141 research outputs found
Many-body Green's function approach to attosecond nonlinear X-ray spectroscopy
Closed expressions are derived for resonant multidimensional X-ray
spectroscopy using the quasiparticle nonlinear exciton representation of
optical response. This formalism is applied to predict coherent four wave
mixing signals which probe single and two core-hole states. Nonlinear X-ray
signals are compactly expressed in terms of one- and two- particle Green's
functions which can be obtained from the solution of Hedin-like equations at
the level.Comment: 10 pages and 3 figures (To appear in Physical Review B
Effects of tunable excitation in carotenoids explained by the vibrational energy relaxation approach
V. B. acknowledges funding by the Leverhulme Trust Research Project Grant RPG-2015-337. J. H. and C. N. L. acknowledge funding by the Austrian Science Fund (FWF): START project Y 631-N27. D. A. acknowledges support by the Research Council of Lithuania (No MIP-090/2015). G. C. acknowledges support by the European Research Council Advanced Grant STRATUS (ERC-2011-AdG No. 291198). G. C. and J. H. acknowledge funding by Laserlab-Europe (EU-H2020 654148)
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 pigmentâprotein complex
Femtosecond Coherence and Quantum Control of Single Molecules at Room Temperature
Quantum mechanical phenomena, such as electronic coherence and entanglement,
play a key role in achieving the unrivalled efficiencies of light-energy
conversion in natural photosynthetic light-harvesting complexes, and triggered
the growing interest in the possibility of organic quantum computing. Since
biological systems are intrinsically heterogeneous, clear relations between
structural and quantum-mechanical properties can only be obtained by
investigating individual assemblies. However, single-molecule techniques to
access ultrafast coherences at physiological conditions were not available so
far. Here we show by employing femtosecond pulse-shaping techniques that
quantum coherences in single organic molecules can be created, probed, and
manipulated at ambient conditions even in highly disordered solid environments.
We find broadly distributed coherence decay times for different individual
molecules giving direct insight into the structural heterogeneity of the local
surroundings. Most importantly, we induce Rabi-oscillations and control the
coherent superposition state in a single molecule, thus performing a basic
femtosecond single-qubit operation at room temperature
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
Relaxation and dephasing in open quantum systems time-dependent density functional theory: Properties of exact functionals from an exactly-solvable model system
The dissipative dynamics of many-electron systems interacting with a thermal
environment has remained a long-standing challenge within time-dependent
density functional theory (TDDFT). Recently, the formal foundations of open
quantum systems time-dependent density functional theory (OQS-TDDFT) within the
master equation approach were established. It was proven that the exact
time-dependent density of a many-electron open quantum system evolving under a
master equation can be reproduced with a closed (unitarily evolving) and
non-interacting Kohn-Sham system. This potentially offers a great advantage
over previous approaches to OQS-TDDFT, since with suitable functionals one
could obtain the dissipative open-systems dynamics by simply propagating a set
of Kohn-Sham orbitals as in usual TDDFT. However, the properties and exact
conditions of such open-systems functionals are largely unknown. In the present
article, we examine a simple and exactly-solvable model open quantum system:
one electron in a harmonic well evolving under the Lindblad master equation. We
examine two different representitive limits of the Lindblad equation
(relaxation and pure dephasing) and are able to deduce a number of properties
of the exact OQS-TDDFT functional. Challenges associated with developing
approximate functionals for many-electron open quantum systems are also
discussed.Comment: 12 pages, 9 figure
- âŚ