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探索激发态简并性在与原子尺度光学的振动耦合中的作用。

Exploring the Role of Excited States' Degeneracy on Vibronic Coupling with Atomic-Scale Optics.

作者信息

Vasilev Kirill, Canola Sofia, Scheurer Fabrice, Boeglin Alex, Lotthammer Fanny, Chérioux Frédéric, Neuman Tomáš, Schull Guillaume

机构信息

Université de Strasbourg, CNRS, IPCMS, UMR 7504, F-67000 Strasbourg, France.

Institute of Physics, Czech Academy of Sciences, Cukrovarnická 10, 16200 Prague, Czech Republic.

出版信息

ACS Nano. 2024 Oct 15;18(41):28052-28059. doi: 10.1021/acsnano.4c07136. Epub 2024 Oct 3.

DOI:10.1021/acsnano.4c07136
PMID:39363581
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11483947/
Abstract

Interactions between molecular electronic and vibrational states manifest themselves in a variety of forms and have a strong impact on molecular physics and chemistry. For example, the efficiency of energy transfer between organic molecules, ubiquitous in biological systems and in organic optoelectronics, is strongly influenced by vibronic coupling. Using an approach based on scanning tunneling microscope-induced luminescence (STML), we reveal vibronic interactions in optical spectra of a series of single phthalocyanine derivative molecules featuring degenerate or near-degenerate excited states. Based on detailed theoretical simulations, we disentangle spectroscopic signatures belonging to Franck-Condon and Herzberg-Teller vibronic progressions in tip-position-resolved STML spectra, and we directly map out the vibronic coupling between the close-lying excited states of the molecules.

摘要

分子电子态与振动态之间的相互作用以多种形式表现出来，并对分子物理和化学产生强烈影响。例如，在生物系统和有机光电子学中普遍存在的有机分子之间的能量转移效率，受到振动电子耦合的强烈影响。我们采用基于扫描隧道显微镜诱导发光（STML）的方法，揭示了一系列具有简并或近简并激发态的单酞菁衍生物分子的光谱中的振动电子相互作用。基于详细的理论模拟，我们在针尖位置分辨的STML光谱中区分出属于弗兰克 - 康登和赫兹伯格 - 泰勒振动电子跃迁的光谱特征，并直接绘制出分子近邻激发态之间的振动电子耦合。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/354f2ae3b4ca/nn4c07136_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/a71c7401c4be/nn4c07136_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/b37b426f1e7c/nn4c07136_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/62ab4a180894/nn4c07136_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/354f2ae3b4ca/nn4c07136_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/a71c7401c4be/nn4c07136_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/b37b426f1e7c/nn4c07136_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/62ab4a180894/nn4c07136_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/669b/11483947/354f2ae3b4ca/nn4c07136_0004.jpg

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