scholarly journals Dynamic mapping of conical intersection seams: A general method for incorporating the geometric phase in adiabatic dynamics in polyatomic systems

2017 ◽  
Vol 147 (4) ◽  
pp. 044109 ◽  
Author(s):  
Changjian Xie ◽  
Christopher L. Malbon ◽  
David R. Yarkony ◽  
Hua Guo
Keyword(s):  
Geometric Phase ◽  
Conical Intersection ◽  
Dynamic Mapping ◽  
Polyatomic Systems ◽  
Adiabatic Dynamics ◽  
General Method

Observation of the geometric phase effect in the H + HD → H2+ D reaction

Science ◽  
2018 ◽  
Vol 362 (6420) ◽  
pp. 1289-1293 ◽  
Author(s):  
Daofu Yuan ◽  
Yafu Guan ◽  
Wentao Chen ◽  
Hailin Zhao ◽  
Shengrui Yu ◽  
...  
Keyword(s):  
Cross Sections ◽  
Geometric Phase ◽  
Potential Energy Surfaces ◽  
Molecular Beams ◽  
Conical Intersection ◽  
Molecular Systems ◽  
Quantum State Resolved ◽  
State Potential ◽  
Energy Surfaces ◽  
Angular Oscillations

Theory has established the importance of geometric phase (GP) effects in the adiabatic dynamics of molecular systems with a conical intersection connecting the ground- and excited-state potential energy surfaces, but direct observation of their manifestation in chemical reactions remains a major challenge. Here, we report a high-resolution crossed molecular beams study of the H + HD → H2+ D reaction at a collision energy slightly above the conical intersection. Velocity map ion imaging revealed fast angular oscillations in product quantum state–resolved differential cross sections in the forward scattering direction for H2products at specific rovibrational levels. The experimental results agree with adiabatic quantum dynamical calculations only when the GP effect is included.

scholarly journals Polariton Induced Conical Intersection and Berry Phase

2021 ◽  
Author(s):  
Marwa Farag ◽  
Arkajit Mandal ◽  
Pengfei Huo
Keyword(s):  
Population Dynamics ◽  
Angular Distribution ◽  
Geometric Phase ◽  
Quantum Dynamics ◽  
Berry Phase ◽  
Optical Cavity ◽  
The Other ◽  
Conical Intersection ◽  
Fragment Angular Distribution ◽  
Molecular Rotations

We investigate the Polariton induced conical intersection (PICI) created from coupling a diatomicmolecule with the quantized photon mode inside an optical cavity, and the corresponding BerryPhase effects. We use the rigorous Pauli-Fierz Hamiltonian to describe the quantum light-matterinteractions between a LiF molecule and the cavity, and exact quantum propagation to investigatethe polariton quantum dynamics. The molecular rotations relative to the cavity polarization directionplay a role as the tuning mode of the PICI, resulting in an effective CI even within a diatomic molecule.To clearly demonstrate the dynamical effects of the Berry phase, we construct two additional modelsthat have the same Born-Oppenheimer surface, but the effects of the geometric phase are removed.We find that when the initial wavefunction is placed in the lower polaritonic surface, the Berryphase causes aπphase-shift in the wavefunction after the encirclement around the CI, indicatedfrom the nuclear probability distribution. On the other hand, when the initial wavefunction is placedin the upper polaritonic surface, the geometric phase significantly influences the couplings betweenpolaritonic states and therefore, the population dynamics between them. These BP effects are furtherdemonstrated through the photo-fragment angular distribution. PICI created from the quantizedradiation field has the promise to open up new possibilities to modulate photochemical reactivities.

Mixed state `on the fly' non-adiabatic dynamics: the role of the conical intersection topology

1998 ◽  
Vol 292 (3) ◽  
pp. 259-266 ◽  
Author(s):  
Stéphane Klein ◽  
Michael J. Bearpark ◽  
Barry R. Smith ◽  
Michael A. Robb ◽  
Massimo Olivucci ◽  
...  
Keyword(s):  
Mixed State ◽  
Conical Intersection ◽  
Adiabatic Dynamics

scholarly journals Polariton Induced Conical Intersection and Berry Phase

2021 ◽  
Author(s):  
Marwa Farag ◽  
Arkajit Mandal ◽  
Pengfei Huo
Keyword(s):  
Population Dynamics ◽  
Angular Distribution ◽  
Geometric Phase ◽  
Quantum Dynamics ◽  
Berry Phase ◽  
Optical Cavity ◽  
The Other ◽  
Conical Intersection ◽  
Fragment Angular Distribution ◽  
Molecular Rotations

We investigate the Polariton induced conical intersection (PICI) created from coupling a diatomicmolecule with the quantized photon mode inside an optical cavity, and the corresponding BerryPhase effects. We use the rigorous Pauli-Fierz Hamiltonian to describe the quantum light-matterinteractions between a LiF molecule and the cavity, and exact quantum propagation to investigatethe polariton quantum dynamics. The molecular rotations relative to the cavity polarization directionplay a role as the tuning mode of the PICI, resulting in an effective CI even within a diatomic molecule.To clearly demonstrate the dynamical effects of the Berry phase, we construct two additional modelsthat have the same Born-Oppenheimer surface, but the effects of the geometric phase are removed.We find that when the initial wavefunction is placed in the lower polaritonic surface, the Berryphase causes aπphase-shift in the wavefunction after the encirclement around the CI, indicatedfrom the nuclear probability distribution. On the other hand, when the initial wavefunction is placedin the upper polaritonic surface, the geometric phase significantly influences the couplings betweenpolaritonic states and therefore, the population dynamics between them. These BP effects are furtherdemonstrated through the photo-fragment angular distribution. PICI created from the quantizedradiation field has the promise to open up new possibilities to modulate photochemical reactivities.

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