在这项理论研究中，研究人员展示了如何利用时间能量纠缠光子对生成的光电子信号来监测分子的超快激发态动力学，同时具有高联合光谱和时间分辨率。与传统的经典光相比，这种技术不受傅里叶不确定性的限制。这种技术与泵浦强度呈线性关系，而不是二次关系，因此可以研究具有低光子通量的易碎生物样品。通过光电子探测实现光谱分辨率，结合可变相位延迟实现时间分辨率，该技术无需扫描泵浦频率和纠缠时间，大大简化了实验装置，目前的仪器条件下也可行。
研究人员将这种技术应用于吡咯光解离动力学的精确非绝热波包模拟计算中，在约化的两核坐标空间中进行研究。这项研究展示了超快量子光谱的独特优势。
附：英文原文
Title: Photoelectron spectroscopy with entangled photons; enhanced spectrotemporal resolution
Author: Gu, Bing, Sun, Shichao, Chen, Feng, Mukamel, Shaul
Issue&Volume: 2023-5-15
Abstract: In this theoretical study, we show how photoelectron signals generated by time-energy entangled photon pairs can monitor ultrafast excited state dynamics of molecules with high joint spectral and temporal resolutions, not limited by the Fourier uncertainty of classical light. This technique scales linearly, rather than quadratically, with the pump intensity, allowing the study of fragile biological samples with low photon fluxes. Since the spectral resolution is achieved by electron detection and the temporal resolution by a variable phase delay, this technique does not require scanning the pump frequency and the entanglement times, which significantly simplifies the experimental setup, making it feasible with current instrumentation. Application is made to the photodissociation dynamics of pyrrole calculated by exact nonadiabatic wave packet simulations in a reduced two nuclear coordinate space. This study demonstrates the unique advantages of ultrafast quantum light spectroscopy.
DOI: 10.1073/pnas.2300541120
Source: https://www.pnas.org/doi/10.1073/pnas.2300541120