Efficient long-distance energy transport in molecular systems through adiabatic passage

Dijkstra, Arend G.; Beige, Almut

doi:10.1063/1.5100210

Cited by 12 publications

(6 citation statements)

References 38 publications

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“…The excitation with an arbitrary time-dependent (classical) electric field E(t) can be incorporated into HEOM formalism by augmenting Hamiltonian H M by the purely electronic and time-dependent Hamiltonian H M−R (t) [38,39]. Indeed, all the steps in the derivation conducted in Ref.…”

Section: Equations Of Motion: Semiclassical Treatment Of Light-matter...mentioning

confidence: 99%

“…( 38) is partucularly useful. Equation (38) suggests that Eq. ( 67) is reduced to the Förster limit by enforcing the global chronological order in the hyperoperator product acting on |D D|, i.e.,…”

Section: Nonequilibrium Generalization Of Förster Theorymentioning

confidence: 99%

“…While the explicit inclusion of light-matter coupling is typically accompanied by a perturbative treatment of excitation-environment coupling, there are also studies concentrating on a (numerically) exact treatment of the latter, at the expense of a less transparent inclusion of the former [36][37][38]. When the semiclassical description of light-matter interaction is appropriate, the timedependent electric field can be straightforwardly incorporated in the HEOM formalism [38,39], whose relation to the spectroscopic picture of sequential interactions with light is not manifest. When the quantum description of light-matter interaction is in place [36,37], the interaction with the radiation is treated from the standpoint of quantum optics, using the so-called hybrid masterequation-HEOM approach [40].…”

Section: Introductionmentioning

confidence: 99%

“…Section II introduces the Frenkel exciton model of a molecular light-harvesting aggregate, while the theory of nonlinear spectroscopy is employed in Sec. III to shed new light on the existing approaches [38,39] to include semiclassical light-matter coupling into HEOM formalism. Section IV presents the central result of our analysis.…”

Section: Introductionmentioning

confidence: 99%

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Exact description of excitonic dynamics in molecular aggregates weakly driven by light

Janković,

Mančal

2020

Preprint

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We present a rigorous theoretical description of excitonic dynamics in molecular light-harvesting aggregates photoexcited by weak-intensity radiation of arbitrary properties. While the interaction with light is included up to the second order, the treatment of the excitation-environment coupling is exact and results in an exact expression for the reduced excitonic density matrix that is manifestly related to the spectroscopic picture of the photoexcitation process. This expression takes fully into account the environmental reorganization processes triggered by the two interactions with light. This is particularly important for slow environments and/or strong excitation-environment coupling. Within the exponential decomposition scheme, we demonstrate how our result can be recast as the hierarchy of equations of motion (HEOM) that explicitly and consistently includes the photoexcitation step. We analytically describe the environmental reorganization dynamics triggered by a delta-like excitation of a single chromophore, and demonstrate how our HEOM, in appropriate limits, reduces to the Redfield equations comprising a pulsed photoexcitation and the nonequilibrium Förster theory. We also discuss the relation of our formalism to the combined Born-Markov-HEOM approaches in the case of excitation by thermal light.I.

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Section: Equations Of Motion: Semiclassical Treatment Of Light-matter...mentioning

confidence: 99%

Section: Nonequilibrium Generalization Of Förster Theorymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Exact description of excitonic dynamics in molecular aggregates weakly driven by light

Janković,

Mančal

2020

Preprint

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“…Different initializations of the electronic subsystem have been recently compared for a model trimer presenting the so-called Λ scheme between a donor and an acceptor via a bridge 40 . This Λ arrangement should allow a transfer by an adiabatic passage inspired by the STIRAP strategy 41 .…”

Section: Introductionmentioning

confidence: 99%

Funneling dynamics in a phenylacetylene trimer: Coherent excitation of donor excitonic states and their superposition

Breuil

Mangaud

Lasorne

et al. 2021

The Journal of Chemical Physics

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Funneling dynamics in conjugated dendrimers has raised great interest in the context of artificial light-harvesting processes. Photoinduced relaxation has been explored by time-resolved spectroscopy and simulations, mainly by semiclassical approaches or referring to open quantum systems methods, within the Redfield approximation. Here, we take the benefit of an ab initio investigation of a phenylacetylene trimer, and in the spirit of a divide-and-conquer approach, we focus on the early dynamics of the hierarchy of interactions. We build a simplified but realistic model by retaining only bright electronic states and selecting the vibrational domain expected to play the dominant role for timescales shorter than 500 fs. We specifically analyze the role of the in-plane high-frequency skeletal vibrational modes involving the triple bonds. Open quantum system non-adiabatic dynamics involving conical intersections is conducted by separating the electronic subsystem from the high-frequency tuning and coupling vibrational baths. This partition is implemented within a robust non-perturbative and non-Markovian method, here the hierarchical equations of motion. We will more precisely analyze the coherent preparation of donor states or of their superposition by short laser pulses with different polarizations. In particular, we extend the π-pulse strategy for the creation of a superposition to a V-type system. We study the relaxation induced by the high-frequency vibrational collective modes and the transitory dissymmetry, which results from the creation of a superposition of electronic donor states.

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Quantum Information and Algorithms for Correlated Quantum Matter

et al. 2020

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Efficient long-distance energy transport in molecular systems through adiabatic passage

Cited by 12 publications

References 38 publications

Exact description of excitonic dynamics in molecular aggregates weakly driven by light

Exact description of excitonic dynamics in molecular aggregates weakly driven by light

Funneling dynamics in a phenylacetylene trimer: Coherent excitation of donor excitonic states and their superposition

Quantum Information and Algorithms for Correlated Quantum Matter

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