Efficient Modeling of Organic Chromophores for Entangled Two-Photon Absorption

• DOI: 10.1021/jacs.0c02808
• Publication Date: 2020-05-13T12:51:57Z
• Authors: Gyeongwon Kang; Kobra Nasiri Avanaki; Martín A. Mosquera; Ryan K. Burdick; Juan P. Villabona...; Theodore Goodson; George C. Schatz
• Keywords: Chromophore; Two-Photon Absorption

The use of a nonclassical light source for studying molecular electronic structure has been great interest in many applications. Here we report theoretical study entangled two-photon absorption (ETPA) organic chromophores, and provide new insight into the quantitative relation between ETPA corresponding unentangled TPA based on significantly different line widths associated with processes. A sum-over-states approach is used to obtain classical cross sections explore contribution each state process. transition moments energies needed this calculation were obtained from second linear-response (SLR) TDDFT method [J. Chem. Phys., 2016, 144, 204105], which enables treatment relatively large polythiophene dendrimers that serve as absorbers. In addition, SLR calculations estimates excited radiative width, relate density states using quantum electrodynamic analysis. This analysis shows being studied, width orders magnitude narrower than TPA, highly photons Schmidt number. calculated are good agreement experimentally reported values. We also carried out state-resolved unveil pathways process, these demonstrate significant interference behavior. emphasize process plays critical role probing detailed molecule by light-matter nature limit.