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

Physical Review A

Time delay in scattering at a resonance

Arvid Herzenberg, E. Stryjewski

Published Jan 1, 1977• 5 citations
Publisher

Abstract

Pulses of laser light which undergo Raman scattering by a molecule at a resonance are observed to consist of two components: a short pulse which lasts as long as the driving pulse, and a long tail which falls off with the lifetime of the excited state. It is shown that the recent observations of Williams, Rousseau, and Dworetsky on ${\mathrm{I}}_{2}$ can be fitted by theory; one has to suppose that the frequency spectrum of the driving pulses is broadened to an extent equivalent to a reduction of the stated rise and fall times by a factor of 10.

DOI
10.1103/physreva.15.234

Related papers

On the theory of time resolved near-resonance light scattering

Horia I. Metiu, John Ross, Abraham Nitzan

Time resolved resonance and near-resonance light scattering is analyzed by means of Green’s operator formalism. We study the process of a photon wavepacket colliding with and scattered from a given molecule. Two decay components similar to those observed by Williams, Rousseau, and Dworetsky are obtained under appropriate conditions. Unlike other recent treatments of this problem, the light pulse is not treated as a pure quantum state (minimum uncertainty wavepacket) but rather as a mixture having characteristic time and energy profiles. It is shown that the nature of the light pulse may strongly influence the ratio of the short time to the long time decay intensities.

The Journal of Chemical Physics•Aug 1, 1975•35 citations

Lifetimes for resonance fluorescence and near resonance Raman scattering

Shaul Mukamel, Joshua Jortner

In this paper we present a quantum mechanical treatment of time resolved resonant and near resonant light scattering from a molecular system. The time resolved decay pattern is characterized by just two types of lifetimes, those specifying the molecular system and those characterizing the light pulse, while the off resonance energy parameter affects the total intensity and, in some cases, the relative intensities of the different decay components. The theoretical results for the ’’isolated’’ molecule are confronted with the recent experimental data of Williams, Rousseau, and Dworetzky [Phys. Rev. Lett. 32, 196 (1974)] for resonance and near resonance photon scattering from I2. Finally, we present a general scheme for handling photon scattering from a multilevel molecular system.

The Journal of Chemical Physics•May 1, 1975•95 citations

Comment on "Resonant fluorescence and Raman scattering"

Stephen E. Schwartz

The uncertainty-principle implications of the recent study of Williams, Rousseau, and Dworetsky are considered. The incompatible requirements of excitation pulse duration and bandwidth rule out a test of their proposed relation between excitation frequency and scattering time in the transition from resonance fluorescence to Raman scattering.

Physical Review A•Mar 1, 1975•14 citations

Green Function Theory of Resonance Light-Pulse Scattering. I: Simple Application to Molecular Spectroscopy

Masami Kusunoki

A thermal Green function theory of resonance long-laser-pulse scattering is developed, correctly taking account of the uncertainty-relation between the time-resolved and the energy-resolved experiments and the effect of the sample surface. The transient scattering efficiency can be calculated by folding the retarded Green's functions which are given by the thermal average of the chronological products of the pulse-current (or -density) and current operators into an uncertainty-principle broadening function. The theory is applied to resonance light scattering from a simple molecule in gas for steady and transient cases, where all the collision processes are treated quantum-statistically. At low pressure, the resonance scattering is mainly composed of Raman scattering (RS), final-state redistribution scattering (FRS), final-state transfer scattering (FTS) and collision-induced redistribution scattering (CIRS). In the steady state, it is shown that ordinary resonance Raman scattering is equivalent to RS in collisionless case, that absorption followed by emission contains RS, FRS and FTS, and that absorption followed by redistribution followed by emission is the same phenomenon as CIRS which is weighted by rotational population of excited molecules. Moreover, recent laser-pulse data by Roussea, Patterson and Williams are satisfactorily explained. Connection between this theory and other work is discussed.

Progress of Theoretical Physics•Mar 1, 1976•6 citations

Pulse shapes of Raman and Rayleigh scattering

V. A. Morozov, P. P. Shorygin

Abstract The expressions for the pulse shapes of secondary radiation in the frequency range of Rayleigh scattering and resonance fluorescence and in the range of Raman scattering and shifted resonance fluorescence are obtained on the basis of the quantum treatment of transformation of light pulses, the resonance conditions for Raman and Rayleigh scattering being considerably different. The characteristic cases of different pulse shapes of Raman and Rayleigh scattering are considered for the condition when the molecules are irradiated by light pulses which are shorter then the lifetime of the excited state of the molecule and are weak enough not to result in saturation.

Journal of Raman Spectroscopy•Feb 1, 1986•1 citation

Resonance fluorescence and Raman scattering pumped by an adiabatic pulse

Б. В. Крыжановский, A. O. Melikyan

The approximation of nonoverlapping lines is used to calculate spectra of resonance fluorescence and Raman scattering when two- and three-level atoms are pumped by a smooth pulse of duration comparable with the excited-state lifetime. The difference between the quasienergy terms, that determines the satellite frequency, depends on time and has the same value twice, at the pulse leading and trailing edges, so that interference may occur between the radiation produced in the appropriate parts of the pulse. However, the interference pattern is blurred since radiative broadening destroys the coherence. Relationships are obtained between the parameters for which interference may be observed. An analysis is made of the change to short pulses when allowance can be made for the scattered field using the first order of perturbation theory.

Soviet Journal of Quantum Electronics•Jan 31, 1984•1 citation
Pulses of laser light which undergo Raman scattering by a molecule at a resonance are observed to consist of two components: a short pulse which lasts as long as the driving pulse, and a long tail which falls off with the lifetime of the excited state. It is shown that the recent observations of Williams, Rousseau, and Dworetsky on I2{\mathrm{I}}_{2}I2​ can be fitted by theory; one has to suppose that the frequency spectrum of the driving pulses is broadened to an extent equivalent to a reduction of the stated rise and fall times by a factor of 10.
Time resolved resonance and near-resonance light scattering is analyzed by means of Green’s operator formalism. We study the process of a photon wavepacket colliding with and scattered from a given molecule. Two decay components similar to those observed by Williams, Rousseau, and Dworetsky are obtained under appropriate conditions. Unlike other recent treatments of this problem, the light pulse is not treated as a pure quantum state (minimum uncertainty wavepacket) but rather as a mixture having characteristic time and energy profiles. It is shown that the nature of the light pulse may strongly influence the ratio of the short time to the long time decay intensities.
In this paper we present a quantum mechanical treatment of time resolved resonant and near resonant light scattering from a molecular system. The time resolved decay pattern is characterized by just two types of lifetimes, those specifying the molecular system and those characterizing the light pulse, while the off resonance energy parameter affects the total intensity and, in some cases, the relative intensities of the different decay components. The theoretical results for the ’’isolated’’ molecule are confronted with the recent experimental data of Williams, Rousseau, and Dworetzky [Phys. Rev. Lett. 32, 196 (1974)] for resonance and near resonance photon scattering from I2. Finally, we present a general scheme for handling photon scattering from a multilevel molecular system.
A thermal Green function theory of resonance long-laser-pulse scattering is developed, correctly taking account of the uncertainty-relation between the time-resolved and the energy-resolved experiments and the effect of the sample surface. The transient scattering efficiency can be calculated by folding the retarded Green's functions which are given by the thermal average of the chronological products of the pulse-current (or -density) and current operators into an uncertainty-principle broadening function. The theory is applied to resonance light scattering from a simple molecule in gas for steady and transient cases, where all the collision processes are treated quantum-statistically. At low pressure, the resonance scattering is mainly composed of Raman scattering (RS), final-state redistribution scattering (FRS), final-state transfer scattering (FTS) and collision-induced redistribution scattering (CIRS). In the steady state, it is shown that ordinary resonance Raman scattering is equivalent to RS in collisionless case, that absorption followed by emission contains RS, FRS and FTS, and that absorption followed by redistribution followed by emission is the same phenomenon as CIRS which is weighted by rotational population of excited molecules. Moreover, recent laser-pulse data by Roussea, Patterson and Williams are satisfactorily explained. Connection between this theory and other work is discussed.
Abstract The expressions for the pulse shapes of secondary radiation in the frequency range of Rayleigh scattering and resonance fluorescence and in the range of Raman scattering and shifted resonance fluorescence are obtained on the basis of the quantum treatment of transformation of light pulses, the resonance conditions for Raman and Rayleigh scattering being considerably different. The characteristic cases of different pulse shapes of Raman and Rayleigh scattering are considered for the condition when the molecules are irradiated by light pulses which are shorter then the lifetime of the excited state of the molecule and are weak enough not to result in saturation.
The approximation of nonoverlapping lines is used to calculate spectra of resonance fluorescence and Raman scattering when two- and three-level atoms are pumped by a smooth pulse of duration comparable with the excited-state lifetime. The difference between the quasienergy terms, that determines the satellite frequency, depends on time and has the same value twice, at the pulse leading and trailing edges, so that interference may occur between the radiation produced in the appropriate parts of the pulse. However, the interference pattern is blurred since radiative broadening destroys the coherence. Relationships are obtained between the parameters for which interference may be observed. An analysis is made of the change to short pulses when allowance can be made for the scattered field using the first order of perturbation theory.