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Hao-Yue Zhang

Publications and source records attributed to Hao-Yue Zhang.

4 recordsLinked to original sources

Numerically-Exact Quantum-Simulation Approach for Two-Dimensional Spectroscopy of Open Quantum Systems

Two-dimensional spectroscopy (2DS) is a powerful ultrafast technique for probing electronic and vibrational dynamics in complex microscopic systems. Extracting detailed information on system dynamics and system-bath interactions from 2DS experiments requires precise theoretical simulations for comparison, which motivates the development of numerically-exact and computationally-efficient simulation approaches. Here, we propose a quantum-simulation approach for 2DS based on the bath-engineering technique (BET), which has been successfully employed in quantum simulations of open quantum dynamics. To demonstrate our approach, we first simulate the 2DS of a driven four-level system in chiral enantiodetection, where we also assess the applicability of the center-line slope (CLS) method for extracting time correlation functions (TCFs) from the 2DS. We further apply our approach to the 2DS of ${\rm Rh(CO)_2C_5H_7O_2}$ (RDC) dissolved in chloroform, where the results reproduce the main spectral patterns observed in experiments. Our work provides a numerically-exact and efficient framework for simulating 2DS, and can offer additional insight into the dynamics of open quantum systems.

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Non-Hermitian Hamiltonian Approach for Two-Dimensional Coherent Spectra of Driven Systems

Two-dimensional coherent spectroscopy (2DCS) offers significant advantages in terms of high temporal and frequency resolutions and signal-to-noise ratio. Until now, the response-function (RF) formalism has been the prevalent theoretical description. In this study, we compare the non-Hermitian Hamiltonian (NHH) method with the RF formalism in a three-level system with a constant control field. We obtain the signals from both approaches and compare their population dynamics and 2DCS. We propose the quasi-Green functions for the NHH method, which allows all dominant Liouville paths to be inferred. We further simulate the 2DCS of Rh(CO)$_2$C$_5$H$_7$O$_2$ (RDC) dissolved in hexane with the NHH method, which is in good agreement with the previous experiments. Although the NHH method overestimates relaxations, it provides all important paths by analytical solutions, which are different from the four paths used in the RF formalism. Our results demonstrate that the NHH method is more suitable than the RF formalism for investigating the systems including relaxation and control fields via the 2DCS.

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Observing Quantum Coherent Oscillations in a Three-Level Atoms via Electromagnetically Induced Transparency by Two-Dimensional Spectroscopy

Two-dimensional electronic spectroscopy (2DES) has high spectral resolution and is a useful tool for studying atom dynamics. In this paper, we show a smallest unit of electromagnetically induced transparency (EIT) for 2DES, that is, a three-level system. It is found that the original main peak is split into four small ones due to the introduction of the EIT. It suggests that the homogeneous broadening of 2DES can be effectively reduced by the 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.

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

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.

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