Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

physica status solidi (b)

Theory of Absorption Profiles of Molecular Transitions in Dense Media

H. Paerschke, K.‐E. Süsse, D.‐G. Welsch

Published Mar 1, 1980• 2 citations
Publisher

Abstract

Abstract Within the framework of quantum theory the radiationless phase relaxation of a molecular transition in a dense medium is described by an integro‐differential equation. From the Fourier transform of this equation formulas are derived for calculating the corresponding absorption profiles. For the case that the acoustic phonons of the medium are responsible for the phase relaxation a detailed discussion of the resulting absorption profiles is given.

DOI
10.1002/pssb.2220980125

Related papers

Theory of Absorption and Dispersion Profiles of Molecular Transitions in Dense Media

H. Paeeschke, K.‐E. Süsse, D.‐G. Welsch +1 more

Abstract Starting from quantum theoretical principles the phase relaxation is described of a molecule localized in a dense medium by an integro‐differential equation. Using this equation, which leads to a non‐exponential phase decay, general formulas are derived for calculating the absorption and dispersion profiles of vibronic and vibrational transitions of the guest molecule. In detail the calculations are performed for the case that the acoustic phonons of the medium are responsible for the phase relaxation. Especially it is shown, that in comparison with the Lorentz profile the wings of a real absorption profile become steeper with increasing ratio between dephasing rate y and Debye frequency wD‐ Only for γ/wD ≪ 1 the absorption profiles are expected to be Lorentz profiles. The dispersion is found to increase with increasing ratio γ/wD. Both the real absorption and dispersion curves are asymmetric ones.

physica status solidi (b)•Aug 1, 1977•2 citations

Absorption of Ultrashort Laser Pulses in an Optically Dense Medium

Valery Alexandrovich Astapenko

Abstract In the framework of the consistent microscopic theory, universal analytic expressions describing absorption of laser pulses of an arbitrary duration in an optically dense medium have been derived, and their limiting cases have been considered. For the Gaussian and Lorentzian spectral profiles, simple expressions have been obtained for the absorption coefficient as a function of dimensionless parameters (optical thickness of the medium, the pulse duration and carrier frequency). Based on the performed calculations, the effect of the optical thickness of the medium on the dependences of the absorption coefficient on the pulse parameters has been revealed.

Journal of Experimental and Theoretical Physics•Jun 1, 2024•0 citations

Comments on a semigroup formalism for the description of phase and population relaxation processes

Ronnie Kosloff, Stuart A. Rice

Population and phase relaxation in two molecular models is studied. The analysis is based on recent work by Lindblad, in which the time evolution of an N-level quantum system is described using the coresponding generator of a completely positive semigroup. One of the models studied corresponds to a diatomic molecule in a dense medium. New results are obtained for the influence of two quantum transitions on population and phase relaxation. The other model studied corresponds to the case of exchange dephasing in a polyatomic molecule embedded in a dense medium. The formalism permits inclusion of coupling terms neglected by Harris, Shelby, and Cornelius; it is shown that inclusion of these terms leads to a rich range of line shapes, which information is not available from the approximation used by Harris et al.

The Journal of Chemical Physics•Apr 15, 1980•41 citations

Interaction of a light pulse with a multilevel molecular system

Maria V. Bogdanova, Tamara M. Il'inova, R. V. Khokhlov

The results are given of a theoretical investigation of the interaction of a laser pulse with a molecular medium. Allowance for the vibrational relaxation processes is made within the diffusion approximation framework which makes it possible to describe relaxation as the diffusion of particles in continuous electron energy bands. A simultaneous solution is obtained of the diffusion equations for the medium and the equations for the radiation field in the special cases of slow and fast vibrational relaxation. It is shown that the fast relaxation, which prevents gain saturation, increases the signal energy compared with the case of slow relaxation in an amplifying medium and reduces this energy compared with such relaxation in an absorbing medium. Expressions are obtained for the functions which describe the distributions of the band particles established by the investigated signal. The analysis made shows that the diffusion model can be applied to the interaction between laser pulses and molecular media.

Soviet Journal of Quantum Electronics•Sep 30, 1976•1 citation

Vibrational relaxation of a molecule in a dense medium

Abraham Nitzan, Joshua Jortner

In this paper we consider some features of vibrational relaxation of a guest molecule in a host matrix. The model system involves a harmonic molecule interacting with a harmonic medium. The molecule-medium coupling was handled by the rotating wave approximation considering linear terms in the intramolecular displacements and high terms in the medium displacements. Three specific models for the molecule-medium coupling were considered, which involve single phonon decay, vibron-phonon decay and multiphonon decay. Within the framework of the random phase approximation the Heisenberg equations of motion for the system could be expressed in terms of a unified scheme which is valid for both single phonon and multiphonon processes. Explicit solutions were derived utilizing the Wigner-Weisskopf approximation. This generalized formalism was applied for the study of the time evolution of the distribution, the cooling and the heating processes of the oscillator by a thermal field and for the coupling between vibrational relaxation and infra-red emission.

Molecular Physics•Mar 1, 1973•202 citations

A kinetic equation is derived for the forced population relaxation in a gas in the limiting case of sharp col- lisions (with complete loss of phase coherence). The solution is examined for the conditions under which it satisfies the basic kinetic equation of the transition model.

Anatoly I. Burshtein

It is possible to calculate exactly the effects of monochromatic light on a gas molecule (two-level system) in free flight. The absorption kinetics (with allowance for molecular interactions) may also be discussed exactly from Lorenz's model: instantaneous collisions with complete loss of phase memory. The population of the ground state may be put in the form

•Jan 1, 1965•0 citations
Abstract Within the framework of quantum theory the radiationless phase relaxation of a molecular transition in a dense medium is described by an integro‐differential equation. From the Fourier transform of this equation formulas are derived for calculating the corresponding absorption profiles. For the case that the acoustic phonons of the medium are responsible for the phase relaxation a detailed discussion of the resulting absorption profiles is given.
Abstract Starting from quantum theoretical principles the phase relaxation is described of a molecule localized in a dense medium by an integro‐differential equation. Using this equation, which leads to a non‐exponential phase decay, general formulas are derived for calculating the absorption and dispersion profiles of vibronic and vibrational transitions of the guest molecule. In detail the calculations are performed for the case that the acoustic phonons of the medium are responsible for the phase relaxation. Especially it is shown, that in comparison with the Lorentz profile the wings of a real absorption profile become steeper with increasing ratio between dephasing rate y and Debye frequency wD‐ Only for γ/wD ≪ 1 the absorption profiles are expected to be Lorentz profiles. The dispersion is found to increase with increasing ratio γ/wD. Both the real absorption and dispersion curves are asymmetric ones.
Abstract In the framework of the consistent microscopic theory, universal analytic expressions describing absorption of laser pulses of an arbitrary duration in an optically dense medium have been derived, and their limiting cases have been considered. For the Gaussian and Lorentzian spectral profiles, simple expressions have been obtained for the absorption coefficient as a function of dimensionless parameters (optical thickness of the medium, the pulse duration and carrier frequency). Based on the performed calculations, the effect of the optical thickness of the medium on the dependences of the absorption coefficient on the pulse parameters has been revealed.
Population and phase relaxation in two molecular models is studied. The analysis is based on recent work by Lindblad, in which the time evolution of an N-level quantum system is described using the coresponding generator of a completely positive semigroup. One of the models studied corresponds to a diatomic molecule in a dense medium. New results are obtained for the influence of two quantum transitions on population and phase relaxation. The other model studied corresponds to the case of exchange dephasing in a polyatomic molecule embedded in a dense medium. The formalism permits inclusion of coupling terms neglected by Harris, Shelby, and Cornelius; it is shown that inclusion of these terms leads to a rich range of line shapes, which information is not available from the approximation used by Harris et al.
The results are given of a theoretical investigation of the interaction of a laser pulse with a molecular medium. Allowance for the vibrational relaxation processes is made within the diffusion approximation framework which makes it possible to describe relaxation as the diffusion of particles in continuous electron energy bands. A simultaneous solution is obtained of the diffusion equations for the medium and the equations for the radiation field in the special cases of slow and fast vibrational relaxation. It is shown that the fast relaxation, which prevents gain saturation, increases the signal energy compared with the case of slow relaxation in an amplifying medium and reduces this energy compared with such relaxation in an absorbing medium. Expressions are obtained for the functions which describe the distributions of the band particles established by the investigated signal. The analysis made shows that the diffusion model can be applied to the interaction between laser pulses and molecular media.
In this paper we consider some features of vibrational relaxation of a guest molecule in a host matrix. The model system involves a harmonic molecule interacting with a harmonic medium. The molecule-medium coupling was handled by the rotating wave approximation considering linear terms in the intramolecular displacements and high terms in the medium displacements. Three specific models for the molecule-medium coupling were considered, which involve single phonon decay, vibron-phonon decay and multiphonon decay. Within the framework of the random phase approximation the Heisenberg equations of motion for the system could be expressed in terms of a unified scheme which is valid for both single phonon and multiphonon processes. Explicit solutions were derived utilizing the Wigner-Weisskopf approximation. This generalized formalism was applied for the study of the time evolution of the distribution, the cooling and the heating processes of the oscillator by a thermal field and for the coupling between vibrational relaxation and infra-red emission.