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

Journal of the Physical Society of Japan

Duality in Resonance Raman Scattering

Yutaka Toyozawa, A. Kotani, Atsuko Sumi

Published May 1, 1977• 97 citations
Publisher

Abstract

Two complementary pictures for the resonance Raman scattering are presented, corresponding to two different ways of decomposing the four-time correlation function of dipole moment for this second-order process into a pair of two-time correlation functions. One is to take the auto-correlation of polarizability following the semi-classical picture for Raman scattering and expand it in powers of intra-system coupling; how the Raman spectra of higher orders approach the so-called luminescence is shown in the weak and strong coupling limits. Another is to study the correlation between absorption and emission processes; one can see how the relaxation of the strong coupled system after photoexcitation is reflected in the time-resolved emission spectra.

DOI
10.1143/jpsj.42.1495

Related papers

Resonance and Relaxation in Light Scattering

Yutaka Toyozawa

Time dependent description of resonance Raman scattering is performed for a general system, by a density matrix reformulation of damping theory originally used for resonance fluorescence of atom. Radiative damping in the intermediate states can be described in terms of "damping operator" in realistic situations. In large ergodic systems, the scattering reduces to luminescence if the relaxation time within the excited states is much shorter than the radiative lifetime. In a typical case, time resolved emission spectra consist of various stages (i) scattering complex where absorption and emission are inseparable, (ii) dynamical and then (iii) kinetic relaxations giving rise to the hot luminescence, which finally converges to (iv) the ordinary luminescence from relaxed excited states. Hot luminescence does not appear within a motionally narrowed line. The interpretation of spectra depends also on the method of observation.

Journal of the Physical Society of Japan•Aug 1, 1976•156 citations

Relative intensities and time characteristics of Raman scattering and luminescence under nearly resonant light excitation

Takashi Kushida, Shuichi Kinoshita

Various characteristics of frequency-integrated intensities of secondary radiation components near the resonance excitation region have been calculated for a three-level system coupled with a reservoir using a stochastic model. It has been found that the spectral and temporal characteristics of the resonant second-order optical processes can be understood consistently by considering that Raman scattering results from the average value of the induced-dipole moment with respect to the energy fluctuation due to the system-reservoir interaction, while luminescence results from its deviation from the average value. A simple method to determine parameter values that characterize the excited-state dynamics in condensed phases from the secondary radiation data is also discussed.

Physical Review A•Jun 1, 1990•14 citations

Time and spectral resolution in resonance scattering and resonance fluorescence

E. Courtens, A. Szöke

The theory of resonance Raman effect, resonantly enhanced two-photon absorption, and resonance fluorescence---valid also for strong fields---is treated in a unified and simplified way. Dressed states, Bloch equations, and perturbation theory are used to calculate line positions, and integrated intensities both for steady state and transient excitation. The case of adiabatic following is solved explicitly; it occurs when an off-resonance incident pulse is turned on and off slowly. It leads to the identification of Raman scattering, two-photon absorption, and Rayleigh scattering with an adiabatic process while fluorescence and consecutive two-photon absorption with nonadiabaticity. Time-dependent spectra are defined in a rigorous way. Our formulas agree in the various limits with those that appear in the literature.

Physical Review A•Apr 1, 1977•196 citations

Distinction between resonance Raman scattering and hot luminescence

Y. R. Shen

Using density-matrix formalism which takes into account relaxation more correctly, we show that resonance Raman scattering and hot luminescence are two distinct physical processes, although they are always simultaneously present and can interfere with each other. The transient response of the two processes are, however, different.

Physical review. B, Solid state•Jan 15, 1974•242 citations

Nonequilibrium DMFT approach to time-resolved Raman spectroscopy

Philipp Werner, Martin Eckstein, Naoto Tsuji

Raman spectroscopy uses light scattering to extract information on low-energy excitations of solids. The Raman process is described by diagrams which are fourth order in the light-matter interaction and in particular the resonant contribution, which involves four different space-time arguments, is difficult to evaluate. If one instead simulates explicitly the incoming (classical) light pulse, the Raman signal is given by the outgoing photon flux and can be determined from a two-point correlation function. Such a formalism can be used to compute the time-resolved Raman spectrum of nonequilibrium systems, as well as nonlinear signals which are higher order in the incoming field, such as hyper-Raman scattering. Here we explain how to implement this time-dependent formalism within the dynamical mean field theory framework. The method is illustrated with applications to the Holstein-Hubbard model in the strong electron-phonon coupling regime. We demonstrate hyper-Raman scattering in measurements with strong probe fields and frequency mixing signals in the presence of a pump field and simulate the evolution of Stokes and anti-Stokes features after photoexcitations of metallic and Mott insulating systems.

arXiv:2309.02866•Physical review. B./Physical review. B•Dec 27, 2023•2 citations

Resonance Raman Scattering and Luminescence from Highly Excited States

T. Takagahara

Resonance Raman scattering and luminescence under an intense excitation field are studied for both stationary and transient excitation regimes. By means of the Green function theory of resonance Raman scattering and luminescence we explain the characteristic features of the recent experiments on two-photon resonance Raman scattering via excitonic molecule in CuCl where the resonance dip and the asymmetry of the Raman yield around the resonance were observed. We ascribe the origin of the resonance dip of the Raman yield to the resonance enhancement of collisional damping of excitonic molecule and exciton states. The asymmetry of the Raman yield can be naturally understood in terms of the frequency and wave-vector dependent relaxation constants. Furthermore an approach is proposed which incorporates the coherence and correlation among excitonic molecules and excitons in their non-equilibrium state and clarifies their effects on the optical spectra.

Progress of Theoretical Physics Supplement•May 14, 2013•0 citations
Two complementary pictures for the resonance Raman scattering are presented, corresponding to two different ways of decomposing the four-time correlation function of dipole moment for this second-order process into a pair of two-time correlation functions. One is to take the auto-correlation of polarizability following the semi-classical picture for Raman scattering and expand it in powers of intra-system coupling; how the Raman spectra of higher orders approach the so-called luminescence is shown in the weak and strong coupling limits. Another is to study the correlation between absorption and emission processes; one can see how the relaxation of the strong coupled system after photoexcitation is reflected in the time-resolved emission spectra.
Time dependent description of resonance Raman scattering is performed for a general system, by a density matrix reformulation of damping theory originally used for resonance fluorescence of atom. Radiative damping in the intermediate states can be described in terms of "damping operator" in realistic situations. In large ergodic systems, the scattering reduces to luminescence if the relaxation time within the excited states is much shorter than the radiative lifetime. In a typical case, time resolved emission spectra consist of various stages (i) scattering complex where absorption and emission are inseparable, (ii) dynamical and then (iii) kinetic relaxations giving rise to the hot luminescence, which finally converges to (iv) the ordinary luminescence from relaxed excited states. Hot luminescence does not appear within a motionally narrowed line. The interpretation of spectra depends also on the method of observation.
Various characteristics of frequency-integrated intensities of secondary radiation components near the resonance excitation region have been calculated for a three-level system coupled with a reservoir using a stochastic model. It has been found that the spectral and temporal characteristics of the resonant second-order optical processes can be understood consistently by considering that Raman scattering results from the average value of the induced-dipole moment with respect to the energy fluctuation due to the system-reservoir interaction, while luminescence results from its deviation from the average value. A simple method to determine parameter values that characterize the excited-state dynamics in condensed phases from the secondary radiation data is also discussed.
The theory of resonance Raman effect, resonantly enhanced two-photon absorption, and resonance fluorescence---valid also for strong fields---is treated in a unified and simplified way. Dressed states, Bloch equations, and perturbation theory are used to calculate line positions, and integrated intensities both for steady state and transient excitation. The case of adiabatic following is solved explicitly; it occurs when an off-resonance incident pulse is turned on and off slowly. It leads to the identification of Raman scattering, two-photon absorption, and Rayleigh scattering with an adiabatic process while fluorescence and consecutive two-photon absorption with nonadiabaticity. Time-dependent spectra are defined in a rigorous way. Our formulas agree in the various limits with those that appear in the literature.
Raman spectroscopy uses light scattering to extract information on low-energy excitations of solids. The Raman process is described by diagrams which are fourth order in the light-matter interaction and in particular the resonant contribution, which involves four different space-time arguments, is difficult to evaluate. If one instead simulates explicitly the incoming (classical) light pulse, the Raman signal is given by the outgoing photon flux and can be determined from a two-point correlation function. Such a formalism can be used to compute the time-resolved Raman spectrum of nonequilibrium systems, as well as nonlinear signals which are higher order in the incoming field, such as hyper-Raman scattering. Here we explain how to implement this time-dependent formalism within the dynamical mean field theory framework. The method is illustrated with applications to the Holstein-Hubbard model in the strong electron-phonon coupling regime. We demonstrate hyper-Raman scattering in measurements with strong probe fields and frequency mixing signals in the presence of a pump field and simulate the evolution of Stokes and anti-Stokes features after photoexcitations of metallic and Mott insulating systems.
Resonance Raman scattering and luminescence under an intense excitation field are studied for both stationary and transient excitation regimes. By means of the Green function theory of resonance Raman scattering and luminescence we explain the characteristic features of the recent experiments on two-photon resonance Raman scattering via excitonic molecule in CuCl where the resonance dip and the asymmetry of the Raman yield around the resonance were observed. We ascribe the origin of the resonance dip of the Raman yield to the resonance enhancement of collisional damping of excitonic molecule and exciton states. The asymmetry of the Raman yield can be naturally understood in terms of the frequency and wave-vector dependent relaxation constants. Furthermore an approach is proposed which incorporates the coherence and correlation among excitonic molecules and excitons in their non-equilibrium state and clarifies their effects on the optical spectra.