Multiphoton transitions in molecules with permanent dipole moments

Y. B. Band; R. Bavli; D. F. Heller

doi:10.1016/0009-2614(89)87117-9

Multiphoton transitions in molecules with permanent dipole moments

Y. B. Band, R. Bavli, D. F. Heller

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Abstract

We use a nonperturbative treatment to study multiphoton transitions in molecules with permanent dipole moments. This generalizes the perturbative treatment of Scharf and Band (Chem. Phys. Letters 144 (1988) 165) for two-photon transitions in molecules with permanent dipole moments in the presence of electromagnetic fields of two frequencies, one near resonance and the other small, Our nonperturbative density matrix treatment accounts for level population decay (T₁) effects and optical transition dephasing (T₂) effects, both neglected in earlier approaches. Our results are applicable even in the regime where perturbation theory breaks down. In particular, when the sum of the field frequencies approaches a molecular resonance a substantial enhancement of the photo-absorption rate (by a two-photon process) occurs even when one frequency becomes as small as the transition linewidth.

Original language	English
Pages (from-to)	405-410
Number of pages	6
Journal	Chemical Physics Letters
Volume	156
Issue number	4
DOIs	https://doi.org/10.1016/0009-2614(89)87117-9
State	Published - 7 Apr 1989
Externally published	Yes

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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title = "Multiphoton transitions in molecules with permanent dipole moments",

abstract = "We use a nonperturbative treatment to study multiphoton transitions in molecules with permanent dipole moments. This generalizes the perturbative treatment of Scharf and Band (Chem. Phys. Letters 144 (1988) 165) for two-photon transitions in molecules with permanent dipole moments in the presence of electromagnetic fields of two frequencies, one near resonance and the other small, Our nonperturbative density matrix treatment accounts for level population decay (T1) effects and optical transition dephasing (T2) effects, both neglected in earlier approaches. Our results are applicable even in the regime where perturbation theory breaks down. In particular, when the sum of the field frequencies approaches a molecular resonance a substantial enhancement of the photo-absorption rate (by a two-photon process) occurs even when one frequency becomes as small as the transition linewidth.",

author = "Band, {Y. B.} and R. Bavli and Heller, {D. F.}",

note = "Funding Information: This work was supportedi n part by a grant from the US-Israel Binational Science Foundation, We wish to thank ProfessorB enjamin E. Scharf for helpful commentsa nd discussions.",

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T1 - Multiphoton transitions in molecules with permanent dipole moments

AU - Band, Y. B.

AU - Bavli, R.

AU - Heller, D. F.

N1 - Funding Information: This work was supportedi n part by a grant from the US-Israel Binational Science Foundation, We wish to thank ProfessorB enjamin E. Scharf for helpful commentsa nd discussions.

PY - 1989/4/7

Y1 - 1989/4/7

N2 - We use a nonperturbative treatment to study multiphoton transitions in molecules with permanent dipole moments. This generalizes the perturbative treatment of Scharf and Band (Chem. Phys. Letters 144 (1988) 165) for two-photon transitions in molecules with permanent dipole moments in the presence of electromagnetic fields of two frequencies, one near resonance and the other small, Our nonperturbative density matrix treatment accounts for level population decay (T1) effects and optical transition dephasing (T2) effects, both neglected in earlier approaches. Our results are applicable even in the regime where perturbation theory breaks down. In particular, when the sum of the field frequencies approaches a molecular resonance a substantial enhancement of the photo-absorption rate (by a two-photon process) occurs even when one frequency becomes as small as the transition linewidth.

AB - We use a nonperturbative treatment to study multiphoton transitions in molecules with permanent dipole moments. This generalizes the perturbative treatment of Scharf and Band (Chem. Phys. Letters 144 (1988) 165) for two-photon transitions in molecules with permanent dipole moments in the presence of electromagnetic fields of two frequencies, one near resonance and the other small, Our nonperturbative density matrix treatment accounts for level population decay (T1) effects and optical transition dephasing (T2) effects, both neglected in earlier approaches. Our results are applicable even in the regime where perturbation theory breaks down. In particular, when the sum of the field frequencies approaches a molecular resonance a substantial enhancement of the photo-absorption rate (by a two-photon process) occurs even when one frequency becomes as small as the transition linewidth.

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DO - 10.1016/0009-2614(89)87117-9

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VL - 156

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JO - Chemical Physics Letters

JF - Chemical Physics Letters

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Multiphoton transitions in molecules with permanent dipole moments

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