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Threshold dependence of the vibrational excitation of molecules on laser radiation intensity

  • Elementary Physicochemical Processes
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Abstract

The collisionless vibrational excitation of a polyatomic molecule in an IR laser radiation field has been theoretically studied. It has been shown that (i) the degree of vibrational excitation (namely, number 0000 of vibrational quanta of a molecular mode near-resonant with the IR laser field that are absorbed by the molecule) is low if laser pulse intensity P (energy flux density in the laser beam) is lower than a certain critical value P cr; (ii) the degree of excitation abruptly increases after crossing the boundary where P = P cr; (iii) this effect is attributed to two properties inherent in polyatomic molecules, namely, the anharmonicity of the vibrational mode interacting with the laser field and the energy exchange with other modes; and (iv) at P > P cr, number 00000 is determined only by energy density Φ = PτP, where τP is the laser pulse duration, 00000 monotonically increases with increasing Φ. The model is in good agreement with the experimental data.

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References

  1. R. V. Ambartzumian, N. V. Chekalin, V. S. Dolinnikov, V. S. Letokhov, and E. A. Ryabov, Chem. Phys. Lett. 25, 515 (1974).

    Article  Google Scholar 

  2. V. S. Letokhov and A. A. Makarov, Sov. Phys. Usp. 24, 366 (1981).

    Article  Google Scholar 

  3. V. S. Letokhov and E. A. Ryabov, in Isotopes: Properties, Production, Application, Ed. by V. Yu. Baranov (IzdAT, Moscow, 2000), p. 329 [in Russian].

  4. N. G. Basov, E. M. Belenov, V. A. Isakov, et al., Sov. Phys. Usp. 20, 209 (1977).

    Article  Google Scholar 

  5. G. N. Makarov, Phys. Usp. 48, 37 (2005).

    Article  CAS  Google Scholar 

  6. S. N. Gordienko and A. V. Dem’yanenko, JETP Lett. 64, 13 (1996).

    Article  CAS  Google Scholar 

  7. Laser Spectroscopy of Highly Vibrationally Excited Molecules, Ed. by V. S. Letokhov (Adam Hilger, Bristol, 1989; Nauka, Moscow, 1990).

  8. G. A. Askar’yan, Sov. Phys. JETP 19, 273 (1964).

    Google Scholar 

  9. G. A. Askar’yan, Sov. Phys. JETP 21, 658 (1965).

    Google Scholar 

  10. F. V. Bunkin, R. V. Karapetyan, and A. M. Prokhorov, Sov. Phys. JETP 20, 145 (1964).

    Google Scholar 

  11. A. A. Makarov, A. L. Malinovsky, and E. A. Ryabov, Phys. Usp. 55, 977 (2012).

    Article  CAS  Google Scholar 

  12. P. V. Ambartsumyan, V. S. Letokhov, E. A. Ryabov, and N. V. Chekalin, JETP Lett. 20, 273 (1974).

    Google Scholar 

  13. V. Yu. Baranov, E. I. Kozlova, Yu. A. Kolesnikov, and A. A. Kotov, in Isotopes: Properties, Production, Application, Ed. by V. Yu. Baranov (IzdAT, Moscow, 2000), p. 357 [in Russian].

  14. H. Bergh, Laser Optoelectron., No. 3, 263 (1985).

    Google Scholar 

  15. J. W. Earkens and J. Kim, AIChE J. 56, 2331 (2010).

    Google Scholar 

  16. P. V. Ambartsumyan, Yu. A. Gorokhov, V. S. Letokhov, G. N. Makarov, and A. A. Puretskii, Sov. Phys. JETP 44, 231 (1976).

    Google Scholar 

  17. P. Kolodner, C. Winterfeld, and E. Yablonovitch, Opt. Commun. 20, 119 (1977).

    Article  CAS  Google Scholar 

  18. P. Rabinowitz, A. Stein, and A. Caldor, Opt. Commun. 27, 381 (1978).

    Article  CAS  Google Scholar 

  19. R. Kubo, H. Ichimura, T. Usui, and N. Hashitsume, Statistical Mechanics. An Advanced Course with Problems and Solutions (North-Holland, Amsterdam, 1965).

    Google Scholar 

  20. L. D. Landau and E. M. Lifshitz, Course of Theoretical Physics, Vol. 5: Statistical Physics (Fizmatlit, Moscow, 2002; Pergamon, Oxford, 1980), rus. p.29.

    Google Scholar 

  21. N. Bloembergen, C. D. Cantrell, and D. M. Larsen, in Proceedings of the Loen Conference on Tunable Lasers and Applications, Norway, June 6–11, 1976, Ed. by A. Mooradian, T. Jaeger, and P. Stokseth, Springer Ser. Opt. Sci. (Springer, 1976), p.162.

  22. A. A. Makarov, I. Yu. Petrova, E. A. Ryabov, and V. S. Letokhov, J. Phys. Chem. A 102, 1438 (1998).

    Article  CAS  Google Scholar 

  23. A. L. Malinovsky, I. Yu. Petrova, E. A. Ryabov, A. A. Makarov, and V. S. Letokhov, J. Phys. Chem. A 102, 9353 (1998).

    Article  CAS  Google Scholar 

  24. V. N. Lokhman, A. N. Petin, E. A. Ryabov, and V. S. Letokhov, J. Phys. Chem. A 103, 11293 (1999).

    Article  CAS  Google Scholar 

  25. V. N. Lokhman, A. A. Makarov, I. Yu. Petrova, E. A. Ryabov, and V. S. Letokhov, J. Phys. Chem. A 103, 11299 (1999).

    Article  CAS  Google Scholar 

  26. V. M. Apatin and G. N. Makarov, Appl. Phys. B 28, 367 (1982).

    Article  Google Scholar 

  27. V. M. Apatin, T. V. Bezuglova, and G. N. Makarov, Opt. Commun. 42, 255 (1982).

    Article  CAS  Google Scholar 

  28. V. M. Apatin and G. N. Makarov, Sov. J. Quantum Electron. 12, 1067 (1982).

    Article  Google Scholar 

  29. V. M. Apatin, L. M. Dorozhkin, G. N. Makarov, and L. M. Pleshkov, Appl. Phys. B 29, 273 (1982).

    Article  Google Scholar 

  30. V. M. Apatin and G. N. Makarov, Sov. Phys. JETP 57, 8 (1983).

    Google Scholar 

  31. V. M. Apatin and G. N. Makarov, Appl. Phys. B 30, 207 (1983).

    Article  Google Scholar 

  32. V. M. Apatin, V. M. Krivtsun, Yu. A. Kuritsyn, et al., JETP Lett. 37, 431 (1983).

    Google Scholar 

  33. V. M. Apatin and G. N. Makarov, Sov. J. Quantum Electron. 13, 847 (1983).

    Article  Google Scholar 

  34. V. M. Apatin, V. M. Krivtsyn, Yu. A. Kuritsyn, G. N. Makarov, and I. Pak, Opt. Commun. 47, 251 (1983).

    Article  CAS  Google Scholar 

  35. V. M. Krivtsyn, G. N. Makarov, I. Pak, and M. V. Sotnikov, Chem. Phys. 122, 97 (1988).

    Article  Google Scholar 

  36. Yu. A. Kuritsyn, G. N. Makarov, I. Pak, and M. V. Sotnikov, Sov. Phys. JETP 67, 1122 (1988).

    Google Scholar 

  37. G. N. Makarov, E. Ronander, S. P. van Heerden, M. Gouws, and K. van der Merwe, Appl. Phys. B 65, 583 (1997).

    Article  CAS  Google Scholar 

  38. G. N. Makarov, V. N. Lokhman, and E. Ronander, Opt. Spectrosc. 83, 215 (1997).

    Google Scholar 

  39. G. P. Quigley and O. P. Judd, Multiple-Photon Excitation and Dissociation of Polyatomic Molecules, Ed. by C. Cantrell (Springer, Berlin, Heidelberg, New York, 1981), p.9.

  40. V. N. Bagrataschvili, V. S. Letokhov, A. A. Makarov, and E. A. Ryabov, Multiple Photon Infrared Laser Photophysics and Photochemistry (Harwood Academic, London, Paris, New York, 1985), p.366.

    Google Scholar 

  41. R. P. Feynman, Phys. Rev. 80, 440 (1950).

    Article  Google Scholar 

  42. R. P. Feynman, Phys. Rev. 84, 108 (1951).

    Article  Google Scholar 

  43. T. Ree, Y. H. Kim, and H. K. Shin, Chem. Phys. Lett. A 103, 149 (1983).

    Article  CAS  Google Scholar 

  44. R. J. Glauber, Phys. Lett. A 21, 650 (1966).

    Article  Google Scholar 

  45. R. Glauber, Coherent States in Quantum Theory, Ed. by V. I. Man’ko (Mir, Moscow, 1972), p. 26 [in Russian].

  46. B. Ya. Zel’dovich, A. M. Perelomov, and V. S. Popov, Sov. Phys. JETP 28, 308 (1968).

    Google Scholar 

  47. B. Ya. Zel’dovich, A. M. Perelomov, and V. S. Popov, Sov. Phys. JETP 30, 111 (1969).

    Google Scholar 

  48. N. M. Krylov and N. N. Bogolyubov, Introduction to Nonlinear Mechanics (Akad. Nauk Ukr. SSR, Kiev, 1937), p. 293 [in Russian].

    Google Scholar 

  49. N. N. Bogolyubov and Yu. A. Mitropol’skii, Asymptotic Methods in the Theory of Nonlinear Oscillations (Gostekhizdat, Moscow, 1955), p. 185 [in Russian].

    Google Scholar 

  50. Yu. A. Mitropol’skii, in Nonstationary Processes in Nonlinear Oscillatory Systems, Ed. by N. N. Bogolyubov (Akad. Nauk Ukr. SSR, Kiev, 1955), p. 57 [in Russian].

  51. Yu. A. Mitropol’skii, Problems of Asymptotic Theory of Nonstationary Oscillations (Nauka, Moscow, 1964), p. 89 [in Russian].

    Google Scholar 

  52. L. D. Landau and E. M. Lifshitz, Course of Theoretical Physics, Vol. 1: Mechanics (Nauka, Moscow, 1973; Pergamon Press, New York, 1988), p.117.

    Google Scholar 

  53. E. M. Lifshits and L. P. Pitaevskii, Physical Kinetics (Nauka, Moscow, 1979; Pergamon, Oxford, 1981), rus. p.510.

    Google Scholar 

  54. P. L. Houston and J. I. Steinfeld, J. Mol. Spectrosc. 54, 335 (1975).

    Article  CAS  Google Scholar 

  55. V. S. Letokhov and C. B. Moore, Sov. J. Quantum Electron. 6, 129 (1976).

    Article  Google Scholar 

  56. V. S. Letokhov and C. B. Moore, Sov. J. Quantum Electron. 6, 259 (1976).

    Article  Google Scholar 

  57. V. N. Bagrataschvili, I. N. Knyazev, V. S. Letokhov, and V. V. Lobko, Opt. Commun. 18, 525 (1976).

    Article  Google Scholar 

  58. Yu. S. Dolzhikov, V. S. Letokhov, A. A. Makarov, A. L. Malinovskii, and E. A. Ryabov, Sov. Phys. JETP 63, 1161 (1986).

    Google Scholar 

  59. K. S. Rutkovskii and K. G. Tokhadze, Sov. Phys. JETP 48, 204 (1978).

    Google Scholar 

  60. W. D. Breshears and L. S. Blair, J. Chem. Phys. 59, 5824 (1973).

    Article  CAS  Google Scholar 

  61. Y. Okada, S. Yamaguchi, and K. Takeuchi, Appl. Phys. B 72, 507 (2001).

    Article  CAS  Google Scholar 

  62. www.cae-club.ru/content/uchebnik-ak1.

  63. D. Cravens, F. D. Shields, H. E. Bass, and W. D. Breshears, J. Chem. Phys. 71, 2798 (1979).

    Article  Google Scholar 

  64. H. E. Bass, F. D. Shields, W. D. Breshears, and L. B. Asprey, J. Chem. Phys. 67, 1136 (1977).

    Article  CAS  Google Scholar 

  65. H. E. Bass and R. Rogers, J. Chem. Phys. 81, 2981 (1984).

    Article  CAS  Google Scholar 

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Authors and Affiliations

  1. Russian Research Center Kurchatov Institute, Moscow, 123182, Russia

    G. Yu. Grigor’ev, L. I. Men’shikov, P. L. Men’shikov & Sh. Sh. Nabiev

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  1. G. Yu. Grigor’ev
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  2. L. I. Men’shikov
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  3. P. L. Men’shikov
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  4. Sh. Sh. Nabiev
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Correspondence to P. L. Men’shikov.

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Original Russian Text © G.Yu. Grigor’ev, L.I. Men’shikov, P.L. Men’shikov, Sh.Sh. Nabiev, 2017, published in Khimicheskaya Fizika, 2017, Vol. 36, No. 2, pp. 22–31.

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Grigor’ev, G.Y., Men’shikov, L.I., Men’shikov, P.L. et al. Threshold dependence of the vibrational excitation of molecules on laser radiation intensity. Russ. J. Phys. Chem. B 11, 24–33 (2017). https://doi.org/10.1134/S1990793117010195

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