A highly stable version of spectral interferometry is demonstrated, allowing single shot measurement of ultrafast high field processes using modest energy lasers, with pump and probe pulses totaling less than 1 mJ. The technique makes possible reconstruction of ultrafast refractive index transients with one-dimensional spatial resolution, limited only by the bandwidth of the supercontinuum pulse (~100 nm) and instrument resolution. The ultrafast nonlinear Kerr effect in glass, and in Ar, N₂, and N₂O gases is measured, along with plasma generation in Ar. The inertial contribution to the nonlinear index from N₂ and N₂O molecular rotation is also observed.

© 2007 Optical Society of America

1. Cl. Froehly, A. Lacourt and J. Ch. Vienot, "Time impulse response and time frequency response of optical pupils.: Experimental confirmations and applications," Nouvelle Revue d’Optique 4, 183-196 (1973). [CrossRef]
2. E. Tokunaga, A. Terasaki, and T. Kobayashi, "Frequency-domain interferometer for femtosecond time-resolved phase spectroscopy," Opt. Lett. 17, 1131-1133 (1992). [CrossRef] [PubMed]
3. F. Reynaud, F. Salin, and A. Barthelemy, "Measurement of phase shifts introduced by nonlinear optical phenomena on subpicosecond pulses," Opt. Lett. 14, 275-277 (1989). [CrossRef] [PubMed]
4. C. X. Yu, M. Margalit, E. P. Ippen, and H. A. Haus, "Direct measurement of self-phase shift due to fiber nonlinearity," Opt. Lett. 23, 679-681 (1998). [CrossRef]
5. J. P. Geindre, P. Audebert, A. Rousse, F. Fallies, J. C. Gauthier, A. Mysyrowicz, A. Dos Santos, and G. Hamoniaux A. Antonetti, "Frequency-domain interferometer for measuring the phase and amplitude of a femtosecond pulse probing a laser-produced plasma," Opt. Lett. 19, 1997-1999 (1994). [CrossRef] [PubMed]
6. P. Salieres, L. LeDeroff, T. Auguste, P. Monot, P. d’Oliveira, D. Campo, J.-F. Hergott, H. Merdji, and B. Carre, "Frequency-Domain Interferometry in the XUV with High-Order Harmonics," Phys. Rev. Lett. 83, 5483-5486 (1999). [CrossRef]
7. R. Evans, A. D. Badger, F. Fallies, M. Mahdieh, T. A. Hall, P. Audebert, J.-P. Geindre, J.-C. Gauthier, A. Mysyrowicz, G. Grillon, and A. Antonetti, "Time- and space-resolved optical probing of femtosecond-laser-driven shock waves in aluminum," Phys. Rev. Lett. 77, 3359-3362 (1996). [CrossRef] [PubMed]
8. K. Y. Kim, I. Alexeev, E. Parra, and H. M. Milchberg, "Time-resolved explosion of intense-laser-heated clusters," Phys. Rev. Lett. 90, 023401 (2003); I. Alexeev, T. M. Antonsen, K. Y. Kim, and H. M. Milchberg, "Self- focusing of intense laser pulses in a clustered gas," Phys. Rev. Lett. 90, 103402 (2003). [CrossRef] [PubMed]
9. J. R. Marques, J. P. Geindre, F. Amiranoff, P. Audebert, J. C. Gauthier, A. Antonetti, and G. Grillon, "Temporal and spatial measurements of the electron density perturbation produced in the wake of an ultrashort laser pulse," Phys. Rev. Lett. 76, 3566-3569 (1996). [CrossRef] [PubMed]
10. C. W. Siders, S. P. Le Blanc, D. Fisher, T. Tajima, M. C. Downer, A. Babine, A. Stepanov, and A. Sergeev, "Laser Wakefield excitation and measurement by Femtosecond Longitudinal Interferometry," Phys. Rev. Lett. 76, 3570-3573 (1996). [CrossRef] [PubMed]
11. J. R. Marques, F. Dorchies, F. Amiranoff, P. Audebert, J. C. Gauthier, J. P. Geindre, A. Antonetti, T. M. Antonsen, Jr., P. Chessa, and P. Mora, "Laser Wakefield: experimental study of nonlinear radial electron oscillations," Phys. Plasmas 5, 1162-1177 (1998). [CrossRef]
12. A. Benuzzi-Mounaix, M. Koenig, J. M. Boudenne, T. A. Hall, D. Batani, F. Scianitti, A. Masini, and D. Di Santo, "Chirped pulse reflectivity and frequency domain interferometry in laser driven shock experiments," Phys. Rev. E 60, R2488-R2491 (1999). [CrossRef]
13. C. Y. Chien, B. La Fontaine, A. Desparois, Z. Jiang, T. W. Johnston, J. C. Kieffer, H. Pepin, F. Vidal, and H. P. Mercure, "Single-shot chirped-pulse spectral interferometry used to measure the femtosecond ionization dynamics of air," Opt. Lett. 25, 578-580 (2000). [CrossRef]
14. J. -P. Geindre, P. Audebert, S. Rebibo, and J. -C. Gauthier, "Single-shot spectral interferometry with chirped pulses," Opt. Lett. 26, 1612-1614 (2001). [CrossRef]
15. S. P. Le Blanc, E. W. Gaul, N. H. Matlis, A. Rundquist, and M. C. Downer, "Single-shot measurement of temporal phase shifts by frequency-domain holography," Opt. Lett. 25, 764-766 (2000). [CrossRef]
16. K. Y. Kim, I. Alexeev, and H. M. Milchberg, "Single-shot supercontinuum spectral interferometry," Appl. Phys. Lett. 81, 4124-4126 (2002). [CrossRef]
17. K. Kim, I. Alexeev, and H. Milchberg, "Single-shot measurement of laser-induced double step ionization of helium," Opt. Express 10, 1563-1572 (2002). [PubMed]
18. K. Y. Kim, I. Alexeev, V. Kumarappan, E. Parra, T. Antonsen, T. Taguchi, A. Gupta, and H. M. Milchberg, "Gases of exploding laser-heated cluster nanoplasmas as a nonlinear optical medium," Phys. Plasmas 11, 2882- 2889 (2004). [CrossRef]
19. K. Y. Kim, I. Alexeev, and H. M. Milchberg, "Measurement of ultrafast dynamics in the interaction of intense laser pulses with gases, clusters, and plasma waveguides," Phys. Plasmas 12, 056712 (2005). [CrossRef]
20. N. H. Matlis, S. Reed, S. S. Bulanov, V. Chvykov, G. Kalintchenko, T. Matsuoka, P. Rousseau, V. Yanovsky, A. Maksimchuk, S. Kalmykov, G. Shvets and M. C. Downer, "Snapshots of laser wakefields," Nature Phys. 2, 749-753 (2006). [CrossRef]
21. J. K. Ranka, R. S. Windeler, and A. J. Stentz, "Visible continuum generation in air silica microstructure optical fibers with anomalous dispersion at 800nm," Opt. Lett. 25, 25-27 (2000). [CrossRef]
22. J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006). [CrossRef]
23. P. B. Corkum, C. Rolland, and T. Srinivasan-Rao, "Supercontinuum Generation in Gases," Phys. Rev. Lett. 57, 2268-2271 (1986). [CrossRef] [PubMed]
24. P. O’Shea, M. Kimmel, X. Gu, and R. Trebino, "Highly simplified device for ultrashort-pulse measurement," Opt. Lett. 26, 932-934 (2001). [CrossRef]
25. P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics (Cambridge University Press, 1990).
26. S. Augst, A. Talebpour, S. L. Chin, Y. Beaudoin, and M. Chaker, "Nonsequential triple ionization of argon atoms in a high-intensity laser field," Phys. Rev. A 52, R917-R919 (1995); S. Geltman, "Multiple ionization of argon atoms by intense laser pulses," Phys. Rev. A 54, 2489-2491 (1996). [CrossRef] [PubMed]
27. D. Milam and M. J. Weber, "Measurement of nonlinear refractive-index coefficients using time-resolved interferometry: Application to optical materials for high-power neodymium lasers," J. Appl. Phys. 47, 2497-2501 (1976). [CrossRef]
28. R. Adair, L. L. Chase, and S. A. Payne, "Nonlinear refractive-index measurements of glasses using three-wave frequency mixing," J. Opt. Soc. Am. B 4, 875-881 (1987). [CrossRef]
29. M. Falconieri, E. Palange, and H. L. Fragnito, "Achievement of λ/4000 phase distortion sensitivity in the measurement of optical nonlinearities by using a modulated Z-scan technique," J. Opt. A: Pure Appl. Opt. 4, 404-407 (2002). [CrossRef]
30. H. J. Lehmeier, W. Leupacher, and A. Penzkofer, "Nonresonant third order hyperpolarizability of rare gases and N2 determined by third harmonic generation," Opt. Commun. 56, 67-72 (1985). [CrossRef]
31. B. Friedrich and D. Herschbach, "Alignment and trapping of molecules in intense laser fields," Phys. Rev. Lett. 74, 4623-4626 (1995). [CrossRef] [PubMed]
32. J.-F. Ripoche, G. Grillon, B. Prade, M. Franco, E. Nibbering, R. Lange, A. Mysyrowicz, "Determination of the time dependence of n2 in air," Opt. Commun. 135, 310-314 (1997). [CrossRef]
33. W. Demtroder, Molecular Physics (Wiley-VCH, Weinheim, 2005). [CrossRef]
34. R. A. Toth, "Line positions and strengths of N2O between 3515 and 7800 cm1," J.Mol. Spectrosc. 197, 158-187 (1999). [CrossRef] [PubMed]
35. P. W. Dooley, I. V. Litvinyuk, KevinF. Lee, D. M. Rayner, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Direct imaging of rotational wave-packet dynamics of diatomic molecules," Phys. Rev. A 68, 023406 (2003). [CrossRef]

Appl. Phys. Lett.

• K. Y. Kim, I. Alexeev, and H. M. Milchberg, "Single-shot supercontinuum spectral interferometry," Appl. Phys. Lett. 81, 4124-4126 (2002). [CrossRef]

J. Appl. Phys.

• D. Milam and M. J. Weber, "Measurement of nonlinear refractive-index coefficients using time-resolved interferometry: Application to optical materials for high-power neodymium lasers," J. Appl. Phys. 47, 2497-2501 (1976). [CrossRef]

J. Opt. A: Pure Appl. Opt.

• M. Falconieri, E. Palange, and H. L. Fragnito, "Achievement of λ/4000 phase distortion sensitivity in the measurement of optical nonlinearities by using a modulated Z-scan technique," J. Opt. A: Pure Appl. Opt. 4, 404-407 (2002). [CrossRef]

J. Opt. Soc. Am. B

• R. Adair, L. L. Chase, and S. A. Payne, "Nonlinear refractive-index measurements of glasses using three-wave frequency mixing," J. Opt. Soc. Am. B 4, 875-881 (1987). [CrossRef]

J.Mol. Spectrosc.

• R. A. Toth, "Line positions and strengths of N2O between 3515 and 7800 cm1," J.Mol. Spectrosc. 197, 158-187 (1999). [CrossRef] [PubMed]

Nature Phys.

• N. H. Matlis, S. Reed, S. S. Bulanov, V. Chvykov, G. Kalintchenko, T. Matsuoka, P. Rousseau, V. Yanovsky, A. Maksimchuk, S. Kalmykov, G. Shvets and M. C. Downer, "Snapshots of laser wakefields," Nature Phys. 2, 749-753 (2006). [CrossRef]

Nouvelle Revue d’Optique

• Cl. Froehly, A. Lacourt and J. Ch. Vienot, "Time impulse response and time frequency response of optical pupils.: Experimental confirmations and applications," Nouvelle Revue d’Optique 4, 183-196 (1973). [CrossRef]

Opt. Commun.

• H. J. Lehmeier, W. Leupacher, and A. Penzkofer, "Nonresonant third order hyperpolarizability of rare gases and N2 determined by third harmonic generation," Opt. Commun. 56, 67-72 (1985). [CrossRef]
• J.-F. Ripoche, G. Grillon, B. Prade, M. Franco, E. Nibbering, R. Lange, A. Mysyrowicz, "Determination of the time dependence of n2 in air," Opt. Commun. 135, 310-314 (1997). [CrossRef]

Opt. Express

• K. Kim, I. Alexeev, and H. Milchberg, "Single-shot measurement of laser-induced double step ionization of helium," Opt. Express 10, 1563-1572 (2002). [PubMed]

Opt. Lett.

• C. Y. Chien, B. La Fontaine, A. Desparois, Z. Jiang, T. W. Johnston, J. C. Kieffer, H. Pepin, F. Vidal, and H. P. Mercure, "Single-shot chirped-pulse spectral interferometry used to measure the femtosecond ionization dynamics of air," Opt. Lett. 25, 578-580 (2000). [CrossRef]
• J. -P. Geindre, P. Audebert, S. Rebibo, and J. -C. Gauthier, "Single-shot spectral interferometry with chirped pulses," Opt. Lett. 26, 1612-1614 (2001). [CrossRef]
• S. P. Le Blanc, E. W. Gaul, N. H. Matlis, A. Rundquist, and M. C. Downer, "Single-shot measurement of temporal phase shifts by frequency-domain holography," Opt. Lett. 25, 764-766 (2000). [CrossRef]
• E. Tokunaga, A. Terasaki, and T. Kobayashi, "Frequency-domain interferometer for femtosecond time-resolved phase spectroscopy," Opt. Lett. 17, 1131-1133 (1992). [CrossRef] [PubMed]
• F. Reynaud, F. Salin, and A. Barthelemy, "Measurement of phase shifts introduced by nonlinear optical phenomena on subpicosecond pulses," Opt. Lett. 14, 275-277 (1989). [CrossRef] [PubMed]
• C. X. Yu, M. Margalit, E. P. Ippen, and H. A. Haus, "Direct measurement of self-phase shift due to fiber nonlinearity," Opt. Lett. 23, 679-681 (1998). [CrossRef]
• J. P. Geindre, P. Audebert, A. Rousse, F. Fallies, J. C. Gauthier, A. Mysyrowicz, A. Dos Santos, and G. Hamoniaux A. Antonetti, "Frequency-domain interferometer for measuring the phase and amplitude of a femtosecond pulse probing a laser-produced plasma," Opt. Lett. 19, 1997-1999 (1994). [CrossRef] [PubMed]
• J. K. Ranka, R. S. Windeler, and A. J. Stentz, "Visible continuum generation in air silica microstructure optical fibers with anomalous dispersion at 800nm," Opt. Lett. 25, 25-27 (2000). [CrossRef]
• P. O’Shea, M. Kimmel, X. Gu, and R. Trebino, "Highly simplified device for ultrashort-pulse measurement," Opt. Lett. 26, 932-934 (2001). [CrossRef]

Phys. Plasmas

• J. R. Marques, F. Dorchies, F. Amiranoff, P. Audebert, J. C. Gauthier, J. P. Geindre, A. Antonetti, T. M. Antonsen, Jr., P. Chessa, and P. Mora, "Laser Wakefield: experimental study of nonlinear radial electron oscillations," Phys. Plasmas 5, 1162-1177 (1998). [CrossRef]
• K. Y. Kim, I. Alexeev, V. Kumarappan, E. Parra, T. Antonsen, T. Taguchi, A. Gupta, and H. M. Milchberg, "Gases of exploding laser-heated cluster nanoplasmas as a nonlinear optical medium," Phys. Plasmas 11, 2882- 2889 (2004). [CrossRef]
• K. Y. Kim, I. Alexeev, and H. M. Milchberg, "Measurement of ultrafast dynamics in the interaction of intense laser pulses with gases, clusters, and plasma waveguides," Phys. Plasmas 12, 056712 (2005). [CrossRef]

Phys. Rev. A

• S. Augst, A. Talebpour, S. L. Chin, Y. Beaudoin, and M. Chaker, "Nonsequential triple ionization of argon atoms in a high-intensity laser field," Phys. Rev. A 52, R917-R919 (1995); S. Geltman, "Multiple ionization of argon atoms by intense laser pulses," Phys. Rev. A 54, 2489-2491 (1996). [CrossRef] [PubMed]
• P. W. Dooley, I. V. Litvinyuk, KevinF. Lee, D. M. Rayner, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Direct imaging of rotational wave-packet dynamics of diatomic molecules," Phys. Rev. A 68, 023406 (2003). [CrossRef]

Phys. Rev. E

• A. Benuzzi-Mounaix, M. Koenig, J. M. Boudenne, T. A. Hall, D. Batani, F. Scianitti, A. Masini, and D. Di Santo, "Chirped pulse reflectivity and frequency domain interferometry in laser driven shock experiments," Phys. Rev. E 60, R2488-R2491 (1999). [CrossRef]

Phys. Rev. Lett.

• P. Salieres, L. LeDeroff, T. Auguste, P. Monot, P. d’Oliveira, D. Campo, J.-F. Hergott, H. Merdji, and B. Carre, "Frequency-Domain Interferometry in the XUV with High-Order Harmonics," Phys. Rev. Lett. 83, 5483-5486 (1999). [CrossRef]
• R. Evans, A. D. Badger, F. Fallies, M. Mahdieh, T. A. Hall, P. Audebert, J.-P. Geindre, J.-C. Gauthier, A. Mysyrowicz, G. Grillon, and A. Antonetti, "Time- and space-resolved optical probing of femtosecond-laser-driven shock waves in aluminum," Phys. Rev. Lett. 77, 3359-3362 (1996). [CrossRef] [PubMed]
• K. Y. Kim, I. Alexeev, E. Parra, and H. M. Milchberg, "Time-resolved explosion of intense-laser-heated clusters," Phys. Rev. Lett. 90, 023401 (2003); I. Alexeev, T. M. Antonsen, K. Y. Kim, and H. M. Milchberg, "Self- focusing of intense laser pulses in a clustered gas," Phys. Rev. Lett. 90, 103402 (2003). [CrossRef] [PubMed]
• J. R. Marques, J. P. Geindre, F. Amiranoff, P. Audebert, J. C. Gauthier, A. Antonetti, and G. Grillon, "Temporal and spatial measurements of the electron density perturbation produced in the wake of an ultrashort laser pulse," Phys. Rev. Lett. 76, 3566-3569 (1996). [CrossRef] [PubMed]
• C. W. Siders, S. P. Le Blanc, D. Fisher, T. Tajima, M. C. Downer, A. Babine, A. Stepanov, and A. Sergeev, "Laser Wakefield excitation and measurement by Femtosecond Longitudinal Interferometry," Phys. Rev. Lett. 76, 3570-3573 (1996). [CrossRef] [PubMed]
• B. Friedrich and D. Herschbach, "Alignment and trapping of molecules in intense laser fields," Phys. Rev. Lett. 74, 4623-4626 (1995). [CrossRef] [PubMed]
• P. B. Corkum, C. Rolland, and T. Srinivasan-Rao, "Supercontinuum Generation in Gases," Phys. Rev. Lett. 57, 2268-2271 (1986). [CrossRef] [PubMed]

Rev. Mod. Phys.

• J. M. Dudley, G. Genty, and S. Coen, "Supercontinuum generation in photonic crystal fiber," Rev. Mod. Phys. 78, 1135-1184 (2006). [CrossRef]

Other

• P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics (Cambridge University Press, 1990).
• W. Demtroder, Molecular Physics (Wiley-VCH, Weinheim, 2005). [CrossRef]

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