Davydov <i>Ansatz</i> as an efficient tool for the simulation of nonlinear optical response of molecular aggregates

Sun, Ke; Gelin, Maxim F.; Chernyak, Vladimir; Zhao, Yue

doi:10.1063/1.4921575

Cited by 38 publications

(72 citation statements)

References 70 publications

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“…While finite temperature was included in calculations of Refs. [63,42,43], that was done via a secondary bath, that was not treated on equal footing with the primary bath. The sTDVA, introduced in Ref.…”

Section: Discussionmentioning

confidence: 99%

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Benchmarking the stochastic time-dependent variational approach for excitation dynamics in molecular aggregates

et al. 2016

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Section: Discussionmentioning

confidence: 99%

“…In Refs. [46,39,63,42,43] it was assumed that the phonons couple to each site non-locally. Therefore, the site energy fluctuations were totally correlated, and no incoherent energy transfer was possible.…”

Section: Discussionmentioning

confidence: 99%

Benchmarking the stochastic time-dependent variational approach for excitation dynamics in molecular aggregates

et al. 2016

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“…The initial state of the system is assumed to be the electronic ground state |S 0 (|g ) with the relevant vibrational ground state |0 ph , i.e., |Ψ 0 = |S 0 |0 ph . The time-dependent wavefunction of the excited-state manifold reads 8,[52][53][54] Ψ e(f )…”

Section: Discussionmentioning

confidence: 99%

“…As a normal consideration in studying the 2D electronic spectrum, a model consisting of both the system and the harmonic bath is employed, whose Hamiltonian could be written as 8,39,41…”

Section: Methodsmentioning

confidence: 99%

Beating maps of singlet fission: Simulation of coherent two-dimensional electronic spectroscopy by Davydov ansatz in organic molecules

Sun

Yao

2017

The Journal of Chemical Physics

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The coherent two-dimensional (2D) electronic spectra for both the intra- and inter-molecular singlet fission (SF) processes in organic molecules are simulated by the Davydov ansatz combined with the Frenkel-Dirac time-dependent variational algorithm. By virtue of the dynamical approach, we are able to identify the signals of triplet excitation in the excited-state absorption contribution of the 2D spectra. In order to discuss whether a mediative charge-transfer (CT) state is necessary to SF, we increase the CT-state energy and find, in a theoretical manner, that the beating signal related to the triplet is inhibited. The vibronic coherence is then studied in the beating maps for both the ground and excited states. Except for the normal beating modes adhering to the relevant electronic state, we observe signals that are explicitly related to the triplet excitations. The pathways of transition corresponding to these signals are clarified in the respective Feynman diagram, which can help the experimenters determine the physical origin of relevant measurements.

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“…The details of the derivation are shown in Appendix B. Due to the high efficiency of the D 1 Ansatz method, we can easily perform the calculation of 2D spectra even in the presence of diagonal (off-diagonal) disorder [74,75]. A secondary, low-frequency thermal bath that accounts for solvent effects and protein motion is included by means of an overdamped brownian oscillator model [12,[76][77][78].…”

Section: E Spectroscopymentioning

confidence: 99%

Dynamics of coherence, localization and excitation transfer in disordered nanorings

Somoza

Sun

Molina

et al. 2017

Phys. Chem. Chem. Phys.

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Self-assembled supramolecular aggregates are excellent candidates for the design of efficient excitation transport devices. Both artificially prepared and natural photosynthetic aggregates in plants and bacteria present an important degree of disorder that is supposed to hinder excitation transport. Besides, molecular excitations couple to nuclear motion affecting excitation transport in a variety of ways. We present an exhaustive study of exciton dynamics in disordered nanorings with long-range interactions under the influence of a phonon bath and take the LH2 system of purple bacteria as a model. Nuclear motion is explicitly taken into account by employing the Davydov ansatz description of the polaron and quantum dynamics are obtained using a time-dependent variational method. We reveal an optimal exciton-phonon coupling that suppresses disorder-induced localization and facilitate excitation de-trapping. This excitation transfer enhancement, mediated by environmental phonons, is attributed to energy relaxation toward extended, low-energy excitons provided by the precise LH2 geometry with anti-parallel dipoles and long-range interactions. An analysis of localization and spectral statistics is followed by dynamical measures of coherence and localization, transfer efficiency and superradiance. Linear absorption, 2D photon-echo spectra and diffusion measures of the exciton are examined to monitor the diffusive behavior as a function of the strengths of disorder and exciton-phonon coupling.

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Davydov Ansatz as an efficient tool for the simulation of nonlinear optical response of molecular aggregates

Cited by 38 publications

References 70 publications

Benchmarking the stochastic time-dependent variational approach for excitation dynamics in molecular aggregates

Benchmarking the stochastic time-dependent variational approach for excitation dynamics in molecular aggregates

Beating maps of singlet fission: Simulation of coherent two-dimensional electronic spectroscopy by Davydov ansatz in organic molecules

Dynamics of coherence, localization and excitation transfer in disordered nanorings

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