Orchestrating Nuclear Dynamics in a Permanganate Doped Crystal with Chirped Pump–Probe Spectroscopy,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Orchestrating Nuclear Dynamics in a Permanganate Doped Crystal with Chirped Pump–Probe Spectroscopy
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-06-18 , DOI: 10.1021/acs.jpclett.4c00801
Emanuele Mai _{1,

2} , Partha Malakar ₃ , Giovanni Batignani _{1,

2} , Miles Martinati ₁ , Sanford Ruhman ₃ , Tullio Scopigno _{1,

4}

Affiliation

Pump–probe spectroscopy is a powerful tool to investigate light-induced dynamical processes in molecules and solids. Targeting vibrational excitations occurring on the time scales of nuclear motions is challenging, as pulse durations shorter than a vibrational period are needed to initiate the dynamics, and complex experimental schemes are required to isolate weak signatures arising from wavepacket motion in different electronic states. Here, we demonstrate how introducing a temporal delay between the spectral components of femtosecond beams, namely a chirp resulting in the increase of their duration, can counterintuitively boost the desired signals by 2 orders of magnitude. Measuring the time-domain vibrational response of permanganate ions embedded in a KClO₄ matrix, we identify an intricate dependence of the vibrational response on pulse chirps and probed wavelength that can be exploited to unveil weak signatures of the doping ions─otherwise dominated by the nonresonant matrix─or to obtain vibrational excitations pertaining only to the excited state, suppressing ground-state contributions.

中文翻译：

用啁啾泵浦-探针光谱协调高锰酸盐掺杂晶体中的核动力学

泵浦探针光谱是研究分子和固体中光诱导动力学过程的强大工具。针对核运动时间尺度上发生的振动激发具有挑战性，因为需要比振动周期短的脉冲持续时间来启动动力学，并且需要复杂的实验方案来隔离不同电子态下波包运动产生的微弱特征。在这里，我们演示了如何在飞秒光束的频谱分量之间引入时间延迟，即导致其持续时间增加的线性调频脉冲，可以违反直觉地将所需信号增强 2 个数量级。通过测量嵌入 KClO ₄基质中的高锰酸根离子的时域振动响应，我们发现了振动响应对脉冲啁啾和探测波长的复杂依赖性，可利用该依赖性来揭示掺杂离子的微弱特征（否则由非共振主导）矩阵──或者获得仅与激发态相关的振动激发，抑制基态贡献。

更新日期：2024-06-18

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南