Abstract:
A source of intense coherent high-frequency electromagnetic radiation such as soft x-rays. A circularly polarized incident beam of coherent radiation is directed at a frequency multiplication medium that includes constituents of approximate C n  symmetry, oriented so that the symmetry axes of the constituents are parallel to the incident beam. The interaction of the incident beam and the constituents of the medium produces higher harmonics of the incident frequency, up into the x-ray band. If the C n  symmetry of the medium constituents is exact then the harmonic frequencies are multiples ln±l of the frequency of the incident beam, where l is an integer. If the C n  symmetry is only approximate, then the harmonics are centered around these multiples. Suitable medium constituents include dipolar molecules of C 5v  symmetry and circular rings of nanoparticles.

Description:
FIELD AND BACKGROUND OF THE INVENTION 
     The present invention relates to the production of high frequency coherent electromagnetic radiation such as soft x-rays and, more particularly, to a device and method for producing this radiation in limited frequency bands by frequency multiplication. 
     The development of masers and lasers circa 1960 stimulated speculation about applications of similar sources of coherent electromagnetic radiation that could operate at much shorter wavelengths, for example, at soft x-ray wavelengths, between about 1 nm and about 10 nm. Such applications include holographic imaging of biological structures, plasma diagnostics and the generation of intense plasmas. More recent advances in other fields have suggested other applications of coherent soft x-rays. For example, a coherent source of x-rays for CT scanning could be operated at a much lower power level tan the incoherent sources now in use, reducing the exposure of the subjects to ionizing radiation. Another application is in the fabrication of microdevices The design rule of devices such as integrated circuits is now limited by a lower bound of about 0.1 microns by several factors, not least of which is that the shortest wavelength radiation that can be used for photolithography is ultraviolet radiation. A coherent source of soft x-rays would help make even shorter design rules feasible. Similarly, a coherent source of soft x-rays would enable much denser storage of information in media such as compact disks. A sufficiently intense coherent beam of soft x-rays can be used as a weapon, or as an industrial cutting tool. 
     It is known to produce coherent soft x-rays using soft x-ray lasers. The first soft x-ray laser was developed at Lawrence Livermore National Laboratory in 1984. This device, which was described in general terms by Dennis Matthews and Mordecai Rosen in the December 1988 issue of  Scientific American , uses the Nova laser both to create a plasma including high-Z ions and to create a population inversion among those ions by a process known as collisional excitation. The laser medium in such a device is inherently transient. Essentially, the mere process of creating the laser medium, by evaporating a metal foil to produce a plasma. also destroys the laser medium. The use of the Nova laser, originally developed for controlled fusion research, to create the laser medium also meant that the device was a large, expensive research tool unsuitable for practical applications. More compact soft x-ray lasers have been developed in recent years, but like their giant ancestor at LLNL, they all rely on inherently self-destructive mechanisms to create a population inversion in a highly ionized plasma. 
     Two non-self-destructive strategies for the generation of coherent soft x-rays also have been explored. One is the imposition of spatial periodicity on the trajectories of high energy electrons, in free-electron lasers. This requires the use of a massive high-energy accelerator to create the high energy electrons. The other is the use of frequency multiplication media to create higher harmonics of coherent light, such as ultraviolet light, produced by a conventional laser. This generally produces a broad mixture of wavelengths. For example, N. Sarukura et al. reported in  Phys. Rev. A  Vol 43 p. 1669 (1991) the creation of 9-th to 23-rd order harmonics of light from a KrF laser using helium as a frequency multiplication medium. A review of the technique may be found in A. L&#39;Huiller et al., “High-order harmonics: a coherent source in the XUV range”,  Journal of Nonlinear Optical Physics and Materials , July 1995, Vol. 4 No. 3, pp. 647-665, which is incorporated by reference for all purposes as if fully set forth herein. More recently, Preston et al. ( Phys. Rev. A  Vol. 53 p. R31 (1996)) reported obtaining harmonics up to the 35-th using helium as a frequency multiplication medium. 
     There is thus a widely recognized need for, and it would be highly advantageous to have, a compact, portable, reusable source of coherent, relatively monochromatic soft x-rays. 
     SUMMARY OF THE INVENTION 
     According to the present invention there is provided a device for producing high frequency radiation, including: (a) a source of elliptically polarized radiation; and (b) a frequency multiplication medium including at least one constituent having approximate finite symmetry including an axis of approximate C n  symmetry, wherein n is at least 3, and wherein the at least one constituent is oriented so that the elliptically polarized radiation includes an electrical field that is circularly polarized in a plane perpendicular to the axis. 
     According to the present invention there is provided a method of producing high frequency radiation, including the steps of: (a) providing a frequency multiplication medium including at least one constituent having approximate finite symmetry including an axis of approximate C n  symmetry, wherein n is at least 3; and (b) directing elliptically polarized radiation at an angle to the axis such that the elliptically polarized radiation has an electric field that is circularly polarized in a plane perpendicular to the axis. 
     According to the present invention there is provided a device for producing high frequency radiation, including: (a) a source of elliptically polarized radiation; and (b) a frequency multiplication medium including a multiplicity of constituents sharing a common approximate shape and a common orientation aligned so that the elliptically polarized radiation has an electrical field that is circularly polarized in a plane perpendicular to the common orientation, each of the constituents having a longest dimension of at least about 6 Å. 
     According to the present invention there is provided a method of producing high frequency radiation, including the steps of: (a) providing a frequency multiplication medium including a plurality of constituents sharing a common approximate shape and a common orientation, each of the constituents having a longest dimension of at least about 6 Å; and (b) directing elliptically polarized radiation at an angle to the common orientation such that the elliptically polarized radiation has an electric field that is circularly polarized in a plane perpendicular to the common orientation. 
     An object is said to have an axis of C n  symmetry if the object is invariant under rotations by integral multiples of 2 π/n about this axis. The full point group of the object can be of higher symmetry than C n , for example D n , as long as the object has a C n  axis of symmetry. It is demonstrated in the Appendix that a circularly polarized beam of coherent electromagnetic radiation, incident on a medium whose constituents have commonly oriented C n  symmetry axes, causes the generation and amplification of specific harmonics of the incident beam. If the angular frequency of the incident beam is ω, then the harmonics produced are circularly polarized beams, parallel to the incident beam, of angular frequencies (ln±1)ω, where l is an integer, with the “+” beams circularly polarized in the same direction as the incident beam and the “−” beams circularly polarized in the opposite direction. So, for example, a circularly polarized beam of a wavelength of 500 nm incident on a medium whose constituents have C 5  symmetry axes generates, among others, circularly polarized l=20 harmonics with wavelengths of 5.05 nm (99th harmonic) and 4.95 nm (101st harmonic), in the middle of the soft x-ray band. It should be noted that the scope of the present invention is restricted to the case of n≧3, as the case of n=2 reproduces the selection rules of the prior art. In addition, the incident electromagnetic radiation may be elliptically polarized, rather than circularly polarized, as long as the electric field of the incident electromagnetic radiation is circularly polarized in the plane perpendicular to the symmetry axes. 
     It also is demonstrated in the Appendix that the amplification efficiency of medium grows dramatically with system size, even if the C n  symmetry is not perfect. If the constituents of the medium are large (on an atomic scale) ring-like structures, then the medium produces a range of angular frequencies centered around the frequencies determined by the (ln≧1)ω selection rules, at much higher intensities than are attainable by the prior art methods. In addition, under conditions of only approximate C n  symmetry, the radiation produced is not exactly circularly polarized. 
     It is important to note that to the extent that the present invention relies on the approximate symmetry of the constituents of the frequency multiplication medium, that symmetry is finite. In other words, the constituents which are brought under the scope of the present invention by virtue of having approximate C n  symmetry axes do not have infinite order (e.g., C∞) symmetry axes. In fact, a frequency multiplication medium made of constituents with parallel C∞ symmetry axes would not function within the scope of the present invention, because the photons of the “higher harmonics” that would be generated would have to have infinite frequency, and therefore infinite energy. Thus, the helium atoms of the prior art frequency multiplication media do not fall within the scope of the present invention because they are spherically symmetrical, and have an infinite number of C∞ axes, along with an infinite number of C n  axes for all finite n. Indeed, the mechanism by which helium atoms function as elements of a frequency multiplication medium is totally different from the mechanism described in the Appendix. 
     Several types of media may be used for such frequency multiplication of circularly polarized light from sources based on conventional lasers. One such medium consists of a gas of dipolar molecules of C nv  symmetry, which have C n  symmetry axes in the direction of the dipole moments. The molecules are oriented by an externally applied electric field so that all their C n  axes are parallel. Another such medium consists of circular rings of metallic nanoparticles oriented with their approximate C n  axes parallel, for example by having been deposited on a planar substrate. The incident beam is perpendicular to the plane of the substrate. A third such medium consists of parallel carbon nanotubes, which have parallel, exact or approximate C n  symmetry axes, with n typically between 6 and 9. In all three cases, the incident beam is parallel to the exact or approximate C n  axes. 
     As used herein, the term “constituent” refers to a medium component that, individually, includes the desired exact or approximate C 5  axis. For example, the constituents of the C 5 H 5 Tl gas that have the desired (exact ) C 5  axes are the C 5 H 5 Tl molecules themselves; and the constituents of the array of nanoparticle rings that have the desired (approximate) C n  axes are the nanoparticle rings themselves. 
    
    
     BRIEF DESCRIPTION OF THE DRAWINGS 
     The invention is herein described, by way of example only, with reference to the accompanying drawings, wherein: 
     FIG. 1 illustrates a molecule of C 5 H 5 Tl and its C 5  symmetry axis; 
     FIG. 2 is a schematic diagram of a device of the present invention based on C 5 H 5 Tl gas as a frequency multiplication medium; 
     FIG. 3 is a schematic illustration of a device of the present invention based on nanoparticle rings as a frequency multiplication medium 
     FIG. 4 illustrates an ( 8 , 0 ) carbon nanotube 
     FIG. 5 is a schematic illustration of a device of the present invention based on nanotubes as a frequency multiplication medium. 
    
    
     DESCRIPTION OF THE PREFERRED EMBODIMENTS 
     The present invention is of a device and method for the production and frequency multiplication of coherent circularly polarized light. Specifically, the present invention can be used to produce intense, coherent, relatively monochromatic soft x-rays. 
     The principles and operation of the production of high frequency radiation according to the present invention may be better understood with reference to the drawings and the accompanying description. 
     Referring now to the drawings, FIG. 1 illustrates a molecule of a compound useful as a frequency multiplication medium of the present invention: cyclopentadienyl thallium (C 5 H 5 Tl) This molecule, which consists of a conjugated C 5 H 5  ring  10  and a thallium atom  12 , exhibits C 5v  symmetry, and so has a C 5  symmetry axis. This molecule also has a dipole moment along its C 5  symmetry axis  14 , with the thallium end being positive and the conjugated ring end being negative. C 5 H 5 Tl may be purchased from Aldrich Chemical Co. of Milwaukee Wis. 
     FIG. 2 is a schematic diagram of a device of the present invention based on C 5 H 5 Tl as a frequency multiplication medium. Two parallel, electrically conducting plates  20  and  22  define between them a gap  24  filled with gas-phase C 5 H 5 Tl  26 . A source  32  of DC voltage imposes an electric field  38  on gap  24  that is perpendicular to plates  20  and  22 . Electric field  38  orients the molecules of C 5 H 5 Tl  26  so that the C 5  symmetry axes thereof are perpendicular to plates  20  and  22 . A laser-based device  34  directs a beam  36  of coherent, circularly polarized light through gap  24  via aperture  28  in plate  20  and aperture  30  in plate  22 . Beam  36  is parallel to the C 5  symmetry axes of the molecules of C 5 H 5 Tl  26 . The interaction of beam  36  with oriented C 5 H 5 Tl  26  produces higher harmonics of beam  36 . These higher harmonics emerge from aperture  28  along with beam  36 . Suitable laser-based devices  34  are described in the review article by L&#39;Huiller et al. It also is well-known in the art how to-transform linearly polarized coherent light, such as is emitted by a laser, into circularly polarized coherent light, using beam splitters and quarter wave plates. Suitable quarter wave plates are available inter alia from Spindler &amp; Hoyer GMBH &amp; Co., Göttingen, Germany. 
     The harmonics generated by the device of FIG. 2 are the 4th, 6th, 9th, 11th, etc. harmonics of beam  36 . These harmonics thus are more restricted in frequency content, and also more intense, than the consistently odd harmonics that would be produced by the prior art methods, but they are not in any way monochromatic. Monochromaticity may be approached more closely by using a frequency multiplication medium whose components have a higher degree of rotational symmetry, for example, circular rings of nanoparticles. Pamela Ohara, James Heath and William Gelbart (“Self-assembly of submicrometer rings of particles from solutions of nanoparticles”,  Angew. Chem. Int. Ed. Engl ., Vol. 36 no. 10 pp. 1078-1080 (1997), which is incorporated by reference for all purposes as if fully set forth herein) reported the creation of circular rings of silver nanoparticles on a graphite substrate. These rings have approximate C n  symmetry axes, perpendicular to their planes. In one reported example, a ring 0.9 microns in diameter consisted of silver nanoparticles 2.5 nm across. This ring therefore has an axis of approximate C n  symmetry, with n≈2260. For the purposes of the present invention, “approximate C n  symmetry” means that the geometry of the medium constituent is close enough to having an exact C n  symmetry axis for the medium to function as a frequency multiplication medium. It is the fact that all of the nanoparticles have approximately the same size, as can be seen in FIG. 1 of Ohara et al., that gives the rings approximate C n  symmetry. If the nanoparticle sizes were randomly distributed, the rings would have no rotational symmetry. 
     FIG. 3 is a schematic illustration, partly in perspective, of a device of the present invention based on such rings of nanoparticles as the frequency multiplication medium. Nanoparticle rings  42  are deposited on a planar graphite substrate  40  as taught by Ohara, Heath and Gelbart. Substrate  40  is thermally coupled to a cooling chamber  44  through which flows liquid helium (LHe). The purpose of the cooling is to reduce dissipation in nanoparticle rings  42 . A laser-based device  48 , similar to device  34 , directs a beam  50  of coherent, circularly polarized light towards substrate  40 . Beam  50  is perpendicular to substrate  40 , and so is parallel to the C n  symmetry axes of nanoparticle rings  42 . The interaction of beam  50  with nanoparticle rings  42  produces higher harmonics of beam  50 . Because of the very high order symmetry of nanoparticle rings  42 , the higher harmonics are very restricted in frequency content. Because graphite is transparent to soft x-rays, higher harmonics in the soft x-ray band emerge from the side of substrate  40  opposite to nanoparticle rings  42 . 
     If nanoparticle rings  42  have axes of approximate C 2000  symmetry, and the laser of device  48  is a carbon dioxide laser, so that the wavelength of beam  50  is 10.6 microns, the wavelength of the harmonics is centered around 5.3 nm. As noted by Ohara, Heath and Gelbart, the diameters of nanoparticle rings  42  varies inversely with the concentration of the solution used to produce nanoparticle rings  42 . Ohara, Heath and Gelbart used a concentration of about 10 14  particles per ml. A concentration of about 2×10 5  particles per ml produces nanoparticle rings  42  with axes of approximately C 100  symmetry. A circularly polarized beam  50  with a wavelength of 500 nm, when directed perpendicularly at such nanoparticle rings  42 , produces harmonics with wavelengths centered around the dominant wavelengths of 5.05 nm and 4.95 nm. 
     The amplification efficiency of the device of FIG. 3 is increased if nanoparticle rings  42  are ionized, because the transition dipole moments of ionized systems are higher than the transition dipole moments of neutral systems. This ionization occurs naturally if beam  50  is sufficiently intense (at least about 10 11  W/cm 2 ). 
     It should be noted that the frequency multiplication medium constituents of the present invention are considerably larger than the prior art frequency multiplication medium constituents. The largest prior art constituent used heretofore is the SF 6  molecule. The SF 6  molecule is octahedral, with an S-F bond length of 1.58 Å. Using the 1.33 Å radius of the F −  ion as an upper bound on the radius of an F atom gives an upper bound of 5.82 Å on the largest dimension of the SF 6  molecule. The largest dimension of the frequency multiplication media constituents of the present invention commonly is larger, even much larger, than about 6 Å. For example, the smallest nanoparticle ring is about 100 nm in diameter. 
     Another class of frequency multiplication medium constituents of the present invention is the nanotubes. These are cylinders, typically of carbon, that have a graphitic structure. FIG. 4 illustrates the structure of a carbon nanotube that has eight graphite rings per row. This nanotube has an exact C 8  symmetry axis. More generally, the nanotubes consist of either rings or interleaved helices of carbon, boron nitride, or mixtures thereof. The geometry of a nanotube is described by a pair of numbers, the first of which is the number of graphite rings circumferentially around the nanotube, and the second of which is the helicity of the nanotube. For example, the nanotube of FIG. 4 is a ( 8 , 0 ) nanotube. Nanotubes with zero helicity have exact C n  symmetry axes. Nanotubes with non-zero helicity have approximate C n  symmetry axes. Typically, carbon nanotubes with zero helicity have between 6 and 9 graphite rings per row, and so have exact C n  symmetry axes, with 6≦n≦9. Like nanoparticle rings, nanotubes have a longest (axial) dimension that is considerably longer than 6 Å. 
     Individual nanotubes may be mounted on a suitable substrate, as shown by Honjie Dai et al., “Nanotubes as nanoprobes in scanning probe microscopy”,  Nature , Vol. 384 pp. 147-150 (Nov. 14, 1996), which is incorporated by reference for all purposes as if fully set forth herein. Many nanotubes may be mounted parallel, perpendicular to a polymer substrate, as shown by de Heer et al., “Aligned carbon nanotubes films: production and optical and electronic properties”,  Science , Vol. 268 pp. 845-847 (May 12, 1995), which is incorporated by reference for all purposes as if fully set forth herein. Suitable nanotubes are available from Material and Electrical Research Corp. of Tucson Ariz. 
     FIG. 5 is a schematic illustration, partly in perspective, of a device of the present invention based on an assembly of nanotubes as the frequency multiplication medium. The device of FIG. 5 is similar to the device of FIG. 3, with graphite substrate  40  replaced with a polymer substrate  40 ′, and with nanoparticle rings  42  replaced with nanotubes  42 ′ having their cylindrical axes perpendicular to substrate  40 ′. In addition, device  48  directs a beam  50 ′ of elliptically polarized light towards substrate  40 ′, at an angle a to normal incidence. Beam  50 ′ is such that the electrical field thereof, as a function of time t, is 
     
       
           {overscore (E)}=E   x  cos ω t{circumflex over (x)}+E   y  sin ω tŷ   
       
     
     The angle α is chosen so that the electric field in the plane of substrate  40 ′ is circularly polarized. For example, if E x &gt;E y , then angle α is in the y-z plane, and has a value of cos −1 (E y /E x ). Such oblique incidence is useful in case light reflected back to device  48  would damage device  48 . Although, strictly speaking, tilting beam  50 ′ breaks the C n  symmetry, because of the component of the electric field normal to the substrate  40 ′, so that the (ln±1)ω selection rules also are no longer exact, at sufficiently small angles α the symmetry remains close enough to exact for practical purposes. 
     While the invention has been described with respect to a limited number of embodiments, it will be appreciated that many variations, modifications and other applications of the invention may be made. 
     APPENDIX 
     Selection rules for the Harmonic Generation Spectra