利用超快光谱与可见/红外双激发荧光对长寿命振动热基态的直接观察

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中文摘要：在超快红外光谱测量中观察到的纳秒级弛豫诱导漂白信号被广泛认为是由于红外激发热化产生的局部热效应.本文结合超快红外泵浦/探测、二维红外光谱、可见泵浦/红外探测和超快可见/红外双共振荧光实验,发现甲醇溶液中荧光素二价阴离子的振动热基态寿命出人意料的长,能达到纳秒级.结果表明,在非线性红外实验中观察到的长寿命漂白信号在最初的几纳秒内一定存在这些热基态的重要贡献.类似的机制很可能也适用于其他分子系统.热基态的存在时间能比以往的预期长得多,有可能被应用于调控化学反应.

外文标题：Direct Observation of Long-Lived Vibrational Hot Ground States by Ultrafast Spectroscopy and Visible/Infrared Double Excitation Fluorescence

外文摘要：It is widely believed that the relaxation-induced bleaching signals at nanoseconds observed in ultrafast infrared spectro-scopic measurements are due to the local heat effect resulting from the thermal-ization of the infrared exci-tations.In this work,com-bining ultrafast IR pump/probe,2D-IR,visible pump/IR probe,and ultrafast visible/IR double resonant fluores-cence experiments,the vibrational hot ground states of fluorescein dianion in methanol solu-tions are found to be unexpectedly long,at the time scale of nanoseconds.This result indi-cates that the long-standing bleaching signal observed in the nonlinear IR experiments must have significant contributions from these hot ground states for the initial couple of ns.It is likely that a similar mechanism can also hold for other molecular systems.The hot ground states can last much longer than conventionally expected,which can potentially be applied to modify chemical reactions.

外文关键词：

Ultrafast spectroscopyFluorescenceVisible IR double excitationLong-lived hot ground states2D-IRPump-probe

作者：

喻琪锐、李鑫茂、沈成桢、于志浩、关键鑫、郑俊荣

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作者单位：

北京大学化学与分子工程学院,北京 100871

关键词：

超快光谱荧光可见红外双激发长寿命热基态二维红外光谱泵浦-探测

基金：

国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金Min-istry of Science and Technology of China(a special talent program)Beijing City

项目编号：

222030062192790192261206216278051217401221673004218210042167400121790363

出版年：

2024

DOI：

10.1063/1674-0068/cjcp2311116

化学物理学报(英文版)

中国物理学会

化学物理学报(英文版)

CSTPCDEI

影响因子：0.162

ISSN：1674-0068

年,卷(期)：2024.37(2)

参考文献量60