The Unified Theory of Resonance Energy Transfer According to Molecular Quantum Electrodynamics

Salam, A.

doi:10.3390/atoms6040056

Cited by 37 publications

(40 citation statements)

References 76 publications

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“…For each case, four semiclassical treatments are considered: (i) Hamiltonian #I FCI; (ii) Hamiltonian #I CIS; (iii) Hamiltonian #II, and (iv) the hybrid Hamiltonian. To examine the performance of semiclassical approaches, we will compare them against either the time-dependent perturbative QED result [40,41] or the results of Lehmberg-Agarwal master equation (LAME) [42,43] -the standard quantum approach for describing the dynamics of two-level systems (TLSs) in quantum optics; see Appendix B for details. Note that all LAME results presented below are calculated with FCI.…”

Section: Resultsmentioning

confidence: 99%

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Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance

Chen

Nitzan

et al. 2019

Phys. Rev. A

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Semiclassical electrodynamics [with quantum matter plus classical electrodynamics fields] is an appealing approach for studying light-matter interactions, especially for realistic molecular systems. However, there is no unique semiclassical scheme. On the one hand, intermolecular interactions can be described instantaneously by static two-body interactions connecting two different molecules, while a classical transverse E-field acts as a spectator at short distance; we will call this Hamiltonian #I. On the other hand, intermolecular interactions can also be described as effects that are mediated exclusively through a classical one-body E-field without any quantum effects at all (assuming we ignore electronic exchange); we will call this Hamiltonian #II. Moreover, one can also mix these two different Hamiltonians into a third, hybrid Hamiltonian, which preserves quantum electron-electron correlations for lower excitations but describes higher excitations in a mean-field way. To investigate which semiclassical scheme is most reliable for practical use, here we study the real-time dynamics of a minimalistic many-site model -a pair of identical two-level systems (TLSs) -undergoing either resonance energy transfer (RET) or collectively driven dynamics. While both approaches perform reasonably well (#1 as #2) when there is no strong external excitation, we find that no single approach is perfect for all conditions (and all methods fail when a strong external field is applied). Each method has its own distinct problems: Hamiltonian #I performs best for RET but behaves in a complicated manner for driven dynamics. Hamiltonian #II is always stable, but obviously fails for RET at short distances. One key finding is that, for externally driven dynamics, a full configuration interaction description of Hamiltonian #I (#I-FCI) strongly overestimates the long-time electronic energy, highlighting the not obvious fact that, if one plans to merge quantum molecules with classical light, a full, exact treatment of electron-electron correlations can actually lead to worse results than a simple mean-field electronic structure treatment. Future work will need to investigate (i) how these algorithms behave in the context of more than a pair of TLSs and (ii) whether or not these algorithms can be improved in general by including crucial aspects of spontaneous emission. I. INTRODUCTIONRecent experiments demonstrating collective phenomena with nanoscale light-matter interactions[1-3] have highlighted the need for computational simulations of realistic molecular systems [4][5][6]. Unfortunately, full quantum electrodynamical (QED) calculations scale unfavorably with the number of quantized photonic modes. Moreover, full QED is compatible only with full configuration interactions (CI) for the description of the matter system, such that QED also scales unfavorably with the number of molecules. Thus, mixed quantum-classical electrodynamics are a promising approach with reduced computational cost: one treats electronic/molecular subsystems with ...

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Section: Resultsmentioning

confidence: 99%

“…According to the standard perturbative QED calculations [41,47], in the weak coupling limit, the RET rate between a pair of TLSs [donor (D) + acceptor (A)] can be calculated by Fermi's golden rule:…”

Section: Appendix C the Ret Ratementioning

confidence: 99%

Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance

Chen

Nitzan

et al. 2019

Phys. Rev. A

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“…The long-standing semiclassical treatment encapsulated in the well-known Förster theory is based on a nonretarded description of electromagnetic fields [141], which was shown to strictly fail to conform to the demands of causality [142,143]. By correctly describing the interaction between the transition moments of the donor and acceptor in terms of virtual photon propagation, it emerges from QED analysis that the short-and long-range mechanisms previously considered radiationless and radiative, respectively, are simply two asymptotic limits of a unified theory of energy transfer, fully accommodating both retardation and quantum uncertainty effects [123,124,[144][145][146][147][148]. Inter alia, the QED analysis also showed that the two supposedly different mechanisms can never compete in determining the distance-dependent dynamics of energy transfer.…”

Section: A Differences In Perspectivementioning

confidence: 99%

Quantum electrodynamics in modern optics and photonics: tutorial

et al. 2020

Self Cite

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One of the key frameworks for developing the theory of light-matter interactions in modern optics and photonics is quantum electrodynamics (QED). Contrasting with semiclassical theory, which depicts electromagnetic radiation as a classical wave, QED representations of quantized light fully embrace the concept of the photon. This tutorial review is a broad guide to cutting-edge applications of QED, providing an outline of its underlying foundation and an examination of its role in photon science. Alongside the full quantum methods, it is shown how significant distinctions can be drawn when compared to semiclassical approaches. Clear advantages in outcome arise in the predictive capacity and physical insights afforded by QED methods, which favors its adoption over other formulations of radiation-matter interaction.

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“…(24), leads to the matrix elements I|Ĥ AF |0 , II|Ĥ AF |I , III|Ĥ AF |II , and 0|Ĥ AF |III given, respectively, by Eqs. (24), (39), (26), and (27). Substitution of these matrix elements in Eq.…”

Section: Electric-chiral Paramagnetic-chiral and Chiral-chiral Intementioning

confidence: 99%

Medium-assisted van der Waals dispersion interactions involving chiral molecules

et al. 2020

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The van der Waals dispersion interaction between two chiral molecules in the presence of arbirary magnetoelectric media is derived using perturbation theory. To be general, the molecular polarisabilities are assumed to be of electric, paramagnetic and diamagnetic natures and the material environment is considered to possess a chiral electromagnetic response. The derived formulas of electric-chiral, paramagnetic-chiral, diamagnetic-chiral and chiral-chiral interaction potentials when added to the previously obtained contributions in literature, form a complete set of dispersion interaction formulas. We present them in a unified form making use of electric-magnetic duality. As an application, the case of two anisotropic molecules in free space is considered where we drive the retarded and non-retarded limits with respect to intermolecular distance.

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The Unified Theory of Resonance Energy Transfer According to Molecular Quantum Electrodynamics

Cited by 37 publications

References 76 publications

Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance

Understanding the nature of mean-field semiclassical light-matter dynamics: An investigation of energy transfer, electron-electron correlations, external driving, and long-time detailed balance

Quantum electrodynamics in modern optics and photonics: tutorial

Medium-assisted van der Waals dispersion interactions involving chiral molecules

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