Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

Chen, Hsing-Ta; Li, Tao E.; Sukharev, Maxim; Nitzan, Abraham; Subotnik, Joseph E.

doi:10.1063/1.5057366

Cited by 16 publications

(26 citation statements)

References 39 publications

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“…In order to address some of these challenges, we have recently shown the potential of the Multi-Trajectory Ehrenfest (MTEF) method to capture the correlated dynamics of a one-dimensional QED cavity-setup with a twolevel atomic system coupled to a large set of cavity photonmodes 29 . Furthermore, we note that in contrast to recent work of Subotnik and co-workers, who investigated light-matter interaction with an adjusted Ehrenfest theory based method to simulate spontaneous emission of classical light [30][31][32] , we focus on the description of quantized light fields. light-matter interactions, and a brief introduction of the class of model systems used in this study.…”

Section: Introductionmentioning

confidence: 99%

Benchmarking semiclassical and perturbative methods for real-time simulations of cavity-bound emission and interference

Hoffmann

Schäfer

Säkkinen

et al. 2019

The Journal of Chemical Physics

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We benchmark a selection of semiclassical and perturbative dynamics techniques by investigating the correlated evolution of a cavity-bound atomic system to assess their applicability to study problems involving strong light-matter interactions in quantum cavities. The model system of interest features spontaneous emission, interference, and strong coupling behaviour, and necessitates the consideration of vacuum fluctuations and correlated light-matter dynamics. We compare a selection of approximate dynamics approaches including fewest switches surface hopping, multi-trajectory Ehrenfest dynamics, linearized semiclasical dynamics, and partially linearized semiclassical dynamics. Furthermore, investigating self-consistent perturbative methods, we apply the Bogoliubov-Born-Green-Kirkwood-Yvon hierarchy in the second Born approximation. With the exception of fewest switches surface hopping, all methods provide a reasonable level of accuracy for the correlated light-matter dynamics, with most methods lacking the capacity to fully capture interference effects.Here we broaden our scope by investigating the performance of a comprehensive class of approximate quantum dynamics methods for simulating spontaneous emission in an optical cavity, including Ehrenfest meanfield theory 33,34 , Tully's surface hopping algorithm 35 , fully linearized 36 and partially linearized 37,38 semilclassical dynamics techniques, and a selection of approximate closures for the quantum mechanical Bogoliubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy. Through benchmark comparisons with exact numerical results, we assess the accuracy and efficiency of each method and highlight the possibilities and theoretical challenges involved with extending these approaches towards realistic systems.The remainder of this work is divided into four sections: Sec. II gives a short overview of general quantum mechanical arXiv:1909.07177v2 [quant-ph]

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Section: Introductionmentioning

confidence: 99%

Benchmarking semiclassical and perturbative methods for real-time simulations of cavity-bound emission and interference

Hoffmann

Schäfer

Säkkinen

et al. 2019

The Journal of Chemical Physics

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“…Recently, attempts have been made to include quantum EM-field effects even when evolving classical EM fields [29,30]. For example, in the recently proposed Ehrenfest+R approach [28,[31][32][33], our research group included vacuum fluctuations by propagating a swarm of augmented Maxwell-Schrödinger equations. Nevertheless, because Ehrenfest+R was developed in free space, the performance of the method in cavities is unknown.…”

Section: Introductionmentioning

confidence: 99%

Quasiclassical modeling of cavity quantum electrodynamics

Chen

Nitzan

et al. 2020

Phys. Rev. A

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We model a collection of N two-level systems (TLSs) coupled to a multimode cavity via Meyer-Miller-Stock-Thoss (MMST) dynamics, sampling both electronic and photonic zero-point energies (ZPEs) and propagating independent trajectories in Wigner phase space. By investigating the ground state stability of a single TLS, we use MMST dynamics to separately study both electronic ZPE effects (which would naively lead to the breakdown of the electronic ground state) as well as photonic ZPE effects (which would naively lead to spontaneous absorption). By contrast, including both effects (i.e., sampling both electronic and photonic ZPEs) leads to the dynamical stability of the electronic ground state. Therefore, MMST dynamics provide a practical way to identify the contributions of self-interaction and vacuum fluctuations. More importantly, we find that MMST dynamics can predict accurate quantum dynamics for both electronic populations and electromagnetic field intensity in the high saturation limit. For a single TLS in a cavity, MMST dynamics correctly predict the initial exponential decay of spontaneous emission, Poincaré recurrences, and the positional dependence of a spontaneous emission rate. For an array of N equally spaced TLSs with only one TLS excited initially, MMST dynamics correctly predict the modification of spontaneous emission rate as a function of the spacing between TLSs. Finally, MMST dynamics also correctly model Dicke's superradiance and subradiance (i.e., the dynamics when all TLSs are excited initially) including the correct quantum statistics for the delay time (as found by counting trajectories, for which a full quantum simulation is hard to achieve). Therefore, this work raises the possibility of simulating large-scale collective light-matter interactions with methods beyond mean-field theory.

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“…This led to an identical CRT correction, − h 2ωα g 2 α,I . In choosing our value for λ α , we follow Rubio, 83,91 Subotnik, [65][66][67]123 and others. 82,98 It would be a reasonable choice when one or more molecules is placed within a horizontal plane equidistant from the two mirrors (z = L z /2, where the sine wave reaches its maximum value).…”

Section: B Formaldehydementioning

confidence: 99%

“…52,59,60 In the study of polariton chemistry, it has been common to restrict the description of each electronic system to simplified two-or three-state model. 23,55,56,[61][62][63][64][65][66][67][68] The corresponding input parameters (energy levels and coupling elements), on which the models would heavily rely, are obtained from either experiments or firstprinciples quantum chemistry calculations. Through employing these models, it has been predicted that the coupling of molecular systems to quantized radiation modes could substantially modify the potential energy surfaces and create new conical intersections, 27,28,40,69 suppress or enhance photoisomerization reactions, 47,[70][71][72][73][74] increase the charge transfer and excitation energy trans-fer rates, 52,[75][76][77][78][79] accelerate the singlet fission kinetics, 41,80 and even control the chemical reactions remotely.…”

Section: Introductionmentioning

confidence: 99%

Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation

Yang,

Ou,

Pei

et al. 2021

Preprint

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Inspired by the formulation of quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) by Rubio and coworkers, we propose an implementation that uses dimensionless amplitudes for describing the photonic contributions to QED-TDDFT electron-photon eigenstates. The leads to a symmetric QED-TDDFT coupling matrix, which is expected to facilitate the future development of analytic derivatives. Through a Gaussian atomic basis implementation of the QED-TDDFT method, we examined the effect of dipole self-energy, rotating wave approximation, and the Tamm-Dancoff approximation on the QED-TDDFT eigenstates of model compounds (ethene, formaldehyde, and benzaldehyde) in an optical cavity. We highlight, in the strong coupling regime, the role of higher-energy and off-resonance excited states with large transition dipole moments in the direction of the photonic field, which are automatically accounted for in our QED-TDDFT calculations and might substantially affect the energy and composition of polaritons associated with lower-energy electronic states.

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Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

Cited by 16 publications

References 39 publications

Benchmarking semiclassical and perturbative methods for real-time simulations of cavity-bound emission and interference

Benchmarking semiclassical and perturbative methods for real-time simulations of cavity-bound emission and interference

Quasiclassical modeling of cavity quantum electrodynamics

Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation

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