Abstract

We investigate a method for complete population inversion in three level systems through π -pulse bichromatic two-photon coherent excitation and study the dependence on the chirp of the laser pulses. We observe that the population inversion does not monotonously decrease with increasing the time-bandwidth product, and that the excitation depends on the sign of the chirp of the individual pulses. Our results evidence a strategy for coherent population transfer which is energetically superior to adiabatic methods and opens the door for real-world applications, since it alleviates the need for challenging generation of transform-limited pulses at arbitrary wavelengths.

© 2008 Optical Society of America

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  5. J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
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  6. G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
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  8. D. Meshulach and Y. Silberberg, "Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses," Phys. Rev. A 60, 1287-1292 (1999).
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  9. N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
    [CrossRef] [PubMed]
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    [CrossRef]
  11. A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
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  13. J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
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    [CrossRef]
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  29. B. W. Shore and J. Ackerhalt, "Dynamics of multilevel laser excitation: Three-level atoms," Phys. Rev. A 15, 1640-1647 (1977).
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  30. C. E. Carroll and F. T. Hioe, "Driven three-state model and its analytic solutions," J. Math. Phys. 29, 487 (1988).
    [CrossRef]
  31. S. Chelkowski and A. D. Bandrauk, "Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium," J. Chem. Phys. 89, 3618 (1988).
    [CrossRef]
  32. A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
    [CrossRef] [PubMed]
  33. A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
    [CrossRef] [PubMed]
  34. J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
    [CrossRef]
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2007 (1)

P. Král, I. Thanopulos, and M. Shapiro, "Colloquium: Coherently controlled adiabatic passage," Rev. Mod. Phys. 79, 53 (2007).
[CrossRef]

2006 (4)

J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
[CrossRef]

P. Panek and A. Becker, "Dark pulses for resonant two-photon transitions," Phys. Rev. A 74, 023408 (2006).
[CrossRef]

J. L. Herek, "Coherent control of photochemical and photobiological processes," J. Photochem. Photobiol. A 180, 225 (2006).
[CrossRef]

A. Monmayrant, B. Chatel, and B. Girard, "Real time quantum state holography using coherent transients," Opt. Commun. 264, 256-263 (2006).
[CrossRef]

2005 (2)

V. V. Lozovoy and M. Dantus, "Systematic Control of Nonlinear Optical Processes using Optimally Shaped Femtosecond Pulses," ChemPhysChem 6, 1970-2000 (2005).
[CrossRef] [PubMed]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

2004 (1)

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

2003 (2)

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

J. Biegert and J.-C. Diels, "Feasibility study to create a polychromatic guidestar in atomic sodium," Phys. Rev. A 67, 043403 (2003).
[CrossRef]

2002 (1)

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

2001 (1)

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

2000 (1)

1999 (1)

D. Meshulach and Y. Silberberg, "Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses," Phys. Rev. A 60, 1287-1292 (1999).
[CrossRef]

1998 (2)

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239-242 (1998).
[CrossRef]

K. Bergmann, H. Theuer, and B. W. Shore, "Coherent population transfer among quantum states of atoms and molecules," Rev. Mod. Phys. 70, 1003-1025 (1998).
[CrossRef]

1997 (1)

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

1996 (1)

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

1995 (1)

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

1993 (1)

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

1992 (1)

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

1989 (1)

F. T. Hioe and K. Bergmann, "Adiabatic population transfer in a three-level system driven by delayed laser pulses," Phys. Rev. A 40, 6741-6744 (1989).
[CrossRef] [PubMed]

1988 (2)

C. E. Carroll and F. T. Hioe, "Driven three-state model and its analytic solutions," J. Math. Phys. 29, 487 (1988).
[CrossRef]

S. Chelkowski and A. D. Bandrauk, "Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium," J. Chem. Phys. 89, 3618 (1988).
[CrossRef]

1986 (1)

J.-C. Diels and S. Besnainou, "Multiphoton coherent excitation of molecules," J. Chem. Phys. 85, 6347 (1986).
[CrossRef]

1977 (1)

B. W. Shore and J. Ackerhalt, "Dynamics of multilevel laser excitation: Three-level atoms," Phys. Rev. A 15, 1640-1647 (1977).
[CrossRef]

1976 (2)

M. SargentIII and P. Horwitz, "Three-level Rabi flopping," Phys. Rev. A 13, 1962-1964 (1976).
[CrossRef]

J.-C. Diels, "Efficient selective optical excitation for isotope separation, using short laser pulse," Phys. Rev. A 13, 1520-1527 (1976).
[CrossRef]

1975 (1)

R. G. Brewer and E. L. Hahn, "Coherent two-photon processes: Transient and steady-state cases," Phys. Rev. A 11, 1641-1649 (1975).
[CrossRef]

Ackerhalt, J.

B. W. Shore and J. Ackerhalt, "Dynamics of multilevel laser excitation: Three-level atoms," Phys. Rev. A 15, 1640-1647 (1977).
[CrossRef]

Backup, T.

J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
[CrossRef]

Bakos, J. S.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Ballard, J. B.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

Bandrauk, A. D.

S. Chelkowski and A. D. Bandrauk, "Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium," J. Chem. Phys. 89, 3618 (1988).
[CrossRef]

Baumert, T.

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

Becker, A.

P. Panek and A. Becker, "Dark pulses for resonant two-photon transitions," Phys. Rev. A 74, 023408 (2006).
[CrossRef]

Bergmann, K.

K. Bergmann, H. Theuer, and B. W. Shore, "Coherent population transfer among quantum states of atoms and molecules," Rev. Mod. Phys. 70, 1003-1025 (1998).
[CrossRef]

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

F. T. Hioe and K. Bergmann, "Adiabatic population transfer in a three-level system driven by delayed laser pulses," Phys. Rev. A 40, 6741-6744 (1989).
[CrossRef] [PubMed]

Besnainou, S.

J.-C. Diels and S. Besnainou, "Multiphoton coherent excitation of molecules," J. Chem. Phys. 85, 6347 (1986).
[CrossRef]

Biegert, J.

J. Biegert and J.-C. Diels, "Feasibility study to create a polychromatic guidestar in atomic sodium," Phys. Rev. A 67, 043403 (2003).
[CrossRef]

J. Biegert, J.-C. Diels, and P. W. Milonni, "Bichromatic two-photon coherent excitation of sodium to provide a dualwavelength guidestar," Opt. Lett. 25, 683-685 (2000).
[CrossRef]

Borisov, S. K.

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Brewer, R. G.

R. G. Brewer and E. L. Hahn, "Coherent two-photon processes: Transient and steady-state cases," Phys. Rev. A 11, 1641-1649 (1975).
[CrossRef]

Buckup, T.

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

Carroll, C. E.

C. E. Carroll and F. T. Hioe, "Driven three-state model and its analytic solutions," J. Math. Phys. 29, 487 (1988).
[CrossRef]

Chatel, B.

A. Monmayrant, B. Chatel, and B. Girard, "Real time quantum state holography using coherent transients," Opt. Commun. 264, 256-263 (2006).
[CrossRef]

Chelkowski, S.

S. Chelkowski and A. D. Bandrauk, "Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium," J. Chem. Phys. 89, 3618 (1988).
[CrossRef]

Choe, A. S.

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Dam, N.

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

Dantus, M.

V. V. Lozovoy and M. Dantus, "Systematic Control of Nonlinear Optical Processes using Optimally Shaped Femtosecond Pulses," ChemPhysChem 6, 1970-2000 (2005).
[CrossRef] [PubMed]

Dayan, B.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

Demeter, G.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Diels, J.-C.

J. Biegert and J.-C. Diels, "Feasibility study to create a polychromatic guidestar in atomic sodium," Phys. Rev. A 67, 043403 (2003).
[CrossRef]

J. Biegert, J.-C. Diels, and P. W. Milonni, "Bichromatic two-photon coherent excitation of sodium to provide a dualwavelength guidestar," Opt. Lett. 25, 683-685 (2000).
[CrossRef]

J.-C. Diels and S. Besnainou, "Multiphoton coherent excitation of molecules," J. Chem. Phys. 85, 6347 (1986).
[CrossRef]

J.-C. Diels, "Efficient selective optical excitation for isotope separation, using short laser pulse," Phys. Rev. A 13, 1520-1527 (1976).
[CrossRef]

Djotyan, G. P.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Dudovich, N.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

Gallagher Faeder, S. M.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

Gandhi, S. R.

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

Girard, B.

A. Monmayrant, B. Chatel, and B. Girard, "Real time quantum state holography using coherent transients," Opt. Commun. 264, 256-263 (2006).
[CrossRef]

Hahn, E. L.

R. G. Brewer and E. L. Hahn, "Coherent two-photon processes: Transient and steady-state cases," Phys. Rev. A 11, 1641-1649 (1975).
[CrossRef]

Han, P. S.

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Hariharan, A.

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

Hauer, J.

J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
[CrossRef]

Herek, J. L.

J. L. Herek, "Coherent control of photochemical and photobiological processes," J. Photochem. Photobiol. A 180, 225 (2006).
[CrossRef]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

Hetherington, C. L.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

Hioe, F. T.

F. T. Hioe and K. Bergmann, "Adiabatic population transfer in a three-level system driven by delayed laser pulses," Phys. Rev. A 40, 6741-6744 (1989).
[CrossRef] [PubMed]

C. E. Carroll and F. T. Hioe, "Driven three-state model and its analytic solutions," J. Math. Phys. 29, 487 (1988).
[CrossRef]

Holleman, I.

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

Horwitz, P.

M. SargentIII and P. Horwitz, "Three-level Rabi flopping," Phys. Rev. A 13, 1962-1964 (1976).
[CrossRef]

Ignácz, P. N.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Kedves, M. Á.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Kim, J. B.

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

Král, P.

P. Král, I. Thanopulos, and M. Shapiro, "Colloquium: Coherently controlled adiabatic passage," Rev. Mod. Phys. 79, 53 (2007).
[CrossRef]

Kuhn, A.

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

Kuzmina, M. A.

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Lee, J.

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Leone, S. R.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

Linskens, A. F.

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

Lozovoy, V. V.

V. V. Lozovoy and M. Dantus, "Systematic Control of Nonlinear Optical Processes using Optimally Shaped Femtosecond Pulses," ChemPhysChem 6, 1970-2000 (2005).
[CrossRef] [PubMed]

Melinger, J. S.

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

Meshulach, D.

D. Meshulach and Y. Silberberg, "Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses," Phys. Rev. A 60, 1287-1292 (1999).
[CrossRef]

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239-242 (1998).
[CrossRef]

Milonni, P. W.

Mirowski, E.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

Mishin, V. A.

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Monmayrant, A.

A. Monmayrant, B. Chatel, and B. Girard, "Real time quantum state holography using coherent transients," Opt. Commun. 264, 256-263 (2006).
[CrossRef]

Motzkus, M.

J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
[CrossRef]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

Panek, P.

P. Panek and A. Becker, "Dark pulses for resonant two-photon transitions," Phys. Rev. A 74, 023408 (2006).
[CrossRef]

Präkelt, A.

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

Reuss, J.

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

Rhee, Y.

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

Sargent, M.

M. SargentIII and P. Horwitz, "Three-level Rabi flopping," Phys. Rev. A 13, 1962-1964 (1976).
[CrossRef]

Sarpe-Tudoran, C.

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

Schiemann, S.

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

Shapiro, M.

P. Král, I. Thanopulos, and M. Shapiro, "Colloquium: Coherently controlled adiabatic passage," Rev. Mod. Phys. 79, 53 (2007).
[CrossRef]

Shore, B. W.

K. Bergmann, H. Theuer, and B. W. Shore, "Coherent population transfer among quantum states of atoms and molecules," Rev. Mod. Phys. 70, 1003-1025 (1998).
[CrossRef]

B. W. Shore and J. Ackerhalt, "Dynamics of multilevel laser excitation: Three-level atoms," Phys. Rev. A 15, 1640-1647 (1977).
[CrossRef]

Silberberg, Y.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

D. Meshulach and Y. Silberberg, "Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses," Phys. Rev. A 60, 1287-1292 (1999).
[CrossRef]

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239-242 (1998).
[CrossRef]

Sörlei, Zs.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Stauffer, H. U.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

Steuerwald, S.

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

Szigeti, J.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Thanopulos, I.

P. Král, I. Thanopulos, and M. Shapiro, "Colloquium: Coherently controlled adiabatic passage," Rev. Mod. Phys. 79, 53 (2007).
[CrossRef]

Theuer, H.

K. Bergmann, H. Theuer, and B. W. Shore, "Coherent population transfer among quantum states of atoms and molecules," Rev. Mod. Phys. 70, 1003-1025 (1998).
[CrossRef]

Tóth, Z. L.

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

Tull, J. X.

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

Warren, W. S.

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

Wohlleben, W.

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

Wollenhaupt, M.

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

Zhang, B.

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

ChemPhysChem (2)

V. V. Lozovoy and M. Dantus, "Systematic Control of Nonlinear Optical Processes using Optimally Shaped Femtosecond Pulses," ChemPhysChem 6, 1970-2000 (2005).
[CrossRef] [PubMed]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, "Coherent Control for Spectroscopy and Manipulation of Biological Dynamics," ChemPhysChem 6, 850-857 (2005).
[CrossRef] [PubMed]

J. Chem. Phys. (4)

S. Chelkowski and A. D. Bandrauk, "Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium," J. Chem. Phys. 89, 3618 (1988).
[CrossRef]

J. Hauer, T. Backup, and M. Motzkus, "Enhancement of molecular modes by electronically resonant multipulse excitation: Further progress towards mode selective chemistry," J. Chem. Phys. 125, 061101 (2006).
[CrossRef]

J.-C. Diels and S. Besnainou, "Multiphoton coherent excitation of molecules," J. Chem. Phys. 85, 6347 (1986).
[CrossRef]

E. Mirowski, H. U. Stauffer, J. B. Ballard, B. Zhang, C. L. Hetherington, and S. R. Leone, "Effect of nonresonant frequencies on the enhancement of quantum beat amplitudes in rovibrational states of Li2: The role of state spacing," J. Chem. Phys. 117, 11228 (2002).
[CrossRef]

J. Math. Phys. (1)

C. E. Carroll and F. T. Hioe, "Driven three-state model and its analytic solutions," J. Math. Phys. 29, 487 (1988).
[CrossRef]

J. Photochem. Photobiol. A (1)

J. L. Herek, "Coherent control of photochemical and photobiological processes," J. Photochem. Photobiol. A 180, 225 (2006).
[CrossRef]

Nature (London) (1)

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239-242 (1998).
[CrossRef]

Opt. Commun. (1)

A. Monmayrant, B. Chatel, and B. Girard, "Real time quantum state holography using coherent transients," Opt. Commun. 264, 256-263 (2006).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. A (13)

G. P. Djotyan, J. S. Bakos, G. Demeter, P. N. Ignácz, M. Á. Kedves, Zs. Sörlei, J. Szigeti, and Z. L. Tóth, "Coherent population transfer in Rb atoms by frequency-chirped laser pulses," Phys. Rev. A 68, 053409 (2003).
[CrossRef]

J.-C. Diels, "Efficient selective optical excitation for isotope separation, using short laser pulse," Phys. Rev. A 13, 1520-1527 (1976).
[CrossRef]

P. Panek and A. Becker, "Dark pulses for resonant two-photon transitions," Phys. Rev. A 74, 023408 (2006).
[CrossRef]

F. T. Hioe and K. Bergmann, "Adiabatic population transfer in a three-level system driven by delayed laser pulses," Phys. Rev. A 40, 6741-6744 (1989).
[CrossRef] [PubMed]

D. Meshulach and Y. Silberberg, "Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses," Phys. Rev. A 60, 1287-1292 (1999).
[CrossRef]

A. Präkelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

R. G. Brewer and E. L. Hahn, "Coherent two-photon processes: Transient and steady-state cases," Phys. Rev. A 11, 1641-1649 (1975).
[CrossRef]

M. SargentIII and P. Horwitz, "Three-level Rabi flopping," Phys. Rev. A 13, 1962-1964 (1976).
[CrossRef]

B. W. Shore and J. Ackerhalt, "Dynamics of multilevel laser excitation: Three-level atoms," Phys. Rev. A 15, 1640-1647 (1977).
[CrossRef]

A. S. Choe, Y. Rhee, J. Lee, P. S. Han, S. K. Borisov, M. A. Kuzmina, and V. A. Mishin, "Effective excitation method of a three-level medium in a selective photoionization," Phys. Rev. A 52, 382-386 (1995).
[CrossRef] [PubMed]

A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, "Two-photon Rabi oscillations," Phys. Rev. A 54, 4854-4862 (1996).
[CrossRef] [PubMed]

J. B. Kim, J. Lee, A. S. Choe, and Y. Rhee, "Geometrical representation of coherent-excitation methods using delayed and detuned lasers," Phys. Rev. A 55, 3819-3825 (1997).
[CrossRef]

J. Biegert and J.-C. Diels, "Feasibility study to create a polychromatic guidestar in atomic sodium," Phys. Rev. A 67, 043403 (2003).
[CrossRef]

Phys. Rev. Lett. (3)

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-Limited Pulses are not Optimal for Resonant Multiphoton Transitions," Phys. Rev. Lett. 86, 47-50 (2001).
[CrossRef] [PubMed]

J. S. Melinger, S. R. Gandhi, A. Hariharan, J. X. Tull, and W. S. Warren, "Generation of narrowband inversion with broadband laser pulses," Phys. Rev. Lett. 68, 2000-2003 (1992).
[CrossRef] [PubMed]

S. Schiemann, A. Kuhn, S. Steuerwald, and K. Bergmann, "Efficient coherent population transfer in NO molecules using pulsed lasers," Phys. Rev. Lett. 71, 3637-3640 (1993).
[CrossRef] [PubMed]

Rev. Mod. Phys. (2)

K. Bergmann, H. Theuer, and B. W. Shore, "Coherent population transfer among quantum states of atoms and molecules," Rev. Mod. Phys. 70, 1003-1025 (1998).
[CrossRef]

P. Král, I. Thanopulos, and M. Shapiro, "Colloquium: Coherently controlled adiabatic passage," Rev. Mod. Phys. 79, 53 (2007).
[CrossRef]

Other (6)

J. Biegert, Polychromatic Multiphoton Coherent Excitation of Sodium (Der Andere Verlag, Osnabrück, 2001).

S. A. Rice and M. Zhao, Optimal Control of Molecular Dynamics (Wiley Inter-Science, New York, 2000).

M. Shapiro and P. Brumer, Principles of the Quantum Control of Molecular Processes (Wiley Inter-Science, Hoboken, New Jersey, 2003).

S. Mukamel, Nonlinear Optical Spectroscopy (Oxford University Press, New York, 1995).

M. A. Nielsen and I. L. Chuang, Quantum Computation and Quantum Information (Cambridge University Press, Cambridge, England, 2000).

L. Allen and J. H. Eberly, Optical resonance and two-level atoms, (Dover Publications, New York 1975).

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Figures (4)

Fig. 1.
Fig. 1.

Schematic energy level configuration.

Fig. 2.
Fig. 2.

Evolution of the normalized amplitude of the Bloch vector (u,v,w) on the sphere for p-pulse and adiabatic excitation, as indicated, for the three-level system reduced to a pseudo-two-level system (a). Projection of the two trajectories onto the u, v plane (b).

Fig. 3.
Fig. 3.

Final value of the population ρ 22 (in %) as a function of the adimensional chirp parameter for the 589 nm (a 1) and the 1140 nm (a 2) bichromatic pulse components. For instance, a i =10 gives a chirp value of ≈0.14 ps-2. Other parameters are tp =10 ps, E 1=3.25×106 V/m, E 2=4.34×106 V/m, Δ1=94.14 GHz and Δ2=10.95 GHz.

Fig. 4.
Fig. 4.

Final value of the populations ρ00, ρ11 and ρ22 (as indicated) as a function of the chirp parameter (in units of τ-2 i.e. 2ln 2/100ps 2) for a 1=a 2. Other parameters are as in Fig. 3.

Equations (10)

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

ρ ˙ 00 = i E ( t ) h ̅ { d 01 ( ρ 10 ρ 01 ) } ,
ρ ˙ 11 = i E ( t ) h ̅ { d 01 ( ρ 01 ρ 10 ) + d 12 ( ρ 21 ρ 12 ) } ,
ρ ˙ 22 = i E ( t ) h ̅ { d 12 ( ρ 12 ρ 21 ) } ,
ρ ˙ 01 = i ω 10 ρ 01 + i E ( t ) h ̅ { d 01 ( ρ 11 ρ 00 ) d 12 ρ 02 } ,
ρ ˙ 02 = i ω 20 ρ 02 + i E ( t ) h ̅ { d 01 ρ 12 d 12 ρ 01 } ,
ρ ˙ 12 = i ω 21 ρ 12 + i E ( t ) h ̅ { d 12 ( ρ 22 ρ 11 ) d 01 ρ 02 } .
E ( t ) = e ( t τ ) 2 { E 1 cos [ ω 1 t a 1 ( t τ ) 2 ] + E 2 cos [ ω 2 t a 2 ( t τ ) 2 ] } .
u ˙ = Ω 1 2 Ω 2 2 Δ 1 v ,
v ˙ = Ω 1 2 Ω 2 2 Δ 1 u + 2 Ω 1 Ω 2 Δ 1 w
w ˙ = 2 Ω 1 Ω 2 Δ 1 v ,

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