Ultrafast dynamics in the vicinity of quantum light-induced conical intersections

被引:44
作者
Csehi, Andras [1 ,2 ]
Kowalewski, Markus [3 ]
Halasz, Gabor J. [4 ]
Vibok, Agnes [1 ,2 ]
机构
[1] Univ Debrecen, Dept Theoret Phys, POB 400, H-4002 Debrecen, Hungary
[2] ELI HU Nonprofit Ltd, ELI ALPS, Dugonics Ter 13, H-6720 Szeged, Hungary
[3] Stockholm Univ, Dept Phys, AlbaNova Univ Ctr, SE-10691 Stockholm, Sweden
[4] Univ Debrecen, Dept Informat Technol, POB 400, H-4002 Debrecen, Hungary
基金
瑞典研究理事会;
关键词
optical and microwave cavities; Fock states; population transfer; nonadiabatic couplings; light-induced conical intersections; MOLECULAR-DYNAMICS; BORN-OPPENHEIMER; NONADIABATIC PHENOMENA; CHEMISTRY; STATE; PHOTODISSOCIATION; SPECTROSCOPY; ALIGNMENT; CAVITIES;
D O I
10.1088/1367-2630/ab3fcc
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Nonadiabatic effects appear due to avoided crossings or conical intersections (CIs) that are either intrinsic properties in field-free space or induced by a classical laser field in a molecule. It was demonstrated that avoided crossings in diatomics can also be created in an optical cavity. Here, the quantized radiation field mixes the nuclear and electronic degrees of freedom creating hybrid field-matter states called polaritons. In the present theoretical study we go further and create CIs in diatomics by means of a radiation field in the framework of cavity quantum electrodynamics. By treating all degrees of freedom, that is the rotational, vibrational, electronic and photonic degrees of freedom on an equal footing we can control the nonadiabatic quantum light-induced dynamics by means of CIs. First, the pronounced difference between the the quantum light-induced avoided crossing and the CI with respect to the nonadiabatic dynamics of the molecule is demonstrated. Second, we discuss the similarities and differences between the classical and the quantum field description of the light for the studied scenario.
引用
收藏
页数:8
相关论文
共 57 条
[31]   Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings [J].
Kowalewski, Markus ;
Bennett, Kochise ;
Mukamel, Shaul .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2016, 7 (11) :2050-2054
[32]   Non-adiabatic dynamics of molecules in optical cavities [J].
Kowalewski, Markus ;
Bennett, Kochise ;
Mukamel, Shaul .
JOURNAL OF CHEMICAL PHYSICS, 2016, 144 (05)
[33]  
Lim JS, 2010, NAT CHEM, V2, P627, DOI [10.1038/NCHEM.702, 10.1038/nchem.702]
[34]   Multiscale Molecular Dynamics Simulations of Polaritonic Chemistry [J].
Luk, Hoi Ling ;
Feist, Johannes ;
Toppari, J. Jussi ;
Groenhof, Gerrit .
JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2017, 13 (09) :4324-4335
[35]   PHYSICAL CHEMISTRY Seaming is believing [J].
Martinez, Todd J. .
NATURE, 2010, 467 (7314) :412-413
[36]   Can Ultrastrong Coupling Change Ground-State Chemical Reactions? [J].
Martinez-Martinez, Luis A. ;
Ribeiro, Raphael F. ;
Campos-Gonzalez-Angulo, Jorge ;
Yuen-Zhou, Joel .
ACS PHOTONICS, 2018, 5 (01) :167-176
[37]   THE MULTI-CONFIGURATIONAL TIME-DEPENDENT HARTREE APPROACH [J].
MEYER, HD ;
MANTHE, U ;
CEDERBAUM, LS .
CHEMICAL PHYSICS LETTERS, 1990, 165 (01) :73-78
[38]   Laser-induced conical intersections in molecular optical lattices [J].
Moiseyev, Nimrod ;
Sindelka, Milan ;
Cederbaum, Lorenz S. .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 2008, 41 (22)
[39]   Conical intersection dynamics of the primary photoisomerization event in vision [J].
Polli, Dario ;
Altoe, Piero ;
Weingart, Oliver ;
Spillane, Katelyn M. ;
Manzoni, Cristian ;
Brida, Daniele ;
Tomasello, Gaia ;
Orlandi, Giorgio ;
Kukura, Philipp ;
Mathies, Richard A. ;
Garavelli, Marco ;
Cerullo, Giulio .
NATURE, 2010, 467 (7314) :440-U88
[40]   Polariton chemistry: controlling molecular dynamics with optical cavities [J].
Ribeiro, Raphael F. ;
Martinez-Martinez, Luis A. ;
Du, Matthew ;
Campos-Gonzalez-Angulo, Jorge ;
Yuen-Zhou, Joel .
CHEMICAL SCIENCE, 2018, 9 (30) :6325-6339