Polariton Induced Conical Intersection and Berry Phase

Author(s):  
Marwa H Farag ◽  
Arkajit Mandal ◽  
Pengfei Huo

We investigate the Polariton induced conical intersection (PICI) created from coupling a diatomic molecule with the quantized photon mode inside an optical cavity, and the corresponding Berry Phase effects. We...


2021 ◽  
Author(s):  
Marwa Farag ◽  
Arkajit Mandal ◽  
Pengfei Huo

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.



2021 ◽  
Author(s):  
Marwa Farag ◽  
Arkajit Mandal ◽  
Pengfei Huo

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.



2017 ◽  
Vol 31 (12) ◽  
pp. 1750091 ◽  
Author(s):  
A. S. Abdel-Rady ◽  
Samia. S. A. Hassan ◽  
Abdel-Nasser A. Osman ◽  
Ahmed Salah

In this paper, we employ the energy surface method to study a system of a two-level atom Bose–Einstein condensate coupled to a high-finesse optical cavity interacting with a single-mode electromagnetic field in the presence of the Stark-shift. The energy surface, the Phase transitions and the Berry phase of the two-level atom in Dicke model are obtained. Employing the Holstein–Primakoff representation of the angular momentum Lie algebra, the coupling line separation of the normal phase and the superradiant phase which occurs in a collection of fluorescent emitters (such as atoms), between a state containing few electromagnetic excitations are studied and a mean field description of the Dicke model is presented. We notice that in the thermodynamic limit, the energy surface takes a simple form for a direct description of the phase transition. Moreover, we show that the Stark-shift parameters and the atom–atom interactions can strongly affect the phase transition point. The results in the absence of the Stark-shift agree precisely with those obtained by Li, Liu and Zhou, who studied the same model using a different method.





2020 ◽  
Author(s):  
A. Hosseinizadeh ◽  
N. Breckwoldt ◽  
R. Fung ◽  
R. Sepehr ◽  
M. Schmidt ◽  
...  

The structural dynamics of a molecule are determined by the underlying potential energy landscape. Conical intersections are funnels connecting otherwise separate energy surfaces. Posited almost a century ago 1, conical intersections remain the subject of intense scientific investigation 2–4. In biology, they play a pivotal role in vision, photosynthesis, and DNA stability 5,6. In ultrafast radiationless de-excitation 1,7, they are vital to ameliorating photon-induced damage. In chemistry, they tightly couple the normally separable nuclear and electronic degrees of freedom, precluding the Born-Oppenheimer approximation 8. In physics, they manifest a Berry phase, giving rise to destructive interference between clockwise and anti-clockwise trajectories around the conical intersection 9. Accurate theoretical methods for examining conical intersections are at present limited to small molecules. Experimental investigations are challenged by the required time resolution and sensitivity. Current structure-dynamical understanding of conical intersections is thus limited to simple molecules with around 10 atoms, on timescales of about 100 fs or longer 10. Spectroscopy can achieve better time resolution, but provides only indirect structural information. Here, we present single-femtosecond, atomic-resolution movies of a 2,000-atom protein passing through a conical intersection. These movies, extracted from experimental data by geometric machine learning, reveal the dynamical trajectories of de-excitation via a conical intersection, yield the key parameters of the conical intersection controlling the de-excitation process, and elucidate the topography of the electronic potential energy surfaces involved.





2015 ◽  
Vol 3 (21) ◽  
pp. 5377-5382 ◽  
Author(s):  
Kyu-Tae Lee ◽  
Masanori Fukuda ◽  
Suneel Joglekar ◽  
L. Jay Guo

Optical cavity-integrated perovskite solar cells capable of creating distinctive semitransparent colors with high efficiencies are demonstrated.



2013 ◽  
Vol 139 (18) ◽  
pp. 184309 ◽  
Author(s):  
Vladimir S. Petrovic ◽  
Sebastian Schorb ◽  
Jaehee Kim ◽  
James White ◽  
James P. Cryan ◽  
...  


2021 ◽  
Vol 8 (3) ◽  
pp. 034101
Author(s):  
Deependra Jadoun ◽  
Mahesh Gudem ◽  
Markus Kowalewski


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