Radiative thermalization in semiclassical simulations of light-matter interaction

Gadea, Esteban D.; Bustamante, Carlos M.; Todorov, Tchavdar N.; Scherlis, Damián A.

doi:10.1103/physreva.105.042201

Cited by 7 publications

(6 citation statements)

References 24 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In the limit of large N 1 or, equivalently, for the case of small excitations, both models converge to a same result. This coincidence is not surprising since, as we showed elsewhere, 51,52 small displacements from the ground state lead to better agreement with the Fermi golden rule. The additional term in Dicke's formulation is a consequence of spontaneous emission, 2 not present in our semiclassical scheme: when all the emitters are in the excited eigenstate, or N 1 = 0, the dissipated energy is zero because the system does not relax to the ground state.…”

supporting

confidence: 86%

“…51 This approach describes in the velocity gauge the same radiation field as the theory of Rashkovskiy in the length gauge. 52 In the Supporting Information we show that, same as that theory, it leads to the Abraham-Lorentz force, from which it can be expected that this treatment and those in refs 39 and 44 produce comparable dynamics. Our equation of motion is also closely connected to the master equation introduced by Agarwall in his approach to spontaneous emission using a two-level system 53 (see next section).…”

supporting

confidence: 72%

“…Similarly to other semiclassical approaches, this formalism does not include spontaneous emission from a stationary state, meaning with this that the system will not relax from an eigenstate unless it is perturbed. This can lead to discrepancies with respect to the Fermi golden Rule at high temperatures or when the excitated states are highly populated. , The role of the initial state is discussed in the Supporting Information. On the other hand, implicit in the derivation of the equation of motion is the long wave approximation, which assumes that the radiated field instantaneously affects the entire system, neglecting the retardation associated with the spatial separation.…”

mentioning

confidence: 99%

See 2 more Smart Citations

Tailoring Cooperative Emission in Molecules: Superradiance and Subradiance from First-Principles Simulations

Bustamante

Gadea

Todorov

et al. 2022

J. Phys. Chem. Lett.

Self Cite

View full text Add to dashboard Cite

Cooperative optical effects provide a pathway to both the amplification (superradiance) and the suppression (subradiance) of photon emission from electronically excited states. These captivating phenomena offer a rich variety of possibilities for photonic technologies aimed at electromagnetic energy manipulation, including lasers and high-speed emitting devices in the case of superradiance or optical energy storage in that of subradiance. The employment of molecules as the building pieces in these developments requires a precise understanding of the roles of separation, orientation, spatial distribution, and applied fields, which remains challenging for theory and experiments. These questions are addressed here through ab initio quantum dynamics simulations of collective emission on the basis of a novel semiclassical formalism and time-dependent density functional theory. By establishing the configurations leading to decoherence and how the fine-tuning of a pulse can accumulate or release optical energy in H 2 arrays, this report provides fundamental insight toward the design of real superradiant and subradiant devices.

show abstract

supporting

confidence: 86%

supporting

confidence: 72%

mentioning

confidence: 99%

See 1 more Smart Citation

Tailoring Cooperative Emission in Molecules: Superradiance and Subradiance from First-Principles Simulations

Bustamante

Gadea

Todorov

et al. 2022

J. Phys. Chem. Lett.

Self Cite

View full text Add to dashboard Cite

show abstract

“…Taking into account (25), one obtains the vector of the intrinsic magnetic moment of the Pauli field in the hydrogen atom…”

Section: Angular Momentum and Magnetic Moment Of The Pauli Field In T...mentioning

confidence: 99%

“…Semiclassical theories have made significant progress in describing the basic quantum effects that make up the experimental foundation of modern quantum mechanics, such as the Compton effect [1][2][3][4]18], photoelectric effect [5,21], thermal radiation [22,25], spontaneous emission and spontaneous transitions [6-12, 15-17, 19, 24], light-matter interactions [7,20], induced emission [6,7,20,22], Lamb shift [6,7,9], the Lamb-Retherford experiments [23], etc. It can be argued that at present there is not a single basic quantum effect that has not been described within the semiclassical theory.…”

Section: Introductionmentioning

confidence: 99%

Nonlinear Pauli Equation

Rashkovskiy¹

2022

Preprint

View full text Add to dashboard Cite

In the framework of the self-consistent Maxwell-Pauli theory, the non-linear Pauli equation is obtained. Stationary and nonstationary solutions of the nonlinear Pauli equation for the hydrogen atom are studied. We show that spontaneous emission and the related rearrangement of the internal structure of an atom, which is traditionally called a spontaneous transition, have a simple and natural description in the framework of classical field theory without any quantization and additional hypotheses. The behavior of the intrinsic magnetic moment (spin) of an electron wave in an external magnetic field is considered. We show that, according to the self-consistent Maxwell-Pauli theory, in a weak magnetic field, the intrinsic magnetic moment of an electron wave is always oriented parallel to the magnetic field strength vector, while in a strong magnetic field, depending on the initial orientation of the intrinsic magnetic moment, two orientations are realized: either parallel or antiparallel to the magnetic field strength vector.

show abstract

Fluorescence in quantum dynamics: Accurate spectra require post-mean-field approaches

Bustamante

Gadea

Todorov

et al. 2023

The Journal of Chemical Physics

View full text Add to dashboard Cite

Real time modelling of fluorescence with vibronic resolution entails the representation of the light-matter interaction coupled to a quantum-mechanical description of the phonons, and is therefore a challenging problem. In this work, taking advantage of the difference in time-scales characterizing internal conversion and radiative relaxation -which allows us to decouple these two phenomena by sequentially modelling one after the other- we simulate the electron dynamics of fluorescence through a master equation derived from the Redfield formalism. Moreover, we explore the use of a recent semiclassical dissipative equation of motion [ Phys. Rev. Lett. 126, 087401 (2021)], termed CEED, to describe the radiative stage. By comparing the results with those from the full quantum-electrodynamics treatment, we find that the semiclassical model does not reproduce the right amplitudes in the emission spectra when the radiative process involves the deexcitation to a manifold of closely lying states. We argue that this flaw is inherent to any mean-field approach, as it is the case of CEED. This effect is critical for the study of light-matter interaction and this work is, to our knowledge, the first one to report this problem. Besides, CEED reproduces the correct frequencies in agreement with quantum electrodynamics. This is a major asset of the semiclassical model, since the emission peak positions will be rightly predicted without any prior assumption about the nature of the molecular Hamiltonian. This is not so for the quantum electrodynamics approach, where access to the spectral information relies on the knowledge of the Hamiltonian eigenvalues.

show abstract

Radiative thermalization in semiclassical simulations of light-matter interaction

Cited by 7 publications

References 24 publications

Tailoring Cooperative Emission in Molecules: Superradiance and Subradiance from First-Principles Simulations

Tailoring Cooperative Emission in Molecules: Superradiance and Subradiance from First-Principles Simulations

Nonlinear Pauli Equation

Fluorescence in quantum dynamics: Accurate spectra require post-mean-field approaches

Contact Info

Product

Resources

About