Szidarovszky Tamás, Halász Gábor J, Császár Attila G, Cederbaum Lorenz S, Vibók Ágnes
Laboratory of Molecular Structure and Dynamics, Institute of Chemistry , ELTE Eötvös Loránd University and MTA-ELTE Complex Chemical System Research Group , Pázmány Péter sétány 1/A , H-1117 Budapest , Hungary.
Department of Information Technology , University of Debrecen , P.O. Box 400, H-4002 Debrecen , Hungary.
J Phys Chem Lett. 2018 Nov 1;9(21):6215-6223. doi: 10.1021/acs.jpclett.8b02609. Epub 2018 Oct 17.
In classical laser fields with frequencies resonant with the electronic excitation in molecules, it is by now known that conical intersections are induced by the field and are called light-induced conical intersections (LICIs). As optical cavities have become accessible, the question arises whether their quantized modes could also lead to the appearance of LICIs. A theoretical framework is formulated for the investigation of LICIs of diatomics in such quantum light. The eigenvalue spectrum of the dressed states in the cavity is studied, putting particular emphasis on the investigation of absorption spectra of the Na molecule, that is, on the transitions between dressed states, measured by employing a weak probe pulse. The dependence of the spectra on the light-matter coupling strength in the cavity and on the frequency of the cavity mode is studied in detail. The computations demonstrate strong nonadiabatic effects caused by the appearing LICI.
在频率与分子中的电子激发共振的经典激光场中,目前已知场会诱导出锥形交叉点,这些交叉点被称为光诱导锥形交叉点(LICIs)。随着光学腔变得可用,问题随之而来,即它们的量子化模式是否也会导致LICIs的出现。本文建立了一个理论框架,用于研究双原子分子在这种量子光中的LICIs。研究了腔内缀饰态的本征值谱,特别着重于对钠分子吸收光谱的研究,即通过使用弱探测脉冲测量的缀饰态之间的跃迁。详细研究了光谱对腔内光与物质耦合强度以及腔模频率的依赖性。计算结果表明,出现的LICI会引起强烈的非绝热效应。