88 research outputs found
Sum-over-states vs quasiparticle pictures of coherent correlation spectroscopy of excitons in semiconductors; femtosecond analogues of multidimensional NMR
Two-dimensional correlation spectroscopy (2DCS) based on the nonlinear
optical response of excitons to sequences of ultrafast pulses, has the
potential to provide some unique insights into carrier dynamics in
semiconductors. The most prominent feature of 2DCS, cross peaks, can best be
understood using a sum-over-states picture involving the many-body eigenstates.
However, the optical response of semiconductors is usually calculated by
solving truncated equations of motion for dynamical variables, which result in
a quasiparticle picture. In this work we derive Green's function expressions
for the four wave mixing signals generated in various phase-matching directions
and use them to establish the connection between the two pictures. The formal
connection with Frenkel excitons (hard-core bosons) and vibrational excitons
(soft-core bosons) is pointed out.Comment: Accepted to Phys. Rev.
Partially-Time-Ordered Schwinger-Keldysh Loop Expansion of Coherent Nonlinear Optical Susceptibilities
A compact correlation-function expansion is developed for nth order optical
susceptibilities in the frequency domain using the Keldysh-Schwinger loop. By
not keeping track of the relative time ordering of bra and ket interactions at
the two branches of the loop, the resulting expressions contain only n+1 basic
terms, compared to the 2n terms required for a fully time-ordered density
matrix description. Superoperator Green's function expressions for the nth
order suscpeptibility derived using both expansions reflect different types of
interferences between pathways .These are demonstrated for correlation-induced
resonances in four wave mixing signals.Comment: article: 19 pages (preprint style!; including figures) ``paper.tex''
figures:
Excitation Dynamics and Relaxation in a Molecular Heterodimer
The exciton dynamics in a molecular heterodimer is studied as a function of
differences in excitation and reorganization energies, asymmetry in transition
dipole moments and excited state lifetimes. The heterodimer is composed of two
molecules modeled as two-level systems coupled by the resonance interaction.
The system-bath coupling is taken into account as a modulating factor of the
energy gap of the molecular excitation, while the relaxation to the ground
state is treated phenomenologically. Comparison of the description of the
excitation dynamics modeled using either the Redfield equations (secular and
full forms) or the Hierarchical quantum master equation (HQME) is demonstrated
and discussed. Possible role of the dimer as an excitation quenching center in
photosynthesis self-regulation is discussed. It is concluded that the
system-bath interaction rather than the excitonic effect determines the
excitation quenching ability of such a dimer
Probing Interband Coulomb Interactions in Semiconductor Nanocrystals with 2D Double-Quantum Coherence Spectroscopy
Using previously developed exciton scattering model accounting for the
interband, i.e., exciton-biexciton, Coulomb interactions in semiconductor
nanocrystals (NCs), we derive a closed set of equations for 2D double-quantum
coherence signal. The signal depends on the Liouville space pathways which
include both the interband scattering processes and the inter- and intraband
optical transitions. These processes correspond to the formation of different
cross-peaks in the 2D spectra. We further report on our numerical calculations
of the 2D signal using reduced level scheme parameterized for PbSe NCs. Two
different NC excitation regimes considered and unique spectroscopic features
associated with the interband Coulomb interactions are identified.Comment: 11 pages, 5 figure
Revisiting the optical properties of the FMO protein
We review the optical properties of the FMO complex as found by spectroscopic studies of the Qy band over the last two decades. This article emphasizes the different methods used, both experimental and theoretical, to elucidate the excitonic structure and dynamics of this pigment–protein complex
Origin of Long Lived Coherences in Light-Harvesting Complexes
A vibronic exciton model is developed to investigate the origin of long lived
coherences in light-harvesting complexes. Using experimentally determined
parameters and uncorrelated site energy fluctuations, the model predicts
oscillations in the nonlinear spectra of the Fenna-Matthews-Olson (FMO) complex
with a dephasing time of 1.3 ps at 77 K. These oscillations correspond to the
coherent superposition of vibronic exciton states with dominant contributions
from vibrational excitations on the same pigment. Purely electronic coherences
are found to decay on a 200 fs timescale.Comment: 4 pages, 2 figure
Monte Carlo Simulation of Exciton Bimolecular Annihilation Dynamics in Supramolecular Semiconductor Architectures †
Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes
Excitation transfer pathways in excitonic aggregates revealed by the stochastic Schrödinger equation
Chirality-Based Signatures of Local Protein Environments in Two-Dimensional Optical Spectroscopy of Two Species Photosynthetic Complexes of Green Sulfur Bacteria: Simulation Study
Two-dimensional electronic chirality-induced signals of excitons in the photosynthetic Fenna-Matthews-Olson complex from two species of green sulfur bacteria (Chlorobium tepidum and Prosthecochloris aestuarii) are compared. The spectra are predicted to provide sensitive probes of local protein environment of the constituent bacteriochlorophyll a chromophores and reflect electronic structure variations (site energies and couplings) of the two complexes. Pulse polarization configurations are designed that can separate the coherent and incoherent exciton dynamics contributions to the two-dimensional spectra
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