compound of the present invention in a powdery state used in Example 5. 
    
    
     DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS 
     In order to improve a luminescence efficiency of the organic EL device (organic luminescence device), a luminescence center material per se is required to provide a higher yield of luminescence quantum. In addition thereto, when a luminescence layer is comprised of a luminescent material as a guest material and a base or matrix material as a host material, an efficient energy transfer between host material molecules and/or between host material molecule and guest material molecule is also an important factor. 
     Further, the above-described luminescent deterioration in energized state may presumably relate to the luminescent center material per se or an environmental change thereof by its surrounding molecules. 
     The metal coordination compound of the formula (1) used in the present invention produces phosphorescence, and its lowest excited state is believed to be an MLCT* (metal-to-ligand charge transfer) excited state or π-π* excited state in a triplet state, and phosphorescence is caused at the time of transition from such a state to the ground state. 
     The luminescence material of the present invention exhibited a high phosphorescence yield of at least 0.01 and a short phosphorescence life of 1-100 μsec. 
     The shorter phosphorescence life is necessary to provide a resultant EL device with a higher luminescence efficiency. This is because the longer phosphorescence life increases molecules placed in their excited triplet state which is a waiting state for phosphorescence, thus lowering the resultant luminescence efficiency particularly at a higher current density. 
     Accordingly, the metal coordination compound of formula (1) according to the present invention is a suitable luminescent material for an EL device with a higher phosphorescence yield and a shorter phosphorescence life. 
     Further, the shorter phosphorescence life leads to a shorter retention time of molecules in the excited triplet state, i.e., a high-energy state, thus expecting provision of less device deterioration and high durability to the resultant device. 
     The metal coordination compound of the formula (1) used as the luminescent material is binuclear metal coordination compound having two metal atoms in one molecule, thereby to exhibit a stable high-luminescent characteristic. As a result, the metal coordination compound effectively used in the luminescence layer of the organic EL device, particularly being suitable as a phosphorescent material for an organic luminescence device utilizing phosphorescence. 
     The specific reason thereof may be considered as follows. 
     (1) Phosphorescence is emission of light at the time of transition from the excited triplet state to the ground state. In a deactivation process by the phosphorescence, spin is forbidden according to quantum mechanical first-order approximation. However, a heavy atom is present within a molecule to enhance spin-orbit interaction, whereby the forbidden spin is allowed. The spin-orbit interaction becomes stronger as a heavier atom is used. The metal coordination compound used in the present invention has two metal atoms in one molecules, thus effectively encouraging the spin-orbit interaction to produce strong phosphorescence. 
     (2) In a molecular structure of the metal coordination compound of the present invention, the center quadridentate ligand P connecting two metal atoms is sterically surrounded by the two bidentate ligands Q1 and Q2, thus being separated from surrounding or ambient molecules. In the case where the center quadridentate ligand P relates to phosphorescence (luminescence), the quadridentate ligand P is guarded against the surrounding molecules. As a result, a probability of radiationless deactivation due to deactivation passage formed by the intermolecular interaction is considerably decreased thus allowing strong luminescence from the excited state of the metal coordination compound molecule having the center quadridentate ligand P. 
     (3) In the case of an organic EL device, it is important to effect smooth energy transfer from a host molecule to a luminescent guest molecule. In the metal coordination compound of the present invention, the surrounding ligands (the bidentate ligands) Q1 and Q2 function as an energy-trapping ligand liable to promote such energy transfer, and the center ligand (the quadridentate ligand) P functions as a luminescent ligand, thus allowing smooth energy transfer. Further, as described in (2), the center ligand P is guarded against other surrounding molecules, thus being less liable to cause radiationless deactivation to allow strong luminescence with a high luminescence efficiency. 
     Generally, even a compound producing strong luminescence in a dispersion state or a low-concentration solution is liable to cause concentration extinction in such a high-concentration state that molecules thereof are associated or concentrated, thus remarkably lowering a luminescence luminance. This is because energy transfer from an excited molecule to a surrounding molecule is caused to occur, thus being less liable to produce luminescence. In a conventional phosphorescence-type organic luminescence device, a luminescence layer is composed of a material comprising a mixture of a luminescent material and a carrier-transporting material. Accordingly, due to the above-mentioned concentration extinction, a weight proportion of the luminescent material has been restricted to at most 10%. 
     However, the luminescent material used in the present invention has a better concentration extinction-prevention performance, so that the luminescent material can be used in a dispersion state in a host material at a high concentration. 
     In the case where the metal coordination compound of the formula (1) is used as the luminescent material according to the present invention, the concentration extinction is effectively suppressed, thus resulting in a better luminescence efficiency even at a high concentration of the luminescence material. Accordingly, the dispersion concentration (weight proportion) of the luminescent material (the metal coordination compound of the formula (1)) can be increased up to above 10%. Further, it is possible to form a luminescence layer only of the metal coordination compound of the formula (1) (i.e., weight proportion =100%). Accordingly, by the use of the metal coordination compound of the formula (1) according to the present invention, a luminance of light emitted from a resultant organic luminescence device can be increased. 
     Energy levels of the above-mentioned respective ligands may be determined based on a combination of a ligand with a metal atom. 
     For example, in the case of a partial structure (Partial Chemical Structural Formula No. 20 shown hereinafter) having a phenyl-pyridine ligand and Ir as M, an energy level of the partial structure can be determined by measuring a triplet energy level of tri-phenylpyridine-iridium complex (Ir(ppy) 3  shown above). The triplet energy level at room temperature is ca. 2.4 eV. On the other hand, a partial structure having a phenylpyrimidine ligand (as in Partial Chemical Structural Formula No. 1) has a triplet energy level lower than 2.4 eV. 
     When a metal coordination compound of formula (1) (Example Compound No. 1 shown hereinafter) having a center quadridentate ligand P comprising the phenylpyrimidine ligand and surrounding bidentate ligands Q1 and Q2 each comprising the phenylpyridine ligand is used in an organic luminescence device (organic EL device), energy transfer from surrounding host molecules (other molecule) to the phenylpyridine ligands (Q1 and Q2) is first caused to occur to place the phenylpyridine ligands in an excited state. Thereafter, energy thereof is transferred within the metal coordination compound molecule to excite the center phenylpyrimidine ligand (P), thus producing luminescence. 
     Thus, in the case where the center ligand finally causes luminescence based on the above-mentioned energy transfer, it is important to appropriately select functional ligands as described above for preparing the metal coordination compound of the formula (1) according to the present invention. 
     (4) In the case of an organic EL device having a luminescence layer formed of a host material doped with a luminescent material, a resultant device characteristic is largely affected by a carrier-transporting performance of the luminescence material alone. 
     For example, ligands having partial structures (Partial Chemical Structural Formulas Nos. 20, 27, 28 and 34) exhibit a carrier-transporting performance, thus increasing a current value of the resultant device when compared with a device using the host material which is not doped with the luminescent material. This can be confirmed by evaluating current characteristics of organic EL devices using Ir complexes each having three identical charge-transporting ligands (e.g., having the particle structure of Particle Chemical Structural No. 20, 27, 28 or 34). The increase in current value described above is considered to be based on hopping transport of carrier between guest luminescent molecules. Accordingly, when a luminescence material is constituted by a combination of a carrier-transporting ligand for the surrounding bidentate ligands with a luminescent ligand for the center quadridentate ligand, a carrier transport is improved. In addition thereto, the center quadridentate ligand is sterically surrounded by the surrounding bidentate ligands as described above, thus reducing a deactivation probability based on intermolecular interaction to allow a high-efficient luminescence. 
     The organic luminescence device according to the present invention may preferably be an electric field emission device such that an organic compound layer comprising the metal coordination compound of the formula (1) is sandwiched between a pair of opposing electrodes as shown in FIGS. 1A-1D, and a voltage is applied between the electrodes to cause luminescence. 
     A high-efficiency luminescence device according to the present invention is applicable to a product requiring energy economization or a high luminance. More specifically, the luminescence device is applicable to a display apparatus, an illumination apparatus, a printer light source or a backlight for a liquid crystal display apparatus. As for a display apparatus, it allows a flat panel display which is light in weight and provides a highly recognizable display at a low energy consumption. The flat panel display may have a simple matrix structure having a plurality of pixels constituted by intersecting stripe electrode at right angles or an active matrix structure having a plurality of pixels each provided with, e.g., a thin film transistor (TFT) of amorphous silicon or polysilicon. As a printer light source, the luminescence device of the present invention can be used instead of a laser light source of a laser beam printer. Independently addressable devices are arranged in an array form to effect a desired exposure on a photosensitive drum thereby forming an image. The apparatus volume can be remarkably reduced by using the devices of the present invention. For the illumination apparatus or backlight, the energy economization effect according to the present invention can be expected. 
     Hereinbelow, some specific structural formulas (Example Compound Nos. 1-760) of metal coordination compounds represented by the formula (1) according to the present invention are shown in Tables 1-16 appearing hereinafter, which are however only representative examples and are not exhaustive. Partial Chemical Structural Formulas Nos. 1-16 for P and 20-34 for Q1 and Q2 used in the tables represent partial structures shown below, respectively. The following metal coordination compounds include positively charged compounds. Such positively charged compounds can be used as luminescence materials for the organic luminescence device of the present invention by neutralizing the compounds with counter anions, such as halogen ions, PF 6   −  and ClO 4   − .                         
                         
                         
                         
                         
                         
                           
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 1 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 1 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 20 
               
               
                 2 
                 Ir 
                 Ir 
                 2 
                 1 
                 21 
                 21 
               
               
                 3 
                 Ir 
                 Ir 
                 2 
                 1 
                 22 
                 22 
               
               
                 4 
                 Ir 
                 Ir 
                 2 
                 1 
                 23 
                 23 
               
               
                 5 
                 Ir 
                 Ir 
                 2 
                 1 
                 24 
                 24 
               
               
                 6 
                 Ir 
                 Ir 
                 2 
                 1 
                 25 
                 25 
               
               
                 7 
                 Ir 
                 Ir 
                 2 
                 1 
                 26 
                 26 
               
               
                 8 
                 Ir 
                 Ir 
                 2 
                 1 
                 27 
                 27 
               
               
                 9 
                 Ir 
                 Ir 
                 2 
                 1 
                 28 
                 28 
               
               
                 10 
                 Ir 
                 Ir 
                 2 
                 1 
                 29 
                 29 
               
               
                 11 
                 Ir 
                 Ir 
                 2 
                 1 
                 30 
                 30 
               
               
                 12 
                 Ir 
                 Ir 
                 2 
                 1 
                 31 
                 31 
               
               
                 13 
                 Ir 
                 Ir 
                 2 
                 1 
                 32 
                 32 
               
               
                 14 
                 Ir 
                 Ir 
                 2 
                 1 
                 33 
                 33 
               
               
                 15 
                 Ir 
                 Ir 
                 2 
                 1 
                 34 
                 34 
               
               
                 16 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 20 
               
               
                 17 
                 Ir 
                 Ir 
                 2 
                 2 
                 21 
                 21 
               
               
                 18 
                 Ir 
                 Ir 
                 2 
                 2 
                 22 
                 22 
               
               
                 19 
                 Ir 
                 Ir 
                 2 
                 2 
                 23 
                 23 
               
               
                 20 
                 Ir 
                 Ir 
                 2 
                 2 
                 24 
                 24 
               
               
                 21 
                 Ir 
                 Ir 
                 2 
                 2 
                 25 
                 25 
               
               
                 22 
                 Ir 
                 Ir 
                 2 
                 2 
                 26 
                 26 
               
               
                 23 
                 Ir 
                 Ir 
                 2 
                 2 
                 27 
                 27 
               
               
                 24 
                 Ir 
                 Ir 
                 2 
                 2 
                 28 
                 28 
               
               
                 25 
                 Ir 
                 Ir 
                 2 
                 2 
                 29 
                 29 
               
               
                 26 
                 Ir 
                 Ir 
                 2 
                 2 
                 30 
                 30 
               
               
                 27 
                 Ir 
                 Ir 
                 2 
                 2 
                 31 
                 31 
               
               
                 28 
                 Ir 
                 Ir 
                 2 
                 2 
                 32 
                 32 
               
               
                 29 
                 Ir 
                 Ir 
                 2 
                 2 
                 33 
                 33 
               
               
                 30 
                 Ir 
                 Ir 
                 2 
                 2 
                 34 
                 34 
               
               
                 31 
                 Ir 
                 Ir 
                 2 
                 3 
                 20 
                 20 
               
               
                 32 
                 Ir 
                 Ir 
                 2 
                 3 
                 21 
                 21 
               
               
                 33 
                 Ir 
                 Ir 
                 2 
                 3 
                 22 
                 22 
               
               
                 34 
                 Ir 
                 Ir 
                 2 
                 3 
                 23 
                 23 
               
               
                 35 
                 Ir 
                 Ir 
                 2 
                 3 
                 24 
                 24 
               
               
                 36 
                 Ir 
                 Ir 
                 2 
                 3 
                 25 
                 25 
               
               
                 37 
                 Ir 
                 Ir 
                 2 
                 3 
                 26 
                 26 
               
               
                 38 
                 Ir 
                 Ir 
                 2 
                 3 
                 27 
                 27 
               
               
                 39 
                 Ir 
                 Ir 
                 2 
                 3 
                 28 
                 28 
               
               
                 40 
                 Ir 
                 Ir 
                 2 
                 3 
                 29 
                 29 
               
               
                 41 
                 Ir 
                 Ir 
                 2 
                 3 
                 30 
                 30 
               
               
                 42 
                 Ir 
                 Ir 
                 2 
                 3 
                 31 
                 31 
               
               
                 43 
                 Ir 
                 Ir 
                 2 
                 3 
                 32 
                 32 
               
               
                 44 
                 Ir 
                 Ir 
                 2 
                 3 
                 33 
                 33 
               
               
                 45 
                 Ir 
                 Ir 
                 2 
                 3 
                 34 
                 34 
               
               
                 46 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 20 
               
               
                 47 
                 Ir 
                 Ir 
                 2 
                 4 
                 21 
                 21 
               
               
                 48 
                 Ir 
                 Ir 
                 2 
                 4 
                 22 
                 22 
               
               
                 49 
                 Ir 
                 Ir 
                 2 
                 4 
                 23 
                 23 
               
               
                 50 
                 Ir 
                 Ir 
                 2 
                 4 
                 24 
                 24 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 2 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 51 
                 Ir 
                 Ir 
                 2 
                 4 
                 25 
                 25 
               
               
                 52 
                 Ir 
                 Ir 
                 2 
                 4 
                 26 
                 26 
               
               
                 53 
                 Ir 
                 Ir 
                 2 
                 4 
                 27 
                 27 
               
               
                 54 
                 Ir 
                 Ir 
                 2 
                 4 
                 28 
                 28 
               
               
                 55 
                 Ir 
                 Ir 
                 2 
                 4 
                 29 
                 29 
               
               
                 56 
                 Ir 
                 Ir 
                 2 
                 4 
                 30 
                 30 
               
               
                 57 
                 Ir 
                 Ir 
                 2 
                 4 
                 31 
                 31 
               
               
                 58 
                 Ir 
                 Ir 
                 2 
                 4 
                 32 
                 32 
               
               
                 59 
                 Ir 
                 Ir 
                 2 
                 4 
                 33 
                 33 
               
               
                 60 
                 Ir 
                 Ir 
                 2 
                 4 
                 34 
                 34 
               
               
                 61 
                 Ir 
                 Ir 
                 2 
                 5 
                 20 
                 20 
               
               
                 62 
                 Ir 
                 Ir 
                 2 
                 5 
                 21 
                 21 
               
               
                 63 
                 Ir 
                 Ir 
                 2 
                 5 
                 22 
                 22 
               
               
                 64 
                 Ir 
                 Ir 
                 2 
                 5 
                 23 
                 23 
               
               
                 65 
                 Ir 
                 Ir 
                 2 
                 5 
                 24 
                 24 
               
               
                 66 
                 Ir 
                 Ir 
                 2 
                 5 
                 25 
                 25 
               
               
                 67 
                 Ir 
                 Ir 
                 2 
                 5 
                 26 
                 26 
               
               
                 68 
                 Ir 
                 Ir 
                 2 
                 5 
                 27 
                 27 
               
               
                 69 
                 Ir 
                 Ir 
                 2 
                 5 
                 28 
                 28 
               
               
                 70 
                 Ir 
                 Ir 
                 2 
                 5 
                 29 
                 29 
               
               
                 71 
                 Ir 
                 Ir 
                 2 
                 5 
                 30 
                 30 
               
               
                 72 
                 Ir 
                 Ir 
                 2 
                 5 
                 31 
                 31 
               
               
                 73 
                 Ir 
                 Ir 
                 2 
                 5 
                 32 
                 32 
               
               
                 74 
                 Ir 
                 Ir 
                 2 
                 5 
                 33 
                 33 
               
               
                 75 
                 Ir 
                 Ir 
                 2 
                 5 
                 34 
                 34 
               
               
                 76 
                 Ir 
                 Ir 
                 2 
                 6 
                 20 
                 20 
               
               
                 77 
                 Ir 
                 Ir 
                 2 
                 6 
                 21 
                 21 
               
               
                 78 
                 Ir 
                 Ir 
                 2 
                 6 
                 22 
                 22 
               
               
                 79 
                 Ir 
                 Ir 
                 2 
                 6 
                 23 
                 23 
               
               
                 80 
                 Ir 
                 Ir 
                 2 
                 6 
                 24 
                 24 
               
               
                 81 
                 Ir 
                 Ir 
                 2 
                 6 
                 25 
                 25 
               
               
                 82 
                 Ir 
                 Ir 
                 2 
                 6 
                 26 
                 26 
               
               
                 83 
                 Ir 
                 Ir 
                 2 
                 6 
                 27 
                 27 
               
               
                 84 
                 Ir 
                 Ir 
                 2 
                 6 
                 28 
                 28 
               
               
                 85 
                 Ir 
                 Ir 
                 2 
                 6 
                 29 
                 29 
               
               
                 86 
                 Ir 
                 Ir 
                 2 
                 6 
                 30 
                 30 
               
               
                 87 
                 Ir 
                 Ir 
                 2 
                 6 
                 31 
                 31 
               
               
                 88 
                 Ir 
                 Ir 
                 2 
                 6 
                 32 
                 32 
               
               
                 89 
                 Ir 
                 Ir 
                 2 
                 6 
                 33 
                 33 
               
               
                 90 
                 Ir 
                 Ir 
                 2 
                 6 
                 34 
                 34 
               
               
                 91 
                 Ir 
                 Ir 
                 2 
                 7 
                 20 
                 20 
               
               
                 92 
                 Ir 
                 Ir 
                 2 
                 7 
                 21 
                 21 
               
               
                 93 
                 Ir 
                 Ir 
                 2 
                 7 
                 22 
                 22 
               
               
                 94 
                 Ir 
                 Ir 
                 2 
                 7 
                 23 
                 23 
               
               
                 95 
                 Ir 
                 Ir 
                 2 
                 7 
                 24 
                 24 
               
               
                 96 
                 Ir 
                 Ir 
                 2 
                 7 
                 25 
                 25 
               
               
                 97 
                 Ir 
                 Ir 
                 2 
                 7 
                 26 
                 26 
               
               
                 98 
                 Ir 
                 Ir 
                 2 
                 7 
                 27 
                 27 
               
               
                 99 
                 Ir 
                 Ir 
                 2 
                 7 
                 28 
                 28 
               
               
                 100 
                 Ir 
                 Ir 
                 2 
                 7 
                 29 
                 29 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 3 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 101 
                 Ir 
                 Ir 
                 2 
                 7 
                 30 
                 30 
               
               
                 102 
                 Ir 
                 Ir 
                 2 
                 7 
                 31 
                 31 
               
               
                 103 
                 Ir 
                 Ir 
                 2 
                 7 
                 32 
                 32 
               
               
                 104 
                 Ir 
                 Ir 
                 2 
                 7 
                 33 
                 33 
               
               
                 105 
                 Ir 
                 Ir 
                 2 
                 7 
                 34 
                 34 
               
               
                 106 
                 Ir 
                 Ir 
                 2 
                 8 
                 20 
                 20 
               
               
                 107 
                 Ir 
                 Ir 
                 2 
                 8 
                 21 
                 21 
               
               
                 108 
                 Ir 
                 Ir 
                 2 
                 8 
                 22 
                 22 
               
               
                 109 
                 Ir 
                 Ir 
                 2 
                 8 
                 23 
                 23 
               
               
                 110 
                 Ir 
                 Ir 
                 2 
                 8 
                 24 
                 24 
               
               
                 111 
                 Ir 
                 Ir 
                 2 
                 8 
                 25 
                 25 
               
               
                 112 
                 Ir 
                 Ir 
                 2 
                 8 
                 26 
                 26 
               
               
                 113 
                 Ir 
                 Ir 
                 2 
                 8 
                 27 
                 27 
               
               
                 114 
                 Ir 
                 Ir 
                 2 
                 8 
                 28 
                 28 
               
               
                 115 
                 Ir 
                 Ir 
                 2 
                 8 
                 29 
                 29 
               
               
                 116 
                 Ir 
                 Ir 
                 2 
                 8 
                 30 
                 30 
               
               
                 117 
                 Ir 
                 Ir 
                 2 
                 8 
                 31 
                 31 
               
               
                 118 
                 Ir 
                 Ir 
                 2 
                 8 
                 32 
                 32 
               
               
                 119 
                 Ir 
                 Ir 
                 2 
                 8 
                 33 
                 33 
               
               
                 120 
                 Ir 
                 Ir 
                 2 
                 8 
                 34 
                 34 
               
               
                 121 
                 Ir 
                 Ir 
                 2 
                 9 
                 20 
                 20 
               
               
                 122 
                 Ir 
                 Ir 
                 2 
                 9 
                 21 
                 21 
               
               
                 123 
                 Ir 
                 Ir 
                 2 
                 9 
                 22 
                 22 
               
               
                 124 
                 Ir 
                 Ir 
                 2 
                 9 
                 23 
                 23 
               
               
                 125 
                 Ir 
                 Ir 
                 2 
                 9 
                 24 
                 24 
               
               
                 126 
                 Ir 
                 Ir 
                 2 
                 9 
                 25 
                 25 
               
               
                 127 
                 Ir 
                 Ir 
                 2 
                 9 
                 26 
                 26 
               
               
                 128 
                 Ir 
                 Ir 
                 2 
                 9 
                 27 
                 27 
               
               
                 129 
                 Ir 
                 Ir 
                 2 
                 9 
                 28 
                 28 
               
               
                 130 
                 Ir 
                 Ir 
                 2 
                 9 
                 29 
                 29 
               
               
                 131 
                 Ir 
                 Ir 
                 2 
                 9 
                 30 
                 30 
               
               
                 132 
                 Ir 
                 Ir 
                 2 
                 9 
                 31 
                 31 
               
               
                 133 
                 Ir 
                 Ir 
                 2 
                 9 
                 32 
                 32 
               
               
                 134 
                 Ir 
                 Ir 
                 2 
                 9 
                 33 
                 33 
               
               
                 135 
                 Ir 
                 Ir 
                 2 
                 9 
                 34 
                 34 
               
               
                 136 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 20 
               
               
                 137 
                 Ir 
                 Ir 
                 2 
                 10 
                 21 
                 21 
               
               
                 138 
                 Ir 
                 Ir 
                 2 
                 10 
                 22 
                 22 
               
               
                 139 
                 Ir 
                 Ir 
                 2 
                 10 
                 23 
                 23 
               
               
                 140 
                 Ir 
                 Ir 
                 2 
                 10 
                 24 
                 24 
               
               
                 141 
                 Ir 
                 Ir 
                 2 
                 10 
                 25 
                 25 
               
               
                 142 
                 Ir 
                 Ir 
                 2 
                 10 
                 26 
                 26 
               
               
                 143 
                 Ir 
                 Ir 
                 2 
                 10 
                 27 
                 27 
               
               
                 144 
                 Ir 
                 Ir 
                 2 
                 10 
                 28 
                 28 
               
               
                 145 
                 Ir 
                 Ir 
                 2 
                 10 
                 29 
                 29 
               
               
                 146 
                 Ir 
                 Ir 
                 2 
                 10 
                 30 
                 30 
               
               
                 147 
                 Ir 
                 Ir 
                 2 
                 10 
                 31 
                 31 
               
               
                 148 
                 Ir 
                 Ir 
                 2 
                 10 
                 32 
                 32 
               
               
                 149 
                 Ir 
                 Ir 
                 2 
                 10 
                 33 
                 33 
               
               
                 150 
                 Ir 
                 Ir 
                 2 
                 10 
                 34 
                 34 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 4 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 151 
                 Ir 
                 Ir 
                 2 
                 11 
                 20 
                 20 
               
               
                 152 
                 Ir 
                 Ir 
                 2 
                 11 
                 21 
                 21 
               
               
                 153 
                 Ir 
                 Ir 
                 2 
                 11 
                 22 
                 22 
               
               
                 154 
                 Ir 
                 Ir 
                 2 
                 11 
                 23 
                 23 
               
               
                 155 
                 Ir 
                 Ir 
                 2 
                 11 
                 24 
                 24 
               
               
                 156 
                 Ir 
                 Ir 
                 2 
                 11 
                 25 
                 25 
               
               
                 157 
                 Ir 
                 Ir 
                 2 
                 11 
                 26 
                 26 
               
               
                 158 
                 Ir 
                 Ir 
                 2 
                 11 
                 27 
                 27 
               
               
                 159 
                 Ir 
                 Ir 
                 2 
                 11 
                 28 
                 28 
               
               
                 160 
                 Ir 
                 Ir 
                 2 
                 11 
                 29 
                 29 
               
               
                 161 
                 Ir 
                 Ir 
                 2 
                 11 
                 30 
                 30 
               
               
                 162 
                 Ir 
                 Ir 
                 2 
                 11 
                 31 
                 31 
               
               
                 163 
                 Ir 
                 Ir 
                 2 
                 11 
                 32 
                 32 
               
               
                 164 
                 Ir 
                 Ir 
                 2 
                 11 
                 33 
                 33 
               
               
                 165 
                 Ir 
                 Ir 
                 2 
                 11 
                 34 
                 34 
               
               
                 166 
                 Ir 
                 Ir 
                 2 
                 12 
                 20 
                 20 
               
               
                 167 
                 Ir 
                 Ir 
                 2 
                 12 
                 21 
                 21 
               
               
                 168 
                 Ir 
                 Ir 
                 2 
                 12 
                 22 
                 22 
               
               
                 169 
                 Ir 
                 Ir 
                 2 
                 12 
                 23 
                 23 
               
               
                 170 
                 Ir 
                 Ir 
                 2 
                 12 
                 24 
                 24 
               
               
                 171 
                 Ir 
                 Ir 
                 2 
                 12 
                 25 
                 25 
               
               
                 172 
                 Ir 
                 Ir 
                 2 
                 12 
                 26 
                 26 
               
               
                 173 
                 Ir 
                 Ir 
                 2 
                 12 
                 27 
                 27 
               
               
                 174 
                 Ir 
                 Ir 
                 2 
                 12 
                 28 
                 28 
               
               
                 175 
                 Ir 
                 Ir 
                 2 
                 12 
                 29 
                 29 
               
               
                 176 
                 Ir 
                 Ir 
                 2 
                 12 
                 30 
                 30 
               
               
                 177 
                 Ir 
                 Ir 
                 2 
                 12 
                 31 
                 31 
               
               
                 178 
                 Ir 
                 Ir 
                 2 
                 12 
                 32 
                 32 
               
               
                 179 
                 Ir 
                 Ir 
                 2 
                 12 
                 33 
                 33 
               
               
                 180 
                 Ir 
                 Ir 
                 2 
                 12 
                 34 
                 34 
               
               
                 181 
                 Ir 
                 Ir 
                 2 
                 13 
                 20 
                 20 
               
               
                 182 
                 Ir 
                 Ir 
                 2 
                 13 
                 21 
                 21 
               
               
                 183 
                 Ir 
                 Ir 
                 2 
                 13 
                 22 
                 22 
               
               
                 184 
                 Ir 
                 Ir 
                 2 
                 13 
                 23 
                 23 
               
               
                 185 
                 Ir 
                 Ir 
                 2 
                 13 
                 24 
                 24 
               
               
                 186 
                 Ir 
                 Ir 
                 2 
                 13 
                 25 
                 25 
               
               
                 187 
                 Ir 
                 Ir 
                 2 
                 13 
                 26 
                 26 
               
               
                 188 
                 Ir 
                 Ir 
                 2 
                 13 
                 27 
                 27 
               
               
                 189 
                 Ir 
                 Ir 
                 2 
                 13 
                 28 
                 28 
               
               
                 190 
                 Ir 
                 Ir 
                 2 
                 13 
                 29 
                 29 
               
               
                 191 
                 Ir 
                 Ir 
                 2 
                 13 
                 30 
                 30 
               
               
                 192 
                 Ir 
                 Ir 
                 2 
                 13 
                 31 
                 31 
               
               
                 193 
                 Ir 
                 Ir 
                 2 
                 13 
                 32 
                 32 
               
               
                 194 
                 Ir 
                 Ir 
                 2 
                 13 
                 33 
                 33 
               
               
                 195 
                 Ir 
                 Ir 
                 2 
                 13 
                 34 
                 34 
               
               
                 196 
                 Ir 
                 Ir 
                 2 
                 14 
                 20 
                 20 
               
               
                 197 
                 Ir 
                 Ir 
                 2 
                 14 
                 21 
                 21 
               
               
                 198 
                 Ir 
                 Ir 
                 2 
                 14 
                 22 
                 22 
               
               
                 199 
                 Ir 
                 Ir 
                 2 
                 14 
                 23 
                 23 
               
               
                 200 
                 Ir 
                 Ir 
                 2 
                 14 
                 24 
                 24 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 5 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 201 
                 Ir 
                 Ir 
                 2 
                 14 
                 25 
                 25 
               
               
                 202 
                 Ir 
                 Ir 
                 2 
                 14 
                 26 
                 26 
               
               
                 203 
                 Ir 
                 Ir 
                 2 
                 14 
                 27 
                 27 
               
               
                 204 
                 Ir 
                 Ir 
                 2 
                 14 
                 28 
                 28 
               
               
                 205 
                 Ir 
                 Ir 
                 2 
                 14 
                 29 
                 29 
               
               
                 206 
                 Ir 
                 Ir 
                 2 
                 14 
                 30 
                 30 
               
               
                 207 
                 Ir 
                 Ir 
                 2 
                 14 
                 31 
                 31 
               
               
                 208 
                 Ir 
                 Ir 
                 2 
                 14 
                 32 
                 32 
               
               
                 209 
                 Ir 
                 Ir 
                 2 
                 14 
                 33 
                 33 
               
               
                 210 
                 Ir 
                 Ir 
                 2 
                 14 
                 34 
                 34 
               
               
                 211 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 20 
               
               
                 212 
                 Ir 
                 Ir 
                 2 
                 15 
                 21 
                 21 
               
               
                 213 
                 Ir 
                 Ir 
                 2 
                 15 
                 22 
                 22 
               
               
                 214 
                 Ir 
                 Ir 
                 2 
                 15 
                 23 
                 23 
               
               
                 215 
                 Ir 
                 Ir 
                 2 
                 15 
                 24 
                 24 
               
               
                 216 
                 Ir 
                 Ir 
                 2 
                 15 
                 25 
                 25 
               
               
                 217 
                 Ir 
                 Ir 
                 2 
                 15 
                 26 
                 26 
               
               
                 218 
                 Ir 
                 Ir 
                 2 
                 15 
                 27 
                 27 
               
               
                 219 
                 Ir 
                 Ir 
                 2 
                 15 
                 28 
                 28 
               
               
                 220 
                 Ir 
                 Ir 
                 2 
                 15 
                 29 
                 29 
               
               
                 221 
                 Ir 
                 Ir 
                 2 
                 15 
                 30 
                 30 
               
               
                 222 
                 Ir 
                 Ir 
                 2 
                 15 
                 31 
                 31 
               
               
                 223 
                 Ir 
                 Ir 
                 2 
                 15 
                 32 
                 32 
               
               
                 224 
                 Ir 
                 Ir 
                 2 
                 15 
                 33 
                 33 
               
               
                 225 
                 Ir 
                 Ir 
                 2 
                 15 
                 34 
                 34 
               
               
                 226 
                 Ir 
                 Ir 
                 2 
                 16 
                 20 
                 20 
               
               
                 227 
                 Ir 
                 Ir 
                 2 
                 16 
                 21 
                 21 
               
               
                 228 
                 Ir 
                 Ir 
                 2 
                 16 
                 22 
                 22 
               
               
                 229 
                 Ir 
                 Ir 
                 2 
                 16 
                 23 
                 23 
               
               
                 230 
                 Ir 
                 Ir 
                 2 
                 16 
                 24 
                 24 
               
               
                 231 
                 Ir 
                 Ir 
                 2 
                 16 
                 25 
                 25 
               
               
                 232 
                 Ir 
                 Ir 
                 2 
                 16 
                 26 
                 26 
               
               
                 233 
                 Ir 
                 Ir 
                 2 
                 16 
                 27 
                 27 
               
               
                 234 
                 Ir 
                 Ir 
                 2 
                 16 
                 28 
                 28 
               
               
                 235 
                 Ir 
                 Ir 
                 2 
                 16 
                 29 
                 29 
               
               
                 236 
                 Ir 
                 Ir 
                 2 
                 16 
                 30 
                 30 
               
               
                 237 
                 Ir 
                 Ir 
                 2 
                 16 
                 31 
                 31 
               
               
                 238 
                 Ir 
                 Ir 
                 2 
                 16 
                 32 
                 32 
               
               
                 239 
                 Ir 
                 Ir 
                 2 
                 16 
                 33 
                 33 
               
               
                 240 
                 Ir 
                 Ir 
                 2 
                 16 
                 34 
                 34 
               
               
                 241 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 23 
               
               
                 242 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 27 
               
               
                 243 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 28 
               
               
                 244 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 33 
               
               
                 245 
                 Ir 
                 Ir 
                 2 
                 1 
                 20 
                 34 
               
               
                 246 
                 Ir 
                 Ir 
                 2 
                 1 
                 27 
                 33 
               
               
                 247 
                 Ir 
                 Ir 
                 2 
                 1 
                 27 
                 34 
               
               
                 248 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 23 
               
               
                 249 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 27 
               
               
                 250 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 28 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 6 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 251 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 33 
               
               
                 252 
                 Ir 
                 Ir 
                 2 
                 2 
                 20 
                 34 
               
               
                 253 
                 Ir 
                 Ir 
                 2 
                 2 
                 27 
                 33 
               
               
                 254 
                 Ir 
                 Ir 
                 2 
                 2 
                 27 
                 34 
               
               
                 255 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 23 
               
               
                 256 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 27 
               
               
                 257 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 28 
               
               
                 258 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 33 
               
               
                 259 
                 Ir 
                 Ir 
                 2 
                 4 
                 20 
                 34 
               
               
                 260 
                 Ir 
                 Ir 
                 2 
                 4 
                 27 
                 33 
               
               
                 261 
                 Ir 
                 Ir 
                 2 
                 4 
                 27 
                 34 
               
               
                 262 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 23 
               
               
                 263 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 27 
               
               
                 264 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 28 
               
               
                 265 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 33 
               
               
                 266 
                 Ir 
                 Ir 
                 2 
                 10 
                 20 
                 34 
               
               
                 267 
                 Ir 
                 Ir 
                 2 
                 10 
                 27 
                 33 
               
               
                 268 
                 Ir 
                 Ir 
                 2 
                 10 
                 27 
                 34 
               
               
                 269 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 23 
               
               
                 270 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 27 
               
               
                 271 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 28 
               
               
                 272 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 33 
               
               
                 273 
                 Ir 
                 Ir 
                 2 
                 15 
                 20 
                 34 
               
               
                 274 
                 Ir 
                 Ir 
                 2 
                 15 
                 27 
                 33 
               
               
                 275 
                 Ir 
                 Ir 
                 2 
                 15 
                 27 
                 34 
               
               
                 276 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 20 
               
               
                 277 
                 Rh 
                 Rh 
                 2 
                 1 
                 21 
                 21 
               
               
                 278 
                 Rh 
                 Rh 
                 2 
                 1 
                 22 
                 22 
               
               
                 279 
                 Rh 
                 Rh 
                 2 
                 1 
                 23 
                 23 
               
               
                 280 
                 Rh 
                 Rh 
                 2 
                 1 
                 24 
                 24 
               
               
                 281 
                 Rh 
                 Rh 
                 2 
                 1 
                 25 
                 25 
               
               
                 282 
                 Rh 
                 Rh 
                 2 
                 1 
                 26 
                 26 
               
               
                 283 
                 Rh 
                 Rh 
                 2 
                 1 
                 27 
                 27 
               
               
                 284 
                 Rh 
                 Rh 
                 2 
                 1 
                 28 
                 28 
               
               
                 285 
                 Rh 
                 Rh 
                 2 
                 1 
                 29 
                 29 
               
               
                 286 
                 Rh 
                 Rh 
                 2 
                 1 
                 30 
                 30 
               
               
                 287 
                 Rh 
                 Rh 
                 2 
                 1 
                 31 
                 31 
               
               
                 288 
                 Rh 
                 Rh 
                 2 
                 1 
                 32 
                 32 
               
               
                 289 
                 Rh 
                 Rh 
                 2 
                 1 
                 33 
                 33 
               
               
                 290 
                 Rh 
                 Rh 
                 2 
                 1 
                 34 
                 34 
               
               
                 291 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 20 
               
               
                 292 
                 Rh 
                 Rh 
                 2 
                 2 
                 21 
                 21 
               
               
                 293 
                 Rh 
                 Rh 
                 2 
                 2 
                 22 
                 22 
               
               
                 294 
                 Rh 
                 Rh 
                 2 
                 2 
                 23 
                 23 
               
               
                 295 
                 Rh 
                 Rh 
                 2 
                 2 
                 24 
                 24 
               
               
                 296 
                 Rh 
                 Rh 
                 2 
                 2 
                 25 
                 25 
               
               
                 297 
                 Rh 
                 Rh 
                 2 
                 2 
                 26 
                 26 
               
               
                 298 
                 Rh 
                 Rh 
                 2 
                 2 
                 27 
                 27 
               
               
                 299 
                 Rh 
                 Rh 
                 2 
                 2 
                 28 
                 28 
               
               
                 300 
                 Rh 
                 Rh 
                 2 
                 2 
                 29 
                 29 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 7 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 301 
                 Rh 
                 Rh 
                 2 
                 2 
                 30 
                 30 
               
               
                 302 
                 Rh 
                 Rh 
                 2 
                 2 
                 31 
                 31 
               
               
                 303 
                 Rh 
                 Rh 
                 2 
                 2 
                 32 
                 32 
               
               
                 304 
                 Rh 
                 Rh 
                 2 
                 2 
                 33 
                 33 
               
               
                 305 
                 Rh 
                 Rh 
                 2 
                 2 
                 34 
                 34 
               
               
                 306 
                 Rh 
                 Rh 
                 2 
                 3 
                 20 
                 20 
               
               
                 307 
                 Rh 
                 Rh 
                 2 
                 3 
                 21 
                 21 
               
               
                 308 
                 Rh 
                 Rh 
                 2 
                 3 
                 22 
                 22 
               
               
                 309 
                 Rh 
                 Rh 
                 2 
                 3 
                 23 
                 23 
               
               
                 310 
                 Rh 
                 Rh 
                 2 
                 3 
                 24 
                 24 
               
               
                 311 
                 Rh 
                 Rh 
                 2 
                 3 
                 25 
                 25 
               
               
                 312 
                 Rh 
                 Rh 
                 2 
                 3 
                 26 
                 26 
               
               
                 313 
                 Rh 
                 Rh 
                 2 
                 3 
                 27 
                 27 
               
               
                 314 
                 Rh 
                 Rh 
                 2 
                 3 
                 28 
                 28 
               
               
                 315 
                 Rh 
                 Rh 
                 2 
                 3 
                 29 
                 29 
               
               
                 316 
                 Rh 
                 Rh 
                 2 
                 3 
                 30 
                 30 
               
               
                 317 
                 Rh 
                 Rh 
                 2 
                 3 
                 31 
                 31 
               
               
                 318 
                 Rh 
                 Rh 
                 2 
                 3 
                 32 
                 32 
               
               
                 319 
                 Rh 
                 Rh 
                 2 
                 3 
                 33 
                 33 
               
               
                 320 
                 Rh 
                 Rh 
                 2 
                 3 
                 34 
                 34 
               
               
                 321 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 20 
               
               
                 322 
                 Rh 
                 Rh 
                 2 
                 4 
                 21 
                 21 
               
               
                 323 
                 Rh 
                 Rh 
                 2 
                 4 
                 22 
                 22 
               
               
                 324 
                 Rh 
                 Rh 
                 2 
                 4 
                 23 
                 23 
               
               
                 325 
                 Rh 
                 Rh 
                 2 
                 4 
                 24 
                 24 
               
               
                 326 
                 Rh 
                 Rh 
                 2 
                 4 
                 25 
                 25 
               
               
                 327 
                 Rh 
                 Rh 
                 2 
                 4 
                 26 
                 26 
               
               
                 328 
                 Rh 
                 Rh 
                 2 
                 4 
                 27 
                 27 
               
               
                 329 
                 Rh 
                 Rh 
                 2 
                 4 
                 28 
                 28 
               
               
                 330 
                 Rh 
                 Rh 
                 2 
                 4 
                 29 
                 29 
               
               
                 331 
                 Rh 
                 Rh 
                 2 
                 4 
                 30 
                 30 
               
               
                 332 
                 Rh 
                 Rh 
                 2 
                 4 
                 31 
                 31 
               
               
                 333 
                 Rh 
                 Rh 
                 2 
                 4 
                 32 
                 32 
               
               
                 334 
                 Rh 
                 Rh 
                 2 
                 4 
                 33 
                 33 
               
               
                 335 
                 Rh 
                 Rh 
                 2 
                 4 
                 34 
                 34 
               
               
                 336 
                 Rh 
                 Rh 
                 2 
                 5 
                 20 
                 20 
               
               
                 337 
                 Rh 
                 Rh 
                 2 
                 5 
                 21 
                 21 
               
               
                 338 
                 Rh 
                 Rh 
                 2 
                 5 
                 22 
                 22 
               
               
                 339 
                 Rh 
                 Rh 
                 2 
                 5 
                 23 
                 23 
               
               
                 340 
                 Rh 
                 Rh 
                 2 
                 5 
                 24 
                 24 
               
               
                 341 
                 Rh 
                 Rh 
                 2 
                 5 
                 25 
                 25 
               
               
                 342 
                 Rh 
                 Rh 
                 2 
                 5 
                 26 
                 26 
               
               
                 343 
                 Rh 
                 Rh 
                 2 
                 5 
                 27 
                 27 
               
               
                 344 
                 Rh 
                 Rh 
                 2 
                 5 
                 28 
                 28 
               
               
                 345 
                 Rh 
                 Rh 
                 2 
                 5 
                 29 
                 29 
               
               
                 346 
                 Rh 
                 Rh 
                 2 
                 5 
                 30 
                 30 
               
               
                 347 
                 Rh 
                 Rh 
                 2 
                 5 
                 31 
                 31 
               
               
                 348 
                 Rh 
                 Rh 
                 2 
                 5 
                 32 
                 32 
               
               
                 349 
                 Rh 
                 Rh 
                 2 
                 5 
                 33 
                 33 
               
               
                 350 
                 Rh 
                 Rh 
                 2 
                 5 
                 34 
                 34 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 8 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 351 
                 Rh 
                 Rh 
                 2 
                 6 
                 20 
                 20 
               
               
                 352 
                 Rh 
                 Rh 
                 2 
                 6 
                 21 
                 21 
               
               
                 353 
                 Rh 
                 Rh 
                 2 
                 6 
                 22 
                 22 
               
               
                 354 
                 Rh 
                 Rh 
                 2 
                 6 
                 23 
                 23 
               
               
                 355 
                 Rh 
                 Rh 
                 2 
                 6 
                 24 
                 24 
               
               
                 356 
                 Rh 
                 Rh 
                 2 
                 6 
                 25 
                 25 
               
               
                 357 
                 Rh 
                 Rh 
                 2 
                 6 
                 26 
                 26 
               
               
                 358 
                 Rh 
                 Rh 
                 2 
                 6 
                 27 
                 27 
               
               
                 359 
                 Rh 
                 Rh 
                 2 
                 6 
                 28 
                 28 
               
               
                 360 
                 Rh 
                 Rh 
                 2 
                 6 
                 29 
                 29 
               
               
                 361 
                 Rh 
                 Rh 
                 2 
                 6 
                 30 
                 30 
               
               
                 362 
                 Rh 
                 Rh 
                 2 
                 6 
                 31 
                 31 
               
               
                 363 
                 Rh 
                 Rh 
                 2 
                 6 
                 32 
                 32 
               
               
                 364 
                 Rh 
                 Rh 
                 2 
                 6 
                 33 
                 33 
               
               
                 365 
                 Rh 
                 Rh 
                 2 
                 6 
                 34 
                 34 
               
               
                 366 
                 Rh 
                 Rh 
                 2 
                 9 
                 20 
                 20 
               
               
                 367 
                 Rh 
                 Rh 
                 2 
                 9 
                 21 
                 21 
               
               
                 368 
                 Rh 
                 Rh 
                 2 
                 9 
                 22 
                 22 
               
               
                 369 
                 Rh 
                 Rh 
                 2 
                 9 
                 23 
                 23 
               
               
                 370 
                 Rh 
                 Rh 
                 2 
                 9 
                 24 
                 24 
               
               
                 371 
                 Rh 
                 Rh 
                 2 
                 9 
                 25 
                 25 
               
               
                 372 
                 Rh 
                 Rh 
                 2 
                 9 
                 26 
                 26 
               
               
                 373 
                 Rh 
                 Rh 
                 2 
                 9 
                 27 
                 27 
               
               
                 374 
                 Rh 
                 Rh 
                 2 
                 9 
                 28 
                 28 
               
               
                 375 
                 Rh 
                 Rh 
                 2 
                 9 
                 29 
                 29 
               
               
                 376 
                 Rh 
                 Rh 
                 2 
                 9 
                 30 
                 30 
               
               
                 377 
                 Rh 
                 Rh 
                 2 
                 9 
                 31 
                 31 
               
               
                 378 
                 Rh 
                 Rh 
                 2 
                 9 
                 32 
                 32 
               
               
                 379 
                 Rh 
                 Rh 
                 2 
                 9 
                 33 
                 33 
               
               
                 380 
                 Rh 
                 Rh 
                 2 
                 9 
                 34 
                 34 
               
               
                 381 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 20 
               
               
                 382 
                 Rh 
                 Rh 
                 2 
                 10 
                 21 
                 21 
               
               
                 383 
                 Rh 
                 Rh 
                 2 
                 10 
                 22 
                 22 
               
               
                 384 
                 Rh 
                 Rh 
                 2 
                 10 
                 23 
                 23 
               
               
                 385 
                 Rh 
                 Rh 
                 2 
                 10 
                 24 
                 24 
               
               
                 386 
                 Rh 
                 Rh 
                 2 
                 10 
                 25 
                 25 
               
               
                 387 
                 Rh 
                 Rh 
                 2 
                 10 
                 26 
                 26 
               
               
                 388 
                 Rh 
                 Rh 
                 2 
                 10 
                 27 
                 27 
               
               
                 389 
                 Rh 
                 Rh 
                 2 
                 10 
                 28 
                 28 
               
               
                 390 
                 Rh 
                 Rh 
                 2 
                 10 
                 29 
                 29 
               
               
                 391 
                 Rh 
                 Rh 
                 2 
                 10 
                 30 
                 30 
               
               
                 392 
                 Rh 
                 Rh 
                 2 
                 10 
                 31 
                 31 
               
               
                 393 
                 Rh 
                 Rh 
                 2 
                 10 
                 32 
                 32 
               
               
                 394 
                 Rh 
                 Rh 
                 2 
                 10 
                 33 
                 33 
               
               
                 395 
                 Rh 
                 Rh 
                 2 
                 10 
                 34 
                 34 
               
               
                 396 
                 Rh 
                 Rh 
                 2 
                 11 
                 20 
                 20 
               
               
                 397 
                 Rh 
                 Rh 
                 2 
                 11 
                 21 
                 21 
               
               
                 398 
                 Rh 
                 Rh 
                 2 
                 11 
                 22 
                 22 
               
               
                 399 
                 Rh 
                 Rh 
                 2 
                 11 
                 23 
                 23 
               
               
                 400 
                 Rh 
                 Rh 
                 2 
                 11 
                 24 
                 24 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 9 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 401 
                 Rh 
                 Rh 
                 2 
                 11 
                 25 
                 25 
               
               
                 402 
                 Rh 
                 Rh 
                 2 
                 11 
                 26 
                 26 
               
               
                 403 
                 Rh 
                 Rh 
                 2 
                 11 
                 27 
                 27 
               
               
                 404 
                 Rh 
                 Rh 
                 2 
                 11 
                 28 
                 28 
               
               
                 405 
                 Rh 
                 Rh 
                 2 
                 11 
                 29 
                 29 
               
               
                 406 
                 Rh 
                 Rh 
                 2 
                 11 
                 30 
                 30 
               
               
                 407 
                 Rh 
                 Rh 
                 2 
                 11 
                 31 
                 31 
               
               
                 408 
                 Rh 
                 Rh 
                 2 
                 11 
                 32 
                 32 
               
               
                 409 
                 Rh 
                 Rh 
                 2 
                 11 
                 33 
                 33 
               
               
                 410 
                 Rh 
                 Rh 
                 2 
                 11 
                 34 
                 34 
               
               
                 411 
                 Rh 
                 Rh 
                 2 
                 13 
                 20 
                 20 
               
               
                 412 
                 Rh 
                 Rh 
                 2 
                 13 
                 21 
                 21 
               
               
                 413 
                 Rh 
                 Rh 
                 2 
                 13 
                 22 
                 22 
               
               
                 414 
                 Rh 
                 Rh 
                 2 
                 13 
                 23 
                 23 
               
               
                 415 
                 Rh 
                 Rh 
                 2 
                 13 
                 24 
                 24 
               
               
                 416 
                 Rh 
                 Rh 
                 2 
                 13 
                 25 
                 25 
               
               
                 417 
                 Rh 
                 Rh 
                 2 
                 13 
                 26 
                 26 
               
               
                 418 
                 Rh 
                 Rh 
                 2 
                 13 
                 27 
                 27 
               
               
                 419 
                 Rh 
                 Rh 
                 2 
                 13 
                 28 
                 28 
               
               
                 420 
                 Rh 
                 Rh 
                 2 
                 13 
                 29 
                 29 
               
               
                 421 
                 Rh 
                 Rh 
                 2 
                 13 
                 30 
                 30 
               
               
                 422 
                 Rh 
                 Rh 
                 2 
                 13 
                 31 
                 31 
               
               
                 423 
                 Rh 
                 Rh 
                 2 
                 13 
                 32 
                 32 
               
               
                 424 
                 Rh 
                 Rh 
                 2 
                 13 
                 33 
                 33 
               
               
                 425 
                 Rh 
                 Rh 
                 2 
                 13 
                 34 
                 34 
               
               
                 426 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 20 
               
               
                 427 
                 Rh 
                 Rh 
                 2 
                 15 
                 21 
                 21 
               
               
                 428 
                 Rh 
                 Rh 
                 2 
                 15 
                 22 
                 22 
               
               
                 429 
                 Rh 
                 Rh 
                 2 
                 15 
                 23 
                 23 
               
               
                 430 
                 Rh 
                 Rh 
                 2 
                 15 
                 24 
                 24 
               
               
                 431 
                 Rh 
                 Rh 
                 2 
                 15 
                 25 
                 25 
               
               
                 432 
                 Rh 
                 Rh 
                 2 
                 15 
                 26 
                 26 
               
               
                 433 
                 Rh 
                 Rh 
                 2 
                 15 
                 27 
                 27 
               
               
                 434 
                 Rh 
                 Rh 
                 2 
                 15 
                 28 
                 28 
               
               
                 435 
                 Rh 
                 Rh 
                 2 
                 15 
                 29 
                 29 
               
               
                 436 
                 Rh 
                 Rh 
                 2 
                 15 
                 30 
                 30 
               
               
                 437 
                 Rh 
                 Rh 
                 2 
                 15 
                 31 
                 31 
               
               
                 438 
                 Rh 
                 Rh 
                 2 
                 15 
                 32 
                 32 
               
               
                 439 
                 Rh 
                 Rh 
                 2 
                 15 
                 33 
                 33 
               
               
                 440 
                 Rh 
                 Rh 
                 2 
                 15 
                 34 
                 34 
               
               
                 441 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 23 
               
               
                 442 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 27 
               
               
                 443 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 28 
               
               
                 444 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 33 
               
               
                 445 
                 Rh 
                 Rh 
                 2 
                 1 
                 20 
                 34 
               
               
                 446 
                 Rh 
                 Rh 
                 2 
                 1 
                 27 
                 33 
               
               
                 447 
                 Rh 
                 Rh 
                 2 
                 1 
                 27 
                 34 
               
               
                 448 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 23 
               
               
                 449 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 27 
               
               
                 450 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 28 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                                                      TABLE 10 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 451 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 33 
               
               
                 452 
                 Rh 
                 Rh 
                 2 
                 2 
                 20 
                 34 
               
               
                 453 
                 Rh 
                 Rh 
                 2 
                 2 
                 27 
                 33 
               
               
                 454 
                 Rh 
                 Rh 
                 2 
                 2 
                 27 
                 34 
               
               
                 455 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 23 
               
               
                 456 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 27 
               
               
                 457 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 28 
               
               
                 458 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 33 
               
               
                 459 
                 Rh 
                 Rh 
                 2 
                 4 
                 20 
                 34 
               
               
                 460 
                 Rh 
                 Rh 
                 2 
                 4 
                 27 
                 33 
               
               
                 461 
                 Rh 
                 Rh 
                 2 
                 4 
                 27 
                 34 
               
               
                 462 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 23 
               
               
                 463 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 27 
               
               
                 464 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 28 
               
               
                 465 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 33 
               
               
                 466 
                 Rh 
                 Rh 
                 2 
                 10 
                 20 
                 34 
               
               
                 467 
                 Rh 
                 Rh 
                 2 
                 10 
                 27 
                 33 
               
               
                 468 
                 Rh 
                 Rh 
                 2 
                 10 
                 27 
                 34 
               
               
                 469 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 23 
               
               
                 470 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 27 
               
               
                 471 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 28 
               
               
                 472 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 33 
               
               
                 473 
                 Rh 
                 Rh 
                 2 
                 15 
                 20 
                 34 
               
               
                 474 
                 Rh 
                 Rh 
                 2 
                 15 
                 27 
                 33 
               
               
                 475 
                 Rh 
                 Rh 
                 2 
                 15 
                 27 
                 34 
               
               
                 476 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 20 
               
               
                 477 
                 Pt 
                 Pt 
                 1 
                 1 
                 23 
                 23 
               
               
                 478 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 26 
               
               
                 479 
                 Pt 
                 Pt 
                 1 
                 1 
                 27 
                 27 
               
               
                 480 
                 Pt 
                 Pt 
                 1 
                 1 
                 28 
                 28 
               
               
                 481 
                 Pt 
                 Pt 
                 1 
                 1 
                 33 
                 33 
               
               
                 482 
                 Pt 
                 Pt 
                 1 
                 1 
                 34 
                 34 
               
               
                 483 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 20 
               
               
                 484 
                 Pt 
                 Pt 
                 1 
                 2 
                 23 
                 23 
               
               
                 485 
                 Pt 
                 Pt 
                 1 
                 2 
                 26 
                 26 
               
               
                 486 
                 Pt 
                 Pt 
                 1 
                 2 
                 27 
                 27 
               
               
                 487 
                 Pt 
                 Pt 
                 1 
                 2 
                 28 
                 28 
               
               
                 488 
                 Pt 
                 Pt 
                 1 
                 2 
                 33 
                 33 
               
               
                 489 
                 Pt 
                 Pt 
                 1 
                 2 
                 34 
                 34 
               
               
                 490 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 20 
               
               
                 491 
                 Pt 
                 Pt 
                 1 
                 4 
                 23 
                 23 
               
               
                 492 
                 Pt 
                 Pt 
                 1 
                 4 
                 26 
                 26 
               
               
                 493 
                 Pt 
                 Pt 
                 1 
                 4 
                 27 
                 27 
               
               
                 494 
                 Pt 
                 Pt 
                 1 
                 4 
                 28 
                 28 
               
               
                 495 
                 Pt 
                 Pt 
                 1 
                 4 
                 33 
                 33 
               
               
                 496 
                 Pt 
                 Pt 
                 1 
                 4 
                 34 
                 34 
               
               
                 497 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 20 
               
               
                 498 
                 Pt 
                 Pt 
                 1 
                 7 
                 23 
                 23 
               
               
                 499 
                 Pt 
                 Pt 
                 1 
                 7 
                 26 
                 26 
               
               
                 500 
                 Pt 
                 Pt 
                 1 
                 7 
                 27 
                 27 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 11 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 501 
                 Pt 
                 Pt 
                 1 
                 7 
                 28 
                 28 
               
               
                 502 
                 Pt 
                 Pt 
                 1 
                 7 
                 33 
                 33 
               
               
                 503 
                 Pt 
                 Pt 
                 1 
                 7 
                 34 
                 34 
               
               
                 504 
                 Pt 
                 Pt 
                 1 
                 10 
                 20 
                 20 
               
               
                 505 
                 Pt 
                 Pt 
                 1 
                 10 
                 23 
                 23 
               
               
                 506 
                 Pt 
                 Pt 
                 1 
                 10 
                 26 
                 26 
               
               
                 507 
                 Pt 
                 Pt 
                 1 
                 10 
                 27 
                 27 
               
               
                 508 
                 Pt 
                 Pt 
                 1 
                 10 
                 28 
                 28 
               
               
                 509 
                 Pt 
                 Pt 
                 1 
                 10 
                 33 
                 33 
               
               
                 510 
                 Pt 
                 Pt 
                 1 
                 10 
                 34 
                 34 
               
               
                 511 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 20 
               
               
                 512 
                 Pt 
                 Pt 
                 1 
                 15 
                 23 
                 23 
               
               
                 513 
                 Pt 
                 Pt 
                 1 
                 15 
                 26 
                 26 
               
               
                 514 
                 Pt 
                 Pt 
                 1 
                 15 
                 27 
                 27 
               
               
                 515 
                 Pt 
                 Pt 
                 1 
                 15 
                 28 
                 28 
               
               
                 516 
                 Pt 
                 Pt 
                 1 
                 15 
                 33 
                 33 
               
               
                 517 
                 Pt 
                 Pt 
                 1 
                 15 
                 34 
                 34 
               
               
                 518 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 23 
               
               
                 519 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 26 
               
               
                 520 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 27 
               
               
                 521 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 28 
               
               
                 522 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 33 
               
               
                 523 
                 Pt 
                 Pt 
                 1 
                 1 
                 20 
                 34 
               
               
                 524 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 23 
               
               
                 525 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 27 
               
               
                 526 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 28 
               
               
                 527 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 33 
               
               
                 528 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 34 
               
               
                 529 
                 Pt 
                 Pt 
                 1 
                 1 
                 26 
                 30 
               
               
                 530 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 23 
               
               
                 531 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 26 
               
               
                 532 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 27 
               
               
                 533 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 28 
               
               
                 534 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 33 
               
               
                 535 
                 Pt 
                 Pt 
                 1 
                 2 
                 20 
                 34 
               
               
                 536 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 23 
               
               
                 537 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 26 
               
               
                 538 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 27 
               
               
                 539 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 28 
               
               
                 540 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 33 
               
               
                 541 
                 Pt 
                 Pt 
                 1 
                 4 
                 20 
                 34 
               
               
                 542 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 23 
               
               
                 543 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 26 
               
               
                 544 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 27 
               
               
                 545 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 28 
               
               
                 546 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 33 
               
               
                 547 
                 Pt 
                 Pt 
                 1 
                 7 
                 20 
                 34 
               
               
                 548 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 23 
               
               
                 549 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 26 
               
               
                 550 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 27 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 12 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 551 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 28 
               
               
                 552 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 33 
               
               
                 553 
                 Pt 
                 Pt 
                 1 
                 15 
                 20 
                 34 
               
               
                 554 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 20 
               
               
                 555 
                 Pd 
                 Pd 
                 1 
                 1 
                 23 
                 23 
               
               
                 556 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 26 
               
               
                 557 
                 Pd 
                 Pd 
                 1 
                 1 
                 27 
                 27 
               
               
                 558 
                 Pd 
                 Pd 
                 1 
                 1 
                 28 
                 28 
               
               
                 559 
                 Pd 
                 Pd 
                 1 
                 1 
                 33 
                 33 
               
               
                 560 
                 Pd 
                 Pd 
                 1 
                 1 
                 34 
                 34 
               
               
                 561 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 20 
               
               
                 562 
                 Pd 
                 Pd 
                 1 
                 2 
                 23 
                 23 
               
               
                 563 
                 Pd 
                 Pd 
                 1 
                 2 
                 26 
                 26 
               
               
                 564 
                 Pd 
                 Pd 
                 1 
                 2 
                 27 
                 27 
               
               
                 565 
                 Pd 
                 Pd 
                 1 
                 2 
                 28 
                 28 
               
               
                 566 
                 Pd 
                 Pd 
                 1 
                 2 
                 33 
                 33 
               
               
                 567 
                 Pd 
                 Pd 
                 1 
                 2 
                 34 
                 34 
               
               
                 568 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 20 
               
               
                 569 
                 Pd 
                 Pd 
                 1 
                 4 
                 23 
                 23 
               
               
                 570 
                 Pd 
                 Pd 
                 1 
                 4 
                 26 
                 26 
               
               
                 571 
                 Pd 
                 Pd 
                 1 
                 4 
                 27 
                 27 
               
               
                 572 
                 Pd 
                 Pd 
                 1 
                 4 
                 28 
                 28 
               
               
                 573 
                 Pd 
                 Pd 
                 1 
                 4 
                 33 
                 33 
               
               
                 574 
                 Pd 
                 Pd 
                 1 
                 4 
                 34 
                 34 
               
               
                 575 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 20 
               
               
                 576 
                 Pd 
                 Pd 
                 1 
                 7 
                 23 
                 23 
               
               
                 577 
                 Pd 
                 Pd 
                 1 
                 7 
                 26 
                 26 
               
               
                 578 
                 Pd 
                 Pd 
                 1 
                 7 
                 27 
                 27 
               
               
                 579 
                 Pd 
                 Pd 
                 1 
                 7 
                 28 
                 28 
               
               
                 580 
                 Pd 
                 Pd 
                 1 
                 7 
                 33 
                 33 
               
               
                 581 
                 Pd 
                 Pd 
                 1 
                 7 
                 34 
                 34 
               
               
                 582 
                 Pd 
                 Pd 
                 1 
                 10 
                 20 
                 20 
               
               
                 583 
                 Pd 
                 Pd 
                 1 
                 10 
                 23 
                 23 
               
               
                 584 
                 Pd 
                 Pd 
                 1 
                 10 
                 26 
                 26 
               
               
                 585 
                 Pd 
                 Pd 
                 1 
                 10 
                 27 
                 27 
               
               
                 586 
                 Pd 
                 Pd 
                 1 
                 10 
                 28 
                 28 
               
               
                 587 
                 Pd 
                 Pd 
                 1 
                 10 
                 33 
                 33 
               
               
                 588 
                 Pd 
                 Pd 
                 1 
                 10 
                 34 
                 34 
               
               
                 589 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 20 
               
               
                 590 
                 Pd 
                 Pd 
                 1 
                 15 
                 23 
                 23 
               
               
                 591 
                 Pd 
                 Pd 
                 1 
                 15 
                 26 
                 26 
               
               
                 592 
                 Pd 
                 Pd 
                 1 
                 15 
                 27 
                 27 
               
               
                 593 
                 Pd 
                 Pd 
                 1 
                 15 
                 28 
                 28 
               
               
                 594 
                 Pd 
                 Pd 
                 1 
                 15 
                 33 
                 33 
               
               
                 595 
                 Pd 
                 Pd 
                 1 
                 15 
                 34 
                 34 
               
               
                 596 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 23 
               
               
                 597 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 26 
               
               
                 598 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 27 
               
               
                 599 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 28 
               
               
                 600 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 33 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 13 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 601 
                 Pd 
                 Pd 
                 1 
                 1 
                 20 
                 34 
               
               
                 602 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 23 
               
               
                 603 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 27 
               
               
                 604 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 28 
               
               
                 605 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 33 
               
               
                 606 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 34 
               
               
                 607 
                 Pd 
                 Pd 
                 1 
                 1 
                 26 
                 30 
               
               
                 608 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 23 
               
               
                 609 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 26 
               
               
                 610 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 27 
               
               
                 611 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 28 
               
               
                 612 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 33 
               
               
                 613 
                 Pd 
                 Pd 
                 1 
                 2 
                 20 
                 34 
               
               
                 614 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 23 
               
               
                 615 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 26 
               
               
                 616 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 27 
               
               
                 617 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 28 
               
               
                 618 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 33 
               
               
                 619 
                 Pd 
                 Pd 
                 1 
                 4 
                 20 
                 34 
               
               
                 620 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 23 
               
               
                 621 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 26 
               
               
                 622 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 27 
               
               
                 623 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 28 
               
               
                 624 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 33 
               
               
                 625 
                 Pd 
                 Pd 
                 1 
                 7 
                 20 
                 34 
               
               
                 626 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 23 
               
               
                 627 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 26 
               
               
                 628 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 27 
               
               
                 629 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 28 
               
               
                 630 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 33 
               
               
                 631 
                 Pd 
                 Pd 
                 1 
                 15 
                 20 
                 34 
               
               
                 632 
                 Ru 
                 Ru 
                 2 
                 3 
                 20 
                 20 
               
               
                 633 
                 Ru 
                 Ru 
                 2 
                 3 
                 27 
                 27 
               
               
                 634 
                 Ru 
                 Ru 
                 2 
                 3 
                 32 
                 32 
               
               
                 635 
                 Ru 
                 Ru 
                 2 
                 3 
                 34 
                 34 
               
               
                 636 
                 Ru 
                 Ru 
                 2 
                 10 
                 20 
                 20 
               
               
                 637 
                 Ru 
                 Ru 
                 2 
                 10 
                 27 
                 27 
               
               
                 638 
                 Ru 
                 Ru 
                 2 
                 10 
                 32 
                 32 
               
               
                 639 
                 Ru 
                 Ru 
                 2 
                 10 
                 34 
                 34 
               
               
                 640 
                 Ru 
                 Ru 
                 2 
                 16 
                 20 
                 20 
               
               
                 641 
                 Ru 
                 Ru 
                 2 
                 16 
                 27 
                 27 
               
               
                 642 
                 Ru 
                 Ru 
                 2 
                 16 
                 32 
                 32 
               
               
                 643 
                 Ru 
                 Ru 
                 2 
                 16 
                 34 
                 34 
               
               
                 644 
                 Os 
                 Os 
                 2 
                 3 
                 20 
                 20 
               
               
                 645 
                 Os 
                 Os 
                 2 
                 3 
                 27 
                 27 
               
               
                 646 
                 Os 
                 Os 
                 2 
                 3 
                 32 
                 32 
               
               
                 647 
                 Os 
                 Os 
                 2 
                 3 
                 34 
                 34 
               
               
                 648 
                 Os 
                 Os 
                 2 
                 10 
                 20 
                 20 
               
               
                 649 
                 Os 
                 Os 
                 2 
                 10 
                 27 
                 27 
               
               
                 650 
                 Os 
                 Os 
                 2 
                 10 
                 32 
                 32 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 14 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 651 
                 Os 
                 Os 
                 2 
                 10 
                 34 
                 34 
               
               
                 652 
                 Os 
                 Os 
                 2 
                 16 
                 20 
                 20 
               
               
                 653 
                 Os 
                 Os 
                 2 
                 16 
                 27 
                 27 
               
               
                 654 
                 Os 
                 Os 
                 2 
                 16 
                 32 
                 32 
               
               
                 655 
                 Os 
                 Os 
                 2 
                 16 
                 34 
                 34 
               
               
                 656 
                 Ir 
                 Rh 
                 2 
                 1 
                 20 
                 20 
               
               
                 657 
                 Ir 
                 Rh 
                 2 
                 1 
                 23 
                 23 
               
               
                 658 
                 Ir 
                 Rh 
                 2 
                 1 
                 26 
                 26 
               
               
                 659 
                 Ir 
                 Rh 
                 2 
                 1 
                 27 
                 27 
               
               
                 660 
                 Ir 
                 Rh 
                 2 
                 1 
                 28 
                 28 
               
               
                 661 
                 Ir 
                 Rh 
                 2 
                 1 
                 33 
                 33 
               
               
                 662 
                 Ir 
                 Rh 
                 2 
                 1 
                 34 
                 34 
               
               
                 663 
                 Ir 
                 Rh 
                 2 
                 2 
                 20 
                 20 
               
               
                 664 
                 Ir 
                 Rh 
                 2 
                 2 
                 23 
                 23 
               
               
                 665 
                 Ir 
                 Rh 
                 2 
                 2 
                 26 
                 26 
               
               
                 666 
                 Ir 
                 Rh 
                 2 
                 2 
                 27 
                 27 
               
               
                 667 
                 Ir 
                 Rh 
                 2 
                 2 
                 28 
                 28 
               
               
                 668 
                 Ir 
                 Rh 
                 2 
                 2 
                 33 
                 33 
               
               
                 669 
                 Ir 
                 Rh 
                 2 
                 2 
                 34 
                 34 
               
               
                 670 
                 Ir 
                 Rh 
                 2 
                 4 
                 20 
                 20 
               
               
                 671 
                 Ir 
                 Rh 
                 2 
                 4 
                 23 
                 23 
               
               
                 672 
                 Ir 
                 Rh 
                 2 
                 4 
                 26 
                 26 
               
               
                 673 
                 Ir 
                 Rh 
                 2 
                 4 
                 27 
                 27 
               
               
                 674 
                 Ir 
                 Rh 
                 2 
                 4 
                 28 
                 28 
               
               
                 675 
                 Ir 
                 Rh 
                 2 
                 4 
                 33 
                 33 
               
               
                 676 
                 Ir 
                 Rh 
                 2 
                 4 
                 34 
                 34 
               
               
                 677 
                 Ir 
                 Rh 
                 2 
                 10 
                 20 
                 20 
               
               
                 678 
                 Ir 
                 Rh 
                 2 
                 10 
                 23 
                 23 
               
               
                 679 
                 Ir 
                 Rh 
                 2 
                 10 
                 26 
                 26 
               
               
                 680 
                 Ir 
                 Rh 
                 2 
                 10 
                 27 
                 27 
               
               
                 681 
                 Ir 
                 Rh 
                 2 
                 10 
                 28 
                 28 
               
               
                 682 
                 Ir 
                 Rh 
                 2 
                 10 
                 33 
                 33 
               
               
                 683 
                 Ir 
                 Rh 
                 2 
                 10 
                 34 
                 34 
               
               
                 684 
                 Ir 
                 Rh 
                 2 
                 15 
                 20 
                 20 
               
               
                 685 
                 Ir 
                 Rh 
                 2 
                 15 
                 23 
                 23 
               
               
                 686 
                 Ir 
                 Rh 
                 2 
                 15 
                 26 
                 26 
               
               
                 687 
                 Ir 
                 Rh 
                 2 
                 15 
                 27 
                 27 
               
               
                 688 
                 Ir 
                 Rh 
                 2 
                 15 
                 28 
                 28 
               
               
                 689 
                 Ir 
                 Rh 
                 2 
                 15 
                 33 
                 33 
               
               
                 690 
                 Ir 
                 Rh 
                 2 
                 15 
                 34 
                 34 
               
               
                 691 
                 Pt 
                 Pd 
                 1 
                 1 
                 20 
                 20 
               
               
                 692 
                 Pt 
                 Pd 
                 1 
                 1 
                 23 
                 23 
               
               
                 693 
                 Pt 
                 Pd 
                 1 
                 1 
                 26 
                 26 
               
               
                 694 
                 Pt 
                 Pd 
                 1 
                 1 
                 27 
                 27 
               
               
                 695 
                 Pt 
                 Pd 
                 1 
                 1 
                 28 
                 28 
               
               
                 696 
                 Pt 
                 Pd 
                 1 
                 1 
                 33 
                 33 
               
               
                 697 
                 Pt 
                 Pd 
                 1 
                 1 
                 34 
                 34 
               
               
                 698 
                 Pt 
                 Pd 
                 1 
                 2 
                 20 
                 20 
               
               
                 699 
                 Pt 
                 Pd 
                 1 
                 2 
                 23 
                 23 
               
               
                 700 
                 Pt 
                 Pd 
                 1 
                 2 
                 26 
                 26 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 15 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 701 
                 Pt 
                 Pd 
                 1 
                 2 
                 27 
                 27 
               
               
                 702 
                 Pt 
                 Pd 
                 1 
                 2 
                 28 
                 28 
               
               
                 703 
                 Pt 
                 Pd 
                 1 
                 2 
                 33 
                 33 
               
               
                 704 
                 Pt 
                 Pd 
                 1 
                 2 
                 34 
                 34 
               
               
                 705 
                 Pt 
                 Pd 
                 1 
                 4 
                 20 
                 20 
               
               
                 706 
                 Pt 
                 Pd 
                 1 
                 4 
                 23 
                 23 
               
               
                 707 
                 Pt 
                 Pd 
                 1 
                 4 
                 26 
                 26 
               
               
                 708 
                 Pt 
                 Pd 
                 1 
                 4 
                 27 
                 27 
               
               
                 709 
                 Pt 
                 Pd 
                 1 
                 4 
                 28 
                 28 
               
               
                 710 
                 Pt 
                 Pd 
                 1 
                 4 
                 33 
                 33 
               
               
                 711 
                 Pt 
                 Pd 
                 1 
                 4 
                 34 
                 34 
               
               
                 712 
                 Pt 
                 Pd 
                 1 
                 10 
                 20 
                 20 
               
               
                 713 
                 Pt 
                 Pd 
                 1 
                 10 
                 23 
                 23 
               
               
                 714 
                 Pt 
                 Pd 
                 1 
                 10 
                 26 
                 26 
               
               
                 715 
                 Pt 
                 Pd 
                 1 
                 10 
                 27 
                 27 
               
               
                 716 
                 Pt 
                 Pd 
                 1 
                 10 
                 28 
                 28 
               
               
                 717 
                 Pt 
                 Pd 
                 1 
                 10 
                 33 
                 33 
               
               
                 718 
                 Pt 
                 Pd 
                 1 
                 10 
                 34 
                 34 
               
               
                 719 
                 Pt 
                 Pd 
                 1 
                 15 
                 20 
                 20 
               
               
                 720 
                 Pt 
                 Pd 
                 1 
                 15 
                 23 
                 23 
               
               
                 721 
                 Pt 
                 Pd 
                 1 
                 15 
                 26 
                 26 
               
               
                 722 
                 Pt 
                 Pd 
                 1 
                 15 
                 27 
                 27 
               
               
                 723 
                 Pt 
                 Pd 
                 1 
                 15 
                 28 
                 28 
               
               
                 724 
                 Pt 
                 Pd 
                 1 
                 15 
                 33 
                 33 
               
               
                 725 
                 Pt 
                 Pd 
                 1 
                 15 
                 34 
                 34 
               
               
                 726 
                 Os 
                 Ru 
                 1 
                 1 
                 20 
                 20 
               
               
                 727 
                 Os 
                 Ru 
                 1 
                 1 
                 23 
                 23 
               
               
                 728 
                 Os 
                 Ru 
                 1 
                 1 
                 26 
                 26 
               
               
                 729 
                 Os 
                 Ru 
                 1 
                 1 
                 27 
                 27 
               
               
                 730 
                 Os 
                 Ru 
                 1 
                 1 
                 28 
                 28 
               
               
                 731 
                 Os 
                 Ru 
                 1 
                 1 
                 33 
                 33 
               
               
                 732 
                 Os 
                 Ru 
                 1 
                 1 
                 34 
                 34 
               
               
                 733 
                 Os 
                 Ru 
                 1 
                 3 
                 20 
                 20 
               
               
                 734 
                 Os 
                 Ru 
                 1 
                 3 
                 23 
                 23 
               
               
                 735 
                 Os 
                 Ru 
                 1 
                 3 
                 26 
                 26 
               
               
                 736 
                 Os 
                 Ru 
                 1 
                 3 
                 27 
                 27 
               
               
                 737 
                 Os 
                 Ru 
                 1 
                 3 
                 28 
                 28 
               
               
                 738 
                 Os 
                 Ru 
                 1 
                 3 
                 33 
                 33 
               
               
                 739 
                 Os 
                 Ru 
                 1 
                 3 
                 34 
                 34 
               
               
                 740 
                 Os 
                 Ru 
                 1 
                 4 
                 20 
                 20 
               
               
                 741 
                 Os 
                 Ru 
                 1 
                 4 
                 23 
                 23 
               
               
                 742 
                 Os 
                 Ru 
                 1 
                 4 
                 26 
                 26 
               
               
                 743 
                 Os 
                 Ru 
                 1 
                 4 
                 27 
                 27 
               
               
                 744 
                 Os 
                 Ru 
                 1 
                 4 
                 28 
                 28 
               
               
                 745 
                 Os 
                 Ru 
                 1 
                 4 
                 33 
                 33 
               
               
                 746 
                 Os 
                 Ru 
                 1 
                 4 
                 34 
                 34 
               
               
                 747 
                 Os 
                 Ru 
                 1 
                 10 
                 20 
                 20 
               
               
                 748 
                 Os 
                 Ru 
                 1 
                 10 
                 23 
                 23 
               
               
                 749 
                 Os 
                 Ru 
                 1 
                 10 
                 26 
                 26 
               
               
                 750 
                 Os 
                 Ru 
                 1 
                 10 
                 27 
                 27 
               
               
                   
               
             
          
         
       
     
     
       
         
               
               
               
               
               
               
               
             
               
               
               
               
               
               
               
             
           
               
                 TABLE 16 
               
               
                   
               
               
                 No 
                 M1 
                 M2 
                 n 
                 P 
                 Q1 
                 Q2 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 751 
                 Os 
                 Ru 
                 1 
                 10 
                 28 
                 28 
               
               
                 752 
                 Os 
                 Ru 
                 1 
                 10 
                 33 
                 33 
               
               
                 753 
                 Os 
                 Ru 
                 1 
                 10 
                 34 
                 34 
               
               
                 754 
                 Os 
                 Ru 
                 1 
                 15 
                 20 
                 20 
               
               
                 755 
                 Os 
                 Ru 
                 1 
                 15 
                 23 
                 23 
               
               
                 756 
                 Os 
                 Ru 
                 1 
                 15 
                 26 
                 26 
               
               
                 757 
                 Os 
                 Ru 
                 1 
                 15 
                 27 
                 27 
               
               
                 758 
                 Os 
                 Ru 
                 1 
                 15 
                 28 
                 28 
               
               
                 759 
                 Os 
                 Ru 
                 1 
                 15 
                 33 
                 33 
               
               
                 760 
                 Os 
                 Ru 
                 1 
                 15 
                 34 
                 34 
               
               
                   
               
             
          
         
       
     
     The metal coordination compound of the formula (1) according to the present invention may be synthesized through the following reaction schemes representing a synthesis process of iridium complex as an example. 
     
       
         IrCl 3 +4L→L 2 IrCl 2 IrL 2   (1)  
       
     
     
       
         L 2 IrCl 2 IrL 2 +2Hacac→2IrL 2 (acac)  (2)  
       
     
     
       
         2IrL 2 (acac)+L′→L 2 IrL′L 2   (3)  
       
     
     Hacac: acetylacetone 
     acac: dehydrogenated acetylacetone 
     First, according to the scheme (1), a binuclear iridium complex bridged with chlorine is synthesized and then made into its acetylacetone derivative (the scheme (2)), followed by reaction with L′ to obtain an objective binuclear iridium complex (the scheme (3)). 
     Hereinafter, the present invention will be described more specifically used on Examples. 
     EXAMPLE 1 
     An organic luminescence device (EL device) having a structure shown in FIG. 1C was prepared in the following manner. 
     On a glass substrate (transparent substrate 15), a 100 nm-thick film (transparent electrode  14 ) of ITO (indium tin oxide) was formed by sputtering, followed by patterning. 
     On the ITO-formed substrate, four organic layers and two metal electrode layers shown below were successively formed by vacuum (vapor) deposition using resistance heating in a vacuum chamber (10 −4  Pa). 
     Organic layer  1  (hole transport layer  13 ) (50 nm): α-NPD 
     Organic layer  2  (luminescence layer  12 ) (40 nm): co-deposited film of CBP: metal coordination compound of formula 1 shown below (93:7 by weight) 
     Organic layer  3  (exciton diffusion prevention layer  17 ) (20 nm): BCP 
     Organic layer  4  (electron transport layer  16 ) (40 nm): Alq3 
     Metal electrode layer  1  (metal electrode  11 ) (15 nm): Al—Li alloy (Li=1.8 wt. %) 
     Metal electrode layer  2  (metal electrode  11 ) (100 nm): Al 
     The metal electrode layers  1  and  2  were patterned to have an effective luminescence area (opposing electrode area) of 3 mm 2 .                           
     EL characteristics of the thus-prepared organic luminescence device using the metal coordination compounds of formula (1) (Ex. Comp. No. (1)) was measured by using a microammeter (“Model 4140B”, mfd. by Hewlett-Packard Co.) for a current-voltage characteristic) and a spectrophotofluoro-meter (“Model SR1”, mfd. by Topcon K. K.) for emission. The organic luminescence device exhibited good rectification characteristic. 
     When a voltage of 12 volts was applied to the organic luminescence device, good luminescence from the device was confirmed. This luminescence was similar to photoluminescence obtained when a toluene solution of the luminescence material (the metal coordination compound (Ex. Comp. No. 1), was used. Accordingly, it was confirmed that the luminescence from the organic luminescence device was that resulting from the luminescence material. 
     When the organic luminescence device was continuously driven for 150 hours, the organic luminescence device produced stable luminescence. 
     EXAMPLE 2 
     An organic luminescence device was prepared and evaluated in the same manner as in Example 1 except for using the following metal coordination compound (Ex. Comp. No. 46) shown below in place of the metal coordination compound (Ex. Comp. No. 1).                           
     As a result when a voltage of 12 volts was applied to the organic luminescence device, good luminescence resulting from the luminescence material (the metal coordination compound (Ex. Comp. No. 46) was confirmed. 
     When the organic luminescence device was continuously driven for 150 hours, the organic luminescence device produced stable luminescence. 
     EXAMPLE 3 
     A simple matrix-type organic luminescence device having a structure shown in FIG. 2 was prepared in the following manner. 
     On a glass substrate 21 measuring 75 mm-length, 75 mm-width and 1.1 mm-thickness, a ca. 100 nm-thick ITO film was formed by sputtering and patterned into 100 lines of 100 μm-wide transparent matrix electrodes (anode side) with a spacing of 40 μm as simple matrix electrodes. Then, a four-layered organic compound layer  23  was formed thereon including a luminescence layer  12  containing the metal coordination compound (Ex. Comp. No. 1) in the same manner as in Example 1. 
     Then, 100 lines of 100 μm-wide metal electrodes 24 were formed with a spacing of 40 μm by mask vacuum deposition so as to be perpendicular to the transparent electrodes by vacuum deposition at a vacuum of 2.7×10 −3  Pa (2×10 −5  Torr). The metal electrodes were formed as a lamination of 10 nm-thick layer of Al/Li alloy (Li: 1.3 wt. %) and then 150 nm-thick layer of Al. 
     The thus-obtained 100×100-simple matrix-type organic luminescence device was subjected to a simple matrix drive in a glove box filled with nitrogen at voltages of 15 volts to 23 volts by using a scanning signal of 19 volts and data signals of ±4 volts as shown in FIG.  3 . As a result of an interlaced drive at a frame frequency of 30 Hz, smooth motion pictures were confirmed. 
     EXAMPLE 4 
     Synthesis of Ex. Comp. No. 46 
     
       
                 
         
             
             
         
      
     
     In a 1 L (litter)-three-necked flask, 10.00 g (60.3 mmol) of 1,4-phenylenebisboronic acid, 19.1 g (121 mmol) of 1-bromopyridine, 120 ml of toluene, 60 ml of ethanol and 25 ml of 2M-sodium carbonate aqueous solution, were placed and stirred at room temperature under a nitrogen stream, followed by addition of 4.74 g (4.10 mmol) of tetrakis(triphenylphosphine)palladium (0). Thereafter, the system was refluxed under stirring and nitrogen stream for 8 hours. After completion of the reaction, the reaction product was cooled and extracted by adding cold water and toluene. The organic layer was washed with saline water and dried with anhydrous magnesium sulfate, followed by removal of the solvent under a reduced pressure to provide dry solid. The residue was purified by silica gel column chromatography (eluent: toluene/ethyl acetate=2/1) to obtain 7.8 g (yield=56%) of 1,4-bis(2-pyridyl)benzene.                           
     In a 10 L-three-necked flask, 50.0 g (142 mmol) of iridium (III) chloride trihydrate (mfd. by Across Co.), 98 g (631 mmol) of 2-phenylpyridine (mfd. by Aldrich Co.), 3870 ml of ethoxyethanol and 1290 ml of distilled water were placed and stirred for 30 min. at room temperature under nitrogen stream, followed by 24 hours of reflux under stirring. The reaction product was cooled to room temperature, and the precipitate was recovered by filtration and washed successively with water, ethanol and acetone. After being dried at room temperature under a reduced pressure, the dried product was dissolved in 9700 ml of methylene chloride to remove an insoluble matter by filtration. To the filtrate, 3200 ml of toluene and 1300 ml of hexane were added, followed by distilling-off of the solvent under reduced pressure until the volume thereof was reduced to 6400 ml. The resultant liquid was cooled on an ice bath to precipitate a crystal. The crystal was recovered by filtration to obtain 49.5 g (Yield: 65.1%) of tetrakis (2-phenylpyridine-C 2 ,N)(μ-dichloro)diiridium (III).                           
     In a 3 L-three-necked flask, 1250 ml of ethoxyethanol, 41.8 g (39.0 mmol) of tetrakis(2-phenylpyridine-C 2 ,N)(μ-dichloro)diiridium, 10.0 g (99.9 mmol) of acetylacetone and 45.0 g (425 mmol) of sodium carbonate, were placed and stirred for 1 hour at room temperature under an argon stream, followed by 15 hours of reflux under stirring. The reaction product was cooled with ice, and the precipitate was filtered out and washed with water. The precipitate was successively washed with diethyl ether and hexane and was purified by silica gel chromatography (eluent: methylene chloride) followed by washing with hexane) to obtain 26.0 g (yield: 55.3%) of bis(2-phenyl-pyridine-C 2 ,N)(acetylacetonato)iridium (III).                           
     In a 3 L-three-necked flask, 1520 ml of glycerol was placed and subjected to bubbling with argon stream for 30 minutes on an oil bath held around 170° C. Under the argon stream, to the glycerol, 1.81 g (7.79 mmol) of 1,4-bis(2-pyridyl)benzene was added and dissolved therein, followed by addition of 19.00 g (31.52 mmol) of bis(2-phenylpyridine-C 2  N)(acetyl-acetonato)iridium (III). The system was gradually heated and stirred for 3 hours around 180° C. (inner temperature). After the reaction, the reaction mixture was cooled to room temperature and poured into 15 liters of ice water to precipitate a crystal. The crystal was filtered out and washed with water, followed by washing with 1.5 liters of diethyl ether under stirring. The crystal was purified by silica gel column chromatography (eluent: toluene/methylene chloride=1/1) to obtain 2.81 g (Yield: 29.3%) of a red powdery objective compound (Ex. Comp. No. 46). 
     The compound was subjected to MALDI-TOF MS (matrix-assisted laser desorption ionization time-of-flight mass spectroscopy), whereby M +  (a mass of an ion obtained by removing one electron from the compound) thereof of 1232.3 was confirmed. 
     EXAMPLE 5 
     The metal coordination compound (Ex. Comp. No. 46) prepared in Example 4 was subjected to emission spectrum analysis in a toluene solution and a powdery (solid) state. 
     FIG. 4 was an emission spectrum chart (exciting light: 550 nm) of the compound in the toluene solution at a concentration of 5×10 −6  mol/l, and FIG. 5 was an emission spectrum chart (exciting light: 550 nm) of the compound in the powdery state. 
     The measured peak emission spectrum wavelength of the compound in the toluene solution was 651 nm and that of the compound in the powdery state was 655 nm. 
     As a result, it has been confirmed that the metal coordination compound of the formula (1) according to the present invention produced strong luminescence even in a powdery state wherein ordinary luminescent materials were liable to cause concentration extinction and provided the emission spectrum (in the powdery state) substantially equal to that in the low-concentration toluene solution, thus possessing a good concentration extinction-suppression performance. 
     Generally, an emission spectrum of a metal coordination compound in a powdery (solid) state is liable to be shifted to the longer wavelength side and have a broaden spectrum shape. In this state, a resultant luminescence intensity is generally lowered. 
     On the other hand, the metal coordination compound of the present invention produced strong luminescence. This may be attributable to a particular molecular structure of the metal coordination compound of the present invention such that the center metals are surrounded by the ligands to be less liable to be affected by a surrounding substance. 
     Incidentally, when the metal coordination compound (Ex. Comp. No. 46) used in this example was compared with Ir(ppy) 3 , the metal coordination compound is characterized by its center quadridentate ligand having three rings. 
     Ir(ppy) 3  shows an emission spectrum having a peak wavelength of 515 nm. On the other hand, the metal coordination compound shows the peak emission spectrum wavelength of 655 nm as described above, thus being largely shifted to the longer wavelength side. This may be attributable to the center quadridentate ligand having three rings of the metal coordination compound (Ex. Comp. No. 46) contributing to luminescence, not the phenylpyridine ligand as in Ir(ppy) 3 . 
     Accordingly, luminescence from the metal coordination compound (Ex. Comp. No. 46) as the luminescence material used in the present invention may be considered to be one from the MLCT excited state based on the center quadridentate ligand having three rings. 
     EXAMPLE 6 
     An organic luminescence device having a single organic layer as a luminescence layer  12  as shown in FIG. 1D was prepared in the following manner. 
     On a glass substrate  15 , a 100 nm-thick ITO film  14  was formed by sputtering and patterned. 
     Onto the ITO film, a solution for the luminescence layer  12  of 10 mg of the metal coordination compound (Ex. Comp. No. 46) and 90 mg of polyvinyl carbazole (average molecular weight of 9600) in 10 g of chlorobenzene was applied by spin coating (2000 rpm, 20 sec) in a nitrogen atmosphere, followed by hot curing for 1 hour at 80° C. to obtain a 120 nm-thick luminescence layer  12  (single organic layer). 
     After the thus-treated substrate was set in a vacuum deposition chamber, a cathode  11  having the following two-layer electrode structure was formed by sputtering, followed by patterning to have an effective luminescence area (opposing electrode area) of 3 mm 2 . 
     Metal electrode layer  1  (cathode  11 ) (15 nm): Al—Li alloy (Li=1.8 wt. %) 
     Metal electrode layer  2  (cathode  11 ) (100 nm): Al 
     The thus-prepared organic luminescence device was supplied with a DC voltage between the ITO side ( 14 ) as the anode and the Al side ( 11 ) as the cathode. 
     As a result, the device showed a good rectification (current) characteristic of 12 mA/cm 2  under application of 15 volts. 
     When the device was subjected to measurement of an emission spectrum by using a spectrophoto-fluorometer (“Model SR1”, mfd. by Topcon K. K.), the resultant emission spectrum showed a peak wavelength of 655 nm and a shape substantially identical to those in the powdery state in Example 5. 
     Light emission from the device was clear red luminescence by eye observation and stable even when the device was continuously driven for 200 hours. 
     EXAMPLE 7 
     An organic luminescence device was prepared and evaluated in the same as in Example 6 except that a solution for the luminescence layer  12  was prepared by using 30 mg of the metal coordination compound (Ex. Comp. No. 46), 70 mg of polyvinyl carbazole (average molecular weight of 9600) and 10 g of chlorobenzene. 
     The resultant performances and the resultant emission spectrum of the device were similar to those obtained in Example 6. 
     EXAMPLE 8 
     An organic luminescence device was prepared and evaluated in the same manner as in Example 6 except that a 90 nm-thick luminescence layer  12  was formed with a solution of 10 mg of the metal coordination compound (Ex. Comp. No. 46) in 1 g of chlorobenzene by spin coating (1500 rpm, 10 sec) in a nitrogen atmosphere. 
     As a result, the device showed a good rectification (current) characteristic of 8 mA/cm 2  under application of 16 volts. 
     Further, the device showed a peak emission spectrum wavelength of 660 nm and a shape substantially identical to those in the powdery state in Example 5. 
     Light emission from the device was clear red luminescence by eye observation and stable even when the device was continuously driven for 100 hours. 
     As described above, according to the present invention, the metal coordination compound of the formula (1), which was a binuclear molecular structure characterized by a center quadridentate ligand and surrounding bidentate ligands, exhibits a high phosphorescence yield and has a shorter phosphorescence life. Thus, this compound is suitable as a luminescence material for an organic EL device. Furthermore, the resultant organic EL device (organic luminescence device) having an organic layer comprising the metal coordination compound of the formula (1) exhibits excellent performance including not only a high-efficiency luminescence, but also a high luminance for a long period and less deterioration by continuous energizing. The organic EL device is also excellent as a display device.