Patent Publication Number: US-8119645-B2

Title: Fungicide hydroximoyl-tetrazole derivatives

Description:
CROSS REFERENCE TO RELATED APPLICATION(S) 
     The present application is a 35 U.S.C. §371 national phase conversion of International Application No. PCT/EP2007/057157 filed Jul. 12, 2007, which claims priority of European Application No. 06356093.2 filed Jul. 13, 2006. 
     The present invention relates to hydroximoyl-tetrazoles derivatives, their process of preparation, their use as fungicide active agents, particularly in the form of fungicide compositions, and methods for the control of phytopathogenic fungi, notably of plants, using these compounds or compositions. 
     In European patent application no. 1426371, there are disclosed certain tetrazoyloxime derivatives of the following chemical structure: 
                         
wherein A represents a tetrazolyl group, Het represents either a particular pyridinyl group or a particular thiazolyl group.
 
     In Japanese patent application no. 2004-131392, there are disclosed certain tetrazoyloxime derivatives of the following chemical structure: 
                         
wherein Q can be selected in a list of 15 various heterocycle groups.
 
     In Japanese patent application no. 2004-131416, there are disclosed certain tetrazoyloxime derivatives of the following chemical structure: 
                         
wherein Q can be selected among a pyridinyl group or a thiazolyl group.
 
     The compounds disclosed in these three documents do not prove to provide a comparable utility than the compounds according to the invention. 
     It is always of high-interest in agriculture to use novel pesticide compounds in order to avoid or to control the development of resistant strains to the active ingredients. It is also of high-interest to use novel compounds being more active than those already known, with the aim of decreasing the amounts of active compound to be used, whilst at the same time maintaining effectiveness at least equivalent to the already known compounds. We have now found a new family of compounds which possess the above mentioned effects or advantages. 
     Accordingly, the present invention provides hydroximoyl-tetrazole derivatives of formula (I) 
                         
wherein
         T represents a substituted or non-substituted tetrazolyl group;   L 1  represents a direct bond or a divalent group selected in the list consisting of
           —(CR 1 R 2 ) n — —(CR 1 R 2 ) m —C(═O)—(CR 1 R 2 ) p —   —(CR 1 R 2 ) m —(CR 1 ═CR 2 )—(CR 1 R 2 ) p — —(CR 1 R 2 ) m —C(═O)—(CR 1 R 2 ) p      —(CR 1 R 2 ) m —C≡C—(CR 1 R 2 ) p — —(CR 1 R 2 ) m —O—C(═O)—(CR 1 R 2 ) p —   —(CR 1 R 2 ) m —O—(CR 1 R 2 ) p — —(CR 1 R 2 ) m —C(═O)—NH—(CR 1 R 2 ) p —   —(CR 1 R 2 ) m —NH—(CR 1 R 2 ) p — —(CR 1 R 2 ) m —NH—C(═O)—(CR 1 R 2 ) p —
 
wherein
   
           n represents 1, 2, 3 or 4;   m and p independently represent 0, 1, 2 or 3;   L 2  represents a direct bond or a divalent group selected in the list consisting of
           —(CR 3 R 4 ) q — —(CR 3 R 4 ) a —C(═O)—(CR 3 R 4 ) b —   —(CR 3 R 4 ) a —(CR 3 ═CR 4 )—(CR 3 R 4 ) b — —(CR 3 R 4 ) a —C(═O)—O—(CR 3 R 4 ) b      —(CR 3 R 4 ) a —C≡C—(CR 3 R 4 ) b — —(CR 3 R 4 ) a —O—C(═O)—(CR 3 R 4 ) b —   —(CR 3 R 4 ) a —O—(CR 3 R 4 ) b — —(CR 3 R 4 ) a —C(═O)—NH—(CR 3 R 4 ) b —   —(CR 3 R 4 ) a —NH—(CR 3 R 4 ) b — —(CR 3 R 4 ) a —NH—C(═O)—(CR 3 R 4 ) b —
 
wherein
   
           q represents 1, 2, 3 or 4;   a and b independently represent 0, 1, 2 or 3;   A is selected in the list consisting of A 1  to A 116         

                                                                                                                                                                                                                                                 
wherein
         Z 1 , Z 2 , Z 3 , Z 4 , Z 5 , Z 6 , Z 7 , Z 8  and Z 9  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 5 , —C(═O)OR 5 , —C(═O)NR 5 R 6 , —C(═O)SR 5 , —C(═S)R 5 , —C(═S)OR 5 , —C(═S)NR 5 R 6 , —C(═S)SR 5 , —CR 5 ═NR 6 , —CR 5 ═NOR 6 , —CR 5 ═N—NR 6 R 7 , —OR 5 , —OSiR 5 R 6 R 7 , —OC(═O)R 5 —OC(═O)OR 5 , OC(═O)NR 5 R 6 , —OC(═S)NR 5 R 6 , —NR 5 R 6 , —N(R 5 )C(═O)R 6 , —N(R 5 )C(═O)OR 6 , N(R 5 )C(═O)NR 6 R 7 , —N(R 5 )C(═S)R 6 , —N(R 5 )C(═S)NR 6 R 7 , —N═CR 5 R 6 , —N═C—NR 5 R 6 , —N(R 5 )C(═NR 6 )NR 7 R 8 , —N(R 5 )OR 6 , —N(R 5 )NR 6 R 7 , —N═NR 5 , —N(R 5 )S(═O)R 6 , —N(R 5 )S(═O) 2 R 6 , —N(R 5 )S(═O) 2 OR 6 , —N(R 5 )S(═O)OR 6 , —N(R 5 )S(═O)NR 6 R 7 , —N(R 5 )S(═O) 2 NR 6 R 7 , —SR 5 , —S(═O)R 5 , —S(═O) 2 R 5 , —S(═O)OR 5 , —S(═O)NR 5 R 6 , —S(═O) 2 OR 5 , —S(═O) 2 NR 5 R 6 , nitro, nitroso, azido, cyano, —SF 5  and —SiR 5 R 6 R 7 ;   K 1  and K 2  are independently selected in the list consisting of hydrogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 9 , —C(═O)OR 9 , —C(═O)NR 9 R 10 , —C(═O)SR 9 , —C(═S)R 9 , —C(═S)OR 9 , —C(═S)NR 9 R 10 , —C(═S)SR 9 , —CR 9 ═NR 10 , —CR 9 ═NOR 10 , —CR 9 ═N—NR 10 R 11 , —S(═O)R 9 , —S(═O) 2 R 9 , —S(═O)OR 9 , —S(═O)NR 9 R 10 , —S(═O) 2 OR 9 , —S(═O) 2 NR 9 R 10  and —SiR 9 R 10 R 11 ;   G 1  and G 2  are independently selected in the list consisting of oxygen, sulfur, NR 12 , N—OR 12  and N—NR 12 R 13 ;   Q is selected in the list consisting of Q 1  to Q 72         

                                                                                                                                                                                           
wherein
         X 1 , X 2 , X 3 , X 4  and X 5  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 14 , —C(═O)OR 14 , —C(═O)NR 14 R 15 , —C(═O)SR 14 , —C(═S)R 14 , —C(═S)OR 14 , —C(═S)NR 14 R 15 , —C(═S)SR 14 , —CR 14 ═NR 15 , —CR 14 ═NOR 15 , —CR 14 ═N—NR 15 R 16 , —OR 14 , —OSiR 14 R 15 R 16 , —OC(═O)R 14 —OC(═O)OR 14 , —OC(═O)NR 14 R 15 , —OC(═S)NR 14 R 15 , —NR 14 R 15 , —N(R 14 )C(═O)R 15 , —N(R 14 )C(═O)OR 15 —N(R 14 )C(═O)NR 15 R 16 , —N(R 14 )C(═S)R 15 , —N(R 14 )C(═S)NR 15 R 16 , —N═CR 14 R 15 , —N═C—NR 14 R 15 , —N(R 14 )C(═NR 15 )NR 16 R 17 , —N(R 14 )OR 15 , —N(R 14 )NR 15 R 16 , —N═NR 14 , —N(R 14 )S(═O)R 15 , —N(R 14 )S(═O) 2 R 15 , —N(R 14 )S(═O) 2 OR 15 , —N(R 14 )S(═O)OR 15 , —N(R 14 )S(═O)NR 15 R 16 , —N(R 14 )S(═O) 2 NR 15 R 16 , —SR 14 , —S(═O)R 14 , —S(═O) 2 R 14 , —S(═O)OR 14 , —S(═O)NR 14 R 15 , —S(═O) 2 OR 14 , —S(═O) 2 NR 14 R 15 , nitro, nitroso, azido, cyano, —SF 5  and —SiR 14 R 15 R 16 ;   W 1  is selected in the list consisting of hydrogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 9 , —C(═O)OR 9 , —C(═O)NR 9 R 10 , —C(═O)SR 9 , —C(═S)R 9 , —C(═S)OR 9 , —C(═S)NR 9 R 10 , —C(═S)SR 9 , —CR 9 ═NR 10 , —CR 9 ═NOR 10 , —CR 9 ═N—NR 10 R 11 , —S(═O)R 9 , —S(═O) 2 R 9 , —S(═O)OR 9 , —S(═O)NR 9 R 10 , —S(═O)OR 9 , —S(═O)NR 9 R 10  and —SiR 9 R 10 R 11 ;   R 1 , R 2 , R 3  and R 4  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl, [C 3 -C 5 ]-cycloalkyl, [C 3 -C 5 ]-halocycloalkyl, [C 1 -C 4 ]-alkoxy, [C 1 -C 4 ]-alkoxy-[C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-alkoxy-[C 1 -C 4 ]-alkoxy, [C 1 -C 4 ]-haloalkoxy, [C 1 -C 4 ]-haloalkoxy-[C 1 -C 4 ]-alkyl and cyano;   R 5  to R 17  are independently selected in the list consisting of hydrogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl and aryl-[C 1 -C 8 ]-alkyl;
 
as well as salts, N-oxides, metallic complexes and metalloidic complexes thereof.
       

     Any of the compounds according to the invention can exist as one or more stereoisomers depending on the number of stereogenic units (as defined by the IUPAC rules) in the compound. The invention thus relates equally to all the stereoisomers, and to the mixtures of all the possible stereoisomers, in all proportions. The stereoisomers can be separated according to the methods which are known per se by the man ordinary skilled in the art. 
     According to the invention, the following generic terms are generally used with the following meanings:
         halogen means fluorine, chlorine, bromine or iodine;   heteroatom can be nitrogen, oxygen or sulphur;   halogenated groups, notably haloalkyl, haloalkoxy and cycloalkyl groups, may comprise up to nine identical or different halogen atoms;   the term “aryl” means phenyl or naphthyl, optionally substituted by one to five groups selected in the list consisting of halogen, [C 1 -C 6 ]-alkyl, [C 1 -C 6 ]-haloalkyl, [C 2 -C 6 ]-alkenyl, [C 2 -C 6 ]-haloalkenyl, [C 2 -C 6 ]-alkynyl, [C 2 -C 6 ]-haloalkynyl, [C 1 -C 6 ]-alkoxy, [C 1 -C 4 ]-alkoxy-[C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-alkoxy-[C 1 -C 4 ]-alkoxy, [C 1 -C 6 ]-haloalkoxy and [C 1 -C 4 ]-haloalkoxy-[C 1 -C 4 ]-alkyl.       

     As a further aspect, the present invention provides hydroximoyl-tetrazole derivatives of formula (Ia), (Ib), (Ic) and (Id) 
                         
wherein
         A, Q, L 1  and L 2  are defined in the same manner as the corresponding substituents of the compounds of formula (I) according to the invention;   E 1  is selected in the list consisting of hydrogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —C(═O)SR 18 , —C(═S)R 18 , —C(═S)OR 18 , —C(═S)NR 18 R 19 , —C(═S)SR 18 , —CR 18 ═NR 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —S(═O)R 18 , —S(═O) 2 R 18 , —S(═O)OR 18 , —S(═O)NR 18 R 19 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19 , cyano, and —SiR 18 R 19 R 20 ;   E 2  is selected in the list consisting of hydrogen, halogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl, aryl-[C 1 -C 8 ]-alkyl, hydroxy-[C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-alkoxy-[C 1 -C 8 ]-alkyl, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —C(═O)SR 18 , —C(═S)R 18 , —C(═S)OR 18 , —C(═S)NR 18 R 19 , —C(═S)SR 18 , —CR 18 ═NR 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —OR 18 , —OSiR 18 R 19 R 20 , —OC(═O)R 18 , —OC(═O)OR 18 , —OC(═O)NR 18 R 19 , —OC(═S)NR 18 R 19 , —NR 18 R 19 , —N(R 18 )C(═O)R 19 , —N(R 18 )C(═O)OR 19 , —N(R 18 )C(═O)NR 19 R 20 , —N(R 18 )C(═S)R 19 , —N(R 18 )C(═S)NR 19 R 20 , —N═CR 18 R 19 , —N═C—NR 18 R 19 , —N(R 18 )C(═NR 19 )NR 20 R 21 , —N(R 18 )OR 19 , —N(R 18 )NR 19 R 20 , —N═NR 18 , —N(R 18 )S(═O)R 19 , —N(R 18 )S(═O) 2 R 19 , —N(R 18 )S(═O) 2 OR 19 , —N(R 18 )S(═O)OR 19 , —N(R 18 )S(═O)NR 19 R 20 , —N(R 18 )S(═O) 2 NR 19 R 20 , —SR 18 , —S(═O)R 19 , —S(═O) 2 R 18 , —S(═O)OR 18 , —S(═O)NR 18 R 19 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19 , cyano, —SF 5  and —SiR 18 R 19 R 20 ;   R 18  to R 20  are independently selected in the list consisting of hydrogen, [C 1 -C 8 ]-alkyl, [C 1 -C 8 ]-haloalkyl, [C 2 -C 8 ]-alkenyl, [C 2 -C 8 ]-haloalkenyl, [C 2 -C 8 ]-alkynyl, [C 2 -C 8 ]-haloalkynyl, [C 3 -C 6 ]-cycloalkyl, [C 3 -C 6 ]-halocycloalkyl, aryl and aryl-[C 1 -C 8 ]-alkyl.       

     Preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein L 1  represents a direct bond or a divalent group selected in the list consisting of
         —(CR 1 R 2 ) n — —C(═O)—(CR 1 R 2 ) p —   —(CR 1 R 2 ) m —O—  13  (CR 1 R 2 ) m —C(═O)—O—   —(CR 1 R 2 ) m —NH— —(CR 1 R 2 ) m —C(═O)NH—   —(CR 1 R 2 ) m —C(═O)— —(CR 1 R 2 ) m —NH—C(═O)
 
wherein
   n represents 1 or 2;   m and p independently represent 0 or 1;   R 1  and R 2  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-alkynyl, [C 3 -C 5 ]-cycloalkyl, [C 1 -C 4 ]-alkoxy, [C 1 -C 4 ]-haloalkoxy and cyano.       

     More preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein L 1  represents a direct bond or a divalent group selected in the list consisting of —(CR 1 R 2 )—, —C(═O)—(CR 1 R 2 )— and —C(═O)—; wherein R 1  and R 2  are independently selected in the list consisting of hydrogen, halogen, methyl, ethyl, iso-propyl, trifluoromethyl, difluoromethyl, allyl, ethynyl, propargyl, cyclopropyl, methoxy, trifluoromethoxy and cyano. 
     Other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein L 2  represents a direct bond or a divalent group selected in the list consisting of
         —(CR 3 R 4 ) q — —(CR 3 R 4 ) a —C(═O)—   —(CR 3 ═CR 4 )— —(CR 3 R 4 ) a —C(═O)—O—   —C≡C— —(CR 3 R 4 ) a —O—C(═O)—   —(CR 3 R 4 ) a —O— —(CR 3 R 4 ) a —C(═O)NH—   —(CR 3 R 4 ) a —NH— —(CR 3 R 4 ) a —NH—C(═O)—
 
wherein
   q and a independently represent 1 or 2;   R 3  and R 4  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-alkynyl, [C 3 -C 5 ]-cycloalkyl, [C 1 -C 4 ]-alkoxy, [C 1 -C 4 ]-haloalkoxy and cyano.       

     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein L 2  represents a direct bond or —(CR 3 R 4 )— wherein R 3  and R 4  are independently selected in the list consisting of hydrogen, halogen, methyl, ethyl, iso-propyl, trifluoromethyl, difluoromethyl, allyl, ethynyl, propargyl, cyclopropyl, methoxy, trifluoromethoxy and cyano. 
     Still other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein A is selected in the list consisting of A 1  to A 32 . 
     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein A is selected in the list consisting of A 2 , A 6 , A 8 , A 15 , A 16 , A 17  and A 18 . 
     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Z 1  is selected in the list consisting of hydrogen, —C(═O)R 5 , —C(═O)OR 5 , —C(═O)NR 5 R 6 , —C(═S)NR 5 R 6 , —CR 5 ═NR 6 , —CR 5 ═NOR 6 , —CR 5 ═N—NR 6 R 7 , —OR 5 , —OC(═O)R 5 , —OC(═O)OR 5 , —OC(═O)NR 5 R 6 , —OC(—S)NR 5 R 6 , —NR 5 R 6 , —N(R 5 )C(═O)R 6 , —N(R 5 )C(═O)OR 6 , —N(R 5 )C(═O)NR 6 R 7 , —N(R 5 )C(═S)R 6 , —N(R 5 )C(═S)NR 6 R 7 , —N═CR 5 R 6 , —N═C—NR 5 R 6 , —N(R 5 )C(═NR 6 )NR 7 R 8 , —N(R 5 )OR 6 , —N(R 5 )NR 6 R 7 , —N═NR 5 , —N(R 5 )S(═O) 2 R 6 , —N(R 5 )S(═O) 2 OR 6 , —N(R 5 )S(═O) 2 NR 6 R 7 , —SR 5 , —S(═O) 2 R 5 , —S(═O) 2 OR 5 , —S(═O) 2 NR 5 R 6  and cyano. 
     Other even more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Z 1  is selected in the list consisting of hydrogen, —NR 5 R 6 , —N(R 5 )C(═O)R 6 , —N(R 5 )C(═O)OR 6 , —N(R 5 )C(═O)NR 6 R 7 , —N(R 5 )C(═S)NR 6 R 7 , —N═CR 5 R 6 , —N═C—NR 5 R 6 , —N(R 5 )C(═NR 6 )NR 7 R 8 , —N(R 5 )S(═O) 2 R 6 , —N(R 5 )S(═O) 2 OR 6 , —N(R 5 )S(═O) 2 NR 6 R 7  and cyano. 
     Still other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Z 2 , Z 3 , Z 4 , Z 5 , Z 6 , Z 7 , Z 8  and Z 9  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl, [C 3 -C 5 ]-cycloalkyl, —C(═O)R 5 , —C(═O)OR 5 , —C(═O)NR 5 R 6 , —OR 5 , —OSiR 5 R 6 R 7 , —OC(═O)R 5 , —NR 5 R 6 , —N(R 5 )C(═O)R 6 , —SR 5 , —S(═O) 2 R 5 , —S(═O) 2 OR 5 , —S(═O) 2 NR 5 R 6 , cyano and —SiR 5 R 6 R 7 ; wherein R 5 , R 6 , and R 7  are independently selected in the list consisting of hydrogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl and [C 3 -C 5 ]-cycloalkyl. 
     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Z 2 , Z 3 , Z 4 , Z 5 , Z 6 , Z 7 , Z 8  and Z 9  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, methyl, ethyl, iso-propyl, iso-butyl, tert-butyl, [C 1 -C 4 ]-haloalkyl, trifluoromethyl, difluoromethyl, allyl, ethynyl, propargyl, cyclopropyl, methoxy, trifluoromethoxy, acetyl, trifluoroacetyl and cyano. 
     Still other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein K 1 , K 2  and W 1  are independently selected in the list consisting of hydrogen, [C 1 -C 4 ]-alkyl, methyl, ethyl, iso-propyl, iso-butyl, tert-butyl, allyl, propargyl, cyclopropyl, acetyl, trifluoroacetyl and mesyl. 
     Still other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Q is selected in the list consisting of Q 1  to Q 26 . 
     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein Q is selected in the list consisting of Q 3 , Q 4 , Q 6 , Q 7 , Q 9 , Q 12  and Q 15 . 
     Still other preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein X 1  to X 5  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl, [C 3 -C 5 ]-cycloalkyl, [C 3 -C 5 ]-halocycloalkyl, aryl, aryl-[C 1 -C 2 ]-alkyl, —C(═O)R 14 , —C(═O)OR 14 , —C(═O)NR 14 R 15 , —CR 14 ═NOR 15 , —CR 14 ═N—NR 15 R 16 , —OR 14 , —OSiR 14 R 15 R 16 , —OC(═O)R 14 , —OC(═O)OR 14 , —OC(═O)NR 14 R 15 , —NR 14 R 15 , —N(R 14 )C(═O)R 15 , —SR 14 , —S(═O) 2 R 14 , —S(═O) 2 OR 14 , —S(═O) 2 NR 14 R 15 , cyano and —SiR 14 R 15 R 16 ; wherein R 14 , R 15 , and R 16  are independently selected in the list consisting of hydrogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl and [C 3 -C 5 ]-cycloalkyl, aryl and aryl-[C 1 -C 2 ]-alkyl. 
     Other more preferred compounds of formula (I) and (Ia) to (Id) according to the invention are those wherein X 1  to X 5  are independently selected in the list consisting of hydrogen, halogen, [C 1 -C 4 ]-alkyl, methyl, iso-propyl, iso-butyl, tert-butyl, [C 1 -C 4 ]-haloalkyl, trifluoromethyl, difluoromethyl, allyl, ethynyl, propargyl, cyclopropyl, benzyl, phenethyl, methoxy, trifluoromethoxy, acetyl, trifluoroacetyl and cyano. 
     Preferred compounds of formula (Ia) to (Id) according to the invention are those wherein E 1  is selected in the list consisting of [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl, [C 3 -C 5 ]-cycloalkyl, [C 3 -C 5 ]-halocycloalkyl, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —CR 18 ═NR 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —S(═O) 2 R 18 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19 , cyano and —SiR 18 R 19 R 20 ; wherein R 18 , R 19  and R 20  are independently selected in the list consisting of hydrogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl and cyclopropyl. 
     More preferred compounds of formula (Ia) to (Id) according to the invention are those wherein E 1  is selected in the list consisting of methyl, ethyl, iso-propyl, allyl, propargyl, cyclopropyl, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —CR 18 ═NR 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —S(═O) 2 R 18 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19  and —SiR 18 R 19 R 20 ; wherein R 18 , R 19  and R 20  are independently selected in the list consisting of methyl and trifluoromethyl. 
     Other preferred compounds of formula (Ia) to (Id) according to the invention are those wherein E 2  is selected in the list consisting of halogen, [C 1 -C 4 ]-alkyl, [C 1 -C 4 ]-haloalkyl, [C 2 -C 4 ]-alkenyl, [C 2 -C 4 ]-haloalkenyl, [C 2 -C 4 ]-alkynyl, [C 2 -C 4 ]-haloalkynyl, [C 3 -C 5 ]-cycloalkyl, [C 3 -C 5 ]-halocycloalkyl, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —OR 18 , —OSiR 18 R 19 R 20 , —OC(═O)R 18 , —OC(═O)R 18 , —OC(═O)NR 18 R 19 , —NR 18 R 19 , —N(R 18 )C(═O)R 19 , —N(R 18 )C(═O)OR 19 , —N(R 18 )C(═O)NR 19 R 20 , —N(R 18 )C(═S)R 19 , —N(R 18 )C(═S)NR 19 R 20 , —N═CR 18 R 19 , —N═C—NR 13 R 19 , —N(R 18 )S(═O) 2 R 19 , —N(R 18 )S(═O) 2 OR 19 , —N(R 18 )S(═O)NR 19 R 20 , —SR 18 , —S(═O) 2 R 18 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19 , cyano and —SiR 18 R 19 R 20 ; wherein R 18 , R 19  and R 20  are independently selected in the list consisting of hydrogen, [C 1 -C 4 ]-alkyl and [C 1 -C 4 ]-haloalkyl. 
     Other more preferred compounds of formula (Ia) to (Id) according to the invention are those wherein E 2  is selected in the list consisting of methyl, ethyl, iso-propyl, trifluoromethyl, difluoromethyl, allyl, ethynyl, propargyl, cyclopropyl, cyano, —C(═O)R 18 , —C(═O)OR 18 , —C(═O)NR 18 R 19 , —CR 18 ═NOR 19 , —CR 18 ═N—NR 19 R 20 , —OR 18 , —OSiR 18 R 19 R 20 , —OC(═O)R 18 , —OC(═O)OR 18 , —OC(═O)NR 18 R 19 , —NR 18 R 19 , —N(R 18 )C(═O)R 19 , —N(R 18 )C(═O)OR 19 , —N(R 18 )C(═O)NR 19 R 20 , —N(R 18 )C(═S)R 19 , —N(R 18 )C(═S)NR 19 R 20 , —N═CR 18 R 19 , —N═C—NR 18 R 19 , —N(R 18 )S(═O) 2 R 19 , —N(R 18 )S(═O) 2 OR 19 , —N(R 18 )S(═O) 2 NR 19 R 20 , —SR 18 , —S(═O) 2 R 18 , —S(═O) 2 OR 18 , —S(═O) 2 NR 18 R 19  and —SiR 18 R 19 R 20 ; wherein R 18 , R 19  and R 20  are independently selected in the list consisting of hydrogen, methyl and trifluoromethyl. 
     The above mentioned preferences with regard to the substituents of the compounds of formula (I) and (Ia) to (Id) according to the invention can be combined in various manners. These combinations of preferred features thus provide sub-classes of compounds according to the invention. Examples of such sub-classes of preferred compounds according to the invention can combine:
         preferred features of A with preferred features of one or more of L 1 , L 2 , Q, E 1  and E 2 ;   preferred features of L 1  with preferred features of one or more of A, L 2 , Q, E 1  and E 2 ;   preferred features of L 2  with preferred features of one or more of A, L 1 , Q, E 1  and E 2 ;   preferred features of Q with preferred features of one or more of A, L 1 , L 2 , E 1  and E 2 ;   preferred features of E 1  with preferred features of one or more of A, L 1 , L 2 , Q and E 2 ;   preferred features of E 2  with preferred features of one or more of A, L 1 , L 2 , Q and E 1 .       

     In these combinations of preferred features of the substituents of the compounds according to the invention, the said preferred features can also be selected among the more preferred features of each of A, Q, L 1 , L 2 , E 1  and E 2 ; so as to form most preferred subclasses of compounds according to the invention. 
     The preferred features of the other substituents of the compounds according to the invention can also be part of such sub-classes of preferred compounds according to the invention, notably the groups of substituents R, Z, K, G, X and W as well as the integers a, b, m, n, p and q. 
     The present invention also relates to a process for the preparation of compounds of formula (I), (Ia), (Ib), (Ic) and (Id). Thus, according to a further aspect of the present invention, there is a provided process P1 for the preparation of compounds of formula (I), (Ia), (Ib), (Ic) and (Id) as herein-defined, as illustrated by the following reaction schemes. 
                         
wherein
 
A, L 1 , L 2 , Q, E 1  and E 2  are as herein-defined and LG represents a leaving group. Suitable leaving groups can be selected in the list consisting of a halogen atom or other customary nucleofugal groups such as triflate, mesylate, or tosylate.
 
     For the compounds of formula (I) according to the invention when Z 1 , Z 2 , Z 3 , Z 4 , Z 5 , Z 6 , Z 7 , Z 8  or Z 9  represents an amino group, process P1 according to the invention can be completed by a further step comprising the additional modification of this group, notably by a reaction of acylation, alkoxycarbonylation, alkylaminocarbonylation or alkylaminothiocarbonylation, according to known methods. In such a case there is provided a process P2 according to the invention and such a process P2 can be illustrated by the following reaction schemes: 
                         
wherein A, L 1 , L 2 , T, Q and R 5  are as herein-defined.
 
     If Z 1 , Z 2 , Z 3 , Z 4 , Z 5 , Z 6 , Z 7 , Z 8  or Z 9  represents a protected amino group, carrying out process P2 would previously require a deprotection step in order to yield the amino group. Amino-protecting groups and related methods of cleavage thereof are known and can be found in T. W. Greene and P. G. M. Wuts,  Protective Group in Organic Chemistry,  3 rd  ed., John Wiley &amp; Sons. 
     According to the invention, processes P1 and P2 may be performed if appropriate in the presence of a solvent and if appropriate in the presence of a base. 
     Suitable solvents for carrying out processes P1 and P2 according to the invention are customary inert organic solvents. Preference is given to using optionally halogenated aliphatic, alicyclic or aromatic hydrocarbons, such as petroleum ether, hexane, heptane, cyclohexane, methylcyclohexane, benzene, toluene, xylene or decalin; chlorobenzene, dichlorobenzene, dichloromethane, chloroform, carbon tetrachloride, dichlorethane or trichlorethane; ethers, such as diethyl ether, diisopropyl ether, methyl tert-butyl ether, methyl tert-amyl ether, dioxane, tetrahydrofuran, 1,2-dimethoxyethane, 1,2-diethoxyethane or anisole; nitriles, such as acetonitrile, propionitrile, n- or iso-butyronitrile or benzonitrile; amides, such as N,N-dimethylformamide, N,N-dimethylacetamide, N-methylformanilide, N-methylpyrrolidone or hexamethylphosphoric triamide; esters, such as methyl acetate or ethyl acetate, sulphoxides, such as dimethyl sulphoxide, or sulphones, such as sulpholane. 
     Suitable bases for carrying out processes P1 and P2 according to the invention are inorganic and organic bases which are customary for such reactions. Preference is given to using alkaline earth metal, alkali metal hydride, alkali metal hydroxides or alkali metal alkoxides, such as sodium hydroxide, sodium hydride, calcium hydroxide, potassium hydroxide, potassium tert-butoxide or other ammonium hydroxide, alkali metal carbonates, such as sodium carbonate, potassium carbonate, potassium bicarbonate, sodium bicarbonate, cesium carbonate, alkali metal or alkaline earth metal acetates, such as sodium acetate, potassium acetate, calcium acetate, and also tertiary amines, such as trimethylamine, triethylamine, diisopropylethylamine, tributylamine, N,N-dimethylaniline, pyridine, N-methylpiperidine, N,N-dimethylaminopyridine, 1,4-diazabicyclo[2.2.2]octane (DABCO), 1,5-diazabicyclo[4.3.0]non-5-ene (DBN) or 1,8-diaza-bicyclo[5.4.0]undec-7-ene (DBU). 
     When carrying out processes P1 and P2 according to the invention, the reaction temperature can independently be varied within a relatively wide range. Generally, process P1 according to the invention is carried out at temperatures between 0° C. and 160° C. 
     Processes P1 and P2 according to the invention are generally independently carried out under atmospheric pressure. However, it is also possible to operate under elevated or reduced pressure. 
     When carrying out process P1 according to the invention, generally 1 mol or an excess of derivative of formula A-L 1 -LG and from 1 to 3 mol of base are employed per mole of hydroximoyl tetrazoles of formula (IVa), (IVb), (Va) or (Vb). It is also possible to employ the reaction components in other ratios. 
     Work-up is carried out by customary methods. Generally, the reaction mixture is treated with water and the organic phase is separated off and, after drying, concentrated under reduced pressure. If appropriate, the remaining residue can be freed by customary methods, such as chromatography or recrystallization, from any impurities that may still be present. 
     Compounds according to the invention can be prepared according to the above described processes. It will nevertheless be understood that, on the basis of his general knowledge and of available publications, the skilled worker will be able to adapt these processes according to the specifics of each of the compounds according to the invention that is desired to be synthesised. 
     The compounds of formula (IVa) and (IVb), useful as a starting material, can be prepared, for example, by reacting hydroxylamine with the corresponding ketones that can be prepared, for example, according to the method described by R. Raap ( Can. J. Chem.  1971, 49, 2139) by addition of a tetrazolyl lithium species to esters of formula Q-L 2 -CO 2 Me or Q-L 2 -CO 2 Et, or any of their suitable synthetic equivalents like, for example: Q-L 2 -C(═O)—N(OMe)Me, Q-L 2 -CN, Q-L 2 -C(═O)Cl. 
     The compounds of general formula (Va) and (Vb), useful as a starting material, can be prepared, for example, from oximes of formula Q-L 2 -CH═N—OH and 5-substituted tetrazoles according to the method described by J. Plenkiewicz et al. ( Bull. Soc. Chim. Belg.  1987, 96, 675). 
     In a further aspect, the present invention also relates to a fungicide composition comprising an effective and non-phytotoxic amount of an active compound of formula (I) or (Ia) to (Id). 
     The expression “effective and non-phytotoxic amount” means an amount of composition according to the invention which is sufficient to control or destroy the fungi present or liable to appear on the crops, and which does not entail any appreciable symptom of phytotoxicity for the said crops. Such an amount can vary within a wide range depending on the fungus to be controlled, the type of crop, the climatic conditions and the compounds included in the fungicide composition according to the invention. This amount can be determined by systematic field trials, which are within the capabilities of a person skilled in the art. 
     Thus, according to the invention, there is provided a fungicide composition comprising, as an active ingredient, an effective amount of a compound of formula (I) or (Ia) to (Id) as herein defined and an agriculturally acceptable support, carrier or filler. 
     According to the invention, the term “support” denotes a natural or synthetic, organic or inorganic compound with which the active compound of formula (I) is combined or associated to make it easier to apply, notably to the parts of the plant. This support is thus generally inert and should be agriculturally acceptable. The support may be a solid or a liquid. Examples of suitable supports include clays, natural or synthetic silicates, silica, resins, waxes, solid fertilisers, water, alcohols, in particular butanol, organic solvents, mineral and plant oils and derivatives thereof. Mixtures of such supports may also be used. 
     The composition according to the invention may also comprise additional components. In particular, the composition may further comprise a surfactant. The surfactant can be an emulsifier, a dispersing agent or a wetting agent of ionic or non-ionic type or a mixture of such surfactants. Mention may be made, for example, of polyacrylic acid salts, lignosulphonic acid salts, phenolsulphonic or naphthalenesulphonic acid salts, polycondensates of ethylene oxide with fatty alcohols or with fatty acids or with fatty amines, substituted phenols (in particular alkylphenols or arylphenols), salts of sulphosuccinic acid esters, taurine derivatives (in particular alkyl taurates), phosphoric esters of polyoxyethylated alcohols or phenols, fatty acid esters of polyols, and derivatives of the above compounds containing sulphate, sulphonate and phosphate functions. The presence of at least one surfactant is generally essential when the active compound and/or the inert support are water-insoluble and when the vector agent for the application is water. Preferably, surfactant content may be comprised from 5% to 40% by weight of the composition. 
     Optionally, additional components may also be included, e.g. protective colloids, adhesives, thickeners, thixotropic agents, penetration agents, stabilisers, sequestering agents. More generally, the active compounds can be combined with any solid or liquid additive, which complies with the usual formulation techniques. 
     In general, the composition according to the invention may contain from 0.05 to 99% by weight of active compound, preferably 10 to 70% by weight. 
     Compositions according to the invention can be used in various forms such as aerosol dispenser, capsule suspension, cold fogging concentrate, dustable powder, emulsifiable concentrate, emulsion oil in water, emulsion water in oil, encapsulated granule, fine granule, flowable concentrate for seed treatment, gas (under pressure), gas generating product, granule, hot fogging concentrate, macrogranule, microgranule, oil dispersible powder, oil miscible flowable concentrate, oil miscible liquid, paste, plant rodlet, powder for dry seed treatment, seed coated with a pesticide, soluble concentrate, soluble powder, solution for seed treatment, suspension concentrate (flowable concentrate), ultra low volume (ULV) liquid, ultra low volume (ULV) suspension, water dispersible granules or tablets, water dispersible powder for slurry treatment, water soluble granules or tablets, water soluble powder for seed treatment and wettable powder. These compositions include not only compositions which are ready to be applied to the plant or seed to be treated by means of a suitable device, such as a spraying or dusting device, but also concentrated commercial compositions which must be diluted before application to the crop. 
     The compounds according to the invention can also be mixed with one or more insecticide, fungicide, bactericide, attractant, acaricide or pheromone active substance or other compounds with biological activity. The mixtures thus obtained have a broadened spectrum of activity. The mixtures with other fungicide compounds are particularly advantageous. 
     Examples of suitable fungicide mixing partners may be selected in the following lists
         B1) a compound capable to inhibit the nucleic acid synthesis like benalaxyl, benalaxyl-M, bupirimate, clozylacon, dimethirimol, ethirimol, furalaxyl, hymexazol, mefenoxam, metalaxyl, metalaxyl-M, ofurace, oxadixyl, oxolinic acid;   B2) a compound capable to inhibit the mitosis and cell division like benomyl, carbendazim, diethofencarb, ethaboxam, fuberidazole, pencycuron, thiabendazole, thiophanate-methyl, zoxamide;   B3) a compound capable to inhibit the respiration for example
           as CI-respiration inhibitor like diflumetorim;   as CII-respiration inhibitor like boscalid, carboxin, fenfuram, flutolanil, furametpyr, furmecyclox, mepronil, oxycarboxin, penthiopyrad, thifluzamide;   as CIII-respiration inhibitor like amisulbrom, azoxystrobin, cyazofamid, dimoxystrobin, enestrobin, famoxadone, fenamidone, fluoxastrobin, kresoxim-methyl, metominostrobin, orysastrobin, picoxystrobin, pyraclostrobin, trifloxystrobin;   
           B4) a compound capable of to act as an uncoupler like dinocap, fluazinam, meptyldinocap;   B5) a compound capable to inhibit ATP production like fentin acetate, fentin chloride, fentin hydroxide, silthiofam;   B6) a compound capable to inhibit AA and protein biosynthesis like andoprim, blasticidin-S, cyprodinil, kasugamycin, kasugamycin hydrochloride hydrate, mepanipyrim, pyrimethanil;   B7) a compound capable to inhibit the signal transduction like fenpiclonil, fludioxonil, quinoxyfen;   B8) a compound capable to inhibit lipid and membrane synthesis like biphenyl, chlozolinate, edifenphos, etridiazole, iodocarb, iprobenfos, iprodione, isoprothiolane, procymidone, propamocarb, propamocarb hydrochloride, pyrazophos, tolclofos-methyl, vinclozolin;   B9) a compound capable to inhibit ergosterol biosynthesis like aldimorph, azaconazole, bitertanol, bromuconazole, cyproconazole, diclobutrazole, difenoconazole, diniconazole, diniconazole-M, dodemorph, dodemorph acetate, epoxiconazole, etaconazole, fenarimol, fenbuconazole, fenhexamid, fenpropidin, fenpropimorph, fluquinconazole, flurprimidol, flusilazole, flutriafol, furconazole, furconazole-cis, hexaconazole, imazalil, imazalil sulfate, imibenconazole, ipconazole, metconazole, myclobutanil, naftifine, nuarimol, oxpoconazole, paclobutrazol, pefurazoate, penconazole, prochloraz, propiconazole, prothioconazole, pyributicarb, pyrifenox, simeconazole, spiroxamine, tebuconazole, terbinafine, tetraconazole, triadimefon, triadimenol, tridemorph, triflumizole, triforine, triticonazole, uniconazole, viniconazole, voriconazole;   B10) a compound capable to inhibit cell wall synthesis like benthiavalicarb, dimethomorph, flumorph, iprovalicarb, mandipropamid, polyoxins, polyoxorim, validamycin A;   B11) a compound capable to inhibit melanine biosynthesis like carpropamid, diclocymet, fenoxanil, phthalide, pyroquilon, tricyclazole;   B12) a compound capable to induce a host defence like acibenzolar-S-methyl, probenazole, tiadinil;   B13) a compound capable to have a multisite action like Bordeaux mixture, captafol, captan, chlorothalonil, copper naphthenate, copper oxide, copper oxychloride, copper preparations such as copper hydroxide, copper sulphate, dichlofluanid, dithianon, dodine, dodine free base, ferbam, fluorofolpet, folpet, guazatine, guazatine acetate, iminoctadine, iminoctadine albesilate, iminoctadine triacetate, mancopper, mancozeb, maneb, metiram, metiram zinc, oxine-copper, propineb, sulphur and sulphur preparations including calcium polysulphide, thiram, tolylfluanid, zineb, ziram;   B14) a compound selected in the following list: (2E)-2-(2-{[6-(3-chloro-2-methylphenoxy-5-fluoropyrimidin-4-yl]oxy}phenyl)-2-(methoxyimino)-N-methylacetamide, (2E)-2-{2-[({[(1E)-1-(3-{[(E)-1-fluoro-2-phenylvinyl]oxy}phenyl)ethylidene]amino}oxy)methyl]phenyl}-2-(methoxyimino)-N-methylacetamide, 1-(4-chlorophenyl)-2-(1H-1,2,4-triazol-1-yl)cycloheptanol, 1-[(4-methoxyphenoxy)methyl]-2,2-dimethylpropyl-1H-imidazole-1-carboxylate, 1-methyl-N-[2-(1,1,2,2-tetrafluoroethoxy)phenyl]-3-(trifluoromethyl)-1H-pyrazole-4-carboxamide, 2,3,5,6-tetrachloro-4-(methylsulfonyl)pyridine, 2-butoxy-6-iodo-3-propyl-4H-chromen-4-one, 2-chloro-N-(1,1,3-trimethyl-2,3-dihydro-1H-inden-4-yl)nicotinamide, 2-phenylphenol and salts, 3-(difluoromethyl)-1-methyl-N-[2-(1,1,2,2-tetrafluoroethoxy)phenyl]-1H-pyrazole-4-carboxamide, 3-(difluoromethyl)-N-[(9R)-9-isopropyl-1,2,3,4-tetrahydro-1,4-methanonaphthalen-5-yl]-1-methyl-1H-pyrazole-4-carboxamide, 3-(difluoromethyl)N-[(9S)-9-isopropyl-1,2,3,4-tetrahydro-1,4-methanonaphthalen-5-yl]-1-methyl-1H-pyrazole-4-carboxamide, 3-(difluoromethyl)-N-[4′-(3,3-dimethylbut-1-yn-1-yl)biphenyl-2-yl]-1-methyl-1H-pyrazole-4-carboxamide, 3,4,5-trichloropyridine-2,6-dicarbonitrile, 3-[5-(4-chlorophenyl)-2,3-dimethylisoxazolidin-3-yl]pyridine, 3-chloro-5-(4-chlorophenyl)-4-(2,6-difluorophenyl)-6-methylpyridazine, 4-(4-chlorophenyl-5-(2,6-difluorophenyl)-3,6-dimethylpyridazine, 5-chloro-7-(4-methylpiperidin-1-yl)-6-(2,4,6-trifluorophenyl)[1,2,4]triazolo[1,5-a]pyrimidine, 8-hydroxyquinoline sulfate, benthiazole, bethoxazin, capsimycin, carvone, chinomethionat, cufraneb, cyflufenamid, cymoxanil, dazomet, debacarb, dichlorophen, diclomezine, dicloran, difenzoquat, difenzoquat methylsulphate, diphenylamine, ecomate, ferimzone, flumetover, fluopicolide, fluoroimide, flusulfamide, fosetyl-aluminium, fosetyl-calcium, fosetyl-sodium, hexachlorobenzene, irumamycin, isotianil, methasulfocarb, methyl (2E) 2 -{2-[({cyclopropyl[(4-methoxyphenyl)imino]methyl}thio)methyl]phenyl}-3-methoxyacrylate, methyl 1-(2,2-dimethyl-2,3-dihydro-1H-inden-1-yl-1H-imidazole-5-carboxylate, methyl isothiocyanate, metrafenone, mildiomycin, N-(3′,4′-dichloro-5-fluorobiphenyl-2-yl)-3-(difluoromethyl)-1-methyl-1H-pyrazole-4-carboxamide, N-(3-ethyl-3,5,5-trimethylcyclohexyl)-3-(formylamino)-2-hydroxybenzamide, N-(4-chloro-2-nitrophenyl)-N-ethyl-4-methylbenzenesulfonamide, N-(4-chlorobenzyl)-3-[3-methoxy-4-(prop-2-yn-1-yloxy)phenyl]propanamide, N-[(4-chlorophenyl)(cyano)methyl]-3-[3-methoxy-4-(prop-2-yn-1-yloxy)phenyl]propanamide, N-[(5-bromo-3-chloropyridin-2-yl)methyl]-2,4-dichloronicotinamide, N-[1-(5-bromo-3-chloropyridin-2-yl)ethyl]-2,4-dichloronicotinamide, N-[1-(5-bromo-3-chloropyridin-2-yl)ethyl]-2-fluoro-4-iodonicotinamide, N-[2-(1,3-dimethylbutyl)phenyl]-5-fluoro-1,3-dimethyl-1H-pyrazole-4-carboxamide, N-{(Z)-[(cyclopropylmethoxy)imino][6-(difluoromethoxy)-2,3-difluorophenyl]methyl}-2-phenylacetamide, N-{2-[1,1′-bi(cyclopropyl)-2-yl]phenyl}-3-(difluoromethyl)-1-methyl-1H-pyrazole-4-carboxamide, N-{2-[3-chloro-5-(trifluoromethyl)pyridin-2-yl]ethyl}-2-(trifluoromethyl)benzamide, natamycin, N-ethyl-N-methyl-N′-{2-methyl-5-(trifluoromethyl)-4-[3-(trimethylsilyl)propoxy]phenyl}imidoformamide, N-ethyl-N-methyl-N′-{2-methyl-5-(difluoromethyl)-4-[3-(trimethylsilyl)propoxy]phenyl}imidoformamide, nickel dimethyldithiocarbamate, nitrothal-isopropyl, O-{1-[(4-methoxyphenoxy)methyl]-2,2-dimethylpropyl}1H-imidazole-1-carbothioate, octhilinone, oxamocarb, oxyfenthiin, pentachlorophenol and salts, phosphorous acid and its salts, piperalin, propamocarb fosetylate, propanosine-sodium, proquinazid, pyribencarb, pyrrolnitrine, quintozene, S-allyl-5-amino-2-isopropyl-4-(2-methylphenyl)-3-oxo-2,3-dihydro-1H-pyrazole-1-carbothioate, tecloftalam, tecnazene, triazoxide, trichlamide, valiphenal, zarilamid.       

     The composition according to the invention comprising a mixture of a compound of formula (I) or (Ia) to (Id) with a bactericide compound may also be particularly advantageous. Examples of suitable bactericide mixing partners may be selected in the following list: bronopol, dichlorophen, nitrapyrin, nickel dimethyldithiocarbamate, kasugamycin, octhilinone, furancarboxylic acid, oxytetracycline, probenazole, streptomycin, tecloftalam, copper sulphate and other copper preparations. 
     The compounds of formula (I) or (Ia) to (Id) and the fungicide composition according to the invention can be used to curatively or preventively control the phytopathogenic fungi of plants or crops. 
     Thus, according to a further aspect of the invention, there is provided a method for curatively or preventively controlling the phytopathogenic fungi of plants or crops characterised in that a compound of formula (I) or (Ia) to (Id) or a fungicide composition according to the invention is applied to the seed, the plant or to the fruit of the plant or to the soil wherein the plant is growing or wherein it is desired to grow. 
     The method of treatment according to the invention may also be useful to treat propagation material such as tubers or rhizomes, but also seeds, seedlings or seedlings pricking out and plants or plants pricking out. This method of treatment can also be useful to treat roots. The method of treatment according to the invention can also be useful to treat the overground parts of the plant such as trunks, stems or stalks, leaves, flowers and fruit of the concerned plant. 
     Among the plants that can be protected by the method according to the invention, mention may be made of cotton; flax; vine; fruit or vegetable crops such as  Rosaceae  sp. (for instance pip fruit such as apples and pears, but also stone fruit such as apricots, almonds and peaches),  Ribesioidae  sp.,  Juglandaceae  sp.,  Betulaceae  sp.,  Anacardiaceae  sp.,  Fagaceae  sp.,  Moraceae  sp.,  Oleaceae  sp., Actinidaceae sp.,  Lauraceae  sp.,  Musaceae  sp. (for instance banana trees and plantins),  Rubiaceae  sp.,  Theaceae  sp.,  Sterculiceae  sp.,  Rutaceae  sp. (for instance lemons, oranges and grapefruit);  Solanaceae  sp. (for instance tomatoes),  Liliaceae  sp.,  Asteraceae  sp. (for instance lettuces),  Umbelliferae  sp.,  Cruciferae  sp.,  Chenopodiaceae  sp.,  Cucurbitaceae  sp.,  Papilionaceae  sp. (for instance peas),  Rosaceae  sp. (for instance strawberries); major crops such as  Graminae  sp. (for instance maize, lawn or cereals such as wheat, rice, barley and triticale),  Asteraceae  sp. (for instance sunflower),  Cruciferae  sp. (for instance colza),  Fabacae  sp. (for instance peanuts),  Papilionaceae  sp. (for instance soybean),  Solanaceae  sp. (for instance potatoes),  Chenopodiaceae  sp. (for instance beetroots) horticultural and forest crops; as well as genetically modified homologues of these crops. 
     Among the diseases of plants or crops that can be controlled by the method according to the invention, mention may be made of:
         Powdery mildew diseases such as:     Blumeria  diseases, caused for example by  Blumeria graminis;        Podosphaera  diseases, caused for example by  Podosphaera leucotricha;        Sphaerotheca  diseases, caused for example by  Sphaerotheca fuliginea;        Uncinula  diseases, caused for example by  Uncinula necator;      Rust diseases such as:     Gymnosporangium  diseases, caused for example by  Gymnosporangium sabinae;        Hemileia  diseases, caused for example by  Hemileia vastatrix;        Phakopsora  diseases, caused for example by  Phakopsora pachyrhizi  or  Phakopsora meibomiae;        Puccinia  diseases, caused for example by  Puccinia recondita;        Uromyces  diseases, caused for example by  Uromyces appendiculatus;      Oomycete diseases such as:     Bremia  diseases, caused for example by  Bremia lactucae;        Peronospora  diseases, caused for example by  Peronospora pisi  or  P. brassicae        Phytophthora  diseases, caused for example by  Phytophthora infestans;        Plasmopara  diseases, caused for example by  Plasmopara viticola;        Pseudoperonospora  diseases, caused for example by  Pseudoperonospora humuli  or  Pseudoperonospora cubensis;        Pythium  diseases, caused for example by  Pythium ultimum;      Leafspot, leaf blotch and leaf blight diseases such as:     Alternaria  diseases, caused for example by  Alternaria solani;        Cercospora  diseases, caused for example by  Cercospora beticola;        Cladiosporum  diseases, caused for example by  Cladiosporium cucumerinum;        Cochliobolus  diseases, caused for example by  Cochliobolus sativus;        Colletotrichum  diseases, caused for example by  Colletotrichum lindemuthanium;        Cycloconium  diseases, caused for example by  Cycloconium oleaginum;        Diaporthe  diseases, caused for example by  Diaporthe citri;        Elsinoe  diseases, caused for example by  Elsinoe fawcettii;        Gloeosporium  diseases, caused for example by  Gloeosporium laeticolor;        Glomerella  diseases, caused for example by  Glomerella cingulata;        Guignardia  diseases, caused for example by  Guignardia bidwelli;        Leptosphaeria  diseases, caused for example by  Leptosphaeria maculans; Leptosphaeria nodorum;        Magnaporthe  diseases, caused for example by  Magnaporthe grisea;        Mycosphaerella  diseases, caused for example by  Mycosphaerella graminicola Mycosphaerella arachidicola; Mycosphaerella fijiensis;        Phaeosphaeria  diseases, caused for example by  Phaeosphaeria nodorum;        Pyrenophora  diseases, caused for example by  Pyrenophora teres;        Ramularia  diseases, caused for example by  Ramularia collo - cygni;        Rhynchosporium  diseases, caused for example by  Rhynchosporium secalis;        Septoria  diseases, caused for example by  Septoria apii  or  Septoria lycopercisi;        Typhula  diseases, caused for example by  Typhula incamata;        Venturia  diseases, caused for example by  Venturia inaequalis;      Root and stem diseases such as:     Corticium  diseases, caused for example by  Corticium graminearum;        Fusarium  diseases, caused for example by  Fusarium oxysporum;        Gaeumannomyces  diseases, caused for example by  Gaeumannomyces graminis;        Rhizoctonia  diseases, caused for example by  Rhizoctonia solani;        Tapesia  diseases, caused for example by  Tapesia acuformis;        Thielaviopsis  diseases, caused for example by  Thielaviopsis basicola;      Ear and panicle diseases such as:     Alternaria  diseases, caused for example by  Alternaria  spp.     Aspergillus  diseases, caused for example by  Aspergillus flavus;        Cladosporium  diseases, caused for example by  Cladosporium  spp.     Claviceps  diseases, caused for example by  Claviceps purpurea;        Fusarium  diseases, caused for example by  Fusarium culmorum;        Gibberella  diseases, caused for example by  Gibberella zeae;        Monographella  diseases, caused for example by  Monographella nivalis;      Smut and bunt diseases such as:     Sphacelotheca  diseases, caused for example by  Sphacelotheca reiliana;        Tilletia  diseases, caused for example by  Tilletia caries;        Urocystis  diseases, caused for example by  Urocystis occulta;        Ustilago  diseases, caused for example by  Ustilago nuda;      Fruit rot and mould diseases such as:     Aspergillus  diseases, caused for example by  Aspergillus flavus;        Botrytis  diseases, caused for example by  Botrytis cinerea;        Penicillium  diseases, caused for example by  Penicillium expansum;        Sclerotinia  diseases, caused for example by  Sclerotinia sclerotiorum;        Verticilium  diseases, caused for example by  Verticilium alboatrum;      Seed and soilborne decay, mould, wilt, rot and damping-off diseases such as:     Fusarium  diseases, caused for example by  Fusarium culmorum;        Phytophthora  diseases, caused for example by  Phytophthora cactorum;        Pythium  diseases, caused for example by  Pythium ultimum;        Rhizoctonia  diseases, caused for example by  Rhizoctonia solani;        Sclerotium  diseases, caused for example by  Sclerotium rolfsii;        Microdochium  diseases, caused for example by  Microdochium nivale;      Canker, broom and dieback diseases such as:     Nectria  diseases, caused for example by  Nectria galligena;      Blight diseases such as:     Monilinia  diseases, caused for example by  Monilinia laxa;      Leaf blister or leaf curl diseases such as:     Taphrina  diseases, caused for example by  Taphrina deformans;      Decline diseases of wooden plants such as:   Esca diseases, caused for example by  Phaemoniella clamydospora;        Eutypa  dyeback, caused for example by  Eutypa lata;      Dutch elm disease, caused for example by  Ceratocystsc ulmi;      Diseases of flowers and Seeds such as:     Botrytis  diseases, caused for example by  Botrytis cinerea;      Diseases of tubers such as:     Rhizoctonia  diseases, caused for example by  Rhizoctonia solani.          

     The fungicide composition according to the invention may also be used against fungal diseases liable to grow on or inside timber. The term “timber” means all types of species of wood, and all types of working of this wood intended for construction, for example solid wood, high-density wood, laminated wood, and plywood. The method for treating timber according to the invention mainly consists in contacting one or more compounds according to the invention, or a composition according to the invention; this includes for example direct application, spraying, dipping, injection or any other suitable means. 
     The dose of active compound usually applied in the method of treatment according to the invention is generally and advantageously from 10 to 800 g/ha, preferably from 50 to 300 g/ha for applications in foliar treatment. The dose of active substance applied is generally and advantageously from 2 to 200 g per 100 kg of seed, preferably from 3 to 150 g per 100 kg of seed in the case of seed treatment. 
     It is clearly understood that the doses indicated herein are given as illustrative examples of the method according to the invention. A person skilled in the art will know how to adapt the application doses, notably according to the nature of the plant or crop to be treated. 
     The fungicide composition according to the invention may also be used in the treatment of genetically modified organisms with the compounds according to the invention or the agrochemical compositions according to the invention. Genetically modified plants are plants into genome of which a heterologous gene encoding a protein of interest has been stably integrated. The expression “heterologous gene encoding a protein of interest” essentially means genes which give the transformed plant new agronomic properties, or genes for improving the agronomic quality of the modified plant. 
     The compounds or mixtures according to the invention may also be used for the preparation of composition useful to curatively or preventively treat human or animal fungal diseases such as, for example, mycoses, dermatoses,  trichophyton  diseases and candidiases or diseases caused by  Aspergillus  spp., for example  Aspergillus fumigatus.    
     The following tables I-III illustrate in a non-limiting manner examples of compounds according to the invention. 
     In the following compound examples, M+H indicates the mass versus charge (m/z value) of the monoprotonated molecular ion, as observed in mass spectroscopy by positive atmospheric-pressure chemical-ionisation (APCI+) or positive electrospray-ionisation (ES+). 
     In the following examples, the logP values were determined in accordance with EEC Directive 79/831 Annex V.A8 by HPLC (High Performance Liquid Chromatography) on a reversed-phase column (C 18), using the method described below: 
     Temperature: 40° C.; Mobile phases: 0.1% aqueous formic acid and acetonitrile; linear gradient from 10% acetonitrile to 90% acetonitrile. 
     Calibration was carried out using unbranched alkan-2-ones (comprising 3 to 16 carbon atoms) with known logP values (determination of the logP values by the retention times using linear interpolation between two successive alkanones). 
     The lambda max values were determined in the maxima of the chromatographic signals using the UV spectra from 190 nm to 400 nm. 
     
       
         
           
               
               
             
               
                 TABLE I 
               
             
            
               
                   
               
               
                   
                 (Ic) 
               
               
                 
                   
                     
                     
                         
                         
                     
                   
                 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 N o   
                 A 
                 L 1   
                 —L 2 —Q 
                 E 2   
                 LogP 
                 M + H 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 1 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.26 
                 454 
               
               
                   
               
               
                 2 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.27 
                 434 
               
               
                   
               
               
                 3 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.65 
                 448 
               
               
                   
               
               
                 4 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.26 
                 460 
               
               
                   
               
               
                 5 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3 
                 460 
               
               
                   
               
               
                 6 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.73 
                 424 
               
               
                   
               
               
                 7 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.3 
                 452 
               
               
                   
               
               
                 8 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.48 
                 466 
               
               
                   
               
               
                 9 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.45 
                 488 
               
               
                   
               
               
                 10 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.21 
                 474 
               
               
                   
               
               
                 11 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.77 
                 496 
               
               
                   
               
               
                 12 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.86 
                 426 
               
               
                   
               
               
                 13 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.59 
                 454 
               
               
                   
               
               
                 14 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.39 
                 350 
               
               
                   
               
               
                 15 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.61 
                 466 
               
               
                   
               
               
                 16 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.19 
                 464 
               
               
                   
               
               
                 17 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.66 
                 452 
               
               
                   
               
               
                 18 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.94 
               
               
                   
               
               
                 19 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.28 
                 316 
               
               
                   
               
               
                 20 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.32 
                 325 
               
               
                   
               
               
                 21 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.88 
                 441 
               
               
                   
               
               
                 22 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.99 
                 435 
               
               
                   
               
               
                 23 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.26 
                 477 
               
               
                   
               
               
                 24 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.86 
                 469 
               
               
                   
               
               
                 25 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.92 
                 447 
               
               
                   
               
               
                 26 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.32 
                 407 
               
               
                   
               
               
                 27 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.22 
                 405 
               
               
                   
               
               
                 28 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.65 
                 433 
               
               
                   
               
               
                 29 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.32 
                 432 
               
               
                   
               
               
                 30 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.25 
                 420 
               
               
                   
               
               
                 31 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.55 
                 392 
               
               
                   
               
               
                 32 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.9 
                 440 
               
               
                   
               
               
                 33 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.14 
                 454 
               
               
                   
               
               
                 34 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.67 
                 426 
               
               
                   
               
               
                 35 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.93 
                 426 
               
               
                   
               
               
                 36 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.39 
               
               
                   
               
               
                 37 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3 
                 400 
               
               
                   
               
               
                 38 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.01 
                 420 
               
               
                   
               
               
                 39 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.05 
                 418 
               
               
                   
               
               
                 40 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.51 
                 390 
               
               
                   
               
               
                 41 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.51 
                 462 
               
               
                   
               
               
                 42 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Et 
                 3.35 
                 420 
               
               
                   
               
               
                 43 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Et 
                 3.04 
                 406 
               
               
                   
               
               
                 44 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.46 
                 470 
               
               
                   
               
               
                 45 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.49 
                 468 
               
               
                   
               
               
                 46 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.24 
                 456 
               
               
                   
               
               
                 47 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.65 
                 485 
               
               
                   
               
               
                 48 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.28 
                 438 
               
               
                   
               
               
                 49 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.3 
                 424 
               
               
                   
               
               
                 50 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —(CH 2 ) 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.16 
                 336 
               
               
                   
               
               
                 51 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —(CH 2 ) 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.19 
                 420 
               
               
                   
               
               
                 52 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                   
                 398 
               
               
                   
               
               
                 53 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.24 
                 482 
               
               
                   
               
               
                 54 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.08 
                 516 
               
               
                   
               
               
                 55 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.7 
                 466 
               
               
                   
               
               
                 56 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.87 
                 468 
               
               
                   
               
               
                 57 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.58 
                 496 
               
               
                   
               
               
                 58 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.47 
                 320 
               
               
                   
               
               
                 59 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.95 
                 404 
               
               
                   
               
               
                 60 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.4 
                 466 
               
               
                   
               
               
                 61 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.15 
                 452 
               
               
                   
               
               
                 62 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.98 
                 416 
               
               
                   
               
               
                 63 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.96 
                 424 
               
               
                   
               
               
                 64 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.26 
                 418 
               
               
                   
               
               
                 65 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.92 
                 438 
               
               
                   
               
               
                 66 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.57 
                 390 
               
               
                   
               
               
                 67 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.12 
                 468 
               
               
                   
               
               
                 68 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.41 
                 388 
               
               
                   
               
               
                 69 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.42 
                 388 
               
               
                   
               
               
                 70 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.23 
                 436 
               
               
                   
               
               
                 71 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.37 
                 422 
               
               
                   
               
               
                 72 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1 
                 314 
               
               
                   
               
               
                 73 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.53 
                 416 
               
               
                   
               
               
                 74 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.04 
                 428 
               
               
                   
               
               
                 75 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.78 
                 462 
               
               
                   
               
               
                 76 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.86 
                 432 
               
               
                   
               
               
                 77 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.03 
                 500 
               
               
                   
               
               
                 78 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 5.94 
                 572 
               
               
                   
               
               
                 79 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.18 
                 502 
               
               
                   
               
               
                 80 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.88 
                 530 
               
               
                   
               
               
                 81 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.83 
                 450 
               
               
                   
               
               
                 82 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.11 
                 520 
               
               
                   
               
               
                 83 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 5.85 
                 590 
               
               
                   
               
               
                 84 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.83 
                 518 
               
               
                   
               
               
                 85 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.78 
                 548 
               
               
                   
               
               
                 86 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.07 
                 402 
               
               
                   
               
               
                 87 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.74 
                 486 
               
               
                   
               
               
                 88 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.04 
                 547 
               
               
                   
               
               
                 89 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.76 
                 533 
               
               
                   
               
               
                 90 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.66 
                 497 
               
               
                   
               
               
                 91 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.61 
                 505 
               
               
                   
               
               
                 92 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.92 
                 499 
               
               
                   
               
               
                 93 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.53 
                 519 
               
               
                   
               
               
                 94 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.22 
                 471 
               
               
                   
               
               
                 95 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.76 
                 549 
               
               
                   
               
               
                 96 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.04 
                 469 
               
               
                   
               
               
                 97 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.08 
                 469 
               
               
                   
               
               
                 98 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.94 
                 518 
               
               
                   
               
               
                 99 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.1 
                 502 
               
               
                   
               
               
                 100 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.02 
                 356 
               
               
                   
               
               
                 101 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3 
                 424 
               
               
                   
               
               
                 102 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.73 
                 440 
               
               
                   
               
               
                 103 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.62 
               
               
                   
               
               
                 104 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.64 
                 503 
               
               
                   
               
               
                 105 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.32 
                 489 
               
               
                   
               
               
                 106 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.12 
                 454 
               
               
                   
               
               
                 107 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.12 
               
               
                   
               
               
                 108 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.85 
                 488 
               
               
                   
               
               
                 109 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.93 
                 490 
               
               
                   
               
               
                 110 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.24 
                 504 
               
               
                   
               
               
                 111 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.88 
                 472 
               
               
                   
               
               
                 112 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.05 
                 458 
               
               
                   
               
               
                 113 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.8 
                 336 
               
               
                   
               
               
                 114 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.88 
                 406 
               
               
                   
               
               
                 115 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.42 
                 420 
               
               
                   
               
               
                 116 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.35 
                 454 
               
               
                   
               
               
                 117 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.17 
                 469 
               
               
                   
               
               
                 118 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.33 
                 483 
               
               
                   
               
               
                 119 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.84 
                 404 
               
               
                   
               
               
                 120 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.76 
                 434 
               
               
                   
               
               
                 121 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.81 
                 482 
               
               
                   
               
               
                 122 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.54 
                 468 
               
               
                   
               
               
                 123 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.88 
                 484 
               
               
                   
               
               
                 124 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.51 
                 330 
               
               
                   
               
               
                 125 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.02 
                 478 
               
               
                   
               
               
                 126 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.34 
                 444 
               
               
                   
               
               
                 127 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.79 
                 428 
               
               
                   
               
               
                 128 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.06 
                 477 
               
               
                   
               
               
                 129 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.6 
                 452 
               
               
                   
               
               
                 130 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.76 
                 438 
               
               
                   
               
               
                 131 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.13 
                 382 
               
               
                   
               
               
                 132 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.28 
                 542 
               
               
                   
               
               
                 133 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.8 
                 480 
               
               
                   
               
               
                 134 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.27 
                 452 
               
               
                   
               
               
                 135 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 5.01 
                 522 
               
               
                   
               
               
                 136 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.39 
                 486 
               
               
                   
               
               
                 137 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.17 
                 450 
               
               
                   
               
               
                 138 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.14 
                 450 
               
               
                   
               
               
                 139 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.58 
                 500 
               
               
                   
               
               
                 140 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.05 
                 528 
               
               
                   
               
               
                 141 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.32 
                 498 
               
               
                   
               
               
                 142 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.03 
                 466 
               
               
                   
               
               
                 143 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.29 
                 496 
               
               
                   
               
            
           
         
       
     
     
       
         
           
               
               
             
               
                 TABLE II 
               
             
            
               
                   
               
               
                   
                 (Id) 
               
               
                 
                   
                     
                     
                         
                         
                     
                   
                 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 N o   
                 A 
                 L 1   
                 —L 2 —Q 
                 E 2   
                 LogP 
                 M + H 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 144 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.6 
                 398 
               
               
                   
               
               
                 145 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.88 
                 466 
               
               
                   
               
               
                 146 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.87 
                 496 
               
               
                   
               
               
                 147 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.18 
                 468 
               
               
                   
               
               
                 148 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.52 
                 482 
               
               
                   
               
               
                 149 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.02 
                 356 
               
               
                   
               
               
                 150 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.29 
                 516 
               
               
                   
               
            
           
         
       
     
     
       
         
           
               
               
             
               
                 TABLE III 
               
             
            
               
                   
               
               
                   
                 (Ia) 
               
               
                 
                   
                     
                     
                         
                         
                     
                   
                 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 N o   
                 A 
                 L 1   
                 —L 2 —Q 
                 E 1   
                 LogP 
                 M + H 
               
               
                   
               
            
           
           
               
               
               
               
               
               
               
            
               
                 151 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.17 
                 322 
               
               
                   
               
               
                 152 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.17 
                 406 
               
               
                   
               
               
                 153 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.39 
                 456 
               
               
                   
               
               
                 154 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 2.39 
                 438 
               
               
                   
               
               
                 155 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —(CH 2 ) 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                   
                 304 
               
               
                   
               
               
                 156 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —(CH 2 ) 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                   
                 321 
               
               
                   
               
               
                 157 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                   
                 317 
               
               
                   
               
               
                 158 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.42 
                 356 
               
               
                   
               
               
                 159 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.72 
                 470 
               
               
                   
               
               
                 160 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.37 
                 454 
               
               
                   
               
               
                 161 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.62 
                 490 
               
               
                   
               
               
                 162 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.25 
                 460 
               
               
                   
               
               
                 163 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.19 
                 474 
               
               
                   
               
               
                 164 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.81 
                 399 
               
               
                   
               
               
                 165 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.85 
                 533 
               
               
                   
               
               
                 166 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.06 
                 547 
               
               
                   
               
               
                 167 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.29 
                 513 
               
               
                   
               
               
                 168 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.85 
                 467 
               
               
                   
               
               
                 169 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.62 
                 503 
               
               
                   
               
               
                 170 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.62 
                 483 
               
               
                   
               
               
                 171 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.94 
                 497 
               
               
                   
               
               
                 172 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.58 
                 517 
               
               
                   
               
               
                 173 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.46 
                 523 
               
               
                   
               
               
                 174 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 1.57 
                 393 
               
               
                   
               
               
                 175 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.72 
                 511 
               
               
                   
               
               
                 176 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 3.7 
                 477 
               
               
                   
               
               
                 177 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.56 
                 507 
               
               
                   
               
               
                 178 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                 4.06 
                 491 
               
               
                   
               
               
                 179 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 —CH 2 — 
                 
                   
                     
                     
                         
                         
                     
                   
                 
                 Me 
                   
                 497 
               
               
                   
               
            
           
         
       
     
     The following examples illustrate in a non-limiting manner the preparation of the compounds of formula (I) according to the invention. 
     5-Methyl-1-(3-thiophenecarbohydroximoyl)-tetrazole and 5-methyl-2-(3-thiophenecarbohydroximoyl)-tetrazole 
     
       
         
         
             
             
         
       
     
     To a solution of 3-thiophene carboxaldehyde oxime (8 g, 62.9 mmol) in DMF (80 ml) is added N-chlorosuccinimide (8.8 g, 66 mmol) portionwise, while maintaining the reaction temperature below 45° C. On complete addition, the mixture is stirred one hour at room temperature before being poured into a saturated aqueous NH 4 Cl solution. The mixture is extracted with ethyl acetate. The organic layer is washed successively with water and brine, dried (MgSO 4 ), filtered and concentrated. The residue and 5-methyltetrazole (5.3 g, 62.9 mmol) are diluted in dichloromethane (80 ml) and treithylamine (11.4 ml, 82.1 mmol) is added dropwise at room temperature. After stirring overnight, a saturated aqueous NH 4 Cl solution is added. The aqueous layer is extracted with ethyl acetate. The combined organic layers are washed successively with water and brine, dried (MgSO 4 ), filtered and concentrated. Silica-gel chromatography of the residue affords 5.5 g of 5-methyl-1-(3-thiophenecarbohydroximoyl)-tetrazole [yield 37.6%;  1 H-NMR (DMSO-d6) δ ppm : 2.48 (s, 3H), 7.42 (d, 1H), 7.51 (d, 1H), 7.74 (dd, 1H), 12.7 (s, 1H)] and 2 g 5-methyl-2-(3-thiophenecarbohydroximoyl)-tetrazole [yield 13.7%;  1 H-NMR (DMSO-d6) δ ppm : 2.62 (s, 3H), 7.40 (m, 2H), 7.73 (dd, 1H), 12.6 (s, 1H)]. 
     O-(2-Amino-1,3-thiazol-4-yl)methyl-(thien-3-yl)-(5-methyltetrazol-1-yl)methanone oxime (compound 20) 
     
       
         
         
             
             
         
       
     
     To a cooled solution (0-5° C.) of 5-methyl-1-(3-thiophenecarbohydroximoyl)tetrazole (18.7 g, 89.4 mmol) in acetonitrile (100 ml) is added DBN (22.4 ml, 187.7 mmol). On complete addition, the mixture is stirred five minutes and 4-chloromethyl-2-amino-1,3-thiazole hydrochloride (18.2 g, 98.3 mmol) is added portionwise. On complete addition, the mixture is stirred five minutes before the removal of the cooling bath. After stirring overnight, the solvent is evaporated. Silica-gel chromatography of the residue affords 18.4 g of compound 20 [yield 60.8%; HPLC/MS: m/z=325 (M+H); LogP=1.32]. 
     O-(2-tert-Butylcarbonylamino-1,3-thiazol-4-yl)methyl-(thien-3-yl)-(5-methyltetrazol-1-yl)methanone oxime (compound 18) 
     
       
         
         
             
             
         
       
     
     To a cooled solution (0-5° C.) of compound 20 (8 g, 24.9 mmol) in dry dichloromethane (250 ml) are added triethylamine (3.6 ml, 26.1 mmol) and a catalytic quantity of DMAP, then pivaloyl chloride (3.2 ml, 26.1 mmol) is added dropwise. On complete addition, the mixture is stirred ten minutes before the removal of the cooling bath. After stirring overnight, water is added. After separation, the organic layer is dried (MgSO 4 ), filtered and concentrated to give an off-white solid. Trituration with methanol, filtration, washing with methanol and drying affords 3.2 g of compound 18 [yield 60.5%; HPLC/MS: m/z=406 (M+H); LogP=2.94]. 
     (2-Phenyl-1,3-thiazol-4-yl)-(1-methyltetrazol-5-yl)methanone 
     
       
         
         
             
             
         
       
     
     To a solution of 1-methyltetrazole (2 g, 23.8 mmol) and TMEDA (10 ml, 66.2 mmol) in THF (100 ml) cooled at −78° C. is added dropwise 2.5 M nBuLi in hexanes (9.5 ml, 23.8 mmol) with vigorous stirring and maintaining the reaction temperature below −65° C. On complete addition, the mixture is stirred 20 minutes before adding dropwise a solution of N-methyl-N-methoxy-2-phenyl-1,3-thiazol-4-yl)carboxamide (5.9 g, 23.8 mmol) in THF. On complete addition, the mixture is stirred for six hours at −78° C. before adding slowly a solution of 1N HCl in water (100 ml). When the reaction mixture reaches room temperature, water is added (500 ml) and the reaction mixture is neutralised with a saturated aqueous NaHCO 3  solution and extracted with ethyl acetate (500 ml). After separation, the organic layer is dried (MgSO 4 ), filtered and concentrated. Silica-gel chromatography of the residue affords 4.7 g of (2-phenyl-1,3-thiazol-4-yl)-1-methyltetrazol-5-yl)methanone [yield 72.8%;  1 H-NMR (CDCl 3 ) δ ppm : 4.48 (s, 3H), 7.5 (m, 3H), 8.08 (m, 2H), 9.44 (s, 1H)]. 
     1-Methyl-5-[(2-phenyl-1,3-thiazol-4-yl)carbohydroximoyl]tetrazole 
     
       
         
         
             
             
         
       
     
     A solution of 1-methyl-5-[(2-phenyl-1,3-thiazol-4-yl)carbohydroximoyl]tetrazole (5.1 g, 18.8 mmol) and hydroxylamine hydrochloride (3.3 g, 47 mmol) in pyridine (60 ml) is stirred three hours at 50° C. and overnight at room temperature. The solvent is evaporated and water is added to the crude mixture. The resulting suspension is filtered. The solid is washed with water and dried to give 5 g of 1-methyl-5-[(2-phenyl-1,3-thiazol-4-yl)carbohydroximoyl]tetrazole [yield 92.9%;  1 H-NMR (DMSO-d6) δ ppm : 4.08 (s, 3H), 7.5 (m, 3H), 7.9 (m, 2H), 8.02 (s, 1H), 12.9 (s, 1H)]. 
     O-(2-Phtalimidopyridin-6-yl)methyl-(2-phenyl-1,3-thiazol-4-yl)-(1-methyitetrazol-5-yl)methanone oxime (compound 173) 
     
       
         
         
             
             
         
       
     
     To a cooled solution (0-5° C.) of 1-methyl-5-[(2-phenyl-1,3-thiazol-4-yl)carbohydroximoyl]tetrazole (2.5 g, 8.7 mmol) in acetonitrile (10 ml) is added DBN (2.2 ml, 18.3 mmol). On complete addition, the mixture is stirred five minutes and 6-bromomethyl-2-phtalimidopyridine (3.05 g, 9.6 mmol) is added portionwise. On complete addition, the mixture is stirred five minutes before the removal of the cooling bath. After stirring overnight, water is added and the reaction mixture is extracted with ethyl acetate. The organic layer is dried (MgSO 4 ), filtered and concentrated. Silica-gel chromatography of the residue affords 2.1 g of compound 173 [yield 41.4%; HPLC/MS: m/z=523 (M+H); LogP=3.46]. 
     O-(2-Aminopyridin-6-yl)methyl-(2-phenyl-1,3-thiazol-4-yl)-(1-methyltetrazol-5-yl)methanone oxime (compound 174) 
     
       
         
         
             
             
         
       
     
     To a solution of compound 173 (1.8 g, 3.1 mmol) in THF (45 ml) is added hydrazine hydrate (0.75 ml, 15.5 mmol). After stirring overnight, the reaction mixture is filtered and concentrated. Silica-gel chromatography of the residue affords 1 g of compound 174 [yield 82.2%; HPLC/MS m/z=393 (M+H); LogP=1.57]. 
     O-(2-Pentylcarbonylaminopyridin-6-yl)methyl-(2-phenyl-1,3-thiazol-4-yl)-(1-methyitetrazol-5-yl)methanone oxime (compound 178) 
     
       
         
         
             
             
         
       
     
     To a solution of compound 174 (0.15 g, 0.38 mmol) in dry dichloromethane (5 ml) are added resin PS-BEMP 2.2 mmol/g (0.34 g) and hexanoyl chloride (77 mg, 0.57 mmol). After stirring overnight, the reaction mixture is filtered and concentrated. Silica-gel chromatography of the residue affords 0.16 g of compound 178 [yield 61.8%; HPLC/MS: m/z=491 (M+H); LogP=4.06]. 
     The following examples illustrate in a non-limiting manner the biological activity of the compounds of formula (I) according to the invention. 
    
    
     EXAMPLE A 
     In Vivo Test on  Peronospora parasitica  (Crucifer Downy Mildew) 
     Cabbage plants (Eminence variety) in starter cups, sown on a 50/50 peat soil-pozzolana substrate and grown at 18-20° C., are treated at the cotyledon stage by spraying with the aqueous suspension described above. Plants, used as controls, are treated with an aqueous solution not containing the active material. After 24 hours, the plants are contaminated by spraying them with an aqueous suspension of  Peronospora parasitica  spores (50 000 spores per ml). The spores are collected from infected plant. The contaminated cabbage plants are incubated for 5 days at 20° C., under a humid atmosphere. Grading is carried out 5 days after the contamination, in comparison with the control plants. 
     Under these conditions, good protection (at least 70%) is observed at a dose of 500 ppm with the following compounds: 1, 2, 3, 5, 13, 16, 17, 18, 19, 20, 22, 23, 24, 25, 26, 27, 28, 30, 31, 32, 33, 34, 36, 37, 38, 39, 42, 43, 44, 46, 48, 49, 50, 51, 62, 63, 64, 65, 66, 67, 68, 69, 72, 73, 74, 75, 88, 90, 92, 93, 95, 96, 97, 98, 101, 106, 107, 110, 111, 112, 114, 115, 116, 118, 119, 120, 123, 124, 125, 126, 127, 128, 129, 130, 151, 152, 153 and 154. 
     EXAMPLE B 
     In Vivo Test on  Phytophthora infestans  (Tomato Late Blight) 
     Tomato plants (Marmande variety) sown in started cups on a 50/50 peat soil-pozzolana subtrate and grown at 20-25° C., are treated at stage Z16 by spraying with the aqueous suspension described above. Plants, used as controls, are treated with an aqueous solution not containing the active material. After 24 hours, the plants are contaminated by spraying them with an aqueous suspension of  Phytophthora infestans  spores (20 000 spores per ml). The spores are collected from infected plants. The contaminated tomato plants are incubated for 5 days at 20° C., under a humid atmosphere. Grading is carried out 5 days after the contamination, in comparison with the control plants. 
     Under these conditions, good protection (at least 70%) is observed at a dose of 500 ppm with the following compounds: 3, 18, 19, 22, 24, 36, 38, 95, 101, 124, 126, 127 and 152. 
     EXAMPLE C 
     In Vivo Test on  Plasmopara viticola  (Vine Downy Mildew) 
     Vine plants (Cabernet variety) grown on a 50/50 peat soil-pozzolana subtrate at 20-22° C., are treated at stage Z15 by spraying with the aqueous suspension described above. Plants, used as controls, are treated with an aqueous solution not containing the active material. After 24 hours, the plants are contaminated by spraying the lower surface of the leaves with an aqueous suspension of  Plasmopara viticola  spores (100 000 spores per ml). The spores are collected from infected plants. The contaminated vine plants are incubated for 7 to 8 days at 20° C., under humid atmosphere. Grading is carried out 7 to 8 days after the contamination, in comparison with the control plants. 
     Under these conditions, good protection (at least 70%) is observed at a dose of 500 ppm with the following compounds: 16, 18, 19, 22, 24, 28, 42, 43, 67, 88, 90, 92, 95, 96, 97, 101, 106, 110, 116, 119, 124, 125, 126, 127, 128 and 152. 
     EXAMPLE D 
     Cell Test on  Pythium ultimum  (Damping-Off) 
     The growth of  Pythium ultimum  is performed in PDB medium at 20° C. during 7 days. The PDB medium is prepared by mixing 24 grams of PDB (Difco) in 1 liter of demineralized water. The medium is sterilized by autoclave 15 minutes at 121° C. After 7 days of growth, the mycelium of  Pythium ultimum  is ground and is used as inoculum. The compounds are solubilized in DMSO and added to sterile liquid glucose/mycopeptone medium (14.6 g/l of D-glucose, 7.1 g/l of mycological peptone (Oxoid) and 1.4 g/l of yeast extract (Merck)) at a concentration of 2 ppm. The medium is inoculated with the ground mycelium at an initial OD at 620 nm of 0.025. The efficacy of the compounds is assessed by OD measurement at 620 nm after 5 days at 20° C. in comparison with a control. 
     Under these conditions, good protection (at least 70%) is observed at a dose of 6 ppm with the following compounds: 1, 2, 3, 4, 6, 7, 8, 9, 10, 11, 12, 13, 14, 16, 17, 18, 19, 21, 22, 23, 24, 25, 26, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 44, 45, 46, 47, 48, 59, 60, 63, 64, 65, 67, 68, 74, 75, 86, 87, 88, 90, 91, 92, 93, 94, 95, 96, 97, 98, 100, 101, 102, 103, 104, 106, 107, 108, 110, 111, 113, 114, 115, 116, 117, 118, 119, 120, 121, 122, 123, 124, 125, 126, 127, 129, 134, 138, 151, 152, 153, 154, 160, 166, 170, 175, 177 and 178.