Abstract

An experimental study of third-harmonic generation in methane with a 100-fs, 820-nm, Ti:sapphire laser in a tight focusing geometry is presented. The harmonic intensity and bandwidth were measured in a range of intensities extending from below to far above the first ionization threshold and at pressures as high as 10 atm (1 atm=760 Torr). The harmonic signal follows a power-law dependence on the laser intensity with an exponent of ∼7 and saturates at an intensity Is4×1014 W/cm2. The conversion efficiency was found to increase with the pressure for laser intensities smaller than the saturation intensity Is and to decrease with the pressure at larger intensities. At laser intensities larger than the saturation intensity a substantial modification in the third-harmonic bandwidth and structure was observed.

© 1999 Optical Society of America

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1999 (1)

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

1998 (3)

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

E. C. Jarque and L. Plaja, “Harmonic generation with ionizing two-level atoms,” J. Phys. B 31, 1687–1694 (1998).
[CrossRef]

J. Peatross, S. Backus, J. Zhou, M. M. Murnane, and H. C. Kapteyn, “Spectral-spatial measurements of fundamental and third-harmonic light of intense 25-fs laser pulses focused in a cell gas,” J. Opt. Soc. Am. B 15, 186–192 (1998).
[CrossRef]

1997 (2)

1996 (7)

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, 62–64 (1996).
[CrossRef] [PubMed]

S. Backus, J. Peatross, Z. Zeek, A. Rundquist, G. Taft, M. M. Murnane, and H. C. Kapteyn, “16-fs, 1-μJ ultraviolet pulses generated by third-harmonic conversion in air,” Opt. Lett. 21, 665–667 (1996).
[CrossRef] [PubMed]

C. Altucci, T. Starczewski, E. Mevel, C. G. Wahlstrom, B. Carre, and A. L’Huillier, “Influence of atomic density in high-order harmonic generation,” J. Opt. Soc. Am. B 13, 148–156 (1996).
[CrossRef]

D. M. Mittleman, D. C. Douglass, Z. Henis, O. R. Wood II, R. R. Freeman, and T. J. McIrath, “High-field harmonic generation in the tight-focusing limit,” J. Opt. Soc. Am. B 13, 170–179 (1996).
[CrossRef]

E. T. J. Nibbering, M. A. Franco, B. S. Prade, G. Grillon, J. P. Chambaret, and A. Mysyrowicz, “Spectral determination of the amplitude and the phase of intense ultrashort optical pulses,” J. Opt. Soc. Am. B 13, 317–329 (1996).
[CrossRef]

C. W. Siders, N. C. Turner III, M. C. Downer, A. Babine, A. Stepanov, and A. M. Sergeev, “Blue-shifted third-harmonic generation and correlated self-guiding during ultrafast barrier suppression ionization of subatmospheric density noble gases,” J. Opt. Soc. Am. B 13, 330 (1996).
[CrossRef]

A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
[CrossRef] [PubMed]

1995 (1)

P. Moreno, L. Plaja, V. Malyshev, and L. Roso, “Influence of barrier supression in high-order harmonic generation,” Phys. Rev. A 51, 4746–4753 (1995).
[CrossRef] [PubMed]

1994 (4)

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

W. Becker, S. Long, and J. K. McIver, “Modeling harmonic generation by a zero-range potential,” Phys. Rev. A 50, 1540–1560 (1994).
[CrossRef] [PubMed]

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

A. E. Kaplan and P. L. Shkolnikov, “Superdressed two-level atom: very high harmonic generation and multiresonances,” Phys. Rev. A 49, 1275–1280 (1994).
[CrossRef] [PubMed]

1993 (6)

X. Liu, D. Umstadter, E. Esarey, and A. Ting, “Harmonic generation by an intense laser pulse in neutral and ionized gases,” IEEE Trans. Plasma Sci. 21, 90–94 (1993).
[CrossRef]

E. V. Vanin, A. V. Kim, A. M. Sergeev, and M. C. Downer, “Excitation of ultrashort bursts of harmonics of the radiation during ionization of a gas by an intense light pulse,” JETP Lett. 58, 905 (1993).

P. B. Corkum, “Plasma perspective on strong-field multiphoton ionization,” Phys. Rev. Lett. 71, 1995–1997 (1993).
[CrossRef]

J. J. Macklin, J. D. Kmetec, and C. L. Gordon III, “High-order harmonic generation using femtosecond pulses,” Phys. Rev. Lett. 70, 766–769 (1993).
[CrossRef] [PubMed]

A. L’Huillier and Ph. Balcou, “High-order harmonic generation in rare gases with a 1 ps 1053 laser,” Phys. Rev. Lett. 70, 774–777 (1993).
[CrossRef]

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

1992 (6)

J. L. Krause, K. J. Schafer, and K. C. Kulander, “High-order harmonic generation from atoms and ions in the high intensity regime,” Phys. Rev. Lett. 68, 3535–3538 (1992).
[CrossRef] [PubMed]

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

S. C. Rae, “Ionization induced defocusing of intense laser pulses in high pressure gases,” Opt. Commun. 89, 1091 (1992).

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

L. Plaja and L. Roso-Franco, “Adiabatic theory of high-order harmonic generation in a two-level model,” J. Opt. Soc. Am. B 9, 2210–2213 (1992).
[CrossRef]

J. K. Crane, M. D. Perry, S. Herman, and R. W. Falcone, “High field harmonic generation in helium,” Opt. Lett. 17, 1256–1258 (1992).
[CrossRef] [PubMed]

1991 (3)

P. L. Shkolnikov and A. E. Kaplan, “X-ray third-harmonic generation in plasmas of alkalilike ions,” Opt. Lett. 16, 1973–1975 (1991).
[CrossRef] [PubMed]

N. Sarukura, K. Hata, T. Adachi, R. Nodomi, M. Watanabe, and S. Watanabe, “Coherent soft x-ray generation by the harmonics of 1064 nm radiation in rare gases,” Phys. Rev. A 43, 1669–1672 (1991).
[CrossRef] [PubMed]

A. L’Huillier, K. J. Schaefer, and K. C. Kulander, “Theoretical aspects of intense field harmonic generation,” J. Phys. B 24, 3315–3341 (1991).
[CrossRef]

1990 (2)

B. Sundaram and P. W. Milonni, “High-order harmonic generation: simplified model and relevance of single-atom theories to experiment,” Phys. Rev. A 41, 6571–6573 (1990).
[CrossRef] [PubMed]

M. S. Malcuit, R. W. Boyd, W. V. Davis, and K. Rzazewski, “Anomalies in optical harmonic generations using high intensity radiation,” Phys. Rev. A 41, 3822 (1990).
[CrossRef] [PubMed]

1989 (2)

R. M. Potvliege and R. Shakeshaft, “Multiphoton processes in an intense laser field: harmonic generation and total ionization rates for atomic hydrogen,” Phys. Rev. A 40, 3061–3079 (1989).
[CrossRef] [PubMed]

J. H. Eberly, Q. Su, and J. Javanainen, “Nonlinear light scattering accompanying multiphoton ionization,” Phys. Rev. Lett. 62, 881–884 (1989).
[CrossRef] [PubMed]

1988 (3)

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

R. Rosman, G. Gibson, K. Boyer, H. Jara, T. S. Luk, I. A. McIntyre, A. McPherson, J. C. Solem, and C. K. Rhodes, “Fifth-harmonic production in neon and argon with picosecond 248-nm radiation,” J. Opt. Soc. Am. B 5, 1237–1242 (1988).
[CrossRef]

1979 (1)

R. Mahon, T. J. McIlrath, V. P. Meyerscough, and D. W. Koopman, “Third-harmonic generation in argon, krypton and xenon: bandwidth limitations in the vicinity of Lyman-α,” IEEE J. Quantum Electron. QE-15, 44–451 (1979).

1969 (1)

J. F. Ward and G. H. C. New, “Optical third harmonic generation in gases by a focused laser beam,” Phys. Rev. 185, 57–72 (1969).
[CrossRef]

1966 (1)

Ph. Balcou, A. L’Huillier, and D. Escande, “High-order harmonic generation process in classical and quantum anharmonic oscillators,” Phys. Rev. A 53, 3456–3468 (1966).
[CrossRef]

Adachi, T.

N. Sarukura, K. Hata, T. Adachi, R. Nodomi, M. Watanabe, and S. Watanabe, “Coherent soft x-ray generation by the harmonics of 1064 nm radiation in rare gases,” Phys. Rev. A 43, 1669–1672 (1991).
[CrossRef] [PubMed]

Altucci, C.

Babine, A.

Backus, S.

Balcou, Ph.

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

A. L’Huillier and Ph. Balcou, “High-order harmonic generation in rare gases with a 1 ps 1053 laser,” Phys. Rev. Lett. 70, 774–777 (1993).
[CrossRef]

Ph. Balcou, A. L’Huillier, and D. Escande, “High-order harmonic generation process in classical and quantum anharmonic oscillators,” Phys. Rev. A 53, 3456–3468 (1966).
[CrossRef]

Bandarage, G.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Becker, W.

W. Becker, S. Long, and J. K. McIver, “Modeling harmonic generation by a zero-range potential,” Phys. Rev. A 50, 1540–1560 (1994).
[CrossRef] [PubMed]

Boyd, R. W.

M. S. Malcuit, R. W. Boyd, W. V. Davis, and K. Rzazewski, “Anomalies in optical harmonic generations using high intensity radiation,” Phys. Rev. A 41, 3822 (1990).
[CrossRef] [PubMed]

Boyer, K.

Burnett, K.

A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
[CrossRef] [PubMed]

Carre, B.

Chambaret, J. P.

Chambers, D. M.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

Ciarroca, M.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

Cooper, J.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Corkum, P. B.

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

P. B. Corkum, “Plasma perspective on strong-field multiphoton ionization,” Phys. Rev. Lett. 71, 1995–1997 (1993).
[CrossRef]

Crane, J. K.

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

J. K. Crane, M. D. Perry, S. Herman, and R. W. Falcone, “High field harmonic generation in helium,” Opt. Lett. 17, 1256–1258 (1992).
[CrossRef] [PubMed]

Curley, P. F.

DaSilva, L. B.

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

Davis, W. V.

M. S. Malcuit, R. W. Boyd, W. V. Davis, and K. Rzazewski, “Anomalies in optical harmonic generations using high intensity radiation,” Phys. Rev. A 41, 3822 (1990).
[CrossRef] [PubMed]

De Silvestri, S.

Ditmire, T.

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

Douglass, D. C.

Downer, M. C.

C. W. Siders, N. C. Turner III, M. C. Downer, A. Babine, A. Stepanov, and A. M. Sergeev, “Blue-shifted third-harmonic generation and correlated self-guiding during ultrafast barrier suppression ionization of subatmospheric density noble gases,” J. Opt. Soc. Am. B 13, 330 (1996).
[CrossRef]

E. V. Vanin, A. V. Kim, A. M. Sergeev, and M. C. Downer, “Excitation of ultrashort bursts of harmonics of the radiation during ionization of a gas by an intense light pulse,” JETP Lett. 58, 905 (1993).

Eberly, J. H.

J. H. Eberly, Q. Su, and J. Javanainen, “Nonlinear light scattering accompanying multiphoton ionization,” Phys. Rev. Lett. 62, 881–884 (1989).
[CrossRef] [PubMed]

Esarey, E.

X. Liu, D. Umstadter, E. Esarey, and A. Ting, “Harmonic generation by an intense laser pulse in neutral and ionized gases,” IEEE Trans. Plasma Sci. 21, 90–94 (1993).
[CrossRef]

Escande, D.

Ph. Balcou, A. L’Huillier, and D. Escande, “High-order harmonic generation process in classical and quantum anharmonic oscillators,” Phys. Rev. A 53, 3456–3468 (1966).
[CrossRef]

Falcone, R. W.

Faldon, M. E.

Ferray, M.

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

Franco, M. A.

Freeman, R. R.

Gibson, G.

Gordon III, C. L.

J. J. Macklin, J. D. Kmetec, and C. L. Gordon III, “High-order harmonic generation using femtosecond pulses,” Phys. Rev. Lett. 70, 766–769 (1993).
[CrossRef] [PubMed]

Grillon, G.

Hata, K.

N. Sarukura, K. Hata, T. Adachi, R. Nodomi, M. Watanabe, and S. Watanabe, “Coherent soft x-ray generation by the harmonics of 1064 nm radiation in rare gases,” Phys. Rev. A 43, 1669–1672 (1991).
[CrossRef] [PubMed]

Henis, Z.

Herman, S.

Hutchinson, M. H. R.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

Ivanov, M. Yu.

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

Jara, H.

Jarque, E. C.

E. C. Jarque and L. Plaja, “Harmonic generation with ionizing two-level atoms,” J. Phys. B 31, 1687–1694 (1998).
[CrossRef]

Javanainen, J.

J. H. Eberly, Q. Su, and J. Javanainen, “Nonlinear light scattering accompanying multiphoton ionization,” Phys. Rev. Lett. 62, 881–884 (1989).
[CrossRef] [PubMed]

Kaplan, A. E.

A. E. Kaplan and P. L. Shkolnikov, “Superdressed two-level atom: very high harmonic generation and multiresonances,” Phys. Rev. A 49, 1275–1280 (1994).
[CrossRef] [PubMed]

P. L. Shkolnikov and A. E. Kaplan, “X-ray third-harmonic generation in plasmas of alkalilike ions,” Opt. Lett. 16, 1973–1975 (1991).
[CrossRef] [PubMed]

Kapteyn, H. C.

Key, M. H.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

Kim, A. V.

E. V. Vanin, A. V. Kim, A. M. Sergeev, and M. C. Downer, “Excitation of ultrashort bursts of harmonics of the radiation during ionization of a gas by an intense light pulse,” JETP Lett. 58, 905 (1993).

Kmetec, J. D.

J. J. Macklin, J. D. Kmetec, and C. L. Gordon III, “High-order harmonic generation using femtosecond pulses,” Phys. Rev. Lett. 70, 766–769 (1993).
[CrossRef] [PubMed]

Koopman, D. W.

R. Mahon, T. J. McIlrath, V. P. Meyerscough, and D. W. Koopman, “Third-harmonic generation in argon, krypton and xenon: bandwidth limitations in the vicinity of Lyman-α,” IEEE J. Quantum Electron. QE-15, 44–451 (1979).

Krause, J. L.

J. L. Krause, K. J. Schafer, and K. C. Kulander, “High-order harmonic generation from atoms and ions in the high intensity regime,” Phys. Rev. Lett. 68, 3535–3538 (1992).
[CrossRef] [PubMed]

Krausz, F.

Kulander, K. C.

J. L. Krause, K. J. Schafer, and K. C. Kulander, “High-order harmonic generation from atoms and ions in the high intensity regime,” Phys. Rev. Lett. 68, 3535–3538 (1992).
[CrossRef] [PubMed]

A. L’Huillier, K. J. Schaefer, and K. C. Kulander, “Theoretical aspects of intense field harmonic generation,” J. Phys. B 24, 3315–3341 (1991).
[CrossRef]

L’Huillier, A.

C. Altucci, T. Starczewski, E. Mevel, C. G. Wahlstrom, B. Carre, and A. L’Huillier, “Influence of atomic density in high-order harmonic generation,” J. Opt. Soc. Am. B 13, 148–156 (1996).
[CrossRef]

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

A. L’Huillier and Ph. Balcou, “High-order harmonic generation in rare gases with a 1 ps 1053 laser,” Phys. Rev. Lett. 70, 774–777 (1993).
[CrossRef]

A. L’Huillier, K. J. Schaefer, and K. C. Kulander, “Theoretical aspects of intense field harmonic generation,” J. Phys. B 24, 3315–3341 (1991).
[CrossRef]

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

Ph. Balcou, A. L’Huillier, and D. Escande, “High-order harmonic generation process in classical and quantum anharmonic oscillators,” Phys. Rev. A 53, 3456–3468 (1966).
[CrossRef]

Larsson, J.

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

Lewenstein, M.

A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
[CrossRef] [PubMed]

M. Lewenstein, Ph. Balcou, M. Yu. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of high-harmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).
[CrossRef] [PubMed]

Li, X. F.

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

Liu, X.

X. Liu, D. Umstadter, E. Esarey, and A. Ting, “Harmonic generation by an intense laser pulse in neutral and ionized gases,” IEEE Trans. Plasma Sci. 21, 90–94 (1993).
[CrossRef]

Lompre, A.

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

Lompre, L. A.

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

Long, S.

W. Becker, S. Long, and J. K. McIver, “Modeling harmonic generation by a zero-range potential,” Phys. Rev. A 50, 1540–1560 (1994).
[CrossRef] [PubMed]

Luk, T. S.

Macklin, J. J.

J. J. Macklin, J. D. Kmetec, and C. L. Gordon III, “High-order harmonic generation using femtosecond pulses,” Phys. Rev. Lett. 70, 766–769 (1993).
[CrossRef] [PubMed]

Mahon, R.

R. Mahon, T. J. McIlrath, V. P. Meyerscough, and D. W. Koopman, “Third-harmonic generation in argon, krypton and xenon: bandwidth limitations in the vicinity of Lyman-α,” IEEE J. Quantum Electron. QE-15, 44–451 (1979).

Mainfray, G.

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

Malcuit, M. S.

M. S. Malcuit, R. W. Boyd, W. V. Davis, and K. Rzazewski, “Anomalies in optical harmonic generations using high intensity radiation,” Phys. Rev. A 41, 3822 (1990).
[CrossRef] [PubMed]

Malyshev, V.

P. Moreno, L. Plaja, V. Malyshev, and L. Roso, “Influence of barrier supression in high-order harmonic generation,” Phys. Rev. A 51, 4746–4753 (1995).
[CrossRef] [PubMed]

Manus, C.

A. L’Huillier, L. A. Lompre, M. Ferray, X. F. Li, G. Mainfray, and C. Manus, “Third-harmonic generation in xenon in a pulsed jet and a gas cell,” Europhys. Lett. 5, 601–605 (1988).
[CrossRef]

M. Ferray, A. L’Huillier, X. F. Li, A. Lompre, G. Mainfray, and C. Manus, “Multiple harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B 25, L31–L35 (1988).
[CrossRef]

Maquet, A.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Marangos, J. P.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

Marjoribanks, R. S.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

McIlrath, T. J.

R. Mahon, T. J. McIlrath, V. P. Meyerscough, and D. W. Koopman, “Third-harmonic generation in argon, krypton and xenon: bandwidth limitations in the vicinity of Lyman-α,” IEEE J. Quantum Electron. QE-15, 44–451 (1979).

McIntyre, I. A.

McIrath, T. J.

McIver, J. K.

W. Becker, S. Long, and J. K. McIver, “Modeling harmonic generation by a zero-range potential,” Phys. Rev. A 50, 1540–1560 (1994).
[CrossRef] [PubMed]

McPherson, A.

Menis, T.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Mevel, E.

Meyerscough, V. P.

R. Mahon, T. J. McIlrath, V. P. Meyerscough, and D. W. Koopman, “Third-harmonic generation in argon, krypton and xenon: bandwidth limitations in the vicinity of Lyman-α,” IEEE J. Quantum Electron. QE-15, 44–451 (1979).

Milonni, P. W.

B. Sundaram and P. W. Milonni, “High-order harmonic generation: simplified model and relevance of single-atom theories to experiment,” Phys. Rev. A 41, 6571–6573 (1990).
[CrossRef] [PubMed]

Mittleman, D. M.

Moreno, P.

P. Moreno, L. Plaja, V. Malyshev, and L. Roso, “Influence of barrier supression in high-order harmonic generation,” Phys. Rev. A 51, 4746–4753 (1995).
[CrossRef] [PubMed]

Muffett, J. E.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

Murnane, M. M.

Mysyrowicz, A.

Neely, D.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

New, G. H. C.

J. F. Ward and G. H. C. New, “Optical third harmonic generation in gases by a focused laser beam,” Phys. Rev. 185, 57–72 (1969).
[CrossRef]

Nibbering, E. T. J.

Nisoli, M.

Nodomi, R.

N. Sarukura, K. Hata, T. Adachi, R. Nodomi, M. Watanabe, and S. Watanabe, “Coherent soft x-ray generation by the harmonics of 1064 nm radiation in rare gases,” Phys. Rev. A 43, 1669–1672 (1991).
[CrossRef] [PubMed]

Norreys, P. A.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

Nyguyen, H.

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

Peatross, J.

Perry, M.

T. Ditmire, J. K. Crane, H. Nyguyen, L. B. DaSilva, and M. Perry, “Energy-yield and conversion-efficiency measurements of high-order harmonic radiation,” Phys. Rev. A 51, R902–R905 (1999).
[CrossRef]

Perry, M. D.

Persson, A.

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

Plaja, L.

E. C. Jarque and L. Plaja, “Harmonic generation with ionizing two-level atoms,” J. Phys. B 31, 1687–1694 (1998).
[CrossRef]

P. Moreno, L. Plaja, V. Malyshev, and L. Roso, “Influence of barrier supression in high-order harmonic generation,” Phys. Rev. A 51, 4746–4753 (1995).
[CrossRef] [PubMed]

L. Plaja and L. Roso-Franco, “Adiabatic theory of high-order harmonic generation in a two-level model,” J. Opt. Soc. Am. B 9, 2210–2213 (1992).
[CrossRef]

Potvliege, R. M.

R. M. Potvliege and R. Shakeshaft, “Multiphoton processes in an intense laser field: harmonic generation and total ionization rates for atomic hydrogen,” Phys. Rev. A 40, 3061–3079 (1989).
[CrossRef] [PubMed]

Prade, B. S.

Preston, S. G.

S. G. Preston, D. M. Chambers, R. S. Marjoribanks, P. A. Norreys, D. Neely, M. Zepf, J. Zhang, M. H. Key, and J. S. Wark, “Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser,” J. Phys. B 31, 1069–1082 (1998).
[CrossRef]

Rae, S. C.

S. C. Rae, “Ionization induced defocusing of intense laser pulses in high pressure gases,” Opt. Commun. 89, 1091 (1992).

Rhodes, C. K.

Rosman, R.

Roso, L.

P. Moreno, L. Plaja, V. Malyshev, and L. Roso, “Influence of barrier supression in high-order harmonic generation,” Phys. Rev. A 51, 4746–4753 (1995).
[CrossRef] [PubMed]

Roso-Franco, L.

Rundquist, A.

Rzazewski, K.

M. S. Malcuit, R. W. Boyd, W. V. Davis, and K. Rzazewski, “Anomalies in optical harmonic generations using high intensity radiation,” Phys. Rev. A 41, 3822 (1990).
[CrossRef] [PubMed]

Salin, F.

Sanpera, A.

A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
[CrossRef] [PubMed]

Sartania, S.

Sarukura, N.

N. Sarukura, K. Hata, T. Adachi, R. Nodomi, M. Watanabe, and S. Watanabe, “Coherent soft x-ray generation by the harmonics of 1064 nm radiation in rare gases,” Phys. Rev. A 43, 1669–1672 (1991).
[CrossRef] [PubMed]

Schaefer, K. J.

A. L’Huillier, K. J. Schaefer, and K. C. Kulander, “Theoretical aspects of intense field harmonic generation,” J. Phys. B 24, 3315–3341 (1991).
[CrossRef]

Schafer, K. J.

J. L. Krause, K. J. Schafer, and K. C. Kulander, “High-order harmonic generation from atoms and ions in the high intensity regime,” Phys. Rev. Lett. 68, 3535–3538 (1992).
[CrossRef] [PubMed]

Sergeev, A. M.

C. W. Siders, N. C. Turner III, M. C. Downer, A. Babine, A. Stepanov, and A. M. Sergeev, “Blue-shifted third-harmonic generation and correlated self-guiding during ultrafast barrier suppression ionization of subatmospheric density noble gases,” J. Opt. Soc. Am. B 13, 330 (1996).
[CrossRef]

E. V. Vanin, A. V. Kim, A. M. Sergeev, and M. C. Downer, “Excitation of ultrashort bursts of harmonics of the radiation during ionization of a gas by an intense light pulse,” JETP Lett. 58, 905 (1993).

Shakeshaft, R.

R. M. Potvliege and R. Shakeshaft, “Multiphoton processes in an intense laser field: harmonic generation and total ionization rates for atomic hydrogen,” Phys. Rev. A 40, 3061–3079 (1989).
[CrossRef] [PubMed]

Shkolnikov, P. L.

A. E. Kaplan and P. L. Shkolnikov, “Superdressed two-level atom: very high harmonic generation and multiresonances,” Phys. Rev. A 49, 1275–1280 (1994).
[CrossRef] [PubMed]

P. L. Shkolnikov and A. E. Kaplan, “X-ray third-harmonic generation in plasmas of alkalilike ions,” Opt. Lett. 16, 1973–1975 (1991).
[CrossRef] [PubMed]

Siders, C. W.

Smith, R. A.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

Solem, J. C.

Spielmann, Ch.

Starczewski, T.

C. Altucci, T. Starczewski, E. Mevel, C. G. Wahlstrom, B. Carre, and A. L’Huillier, “Influence of atomic density in high-order harmonic generation,” J. Opt. Soc. Am. B 13, 148–156 (1996).
[CrossRef]

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

Stepanov, A.

Su, Q.

J. H. Eberly, Q. Su, and J. Javanainen, “Nonlinear light scattering accompanying multiphoton ionization,” Phys. Rev. Lett. 62, 881–884 (1989).
[CrossRef] [PubMed]

Sundaram, B.

B. Sundaram and P. W. Milonni, “High-order harmonic generation: simplified model and relevance of single-atom theories to experiment,” Phys. Rev. A 41, 6571–6573 (1990).
[CrossRef] [PubMed]

Svanberg, S.

C. G. Wahlstrom, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
[CrossRef] [PubMed]

Svelto, O.

Taft, G.

Taieb, R.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Ting, A.

X. Liu, D. Umstadter, E. Esarey, and A. Ting, “Harmonic generation by an intense laser pulse in neutral and ionized gases,” IEEE Trans. Plasma Sci. 21, 90–94 (1993).
[CrossRef]

Tisch, J. W. G.

J. W. G. Tisch, R. A. Smith, J. E. Muffett, M. Ciarroca, J. P. Marangos, and M. H. R. Hutchinson, “Angular resolved high-order harmonic generation in helium,” Phys. Rev. A 49, R28–R31 (1994).
[CrossRef]

M. E. Faldon, M. H. R. Hutchinson, J. P. Marangos, J. E. Muffett, R. A. Smith, and J. W. G. Tisch, “Studies of time-resolved harmonic generation in intense laser fields in xenon,” J. Opt. Soc. Am. B 9, 2094–2099 (1992).
[CrossRef]

Turner III, N. C.

Umstadter, D.

X. Liu, D. Umstadter, E. Esarey, and A. Ting, “Harmonic generation by an intense laser pulse in neutral and ionized gases,” IEEE Trans. Plasma Sci. 21, 90–94 (1993).
[CrossRef]

Vanin, E. V.

E. V. Vanin, A. V. Kim, A. M. Sergeev, and M. C. Downer, “Excitation of ultrashort bursts of harmonics of the radiation during ionization of a gas by an intense light pulse,” JETP Lett. 58, 905 (1993).

Veniard, V.

G. Bandarage, A. Maquet, T. Menis, R. Taieb, V. Veniard, and J. Cooper, “Harmonic generation by laser-driven classical hydrogen atoms,” Phys. Rev. A 46, 380–390 (1992).
[CrossRef] [PubMed]

Wahlstrom, C. G.

C. Altucci, T. Starczewski, E. Mevel, C. G. Wahlstrom, B. Carre, and A. L’Huillier, “Influence of atomic density in high-order harmonic generation,” J. Opt. Soc. Am. B 13, 148–156 (1996).
[CrossRef]

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Figures (7)

Fig. 1
Fig. 1

Schematic of the experimental setup for measuring the third harmonic.

Fig. 2
Fig. 2

Third-harmonic signal in CH4 as a function of the laser intensity at various gas pressures.

Fig. 3
Fig. 3

Intensity of the third harmonic radiation in CH4 at different values of the laser irradiance as a function of pressure.

Fig. 4
Fig. 4

Spectra of the radiation emitted in the vicinity of 275.3 nm (2753 Å) for various laser intensities.

Fig. 5
Fig. 5

Spectra of the third-harmonic at various gas pressures, measured at a laser intensity I=1.15×1014 W/cm2.

Fig. 6
Fig. 6

Spectra of the third harmonic at various gas pressures, measured at a laser intensity I=4.5×1014 W/cm2.

Fig. 7
Fig. 7

Harmonic signal in xenon, argon, and methane measured at 30 psi as a function of the laser intensity.

Equations (7)

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I3I13|χ(3)|2N2|F3(bΔk)|2,
F3(bΔk)=2πbΔk2expbΔk2,Δk<0,
F3(bΔk)=0,Δk>0.
Δk=32πλ(n3-n1),n3-n1=2πN Re[χ(1)(3ω)].
Wcr=(1.22λ)2c256Nχ3,
NeNcrλ2zR.
Δλλ=zRcdndt,

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