Competition between Light-Induced and Intrinsic Nonadiabatic Phenomena in Diatomics

被引:43
|
作者
Csehi, Andras [1 ,2 ]
Halasz, Gabor J. [3 ]
Cederbaum, Lorenz S. [4 ]
Vibok, Agnes [1 ,2 ]
机构
[1] Univ Debrecen, Dept Theoret Phys, POB 400, H-4002 Debrecen, Hungary
[2] ELI HU Non Profit Ltd, ELI ALPS, Dugon Ter 13, H-6720 Szeged, Hungary
[3] Univ Debrecen, Dept Informat Technol, POB 400, H-4002 Debrecen, Hungary
[4] Heidelberg Univ, Phys Chem Inst, Theoret Chem, D-69120 Heidelberg, Germany
来源
关键词
CONICAL INTERSECTION DYNAMICS; WAVE-PACKET DYNAMICS; PHOTODISSOCIATION;
D O I
10.1021/acs.jpclett.7b00413
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nonadiabatic effects arise due to avoided crossings or conical intersections that are either present naturally in field-free space or induced by a classical laser field in a molecule. Recently, it was demonstrated that nonadiabatic effects in diatomics can also be created in an optical cavity. Here, the quantized radiation field mixes the nuclear and electronic degrees of freedom. We show the equivalence of using the cavity's quantized field and the classical laser field as usually done for molecules. This is demonstrated for Nal, which exhibits a pronounced natural (intrinsic) avoided crossing that competes with the avoided crossing induced by the field. Furthermore, rotating molecules exhibit light induced conical intersections (LICIs) in classical laser light, and we also investigate the impact of these intersections. For Nal, we undoubtedly demonstrate a significant difference between the impact of the laser-induced avoided crossing and that of the LICl on the dynamics of the molecule.
引用
收藏
页码:1624 / 1630
页数:7
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