Mandal Haraprasad, Giri Sajal Kumar, Jovanovski Sara, Varnavski Oleg, Zagorska Malgorzata, Ganczarczyk Roman, Chiang Tse-Min, Schatz George C, Goodson Theodore
Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States.
Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
J Phys Chem Lett. 2024 Sep 19;15(37):9493-9501. doi: 10.1021/acs.jpclett.4c01948. Epub 2024 Sep 10.
Investigations of entangled and classical two-photon absorption have been carried out for six donor (D)-acceptor (A)-donor (D) compounds containing the dithieno pyrrole (DTP) unit as donor and acceptors with systematically varied electronic properties. Comparing ETPA (quantum) and TPA (classical) results reveals that the ETPA cross section decreases with increasing TPA cross section for molecules with highly off-resonant excited states for single-photon excitation. Theory (TDDFT) results are in semiquantitative agreement with this anticorrelated behavior due to the dependence of the ETPA cross section but not TPA on the two-photon excited state lifetime. The largest cross section is found for a DTP derivative that has a single photon excitation energy closest to resonance with half the two-photon excitation energy. These results are important for the possible use of quantum light for low-intensity energy-conversion applications.
对六种含有二噻吩并吡咯（DTP）单元作为供体且受体具有系统变化电子性质的供体（D）-受体（A）-供体（D）化合物进行了纠缠和经典双光子吸收的研究。比较电子双光子吸收（ETPA，量子）和双光子吸收（TPA，经典）结果表明，对于单光子激发具有高度非共振激发态的分子，ETPA截面随TPA截面的增加而减小。理论（TDDFT）结果与这种反相关行为半定量一致，这是由于ETPA截面而非TPA对双光子激发态寿命的依赖性。对于单光子激发能量最接近双光子激发能量一半的共振的DTP衍生物，发现了最大截面。这些结果对于量子光在低强度能量转换应用中的可能应用很重要。
