Monitoring Wavepacket Dynamics at Conical Intersections by Entangled Two-Photon Absorption,ACS Photonics

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Monitoring Wavepacket Dynamics at Conical Intersections by Entangled Two-Photon Absorption
ACS Photonics ( IF 6.5 ) Pub Date : 2022-05-11 , DOI: 10.1021/acsphotonics.2c00255
Feng Chen ₁ , Bing Gu ₁ , Shaul Mukamel ₁

Affiliation

In this theoretical study, we show how ultrafast electron–nuclear dynamics in a molecule can be monitored by two-photon absorption of time–energy entangled photon pairs generated by spontaneous parametric down-conversion with a narrow-band pump. The dynamics is tracked by a controllable signal-idler delay. Time correlation of the entangled photons enables an ultrafast measurement even with a monochromatic pump. The frequency anticorrelation of the photon pair allows the projection of the intermediate excited-state wavepacket onto an energy-selected vibrational level on a higher-lying electronic state with high energy resolution. Such joint high temporal and energy resolution is not possible with classical light. We demonstrate our scheme for a conical intersection model with four electronic states and two vibrational modes. The ultrafast nuclear wavepacket dynamics around the conical intersection is imprinted onto the time- and frequency-resolved entangled two-photon absorption signals. Electronic population dynamics is obtained by the frequency-integrated signal.

中文翻译：

通过纠缠双光子吸收监测锥形交叉处的波包动力学

在这项理论研究中，我们展示了如何通过窄带泵自发参数下转换产生的时间能量纠缠光子对的双光子吸收来监测分子中的超快电子核动力学。动态由可控的信号闲置延迟跟踪。即使使用单色泵，纠缠光子的时间相关性也能实现超快测量。光子对的频率反相关允许将中间激发态波包投影到具有高能量分辨率的较高电子态的能量选择振动能级上。这种联合的高时间和能量分辨率对于经典光是不可能的。我们展示了具有四种电子状态和两种振动模式的锥形交叉模型的方案。锥形交叉点周围的超快核波包动力学被印在时间和频率分辨的纠缠双光子吸收信号上。电子种群动力学是通过频率积分信号获得的。

更新日期：2022-05-11

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