Abstract

The full transient macroscopic linear optical susceptibility tensor induced in a transiently aligned molecular gas by a single, linearly polarized intense alignment pulse is studied. We determine the optimal properties of the pulse that forms the rotational wave packet. Significantly, we demonstrate that the optimal pulse for phase modulation differs from the optimal alignment pulse. Finally, we show that the limited information about rotational wave packets obtained by measuring the linear optical susceptibility can be augmented by also measuring the time-varying nonlinear optical susceptibilities.

© 2006 Optical Society of America

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  1. R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
    [PubMed]
  2. S. E. Harris and A. V. Sokolov, "Broadband spectral generation with refractive index control," Phys. Rev. A 55, 4019-4022 (1997).
    [CrossRef]
  3. S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
    [CrossRef]
  4. N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88, (2002).
    [CrossRef] [PubMed]
  5. R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
    [CrossRef] [PubMed]
  6. R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
    [CrossRef]
  7. J. P. Heritage, T. K. Gustafson, and C. H. Lin, "Observation of Coherent Transient Birefringence in Cs2 Vapor," Phys. Rev. Lett. 34, 1299-1302 (1975).
    [CrossRef]
  8. C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
    [CrossRef]
  9. H. Stapelfeldt and T. Seideman, "Colloquium: Aligning molecules with strong laser pulses," Rev. Mod. Phys. 75, 543-557 (2003).
    [CrossRef]
  10. I. S. Averbukh and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 8716, 163,601 (2001).
  11. M. Leibscher, I. S. Averbukh, and H. Rabitz, "Molecular alignment by trains of short laser pulses," Phys. Rev. Lett. 90, (2003).
    [CrossRef] [PubMed]
  12. 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, (2004).
    [CrossRef] [PubMed]
  13. P. M. Felker, "Rotational Coherence Spectroscopy - Studies of the Geometries of Large Gas-Phase Species by Picosecond Time-Domain Methods," J. Phys. Chem. 96, 7844-7857 (1992).
    [CrossRef]
  14. M. Gruebele and A. H. Zewail, "FemtosecondWave Packet Spectroscopy - Coherences, the Potential, and Structural Determination," J. Chem. Phys. 98, 883-902 (1993).
    [CrossRef]
  15. R. A. Bartels, N. L. Wagner, M. D. Baertschy, J. Wyss, M. M. Murnane, and H. C. Kapteyn, "Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases," Opt. Lett. 28, 346-348 (2003).
    [CrossRef] [PubMed]
  16. K. Hartinger, S. Nirmalgandhi, J. Wilson, and R. A. Bartels, "Efficient nonlinear frequency conversion with a dynamically structured nonlinearity," Opt. Express 13, 6919-6930 (2005); http://www.opticsinfobase.org/abstract.cfm?URI=oe-13-18-6919.
    [CrossRef] [PubMed]
  17. B. Friedrich and D. Herschbach, "Polarization of molecules induced by intense nonresonant laser fields," J. Phys. Chem. 99, 15,686-15,693 (1995).
    [CrossRef]
  18. B. Friedrich and D. Herschbach, "Alignment and Trapping of Molecules in Intense Laser Fields," Phys. Rev. Lett. 74, 4623-4626 (1995).
    [CrossRef] [PubMed]
  19. G. Herzberg, Molecular spectra and molecular structure (Krieger, 1950).
  20. J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
    [CrossRef]
  21. J. D. Le Grange, M. G. Kuzyk, and K. D. Singer, "Effects of order on nonlinear optical processes in organic molecular materials," Mol. Cryst. Liq. Cryst. 150, 567-605 (1987).
  22. B. Friedrich, P. P.D., and D. Herschbach, "Alignment and orientation of rotationally cool molecules," J. Phys. Chem. 95, 8118-8129 (1991).
    [CrossRef]
  23. M. Machholm, "Postpulse alignment of molecules robust to thermal averaging," J. Chem. Phys. 115, 10,724-10,730 (2001).
    [CrossRef]
  24. M. Comstock, V. V. Lozovoy, and M. Dantus, "Rotational wavepacket revivals for phase modulation of ultrafast pulses," Chem. Phys. Lett. 372, 739-744 (2003).
    [CrossRef]

2005 (1)

2004 (1)

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, (2004).
[CrossRef] [PubMed]

2003 (5)

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

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

R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
[CrossRef]

M. Comstock, V. V. Lozovoy, and M. Dantus, "Rotational wavepacket revivals for phase modulation of ultrafast pulses," Chem. Phys. Lett. 372, 739-744 (2003).
[CrossRef]

R. A. Bartels, N. L. Wagner, M. D. Baertschy, J. Wyss, M. M. Murnane, and H. C. Kapteyn, "Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases," Opt. Lett. 28, 346-348 (2003).
[CrossRef] [PubMed]

2002 (3)

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88, (2002).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
[CrossRef] [PubMed]

2001 (2)

I. S. Averbukh and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 8716, 163,601 (2001).

M. Machholm, "Postpulse alignment of molecules robust to thermal averaging," J. Chem. Phys. 115, 10,724-10,730 (2001).
[CrossRef]

1999 (1)

J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
[CrossRef]

1998 (1)

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

1997 (1)

S. E. Harris and A. V. Sokolov, "Broadband spectral generation with refractive index control," Phys. Rev. A 55, 4019-4022 (1997).
[CrossRef]

1995 (2)

B. Friedrich and D. Herschbach, "Polarization of molecules induced by intense nonresonant laser fields," J. Phys. Chem. 99, 15,686-15,693 (1995).
[CrossRef]

B. Friedrich and D. Herschbach, "Alignment and Trapping of Molecules in Intense Laser Fields," Phys. Rev. Lett. 74, 4623-4626 (1995).
[CrossRef] [PubMed]

1993 (1)

M. Gruebele and A. H. Zewail, "FemtosecondWave Packet Spectroscopy - Coherences, the Potential, and Structural Determination," J. Chem. Phys. 98, 883-902 (1993).
[CrossRef]

1992 (1)

P. M. Felker, "Rotational Coherence Spectroscopy - Studies of the Geometries of Large Gas-Phase Species by Picosecond Time-Domain Methods," J. Phys. Chem. 96, 7844-7857 (1992).
[CrossRef]

1991 (1)

B. Friedrich, P. P.D., and D. Herschbach, "Alignment and orientation of rotationally cool molecules," J. Phys. Chem. 95, 8118-8129 (1991).
[CrossRef]

1987 (1)

J. D. Le Grange, M. G. Kuzyk, and K. D. Singer, "Effects of order on nonlinear optical processes in organic molecular materials," Mol. Cryst. Liq. Cryst. 150, 567-605 (1987).

1976 (1)

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

1975 (1)

J. P. Heritage, T. K. Gustafson, and C. H. Lin, "Observation of Coherent Transient Birefringence in Cs2 Vapor," Phys. Rev. Lett. 34, 1299-1302 (1975).
[CrossRef]

Arvieu, R.

I. S. Averbukh and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 8716, 163,601 (2001).

Averbukh, I. S.

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

I. S. Averbukh and R. Arvieu, "Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor," Phys. Rev. Lett. 8716, 163,601 (2001).

Backus, S.

R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
[CrossRef]

Baertschy, M.

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

Baertschy, M. D.

Bartels, R. A.

K. Hartinger, S. Nirmalgandhi, J. Wilson, and R. A. Bartels, "Efficient nonlinear frequency conversion with a dynamically structured nonlinearity," Opt. Express 13, 6919-6930 (2005); http://www.opticsinfobase.org/abstract.cfm?URI=oe-13-18-6919.
[CrossRef] [PubMed]

R. A. Bartels, N. L. Wagner, M. D. Baertschy, J. Wyss, M. M. Murnane, and H. C. Kapteyn, "Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases," Opt. Lett. 28, 346-348 (2003).
[CrossRef] [PubMed]

R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
[CrossRef]

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
[CrossRef] [PubMed]

Bisgaard, C. Z.

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, (2004).
[CrossRef] [PubMed]

Chiao, R. Y.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

Comstock, M.

M. Comstock, V. V. Lozovoy, and M. Dantus, "Rotational wavepacket revivals for phase modulation of ultrafast pulses," Chem. Phys. Lett. 372, 739-744 (2003).
[CrossRef]

Dantus, M.

M. Comstock, V. V. Lozovoy, and M. Dantus, "Rotational wavepacket revivals for phase modulation of ultrafast pulses," Chem. Phys. Lett. 372, 739-744 (2003).
[CrossRef]

Felker, P. M.

P. M. Felker, "Rotational Coherence Spectroscopy - Studies of the Geometries of Large Gas-Phase Species by Picosecond Time-Domain Methods," J. Phys. Chem. 96, 7844-7857 (1992).
[CrossRef]

Friedrich, B.

J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
[CrossRef]

B. Friedrich and D. Herschbach, "Alignment and Trapping of Molecules in Intense Laser Fields," Phys. Rev. Lett. 74, 4623-4626 (1995).
[CrossRef] [PubMed]

B. Friedrich and D. Herschbach, "Polarization of molecules induced by intense nonresonant laser fields," J. Phys. Chem. 99, 15,686-15,693 (1995).
[CrossRef]

B. Friedrich, P. P.D., and D. Herschbach, "Alignment and orientation of rotationally cool molecules," J. Phys. Chem. 95, 8118-8129 (1991).
[CrossRef]

Greene, C. H.

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

Gruebele, M.

M. Gruebele and A. H. Zewail, "FemtosecondWave Packet Spectroscopy - Coherences, the Potential, and Structural Determination," J. Chem. Phys. 98, 883-902 (1993).
[CrossRef]

Gupta, M.

J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
[CrossRef]

Gustafson, T. K.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

J. P. Heritage, T. K. Gustafson, and C. H. Lin, "Observation of Coherent Transient Birefringence in Cs2 Vapor," Phys. Rev. Lett. 34, 1299-1302 (1975).
[CrossRef]

Harris, S. E.

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

S. E. Harris and A. V. Sokolov, "Broadband spectral generation with refractive index control," Phys. Rev. A 55, 4019-4022 (1997).
[CrossRef]

Hartinger, K.

Heritage, J. P.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

J. P. Heritage, T. K. Gustafson, and C. H. Lin, "Observation of Coherent Transient Birefringence in Cs2 Vapor," Phys. Rev. Lett. 34, 1299-1302 (1975).
[CrossRef]

Herschbach, D.

B. Friedrich and D. Herschbach, "Alignment and Trapping of Molecules in Intense Laser Fields," Phys. Rev. Lett. 74, 4623-4626 (1995).
[CrossRef] [PubMed]

B. Friedrich and D. Herschbach, "Polarization of molecules induced by intense nonresonant laser fields," J. Phys. Chem. 99, 15,686-15,693 (1995).
[CrossRef]

Kapteyn, H. C.

R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
[CrossRef]

R. A. Bartels, N. L. Wagner, M. D. Baertschy, J. Wyss, M. M. Murnane, and H. C. Kapteyn, "Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases," Opt. Lett. 28, 346-348 (2003).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
[CrossRef] [PubMed]

Korn, G.

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88, (2002).
[CrossRef] [PubMed]

Kuzyk, M. G.

J. D. Le Grange, M. G. Kuzyk, and K. D. Singer, "Effects of order on nonlinear optical processes in organic molecular materials," Mol. Cryst. Liq. Cryst. 150, 567-605 (1987).

Le Grange, J. D.

J. D. Le Grange, M. G. Kuzyk, and K. D. Singer, "Effects of order on nonlinear optical processes in organic molecular materials," Mol. Cryst. Liq. Cryst. 150, 567-605 (1987).

Leibscher, M.

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

Leone, S. R.

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
[CrossRef] [PubMed]

Lin, C. H.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

J. P. Heritage, T. K. Gustafson, and C. H. Lin, "Observation of Coherent Transient Birefringence in Cs2 Vapor," Phys. Rev. Lett. 34, 1299-1302 (1975).
[CrossRef]

Lozovoy, V. V.

M. Comstock, V. V. Lozovoy, and M. Dantus, "Rotational wavepacket revivals for phase modulation of ultrafast pulses," Chem. Phys. Lett. 372, 739-744 (2003).
[CrossRef]

Machholm, M.

M. Machholm, "Postpulse alignment of molecules robust to thermal averaging," J. Chem. Phys. 115, 10,724-10,730 (2001).
[CrossRef]

McTague, J. P.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, "Birefringence Arising from Reorientation of Polarizability Anisotropy of Molecules in Collisionless Gases," Phys. Rev. A 13, 813-829 (1976).
[CrossRef]

Murnane, M. M.

R. A. Bartels, S. Backus, M. M. Murnane, and H. C. Kapteyn, "Impulsive stimulated Raman scattering of molecular vibrations using nonlinear pulse shaping," Chem. Phys. Lett. 374, 326-333 (2003).
[CrossRef]

R. A. Bartels, N. L. Wagner, M. D. Baertschy, J. Wyss, M. M. Murnane, and H. C. Kapteyn, "Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases," Opt. Lett. 28, 346-348 (2003).
[CrossRef] [PubMed]

R. A. Bartels, T. C. Weinacht, N. Wagner, M. Baertschy, C. H. Greene, M. M. Murnane, and H. C. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88, (2002).
[PubMed]

R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, "Nonresonant control of multimode molecular wave packets at room temperature," Phys. Rev. Lett. 88(2) (2002).
[CrossRef] [PubMed]

Nirmalgandhi, S.

Ortigoso, J.

J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
[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, (2004).
[CrossRef] [PubMed]

Poulsen, M. D.

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, (2004).
[CrossRef] [PubMed]

Rabitz, H.

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

Rodriguez, M.

J. Ortigoso, M. Rodriguez, M. Gupta, and B. Friedrich, "Time evolution of pendular states created by the interaction of molecular polarizability with a pulsed nonresonant laser field," J. Chem. Phys. 110, 3870-3875 (1999).
[CrossRef]

Seideman, T.

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

Singer, K. D.

J. D. Le Grange, M. G. Kuzyk, and K. D. Singer, "Effects of order on nonlinear optical processes in organic molecular materials," Mol. Cryst. Liq. Cryst. 150, 567-605 (1987).

Sokolov, A. V.

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

S. E. Harris and A. V. Sokolov, "Broadband spectral generation with refractive index control," Phys. Rev. A 55, 4019-4022 (1997).
[CrossRef]

Stapelfeldt, H.

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, (2004).
[CrossRef] [PubMed]

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

Viftrup, S. S.

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, (2004).
[CrossRef] [PubMed]

Wagner, N.

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Supplementary Material (1)

» Media 1: MOV (4466 KB)     

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Figures (5)

Fig. 1.
Fig. 1.

Expansion coefficients, bL (t), as defined in App. A for the transient molecular alignment induced in CO2 gas at 300 K for (a) τp = 20 fs, I 0 = 2 × 1013 W cm-2, (b) τp = 200 fs, I 0 = 2 × 1013 W cm-2, and (c) τp = 140 fs, I 0 = 6 × 1013 W cm-2. The trace colors correlate with the order of expansion for L = 2 (blue), L = 4 (green), L = 6 (red), and L = 8 (cyan).

Fig. 2.
Fig. 2.

Time-dependent orientational probability densities, G(θ,ϕ,t) generated by the expansion coefficients shown in Fig 1. The animations show the evolution of the orientational probability density with time. The moving circle in the right panels highlights the corresponding alignment cosine of the rotational wave packet. [Media 1]

Fig. 3.
Fig. 3.

Maximum static birefringence (a), transient birefringence (b), slope for frequency shifting (c), and chirp rate for spectral broadening (d) versus alignment pulse duration for a peak pulse intensity of Io = 2 × 1013W cm-2. Results for initial temperatures of 20 K(square), 100 K(circle), and 300 K(triangle) are shown.

Fig. 4.
Fig. 4.

Alignment spectrum given by |aωJ |2 as defined in App. B. at room temperature (300 K) with variation of the alignment pulse duration for a peak intensity of Io = 2 × 1013Wcm-2.

Fig. 5.
Fig. 5.

Maximum static birefringence (a), transient birefringence (b), slope for frequency shifting (c), and chirp rate for spectral broadening (d) versus alignment pulse duration at room temperature (300 K) for peak pulse intensities of I 0 = 6× (square), I 0 = 3× (triangle), I 0 = 2× (circle), and I 0 = 1 × 1013Wcm-2 (x).

Tables (2)

Tables Icon

Table 1. Optimal pulse durations for alignment, static & transient birefringence, and spectral modifications as a function of temperature.

Tables Icon

Table 2. Optimal pulse durations for alignment, static & transient birefringence, and spectral modifications as a function of pulse peak intensity.

Equations (26)

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G θ ϕ t = J o g J o P ( J o ) M o = J o J o ψ J o M o θ ϕ t 2 ,
ψ J o M o θ ϕ t = J M = J J C J M J 0 M 0 Y J M ( θ , ϕ ) e i E J t ħ
P = N μ I ε 0 χ ̿ E ,
χ ij = N ε 0 α IJ ij ,
α IJ ij = α IJ 4 π r iI r jJ G θ ϕ t d Ω ,
α IJ ij = 2 π α IJ L b L ( t ) 0 π r iI r jJ Y L 0 ( θ ) sin θ d θ .
χ xx = χ yy = N ε 0 [ α + 1 3 Δ α ] 2 3 Δ α N ε 0 π 5 b 2 ( t )
χ zz = N ε 0 [ α + 1 3 Δ α ] + 4 3 Δ α N ε 0 π 5 b 2 ( t ) ,
χ ̿ iso = N 3 ε 0 ( α + 2 α ) I ,
G θ ϕ t = L , m b L m ( t ) Y L m ( θ , ϕ ) ,
b L m = 0 4 π Y ¯ L m G θ ϕ t d Ω ,
b L m ( t ) = ( 1 ) L 2 L + 1 4 π J o , M o P ( J o ) J M c J M J o M o J , M c J M J o M o e i ω J , J t L 0 J 0 J 0 L m J M JM ,
b L ( t ) = ( 1 ) L 2 L + 1 4 π J o , M o P ( J o ) J J c J M o J o M o c J M o J o M o e i ω J , J t L 0 J 0 J 0 L 0 J M o J M o
ħ B 1 ω J , Δ J = Δ J ( Δ J + 1 ) + 2 Δ JJ ħ B 1 ( ω off + ω beat J ) ,
χ ij ( 1 ) = N ε 0 α IJ ij = N ε 0 4 π α lab ( θ , ϕ ) ij G ϕ θ t d Ω .
χ xx = N ε 0 L , m b L m ( t ) 4 π { α + Δ α sin 2 θ sin 2 ϕ } Y L m ( θ , ϕ ) d Ω ,
χ yy = N ε 0 L , m b L m ( t ) 4 π { α + Δ α cos 2 θ sin 2 ϕ } Y L m ( θ , ϕ ) d Ω , and
χ zz = N ε 0 L , m b L m ( t ) 4 π { α + Δ α cos 2 ( θ ) } Y L m ( θ , ϕ ) d Ω .
χ xx = χ yy = N ε 0 [ α + 1 3 Δ α ] 2 3 Δ α N ε 0 π 5 b 2 ( t ) ,
χ zz = = N ε 0 [ α + 1 3 Δ α ] + 4 3 Δ α N ε 0 π 5 b 2 ( t ) ,
χ xy = χ yx = χ xz = χ zx = χ yz = χ zy = 0 .
χ xx = χ yy = 1 2 N ε 0 [ α + α ] 1 2 N ε 0 Δ α cos 2 θ ( t )
χ zz = N ε 0 α + N ε 0 Δ α cos 2 θ ( t ) ,
cos 2 θ ( t ) = J 0 P ( J 0 ) M 0 = J 0 J 0 ψ J 0 M 0 cos 2 θ ψ J 0 M 0 = 4 3 π 5 b 2 ( t ) + 1 3 .
Δ χ st = 2 π 5 Δ α N ε 0 b 2 dc = 3 N 2 ε 0 Δ α ( cos 2 θ ( t ) ¯ 1 3 ) ,
Δ χ tr ( t ) = 2 π 5 Δ α N ε 0 b ˜ 2 ( t ) = N 2 ε 0 Δ α ( cos 2 θ ( t ) cos 2 ( t ) ¯ ) .

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