Abstract

Field-free alignment of N2, O2, CO, CO2, CS2, and C2H4 molecules was experimentally achieved at room temperature by using 800 nm, 110 fs laser pulses at an intensity of 6×1013 W/cm2. An enhanced degree of alignment was also demonstrated by using two pulses with appropriate separation times. These results indicate that multi-pulse alignment is a feasible approach to provide macroscopic ensembles of highly aligned molecules for practical applications.

© 2006 Optical Society of America

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  1. P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
    [CrossRef]
  2. H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
    [CrossRef]
  3. L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
    [CrossRef] [PubMed]
  4. J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
    [CrossRef]
  5. T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
    [CrossRef]
  6. T. Seideman, "Revival structure of aligned rotational wave packets," Phys. Rev. Lett. 83, 4971 (1999).
    [CrossRef]
  7. F. Rosca-Pruna, M. J. J. Vrakking, "Experimental observation of revival structures in picosecond laser-induced alignment of I2," Phys. Rev. Lett. 87, 153902 (2001).
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  8. E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
    [CrossRef]
  9. R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
    [CrossRef]
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    [CrossRef] [PubMed]
  12. M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
    [CrossRef] [PubMed]
  13. S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
    [CrossRef] [PubMed]
  14. P. W. Dooley, I. V. Litvinyuk, K. F. 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]
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    [CrossRef] [PubMed]
  16. V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
    [CrossRef] [PubMed]
  17. A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
    [CrossRef]
  18. V. Renard, O. Faucher, and B. Lavorel, "Measurement of laser-induced alignment of molecules by cross defocusing," Opt. Lett. 30, 70-72 (2005).
    [CrossRef] [PubMed]
  19. S. Zamith, Z. Ansari, F. Lepine, and M. J. J. Vrakking, "Single-shot measurement of revival structures in femtosecond laser-induced alignment of molecules," Opt. Lett. 30, 2326-2328 (2005).
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    [CrossRef] [PubMed]
  22. I. Sh. Averbukh, and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 87, 163601 (2001).
    [CrossRef] [PubMed]
  23. M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
    [CrossRef]
  24. K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
    [CrossRef]

2006

S. Ramakrishna, and T. Seideman, "Dissipative dynamics of laser induced nonadiabatic molecular alignment," J. Chem. Phys. 124, 034101 (2006).
[CrossRef] [PubMed]

2005

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
[CrossRef]

J. G. Underwood, B. J. Sussman, and A. Stolow, "Field-free three dimensional molecular axis alignment," Phys. Rev. Lett. 94, 143002 (2005).
[CrossRef] [PubMed]

T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
[CrossRef]

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

V. Renard, O. Faucher, and B. Lavorel, "Measurement of laser-induced alignment of molecules by cross defocusing," Opt. Lett. 30, 70-72 (2005).
[CrossRef] [PubMed]

S. Zamith, Z. Ansari, F. Lepine, and M. J. J. Vrakking, "Single-shot measurement of revival structures in femtosecond laser-induced alignment of molecules," Opt. Lett. 30, 2326-2328 (2005).
[CrossRef] [PubMed]

2004

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
[CrossRef] [PubMed]

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

2003

M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
[CrossRef]

H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

2002

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

2001

F. Rosca-Pruna, M. J. J. Vrakking, "Experimental observation of revival structures in picosecond laser-induced alignment of I2," Phys. Rev. Lett. 87, 153902 (2001).
[CrossRef] [PubMed]

I. Sh. Averbukh, and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 87, 163601 (2001).
[CrossRef] [PubMed]

1999

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

T. Seideman, "Revival structure of aligned rotational wave packets," Phys. Rev. Lett. 83, 4971 (1999).
[CrossRef]

Ansari, Z.

Arvieu, R.

I. Sh. Averbukh, and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 87, 163601 (2001).
[CrossRef] [PubMed]

Aseyev, S.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Averbukh, I. Sh.

M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
[CrossRef]

I. Sh. Averbukh, and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 87, 163601 (2001).
[CrossRef] [PubMed]

Bisgaard, C. Z.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

Corkum, P. B.

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

de Nalda, R.

R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
[CrossRef]

Dietrich, P.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Dooley, P. W.

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

Ejdrup, T.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

Ellert, C.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Faucher, O.

V. Renard, O. Faucher, and B. Lavorel, "Measurement of laser-induced alignment of molecules by cross defocusing," Opt. Lett. 30, 70-72 (2005).
[CrossRef] [PubMed]

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Guerin, S.

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Hamilton, E.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

Hankin, S.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Herrmann, J.

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

Itatani, J.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Ivanov, M.

M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
[CrossRef] [PubMed]

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

Jauslin, H. R.

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Kalosha, V.

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

Kanai, T.

T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
[CrossRef]

Kieffer, J. C.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Lavorel, B.

V. Renard, O. Faucher, and B. Lavorel, "Measurement of laser-induced alignment of molecules by cross defocusing," Opt. Lett. 30, 70-72 (2005).
[CrossRef] [PubMed]

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Lee, K. F.

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

Leibsher, M.

M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
[CrossRef]

Lepine, F.

Levesque, J.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Litvinyuk, I. V.

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

Litvinyuk, L. V.

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

Marangos, J. P.

R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
[CrossRef]

Mehendale, M.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Minemoto, S.

T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
[CrossRef]

Niikura, H.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Pashayan, Y. T

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Patchkovskii, S.

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

Pepin, H.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Peronne, E.

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

Poulsen, M. D.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

Rabitz, H.

M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
[CrossRef]

Ramakrishna, S.

S. Ramakrishna, and T. Seideman, "Dissipative dynamics of laser induced nonadiabatic molecular alignment," J. Chem. Phys. 124, 034101 (2006).
[CrossRef] [PubMed]

Rayner, D.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Rayner, D. M.

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

Renard, M.

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Renard, V.

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

V. Renard, O. Faucher, and B. Lavorel, "Measurement of laser-induced alignment of molecules by cross defocusing," Opt. Lett. 30, 70-72 (2005).
[CrossRef] [PubMed]

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

Rosca-Pruna, F.

F. Rosca-Pruna, M. J. J. Vrakking, "Experimental observation of revival structures in picosecond laser-induced alignment of I2," Phys. Rev. Lett. 87, 153902 (2001).
[CrossRef] [PubMed]

Rouzee, A.

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

Sakai, H.

T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
[CrossRef]

Seideman, T.

S. Ramakrishna, and T. Seideman, "Dissipative dynamics of laser induced nonadiabatic molecular alignment," J. Chem. Phys. 124, 034101 (2006).
[CrossRef] [PubMed]

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

T. Seideman, "Revival structure of aligned rotational wave packets," Phys. Rev. Lett. 83, 4971 (1999).
[CrossRef]

Shapiro, E. A.

M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
[CrossRef] [PubMed]

Spanner, M.

M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
[CrossRef] [PubMed]

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

Stapelfeldt, H.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

Stolow, A.

J. G. Underwood, B. J. Sussman, and A. Stolow, "Field-free three dimensional molecular axis alignment," Phys. Rev. Lett. 94, 143002 (2005).
[CrossRef] [PubMed]

Sussman, B. J.

J. G. Underwood, B. J. Sussman, and A. Stolow, "Field-free three dimensional molecular axis alignment," Phys. Rev. Lett. 94, 143002 (2005).
[CrossRef] [PubMed]

Torres, R.

R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
[CrossRef]

Underwood, J. G.

J. G. Underwood, B. J. Sussman, and A. Stolow, "Field-free three dimensional molecular axis alignment," Phys. Rev. Lett. 94, 143002 (2005).
[CrossRef] [PubMed]

Viftrup, S. S.

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

Villeneuve, D.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

Villeneuve, D. M.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

Vrakking, M. J. J.

S. Zamith, Z. Ansari, F. Lepine, and M. J. J. Vrakking, "Single-shot measurement of revival structures in femtosecond laser-induced alignment of molecules," Opt. Lett. 30, 2326-2328 (2005).
[CrossRef] [PubMed]

F. Rosca-Pruna, M. J. J. Vrakking, "Experimental observation of revival structures in picosecond laser-induced alignment of I2," Phys. Rev. Lett. 87, 153902 (2001).
[CrossRef] [PubMed]

Yudin, G. L.

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

Yurchenko, S. N.

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

Zamith, S.

Zeidler, D.

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

Faraday Discuss.

P. B. Corkum, C. Ellert, M. Mehendale, P. Dietrich, S. Hankin, S. Aseyev, D. Rayner, and D. Villeneuve, "Molecular science with strong laser fields," Faraday Discuss. 113, 47-59 (1999).
[CrossRef]

J. Chem. Phys.

S. Ramakrishna, and T. Seideman, "Dissipative dynamics of laser induced nonadiabatic molecular alignment," J. Chem. Phys. 124, 034101 (2006).
[CrossRef] [PubMed]

J. Phys. B

K. F. Lee, I. V. Litvinyuk, P. W. Dooley, M. Spanner, D. M. Villeneuve, and P. B. Corkum, "Two-pulse alignment of molecules," J. Phys. B 37, 43-48, (2004).
[CrossRef]

A. Rouzee, V. Renard, B. Lavorel, and O. Faucher, "Laser spatial profile effects in measurements of impulsive molecular alignment," J. Phys. B 38, 2329-2335 (2005).
[CrossRef]

Nature (London)

J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, "Tomographic imaging of molecular orbitals," Nature (London) 432, 867-871 (2004).
[CrossRef]

T. Kanai, S. Minemoto, and H. Sakai, "Quantum interference during high-order harmonic generation from aligned molecules," Nature (London) 435, 470-474 (2005).
[CrossRef]

Opt. Lett.

Phys. Rev. A

P. W. Dooley, I. V. Litvinyuk, K. F. 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]

E. Hamilton, T. Seideman, T. Ejdrup, M. D. Poulsen, C. Z. Bisgaard, S. S. Viftrup, and H. Stapelfeldt, "Alignment of symmetric top molecules by short laser pulses," Phys. Rev. A 72, 043402 (2005).
[CrossRef]

R. Torres, R. de Nalda, and J. P. Marangos, "Dynamics of laser-induced molecular alignment in the impulsive and adiabatic regimes: A direct comparison," Phys. Rev. A 72, 023420 (2005).
[CrossRef]

Phys. Rev. Lett.

J. G. Underwood, B. J. Sussman, and A. Stolow, "Field-free three dimensional molecular axis alignment," Phys. Rev. Lett. 94, 143002 (2005).
[CrossRef] [PubMed]

V. Kalosha, M. Spanner, J. Herrmann, and M. Ivanov, "Generation of single dispersion precompensated 1-fs pulses by shaped-pulse optimized high-order stimulated Raman scattering," Phys. Rev. Lett. 88, 103901 (2002).
[CrossRef] [PubMed]

M. Spanner, E. A. Shapiro, and M. Ivanov, "Coherent control of rotational wave-packet dynamics via fractional revivals," Phys. Rev. Lett. 92, 093001 (2004).
[CrossRef] [PubMed]

S. N. Yurchenko, S. Patchkovskii, L. V. Litvinyuk, P. B. Corkum, and G. L. Yudin, "Laser-induced interference, focusing, and diffraction of rescattering molecular photoelectrons," Phys. Rev. Lett. 93, 223003 (2004).
[CrossRef] [PubMed]

T. Seideman, "Revival structure of aligned rotational wave packets," Phys. Rev. Lett. 83, 4971 (1999).
[CrossRef]

F. Rosca-Pruna, M. J. J. Vrakking, "Experimental observation of revival structures in picosecond laser-induced alignment of I2," Phys. Rev. Lett. 87, 153902 (2001).
[CrossRef] [PubMed]

C. Z. Bisgaard, M. D. Poulsen, E. Peronne, S. S. Viftrup, and H. Stapelfeldt, "Observation of enhanced field-free molecular alignment by two laser pulses," Phys. Rev. Lett. 92, 173004 (2004).
[CrossRef] [PubMed]

V. Renard, M. Renard, S. Guerin, Y. T Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, "Postpulse molecular alignment measured by a weak field polarization technique," Phys. Rev. Lett. 90, 153601 (2003).
[CrossRef] [PubMed]

L. V. Litvinyuk, K. F. Lee, P. W. Dooley, D. M. Rayner, D. M. Villeneuve, and P. B. Corkum, "Alignment-dependent strong field ionization of molecules," Phys. Rev. Lett. 90, 233003 (2003).
[CrossRef] [PubMed]

I. Sh. Averbukh, and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 87, 163601 (2001).
[CrossRef] [PubMed]

M. Leibsher, I. Sh. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, 213001 (2003).
[CrossRef]

Rev. Mod. Phys.

H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

Other

G. Herzberg, Molecular spectra and molecular structure, (Van Nostrand Reinhold Company Ltd., 1966).

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Figures (5)

Fig. 1.
Fig. 1.

Experimental setup for measuring field-free alignment of molecules induced by femtosecond laser pulses. BS: beam splitter

Fig. 2.
Fig. 2.

Field-free alignment signal for diatomic molecules (a) N2, (b) O2, and (c) CO irradiated by 800 nm, 110 fs pulses at an intensity of 6×1013 W/cm2

Fig. 3.
Fig. 3.

Field-free alignment signal for polyatomic molecules (a) CO2, (b) CS2, and (c) C2H4 irradiated by 800 nm, 110 fs pulses at an intensity of 6×1013 W/cm2

Fig. 4.
Fig. 4.

Field-free alignment signal of CS2 under different laser intensities

Fig. 5.
Fig. 5.

Field-free alignment signal of CS2. (Lower) Single-pulse alignment signal illustrates the pulse timing for the double-pulse experiment. (Upper) The red line represents the alignment signal at 3Tr /4 induced by the first aligning laser pulse alone, the green line represents the alignment signal at Tr /2 induced by the second aligning laser pulse alone, the black line represents the enhanced alignment signal induced by the two aligning laser pulses with appropriate separation times.

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