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Journal of the Physical Society of Japan

Optical Stark Spectroscopy of a Brownian Oscillator in Intense Fields

Yoshitaka Tanimura, Shaul Mukamel

Published Jan 15, 1994• 91 citations
Publisher

Abstract

The optical Stark effect of a two-level system coupled to a Brownian oscillator (i.e. a harmonic mode which in turn is coupled to a heat bath) is studied using equations of motion for a reduced density matrix. These equations, derived using path integral techniques, can be used to study the combined effects of strong fields and dephasing processes at finite temperature, and interpolate continuously from the coherent to the overdamped limits where they reduce to the stochastic Gaussian-Markovian equation. Numerical calculations of probe absorption spectra for various pump intensities are presented, and show dynamical Stark splitting. In contrast to the Bloch equations which contain an infinite-temperature dephasing, we find that at finite temperature, the Stark peaks may have different heights even when the pump pulse is on resonance.

DOI
10.1143/jpsj.63.66

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The optical Stark effect of a two-level system coupled to a Brownian oscillator (i.e. a harmonic mode which in turn is coupled to a heat bath) is studied using equations of motion for a reduced density matrix. These equations, derived using path integral techniques, can be used to study the combined effects of strong fields and dephasing processes at finite temperature, and interpolate continuously from the coherent to the overdamped limits where they reduce to the stochastic Gaussian-Markovian equation. Numerical calculations of probe absorption spectra for various pump intensities are presented, and show dynamical Stark splitting. In contrast to the Bloch equations which contain an infinite-temperature dephasing, we find that at finite temperature, the Stark peaks may have different heights even when the pump pulse is on resonance.
A comprehensive numerical study of the optical Stark effect and associated phenomena in semiconductors is presented. The results are obtained from numerical solutions of the full semiconductor Bloch equations for bulk and quantum-well structures. Coherent oscillations, the optical Stark effect, and adiabatic following, i.e., ultrafast bleaching and recovery of the exciton, are discussed. The relative importance of the different contributions in the semiconductor Bloch equations is identified. Optical-absorption spectra are computed for different exciton dephasing models and a large variety of pump-probe excitation parameters.
Ultrafast pump-probe measurements evidence the dynamical Stark splitting in the exciton absorption spectrum of a single semiconductor quantum well. The intensity of the Stark sidebands in the spectrum is comparable to the linear absorption and their separation scales as the pump field amplitude. In the time domain the Rabi oscillations are observed. The semiconductor Bloch equations solved in the Hartree-Fock approximation demonstrate that the coherent exciton-light coupling dominates over the many-body dephasing.
Vibrational relaxation of a harmonic oscillator nonlinearly coupled to a heat bath is investigated by the Gaussian–Markovian quantum Fokker–Planck equation approach. The system–bath interaction is assumed to be linear in the bath coordinate, but linear plus square in the system coordinate modeling the elastic and inelastic relaxation mechanisms. Interplay of the two relaxation processes induced by the linear–linear and square–linear interactions in Raman or infrared spectra is discussed for various system–bath couplings, temperatures, and correlation times for the bath fluctuations. The one-quantum coherence state created through the interaction with the pump laser pulse relaxes through different pathways in accordance with the mechanisms of the system–bath interactions. Relations between the present theory, Redfield theory, and stochastic theory are also discussed.
The relaxation processes in a quantum system nonlinearly coupled to a harmonic Gaussian-Markovian heat bath are investigated by the quantum Fokker-Planck equation in the hierarchy form. This model describes frequency fluctuations in the quantum system with an arbitrary correlation time and thus bridges the gap between the Brownian oscillator model and the stochastic model by Anderson and Kubo. The effects of the finite correlation time and the system-bath coupling strength are studied for a harmonic model system by numerically integrating the equation of motion. The one-time correlation function of the system coordinate, which is measured in conventional Raman and infrared absorption experiments, already reflects the inhomogeneous character of the relaxation process. The finite correlation time of the frequency fluctuations, however, is directly evident only in the two- and three-time correlation function as probed by multidimensional spectroscopic techniques such as the Raman echo and the fifth-order 2D Raman experiment.
We examine the radiative properties of a two-level atom driven by a strong bichromatic field with frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$=${\mathrm{\ensuremath{\omega}}}_{0}$-${\mathrm{\ensuremath{\delta}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$=${\mathrm{\ensuremath{\omega}}}_{0}$+${\mathrm{\ensuremath{\delta}}}_{2}$, which can be asymmetrically placed about the atomic transition frequency ${\mathrm{\ensuremath{\omega}}}_{0}$ and can have different Rabi frequencies ${\mathrm{\ensuremath{\Omega}}}_{1}$ and ${\mathrm{\ensuremath{\Omega}}}_{2}$. Applying the optical Bloch equations for the bichromatic excitation, we derive an infinite set of equations of motion for the time evolution of the atomic variables. The equations are solved numerically by matrix inversion and Laplace transforms. Using the quantum regression theorem, we then solve for the steady-state total fluorescence intensity, and the resonance-fluorescence and absorption spectra. The spectra are found to depend on the frequency difference 2\ensuremath{\delta}=${\mathrm{\ensuremath{\delta}}}_{1}$+${\mathrm{\ensuremath{\delta}}}_{2}$, the average detuning \ensuremath{\Delta}=${\mathrm{\ensuremath{\omega}}}_{0}$-1/2(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$), and the Rabi frequencies of the driving fields. For ${\mathrm{\ensuremath{\Omega}}}_{1}$=${\mathrm{\ensuremath{\Omega}}}_{2}$=\ensuremath{\Omega}, the total fluorescent intensity displays a series of maxima for \ensuremath{\Delta}=\ifmmode\pm\else\textpm\fi{}n\ensuremath{\delta}\ensuremath{\mp}${\mathrm{\ensuremath{\Omega}}}^{2}$/4\ensuremath{\delta}, where the n are the odd integers. The intensity-dependent shift from the resonances n\ensuremath{\delta} is explained as an analog of the generalized Bloch-Siegert shift. The resonance-fluorescence spectrum for \ensuremath{\Delta}\ensuremath{\ne}0 appears to contain more peaks than that for \ensuremath{\Delta}=0.This is due to the splitting of the central peak and the even sidebands into doublets. The absorption spectrum of a weak-probe beam for \ensuremath{\Delta}=0 and equal Rabi frequencies consists of a symmetric series of dispersionlike sidebands separated from ${\mathrm{\ensuremath{\omega}}}_{0}$ by integer multiples of \ensuremath{\delta}, together with a central absorption peak at ${\mathrm{\ensuremath{\omega}}}_{0}$, whose amplitude oscillates with \ensuremath{\Omega}. For \ensuremath{\Delta}\ensuremath{\ne}0 and/or ${\mathrm{\ensuremath{\Omega}}}_{1}$\ensuremath{\ne}${\mathrm{\ensuremath{\Omega}}}_{2}$, the odd sidebands remain dispersionlike, while the central peak and the even sidebands split into absorption-emission doublets. A simple physical interpretation of the spectral features is given in terms of the dressed-atom model.
A numerical method is introduced that solves the optical Bloch equations describing a two-level atom interacting with a strong polychromatic pump field with an equidistant spectrum and an arbitrarily intense monochromatic probe field. The method involves a transformation of the optical Bloch equations into a system of equations with time-independent coefficients at steady state via double harmonic expansion of the density-matrix elements, which is then solved by the method of matrix inversion. The solutions so obtained lead immediately to the determination of the polarization of the atomic medium and of the absorption and dispersion spectra. The method is applied to the case when the pump field is bichromatic and trichromatic, and the physical interpretation of the numerically computed spectra is given.