Abstract

A new mechanism of nonlinear absorption of intense femtosecond laser radiation in air in the intensity range I = 1011-1012 W/cm2 when the ionization is not important yet is experimentally observed and investigated. This absorption is much greater than for nanosecond pulses. A model of the nonlinear absorption based on the rotational excitation of molecules by linearly polarized ultrashort pulses through the interaction of an induced dipole moment with an electric field is developed. The observed nonlinear absorption of intense femtosecond laser radiation can play an important role in the process of propagation of such radiation in the atmosphere.

© 2006 Optical Society of America

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  1. A. Braun, G. Korn, X. Liu, D. Du, J. Squier, and G. Mourou, "Self-channeling of high-peak-power femtosecond laser pulses in air," Opt. Lett.,  20,73 (1995).
    [CrossRef] [PubMed]
  2. E. T. J. Nibbering, P. F. Curley, G. Grillon, B. S. Prade, M. A. Franco, F. Salin, and A. Mysyrowicz, "Conical emission from self-guided femtosecond pulses in air,’Opt. Lett.,  21,62 (1996).
    [CrossRef] [PubMed]
  3. A. C. Tam, "Signal Enhancement and Noise Suppression Considerations in Photothermal Spectroscopy" in Photoacoustic and Photothermal Phenomena III., D. Bicanic, ed., Springer-Verlag, Springer series in optical sciences 69, 447-462 (1992).
  4. J. Yu, D. Mondelain, J. Kasparian, E. Salmon, S. Geffroy, C. Favre, V. Boutou, and J.-P. Wolf, "Sonographic probing of laser filaments in air," Appl. Opt.,  42, 7117-7120 (2003).
    [CrossRef]
  5. A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
    [CrossRef]
  6. V. S. Kozlov, M. V. Panchenko, А. B. Tikhomirov, and B. А. Tikhomirov, "Measurements of aerosol absorption of the 694.300 nm radiation in the atmospheric surface layer," Atmos.-Ocean Opt. 15, 684-688 (2002).
  7. C. H. Townes, A. L. Schawlow, Microwave spectroscopy (Dover Publications, New York, 1975).
  8. L. D. Landau, and E. M. Lifshitz, Quantum Mechanics: Non-Relativistic Theory (Pergamon, Oxford, 1977).
  9. H. Stapelfeldt, and T. Seideman, "Aligning molecules with strong laser pulses," Rev. Mod. Phys.,  75, 543 (2003).
    [CrossRef]
  10. J.-M. Heritier, "Electrostrictive limit and focusing effects in pulsed photoacoustic detection," Opt. Comm.,  44, 267-272 (1983).
    [CrossRef]
  11. http://srdata.nist.gov/cccbdb/exp2.asp?casno=7727379.
  12. I. S. Grigoryev and E. Z. Meylikhova eds., Handbook of physical values (in Russian), (Energoatomizdat, Moscow, 1991).
  13. L. Berge, S. Skupin, F. Lederer, G. Mejean, J. Yu, J. Kasparian, E. Salmon, J. P. Wolf, M. Rodriguez, L. Woste, R. Bourayou, and R. Sauerbrey, "Multiple Filamentation of Terawatt Laser Pulses in Air," Phys. Rev. Lett., 92, 225002 1-4 (2004).
    [CrossRef] [PubMed]
  14. G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
    [CrossRef]
  15. G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).
  16. R. P. WayneChemistry of Atmospheres (Oxford University Press, 3-rd Ed., 2000).

2004

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

2003

2002

V. S. Kozlov, M. V. Panchenko, А. B. Tikhomirov, and B. А. Tikhomirov, "Measurements of aerosol absorption of the 694.300 nm radiation in the atmospheric surface layer," Atmos.-Ocean Opt. 15, 684-688 (2002).

2001

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

1996

1995

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

A. Braun, G. Korn, X. Liu, D. Du, J. Squier, and G. Mourou, "Self-channeling of high-peak-power femtosecond laser pulses in air," Opt. Lett.,  20,73 (1995).
[CrossRef] [PubMed]

1983

J.-M. Heritier, "Electrostrictive limit and focusing effects in pulsed photoacoustic detection," Opt. Comm.,  44, 267-272 (1983).
[CrossRef]

Aleksandrov, A. P.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Babin, A. A.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Boutou, V.

Braun, A.

Curley, P. F.

Du, D.

Favre, C.

Fraiman, G. M.

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

Franco, M. A.

Geffroy, S.

Grillon, G.

Heritier, J.-M.

J.-M. Heritier, "Electrostrictive limit and focusing effects in pulsed photoacoustic detection," Opt. Comm.,  44, 267-272 (1983).
[CrossRef]

Kasparian, J.

Kirsanov, A. V.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Kiselev, A. M.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Korn, G.

Kozlov, V. S.

V. S. Kozlov, M. V. Panchenko, А. B. Tikhomirov, and B. А. Tikhomirov, "Measurements of aerosol absorption of the 694.300 nm radiation in the atmospheric surface layer," Atmos.-Ocean Opt. 15, 684-688 (2002).

Kulagin, D. I.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Laedke, W.

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

Liu, X.

Lozhkarev, V. V.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Matvienko, G. G.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Mondelain, D.

Mourou, G.

Mysyrowicz, A.

Nibbering, E. T. J.

Panchenko, M. V.

V. S. Kozlov, M. V. Panchenko, А. B. Tikhomirov, and B. А. Tikhomirov, "Measurements of aerosol absorption of the 694.300 nm radiation in the atmospheric surface layer," Atmos.-Ocean Opt. 15, 684-688 (2002).

Ponomarev, Yu. N.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Prade, B. S.

Salin, F.

Salmon, E.

Seideman, T.

H. Stapelfeldt, and T. Seideman, "Aligning molecules with strong laser pulses," Rev. Mod. Phys.,  75, 543 (2003).
[CrossRef]

Sher, E. M.

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

Squier, J.

Stapelfeldt, H.

H. Stapelfeldt, and T. Seideman, "Aligning molecules with strong laser pulses," Rev. Mod. Phys.,  75, 543 (2003).
[CrossRef]

Stepanov, A. N.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Stepanov, A.N.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Tikhomirov, A. B.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Tikhomirov, B. A.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

Wolf, J.-P.

Yu, J.

Yunakovsky, A. D.

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

Appl. Opt.

Ocean Opt.

G. G. Matvienko, Yu. N. Ponomarev, B. A. Tikhomirov, A. B. Tikhomirov, A. V. Kirsanov, A. M. Kiselev, and A.N. Stepanov, "Photo-acoustic measurements of the Ti:Sa-laser femtosecond radiation absorption by atmospheric air," Atmos.-Ocean Opt.,  17, 95-97 (2004).

V. S. Kozlov, M. V. Panchenko, А. B. Tikhomirov, and B. А. Tikhomirov, "Measurements of aerosol absorption of the 694.300 nm radiation in the atmospheric surface layer," Atmos.-Ocean Opt. 15, 684-688 (2002).

Opt. Comm.

J.-M. Heritier, "Electrostrictive limit and focusing effects in pulsed photoacoustic detection," Opt. Comm.,  44, 267-272 (1983).
[CrossRef]

Opt. Lett.

Physica D

G. M. Fraiman, E. M. Sher, A. D. Yunakovsky, and W. Laedke, "Long-term evolution of strong 2-D NSE turbulence," Physica D,  87, 325-334 (1995).
[CrossRef]

Quantum. Electron.

A. P. Aleksandrov, A. A. Babin, A. M. Kiselev, D. I. Kulagin, V. V. Lozhkarev, and A. N. Stepanov, "Terawatt femtosecond Ti:Sa laser complex," Quantum. Electron.,  31,398-400 (2001).
[CrossRef]

Rev. Mod. Phys.

H. Stapelfeldt, and T. Seideman, "Aligning molecules with strong laser pulses," Rev. Mod. Phys.,  75, 543 (2003).
[CrossRef]

Other

C. H. Townes, A. L. Schawlow, Microwave spectroscopy (Dover Publications, New York, 1975).

L. D. Landau, and E. M. Lifshitz, Quantum Mechanics: Non-Relativistic Theory (Pergamon, Oxford, 1977).

http://srdata.nist.gov/cccbdb/exp2.asp?casno=7727379.

I. S. Grigoryev and E. Z. Meylikhova eds., Handbook of physical values (in Russian), (Energoatomizdat, Moscow, 1991).

L. Berge, S. Skupin, F. Lederer, G. Mejean, J. Yu, J. Kasparian, E. Salmon, J. P. Wolf, M. Rodriguez, L. Woste, R. Bourayou, and R. Sauerbrey, "Multiple Filamentation of Terawatt Laser Pulses in Air," Phys. Rev. Lett., 92, 225002 1-4 (2004).
[CrossRef] [PubMed]

R. P. WayneChemistry of Atmospheres (Oxford University Press, 3-rd Ed., 2000).

A. C. Tam, "Signal Enhancement and Noise Suppression Considerations in Photothermal Spectroscopy" in Photoacoustic and Photothermal Phenomena III., D. Bicanic, ed., Springer-Verlag, Springer series in optical sciences 69, 447-462 (1992).

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Figures (4)

Fig. 1.
Fig. 1.

Experimental setup for photoacoustic absorption measurement in atmosphere.

Fig. 2.
Fig. 2.

Dependence of the peak of acoustic signal on laser energy. Circles – nanosecond pulses, squares – femtosecond pulses, solid line – model.

Fig. 3.
Fig. 3.

Distribution of normalized intensity of a beam at different energies in a pulse.

Fig. 4.
Fig. 4.

Acoustic signals for linear (magenta) and circular (blue) polarizations.

Equations (7)

Equations on this page are rendered with MathJax. Learn more.

w ij = 1 ħ 2 V ij e i ω ij t dt 2
V = 1 4 α E 0 2 e t 2 τ 2 cos 2 ( ω t ) cos θ 2
w j , j + 2 = π 3 15 ( α τ I ħc ) 2 e 2 B 2 ħ 2 ( 2 j + 3 ) 2 τ 2 ( j + 1 ) ( 2 j 3 + 4 j 2 + 26 j + 15 ) ( 2 j + 3 ) 2 ( 2 j + 5 ) ,
dE = π 3 15 ( α τ I c ) 2 1 JQ S
dW dz = π 15 Q α 2 n W 2 J c 2 a 2 S
p max 0.42 Q S α 2 n W 2 v 2 c p r 0 1 2 T . J c 2 a 7 2
a = a 0 ( 1 + 0.00167 W 0.005 W 2 )

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