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arXiv:2405.01837 · Physical Review A

Anomalously reduced homogeneous broadening of two-dimensional electronic spectroscopy at high temperature by detailed balance

Ru-Qiong Deng, Cheng-Ge Liu, Yi-Xuan Yao, Jing-Yi-Ran Jin, Hao-Yue Zhang, Yin Song, Qing Ai

Published May 1, 2024• 3 citations
arXivHTMLPDF

Abstract

Dissipation and decoherence of quantum systems in thermal environments is important to various spectroscopies. It is generally believed that dissipation can broaden the line shape of spectroscopies, and thus stronger system-bath interaction can result in more significant homogeneous broadening of two-dimensional electronic spectroscopy (2DES). Here we show that the case can be the opposite in the regime of electromagnetically induced transparency (EIT). We predict that assisted by EIT, the homogeneous broadening of the 2DES at a higher temperature can be significantly reduced due to the detailed balance. This anomalous effect is due to the long-lasting off-diagonal peaks in 2DES.

DOI
10.1103/physreva.109.052801

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Dissipation and decoherence of quantum systems in thermal environments is important to various spectroscopies. It is generally believed that dissipation can broaden the line shape of spectroscopies, and thus stronger system-bath interaction can result in more significant homogeneous broadening of two-dimensional electronic spectroscopy (2DES). Here we show that the case can be the opposite in the regime of electromagnetically induced transparency (EIT). We predict that assisted by EIT, the homogeneous broadening of the 2DES at a higher temperature can be significantly reduced due to the detailed balance. This anomalous effect is due to the long-lasting off-diagonal peaks in 2DES.
Two-dimensional electronic spectroscopy (2DES) has high spectral resolution and is a useful tool for studying atomic dynamics. In this paper, we show a smallest unit of electromagnetically induced transparency (EIT) for 2DES, i.e., a three-level system. It is found that the original main peak is split into four small ones due to the introduction of EIT. It suggests that the homogeneous broadening of 2DES can be effectively reduced by EIT. Moreover, in sharp contrast to a constant height, the height of the peaks will manifest a damped oscillation with respect to the population time. It seems that the quantum-beat phenomenon appears. These findings may help us obtain more information about the dynamics of excited states.
We study, theoretically and experimentally, electromagnetically induced transparency (EIT) in two different solid-state systems. Unlike many implementations in homogeneously broadened media, these systems exhibit inhomogeneous broadening of their optical and spin transitions typical of solid-state materials. We observe EIT lineshapes typical of atomic gases, including a crossover into the regime of Autler-Townes splitting, but with the substitution of the inhomogeneous widths for the homogeneous values. We obtain quantitative agreement between experiment and theory for the width of the transparency feature over a range of optical powers and inhomogeneous linewidths. We discuss regimes over which analytical and numerical treatments capture the behavior. As solid-state systems become increasingly important for scalable and integratable quantum optical and photonic devices, it is vital to understand the effects of the inhomogeneous broadening that is ubiquitous in these systems. The treatment presented here can be applied to a variety of systems, as exemplified by the common scaling of experimental results from two different systems.
The key feature of photon echo-based spectroscopies is a selective elimination of the inhomogeneous broadening. Fast homogeneous dephasing typical for large macromolecules makes it difficult to resolve the congested spectra even if the inhomogeneous component is eliminated. We propose a novel two-dimensional spectroscopy in which a series of temporally separated probe pulses are combined with the strong narrowband control pulse. Using electromagnetically induced transparency originating from the interference between the control and probe pulses, we achieve an observation window for molecular response in narrow spectral intervals significantly smaller than the homogeneous dephasing limit.
We identify carrier scattering at densities below that which has previously been observed in semiconductor quantum wells. These effects are evident in the peak shapes of 2D double-quantum spectra, which change as a function of excitation density. At high excitation densities (>109 excitons/cm2), we observe untilted peaks similar to those reported in previous experiments. At low excitation densities (<108 excitons/cm2), we observe narrower tilted peaks. Using a simple simulation, we show that tilted peak shapes are expected in double-quantum spectra when inhomogeneous broadening is much larger than homogeneous broadening, and that fast pure-decoherence of the double-quantum coherence can obscure this peak tilt. These results show that carrier interactions are important at lower densities than previously expected, and that the “natural” double-quantum peak shapes are hidden by carrier interactions at the excitation densities typically used. Furthermore, these results demonstrate that analysis of 2D peak shapes in double-quantum spectroscopy provides an incisive tool for identifying interactions at low excitation density.
Electromagnetically coupled two-level systems play a central role in several condensed matter components being considered for quantum information processing applications. If the states couple to phonon excitations, their electromagnetic response is altered via phonon-assisted transitions and lifetime broadening. The former has been treated extensively for a number of specific two-level systems (e.g., excitons in artificial quantum dots, localized states associated with impurities or defects, etc.), but the latter has received less attention. Here we study a microscopic model of the dipole transition of a two-level system under the influence of both diagonal and nondiagonal interactions with a bath of phonons. Our results capture both the influence of the frequency distribution of phonons on the relative spectral weight of the zero-phonon transition and the phonon sidebands, and the broadening of the zero-phonon line due to nondiagonal electron-phonon coupling. We use a formalism that includes non-Markovian effects related to the feedback mechanism between the two-level system and the phonon bath. For simplified forms of the phonon spectral functions we provide analytical expressions up to second order in the coupling strength that demonstrate the importance of including both forms of electron-phonon coupling in studies of these systems. Our formalism can be generalized to higher orders of coupling and for realistic phonon spectral functions.