AI 中文总结
本研究提出了名为cQUEDA的从头算框架，可模拟分子极化激元的超快非线性腔QED光谱，计算高效且适用性广，解决了腔QED中极化激元超快动力学模拟的核心问题。
AI 中文摘要
在本通讯中，我们提出了一种用于模拟分子极化激元的超快瞬态吸收泵浦-探测光谱的理论框架。我们在准经典 doorway-Window 近似下推导并实现了极化激元态的腔量子电动力学（QED）演化方程，该框架简称为 cQUEDA /sikeda/。此框架利用无腔情况下混合量子-经典动力学模拟的输出，再计入包含腔损耗率、耦合强度和频率失谐量的腔参数，进而模拟瞬态吸收泵浦-探测光谱。由此，我们解决了腔 QED 领域的一个核心悬而未决问题，即极化激元超快动力学与非线性光学性质的模拟。我们通过计算强耦合至腔的吡嗪的瞬态吸收泵浦-探测光谱的基态漂白（GSB）、受激发射（SE）和激发态吸收（ESA）贡献，验证了该方法的性能。cQUEDA 是一种即时计算高效的框架，对计算机要求低：例如，吡嗪的计算在现代笔记本电脑上仅需数分钟。cQUEDA 适用范围广泛，可推广用于模拟各类非线性光谱信号和量子光学响应。
英文摘要
In this letter we introduce a theoretical framework for the simulation of ultrafast transient absorption pump-probe spectra of molecular polaritons. We derive and implement the cavity quantum electrodynamics (QED) evolution equations of polaritonic states within the framework of the quasi-classical doorway-Window pproximation, hereto referred cQUEDA /sikeda/. This framework uses outputs from mixed quantum-classical dynamics simulations in the absence of the cavity. Then by including cavity parameters accounting for cavity rate loss, coupling strength, and frequency detuning, we simulate transient absorption pump-probe spectra. Consequently, we address one of the main standing problems of cavity QED, the simulation of polaritons ultrafast dynamics and nonlinear optical properties. We demonstrate the performance of our method by computing the ground-state bleach (GSB), stimulated emission (SE), and excited-state absorption (ESA) contributions of transient absorption pump-probe spectra of pyrazine strongly coupled to a cavity. The cQUEDA is an on-the-fly computationally efficient framework with low computer requirements: the pyrazine calculations, for example, took minutes on modern laptops. cQUEDA offers wide-ranging applicability and can be generalized to model diverse nonlinear spectroscopic signals and quantum optics responses.
Comments18 pages, 1 figure
