Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives

Abramavičius, Darius; Palmieri, Benoit; Voronine, Dmitri V.; Šanda, František; Mukamel, Shaul

doi:10.1021/cr800268n

Cited by 485 publications

(867 citation statements)

References 354 publications

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“…Thus the NZ 2 will lead to a contribution to the tensor R (eeee) τ in Eq. (39). However, the parametric projection operator technique allows us to keep the convolution form of the equation if it is desired.…”

Section: B Parametric Master Equationmentioning

confidence: 99%

Parametric projection operator technique for second order non-linear response

Olšina¹,

Mančal²

2012

Chemical Physics

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We demonstrate the application of the recently introduced parametric projector operator technique to a calculation of the second order non-linear optical response of a multilevel molecular system. We derive a parametric quantum master equation (QME) for the time evolution of the excited state of an excitonic system after excitation by the first two pulses in the usual spectroscopic four-wave-mixing scheme. This master equation differs from the usual QME by a correction term which depends on the delay τ between the pulses. In the presence of environmental degrees of freedom with finite bath correlation time and in the presence of intramolecular vibrations we find distinct dynamics of both the excite state populations and the electronic coherence for different delays τ .

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Section: B Parametric Master Equationmentioning

confidence: 99%

Parametric projection operator technique for second order non-linear response

Olšina¹,

Mančal²

2012

Chemical Physics

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“…The environment (heat bath) is described by the infinite number of uncoupled harmonic oscillators, which are linearly coupled to the system and induce the fluctuations of the chromophore energies. These fluctuations are completely characterized by the correlation function [9]. For the energy of the i-th chromophore we have the correlation function…”

Section: Modelmentioning

confidence: 99%

“…Characteristics of the system are obtained by calculating the chromophore populations and the system entropy. We also compare the results calculated using the Debye (or the over damped Brownian oscillator) spectral density [9] and the one obtained from FMO molecular dynamics simulations [10].…”

Section: Introductionmentioning

confidence: 99%

Nonclassical energy transfer in photosynthetic FMO complex

Abramavicius

Abramavičius

2013

EPJ Web of Conferences

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Abstract. Excitation energy transfer in a photosynthetic FMO complex has been simulated using the stochastic Schrödinger equation. Fluctuating chromophore transition energies are simulated from the quantum correlation function which allows to properly include the finite temperature. The resulting excitation dynamics shows fast thermalization of chromophore occupations into proper thermal equilibrium. The relaxation process is characterized by entropy dynamics, which shows nonclassical behavior.

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“…In general the polarisation, created by three pulses applied to the quantum dots, is described by many quantum pathways in Liouville space 8 . In the following way, we can extract a subset of the Liouville pathways by extracting a a) b)…”

Section: B Phase Cycling Detection Of Coherent Signalsmentioning

confidence: 99%

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

et al. 2012

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We show how coherent, spatially resolved spectroscopy can disentangle complex hybrid wave functions into wave functions of the individual emitters. This way, detailed information on the coupling of the individual emitters, not available in far-field spectroscopy, can be revealed. Here we propose a quantum state tomography protocol that relies on the ability to selectively excite each emitter individually by spatially localized pulses. Simulations of coupled semiconductor GaAs/InAs quantum dots using light fields available in current nanoplasmonics show, that undesired resonances can be removed from measured spectra. The method can be applied on a broad range of coupled emitters to study the internal coupling, including pigments in photosynthesis and artificial light harvesting.

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Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives

Cited by 485 publications

References 354 publications

Parametric projection operator technique for second order non-linear response

Parametric projection operator technique for second order non-linear response

Nonclassical energy transfer in photosynthetic FMO complex

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

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