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Izvestiya of Saratov University Physics

Temperature Effects in Vibronic Intensity of Absorption and Resonance Fluorescence Spectra

Maxim K. Berezin, M. L. Chernavina, Anna V. Novoselova, V. I. Berezin

Published Jan 1, 2014• 0 citations
Publisher
DOI
10.18500/1817-3020-2014-14-1-46-52

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The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
We investigate a quantum dot (QD) system coupled to a vibrational environment with a super-Ohmic spectral density and weakly to a leaky cavity mode, a model relevant for semiconductor-based single-photon sources. The phonon coupling induces dephasing and broadens the absorption and emission line shapes, while the weakly coupled cavity mode leads to effective driving of the QD. To capture non-Markovian effects, we use non-Markovian Quantum State Diffusion and its hierarchical extension the Hierarchy of Pure States to compute multitime correlation functions underlying absorption and resonance fluorescence spectra. We present numerical results for the absorption spectra at strong phonon coupling and finite temperature, as well as for resonance fluorescence spectra at varying phonon coupling strengths and temperatures, and analyse the visibility of the resonance fluorescence spectra to provide insights into how phonon coupling and thermal effects influence the spectral features.
A dressed-atom approach to resonance fluorescence in intense laser fields is presented. Simple and general results are derived which include the now well known predictions concerning two-level atoms but are not restricted to such simple cases. The positions of the various components of the fluorescence and absorption spectra are given by the allowed Bohr frequencies of the total system: atom+laser mode (dressed atom). The master equation, describing spontaneous emission from the dressed atom is solved in the limit of high intensities. Simple expressions, taking into account the effect of cascades, are derived for the widths of the components.