Asban Shahaf, Chernyak Vladimir Y, Mukamel Shaul
Department of Chemistry and Physics and Astronomy, University of California, Irvine, California 92697-2025, USA.
Department of Chemistry, Wayne State University, 5101 Cass Ave., Detroit, Michigan 48202, USA.
J Chem Phys. 2022 Mar 7;156(9):094202. doi: 10.1063/5.0079049.
We develop closed expressions for a time-resolved photon counting signal induced by an entangled photon pair in an interferometric spectroscopy setup. Superoperator expressions in Liouville-space are derived that can account for relaxation and dephasing induced by coupling to a bath. Interferometric setups mix matter and light variables non-trivially, which complicates their interpretation. We provide an intuitive modular framework for this setup that simplifies its description. Based on the separation between the detection stage and the light-matter interaction processes, we show that the pair entanglement time and the interferometric time-variables control the observed physics time scale. Only a few processes contribute in the limiting case of small entanglement time with respect to the sample response, and specific contributions can be singled out.
我们推导了在干涉光谱装置中由纠缠光子对诱导产生的时间分辨光子计数信号的闭式表达式。得出了刘维尔空间中的超算符表达式，该表达式能够解释与热库耦合引起的弛豫和退相。干涉装置以一种不平凡的方式混合了物质和光变量，这使其解释变得复杂。我们为该装置提供了一个直观的模块化框架，简化了其描述。基于检测阶段与光 - 物质相互作用过程之间的分离，我们表明，双光子纠缠时间和干涉时间变量控制着所观测到的物理时间尺度。在相对于样品响应的纠缠时间较短的极限情况下，只有少数过程起作用，并且可以区分出特定的贡献。
