Abstract

Scanning through laser field strength and ellipticity, we show that the ellipticity anomaly in harmonic generation in C60 results from uneven saturations at different laser ellipticities. The smaller the laser ellipticity is, the faster the harmonic generation yield saturates with the laser strength. Harmonic generations at nonzero ellipticities take advantage of the earlier saturation at zero ellipticity, continue to grow with the laser field strength and eventually surpass the zero-ellipticity harmonic generation, which leads to the anomalous dependence. The theory predicts that the ellipticity dependence in C60 is much richer than those found in atoms: With an increase in laser field strength, a single maximum can be split into multiple maxima, and the global maximum comes back to zero ellipticity and reclaims its dominance over all other peaks.

© 2007 Optical Society of America

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  1. J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
    [CrossRef]
  2. F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
    [CrossRef]
  3. G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
    [CrossRef]
  4. Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
    [CrossRef]
  5. G. P. Zhang, 'Optical high harmonic generation in C60,' Phys. Rev. Lett. 95, 047401 (2005).
    [CrossRef] [PubMed]
  6. G. P. Zhang, 'Hartree-Fock dynamical electron-correlation effects in C60 after laser excitation,' Phys. Rev. Lett. 91, 176801 (2003).
    [CrossRef] [PubMed]
  7. G. P. Zhang and T. F. George, 'Ellipticity dependence of optical harmonic generation in C60,' Phys. Rev. A 74, 023811 (2006).
    [CrossRef]
  8. N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
    [CrossRef] [PubMed]
  9. F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
    [CrossRef] [PubMed]
  10. H. Stapelfeldt and T. Seideman, 'Colloquium: aligning molecules with strong laser pulses,' Rev. Mod. Phys. 75, 543-557 (2003).
    [CrossRef]
  11. D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
    [CrossRef] [PubMed]
  12. T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
    [CrossRef] [PubMed]
  13. T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
    [CrossRef] [PubMed]
  14. C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
    [CrossRef] [PubMed]
  15. N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
    [CrossRef]
  16. V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
    [CrossRef] [PubMed]
  17. N. L. Manakov, 'Dissipation-induced effects in generation of harmonic of a strong elliptically polarized field by gases,' JETP 83, 685-689 (1996).
  18. N. L. Manakov and V. P. Ovsyannikov, 'High-order nonlinear susceptibilities for generation of optical radiation harmonies in atomic gases,' Sov. Phys. JETP 52, 895-900 (1980).
  19. V. Averbukh, 'High-order harmonic generation by excited helium: the atomic polarization effect,' Phys. Rev. A 69, 043406 (2004).
    [CrossRef]
  20. N. L. Manakov, 'Circular dichroism and related effects in multiphoton transitions,' in Super-Intense Laser-Atom Physics IV, H. M. Muller and M. V. Fedorov, eds. (Kluwer Academic, 1996), pp. 153-162.
  21. M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
    [CrossRef]
  22. G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
    [CrossRef]
  23. T. Tsang, 'Third- and fifth-harmonic generation at the interfaces of glass and liquids,' Phys. Rev. A 54, 5454-5457 (1996).
    [CrossRef] [PubMed]
  24. W. K. Burns and N. Bloembergen, 'Third-harmonic generation in absorbing media of cubic or isotropic symmetry,' Phys. Rev. B 4, 3437-3450 (1971).
    [CrossRef]

2006

G. P. Zhang and T. F. George, 'Ellipticity dependence of optical harmonic generation in C60,' Phys. Rev. A 74, 023811 (2006).
[CrossRef]

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

2005

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
[CrossRef] [PubMed]

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

G. P. Zhang, 'Optical high harmonic generation in C60,' Phys. Rev. Lett. 95, 047401 (2005).
[CrossRef] [PubMed]

2004

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
[CrossRef] [PubMed]

V. Averbukh, 'High-order harmonic generation by excited helium: the atomic polarization effect,' Phys. Rev. A 69, 043406 (2004).
[CrossRef]

2003

G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
[CrossRef]

H. Stapelfeldt and T. Seideman, 'Colloquium: aligning molecules with strong laser pulses,' Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

G. P. Zhang, 'Hartree-Fock dynamical electron-correlation effects in C60 after laser excitation,' Phys. Rev. Lett. 91, 176801 (2003).
[CrossRef] [PubMed]

1997

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

1996

T. Tsang, 'Third- and fifth-harmonic generation at the interfaces of glass and liquids,' Phys. Rev. A 54, 5454-5457 (1996).
[CrossRef] [PubMed]

N. L. Manakov, 'Dissipation-induced effects in generation of harmonic of a strong elliptically polarized field by gases,' JETP 83, 685-689 (1996).

1995

N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
[CrossRef] [PubMed]

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

1994

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

1992

J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
[CrossRef]

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

1980

N. L. Manakov and V. P. Ovsyannikov, 'High-order nonlinear susceptibilities for generation of optical radiation harmonies in atomic gases,' Sov. Phys. JETP 52, 895-900 (1980).

1971

W. K. Burns and N. Bloembergen, 'Third-harmonic generation in absorbing media of cubic or isotropic symmetry,' Phys. Rev. B 4, 3437-3450 (1971).
[CrossRef]

Altucci, C.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Averbukh, V.

V. Averbukh, 'High-order harmonic generation by excited helium: the atomic polarization effect,' Phys. Rev. A 69, 043406 (2004).
[CrossRef]

Banfi, G. P.

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

Bartoli, F. J.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Bellini, M.

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

Benedetti, E.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Bhardwaj, V. R.

V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
[CrossRef] [PubMed]

Bloembergen, N.

W. K. Burns and N. Bloembergen, 'Third-harmonic generation in absorbing media of cubic or isotropic symmetry,' Phys. Rev. B 4, 3437-3450 (1971).
[CrossRef]

Bucksbaum, P. H.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Burnett, N. H.

N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
[CrossRef] [PubMed]

Burns, W. K.

W. K. Burns and N. Bloembergen, 'Third-harmonic generation in absorbing media of cubic or isotropic symmetry,' Phys. Rev. B 4, 3437-3450 (1971).
[CrossRef]

Calegari, F.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Caumes, J.-P.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Comtois, D.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Corkum, P. B.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
[CrossRef] [PubMed]

N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
[CrossRef] [PubMed]

Daems, D.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Danieli, R.

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Du, D.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Dudovich, N.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Dutta, S. K.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Faucher, O.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Fortusini, D.

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

George, T. F.

G. P. Zhang and T. F. George, 'Ellipticity dependence of optical harmonic generation in C60,' Phys. Rev. A 74, 023811 (2006).
[CrossRef]

G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
[CrossRef]

Guerin, S.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Heesel, E.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Hertz, E.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Ivanov, M. Yu.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Jauslin, H. R.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Kafafi, Z. H.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Kajumba, N.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Kajzar, F.

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Kakehata, M.

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

Kan, C.

N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
[CrossRef] [PubMed]

Kanai, T.

T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
[CrossRef] [PubMed]

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

Korn, G.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Lavorel, B.

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

Levesque, J.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Lindle, J. R.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Lingg, L. J.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Manakov, N. L.

N. L. Manakov, 'Dissipation-induced effects in generation of harmonic of a strong elliptically polarized field by gases,' JETP 83, 685-689 (1996).

N. L. Manakov and V. P. Ovsyannikov, 'High-order nonlinear susceptibilities for generation of optical radiation harmonies in atomic gases,' Sov. Phys. JETP 52, 895-900 (1980).

N. L. Manakov, 'Circular dichroism and related effects in multiphoton transitions,' in Super-Intense Laser-Atom Physics IV, H. M. Muller and M. V. Fedorov, eds. (Kluwer Academic, 1996), pp. 153-162.

Marangos, J. P.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Meth, J. S.

J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
[CrossRef]

Milani, P.

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

Milliken, J.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Minemoto, S.

T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
[CrossRef] [PubMed]

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

Miyazaki, K.

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

Nisoli, M.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Ovsyannikov, V. P.

N. L. Manakov and V. P. Ovsyannikov, 'High-order nonlinear susceptibilities for generation of optical radiation harmonies in atomic gases,' Sov. Phys. JETP 52, 895-900 (1980).

Pong, R. G. S.

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

Rayner, D. M.

V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
[CrossRef] [PubMed]

Rossini, S.

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Sakai, H.

T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
[CrossRef] [PubMed]

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

Sansone, G.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Seideman, T.

H. Stapelfeldt and T. Seideman, 'Colloquium: aligning molecules with strong laser pulses,' Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

Shkolnikov, P. L.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Smirnova, O.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Stagira, S.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Stapelfeldt, H.

H. Stapelfeldt and T. Seideman, 'Colloquium: aligning molecules with strong laser pulses,' Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

Sun, X.

G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
[CrossRef]

Suzuki, T.

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

Takada, H.

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

Taliani, C.

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Torres, R.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Tsang, T.

T. Tsang, 'Third- and fifth-harmonic generation at the interfaces of glass and liquids,' Phys. Rev. A 54, 5454-5457 (1996).
[CrossRef] [PubMed]

Vanherzeele, H.

J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
[CrossRef]

Velotta, R.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Villeneuve, D. M.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Vozzi, C.

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

Wang, Y.

J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
[CrossRef]

Weihe, F. A.

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

Yumoto, H.

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

Zamboni, R.

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Zeidler, D.

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

Zhang, G. P.

G. P. Zhang and T. F. George, 'Ellipticity dependence of optical harmonic generation in C60,' Phys. Rev. A 74, 023811 (2006).
[CrossRef]

G. P. Zhang, 'Optical high harmonic generation in C60,' Phys. Rev. Lett. 95, 047401 (2005).
[CrossRef] [PubMed]

G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
[CrossRef]

G. P. Zhang, 'Hartree-Fock dynamical electron-correlation effects in C60 after laser excitation,' Phys. Rev. Lett. 91, 176801 (2003).
[CrossRef] [PubMed]

Chem. Phys. Lett.

J. S. Meth, H. Vanherzeele, and Y. Wang, 'Dispersion of the third-order optical nonlinearity of C60. A third-harmonic generation study,' Chem. Phys. Lett. 197, 26-31 (1992).
[CrossRef]

F. Kajzar, C. Taliani, R. Danieli, S. Rossini, and R. Zamboni, 'Wave-dispersed third-order nonlinear optical properties of C60 thin films,' Chem. Phys. Lett. 217, 418-422 (1994).
[CrossRef]

Z. H. Kafafi, J. R. Lindle, R. G. S. Pong, F. J. Bartoli, L. J. Lingg, and J. Milliken, 'Off-resonant nonlinear optical properties of C60 studied by degenerate four-wave mixing,' Chem. Phys. Lett. 188, 492-496 (1992).
[CrossRef]

JETP

N. L. Manakov, 'Dissipation-induced effects in generation of harmonic of a strong elliptically polarized field by gases,' JETP 83, 685-689 (1996).

Nature

T. Kanai, S. Minemoto, and H. Sakai, 'Quantum interference during high-order harmonic generation from aligned molecules,' Nature 435, 470-474 (2005).
[CrossRef] [PubMed]

Phys. Rev. A

G. P. Zhang and T. F. George, 'Ellipticity dependence of optical harmonic generation in C60,' Phys. Rev. A 74, 023811 (2006).
[CrossRef]

N. H. Burnett, C. Kan, and P. B. Corkum, 'Ellipticity and polarization effects in harmonic generation in ionizing neon,' Phys. Rev. A 51, R3418-R3421 (1995).
[CrossRef] [PubMed]

F. A. Weihe, S. K. Dutta, G. Korn, D. Du, P. H. Bucksbaum, and P. L. Shkolnikov, 'Polarization of high-intensity high-harmonic generation,' Phys. Rev. A 51, R3433-R3436 (1995).
[CrossRef] [PubMed]

V. Averbukh, 'High-order harmonic generation by excited helium: the atomic polarization effect,' Phys. Rev. A 69, 043406 (2004).
[CrossRef]

M. Kakehata, H. Takada, H. Yumoto, and K. Miyazaki, 'Anomalous ellipticity dependence of high-order harmonic generation,' Phys. Rev. A 55, R861-R864 (1997).
[CrossRef]

T. Tsang, 'Third- and fifth-harmonic generation at the interfaces of glass and liquids,' Phys. Rev. A 54, 5454-5457 (1996).
[CrossRef] [PubMed]

Phys. Rev. B

W. K. Burns and N. Bloembergen, 'Third-harmonic generation in absorbing media of cubic or isotropic symmetry,' Phys. Rev. B 4, 3437-3450 (1971).
[CrossRef]

G. P. Zhang, X. Sun, and T. F. George, 'Laser-induced ultrafast dynamics in C60,' Phys. Rev. B 68, 165410 (2003).
[CrossRef]

G. P. Banfi, D. Fortusini, M. Bellini, and P. Milani, 'Wave-dispersed two-photon absorption of C60,' Phys. Rev. B 56, R10075-R10078 (1997).
[CrossRef]

Phys. Rev. Lett.

G. P. Zhang, 'Optical high harmonic generation in C60,' Phys. Rev. Lett. 95, 047401 (2005).
[CrossRef] [PubMed]

G. P. Zhang, 'Hartree-Fock dynamical electron-correlation effects in C60 after laser excitation,' Phys. Rev. Lett. 91, 176801 (2003).
[CrossRef] [PubMed]

C. Vozzi, F. Calegari, E. Benedetti, J.-P. Caumes,G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel,N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, 'Controlling two-center interference in molecular high harmonic generation,' Phys. Rev. Lett. 95, 153902 (2005).
[CrossRef] [PubMed]

N. Dudovich, J. Levesque, O. Smirnova, D. Zeidler, D. Comtois, M. Yu. Ivanov, D. M. Villeneuve, and P. B. Corkum, 'Attosecond temporal gating with elliptically polarized light,' Phys. Rev. Lett. 97, 253903 (2006).
[CrossRef]

V. R. Bhardwaj, P. B. Corkum, and D. M. Rayner, 'Recollision during the high laser intensity ionization of C60,' Phys. Rev. Lett. 93, 043001 (2004).
[CrossRef] [PubMed]

D. Daems, S. Guerin, E. Hertz, H. R. Jauslin, B. Lavorel, and O. Faucher, 'Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses,' Phys. Rev. Lett. 95, 063005 (2005).
[CrossRef] [PubMed]

T. Suzuki, S. Minemoto, T. Kanai, and H. Sakai, 'Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses,' Phys. Rev. Lett. 92, 133005 (2004).
[CrossRef] [PubMed]

Rev. Mod. Phys.

H. Stapelfeldt and T. Seideman, 'Colloquium: aligning molecules with strong laser pulses,' Rev. Mod. Phys. 75, 543-557 (2003).
[CrossRef]

Sov. Phys. JETP

N. L. Manakov and V. P. Ovsyannikov, 'High-order nonlinear susceptibilities for generation of optical radiation harmonies in atomic gases,' Sov. Phys. JETP 52, 895-900 (1980).

Other

N. L. Manakov, 'Circular dichroism and related effects in multiphoton transitions,' in Super-Intense Laser-Atom Physics IV, H. M. Muller and M. V. Fedorov, eds. (Kluwer Academic, 1996), pp. 153-162.

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Figures (5)

Fig. 1
Fig. 1

Dependence of the harmonic yield on the laser ellipticity ϵ for the (a) off-resonant (third-order) harmonic and (b) resonant harmonic (transition between HOMO and LUMO + 1 ). The laser energy is 0.2 eV , and the pulse duration is eight laser cycles. The laser field strength increases from 0.05 to 0.10 V Å (from bottom to top). (a) Off-resonant harmonic shows a normal dependence with ellipticity. (b) On resonance, the anomalous ellipticity dependence gradually develops with an increase in laser field strength. The harmonic yield peaks at a nonzero ellipticity. The maximum moves slightly toward larger ellipticities as the laser field strength increases.

Fig. 2
Fig. 2

Change in harmonic yield as a function of laser field strength for three ellipticities: ϵ = 0 , 0.5, and 1. The laser parameters are the same as for Fig. 1. (a) Off-resonant excitation. Saturation differences among different ellipticities are not large enough to change the order of harmonic yields. (b) Resonant excitation. The saturation in harmonic yield at ϵ = 0 is faster than that at ϵ 0 . The harmonics at ϵ 0 take advantage of this faster saturation and peak at a nonzero ellipticity. This is the origin of the anomalous ellipticity dependence.

Fig. 3
Fig. 3

For higher laser intensities, the off-resonant harmonic yield still has a normal dependence on the laser ellipticity. The curves are shifted for clarity.

Fig. 4
Fig. 4

Ellipticity dependence at resonant excitation for laser field strength from A 0 = 0.10 to 0.19 V Å . The harmonic yield at ϵ = 0 reclaims its global maximum gradually. The curves are shifted for clarity.

Fig. 5
Fig. 5

For slightly off-resonance excitation ( 0.025 eV above resonance), the ellipticity anomaly appears with the help of a substantial laser field strength. The overall change is similar to the resonant case. The curves are shifted for clarity.

Equations (3)

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

i ρ ̇ = [ H , ρ ] ,
H 0 = i j , σ t i j ( c i , σ c j , σ + H.c. ) ,
H I = F D = e i σ F r i n i σ .

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