63 research outputs found
Pseudomodes and the corresponding transformation of the temperature-dependent bath correlation function
In open system approaches with non-Markovian environments, the process of
inserting an individual mode (denoted as "pseudomode") into the bath or
extracting it from the bath is widely employed. This procedure, however, is
typically performed on basis of the spectral density (SD) and does not
incorporate temperature. Here, we show how the - temperature-dependent - bath
correlation function (BCF) transforms in such a process. We present analytic
formulae for the transformed BCF and numerically study the differences between
factorizing initial state and global thermal (correlated) initial state of mode
and bath, respectively. We find that in the regime of strong coupling of the
mode to both system and bath, the differences in the BCFs give rise to
pronounced differences in the dynamics of the system.Comment: 12 pages, 4 figure
Excitonic Wave Function Reconstruction from Near-Field Spectra Using Machine Learning Techniques
A general problem in quantum mechanics is the reconstruction of eigenstate
wave functions from measured data. In the case of molecular aggregates,
information about excitonic eigenstates is vitally important to understand
their optical and transport properties. Here we show that from spatially
resolved near field spectra it is possible to reconstruct the underlying
delocalized aggregate eigenfunctions. Although this high-dimensional nonlinear
problem defies standard numerical or analytical approaches, we have found that
it can be solved using a convolutional neural network. For both one-dimensional
and two-dimensional aggregates we find that the reconstruction is robust to
various types of disorder and noise
Probing weak dipole-dipole interaction using phase-modulated non-linear spectroscopy
Phase-modulated non-linear spectroscopy with higher harmonic demodulation has
recently been suggested to provide information on many-body excitations. In the
present work we theoretically investigate the application of this method to
infer the interaction strength between two particles that interact via weak
dipole-dipole interaction. To this end we use full numerical solution of the
Schr\"odinger equation with time-dependent pulses. For interpretation purpose
we also derive analytical expressions in perturbation theory. We find one can
detect dipole-dipole interaction via peak intensities (in contrast to
line-shifts which typically are used in conventional spectroscopy). We provide
a detailed study on the dependence of these intensities on the parameters of
the laser pulse and the dipole-dipole interaction strength. Interestingly, we
find that there is a phase between the first and second harmonic demodulated
signal, whose value depends on the sign of the dipole-dipole interaction.Comment: 12 pages, 8 figures, Supporting information provided with the source
file
Analytic Representations of Bath Correlation Functions for Ohmic and Superohmic Spectral Densities Using Simple Poles
We present a scheme to express a bath correlation function (BCF)
corresponding to a given spectral density (SD) as a sum of damped harmonic
oscillations. Such a representation is needed, for example, in many open
quantum system approaches. To this end we introduce a class of fit functions
that enables us to model ohmic as well as superohmic behavior. We show that
these functions allow for an analytic calculation of the BCF using pole
expansions of the temperature dependent hyperbolic cotangent. We demonstrate
how to use these functions to fit spectral densities exemplarily for cases
encountered in the description of photosynthetic light harvesting complexes.
Finally, we compare absorption spectra obtained for different fits with exact
spectra and show that it is crucial to take properly into account the behavior
at small frequencies when fitting a given SD.Comment: 16 pages, 9 figure
Vibronic Lineshapes of PTCDA Oligomers in Helium Nanodroplets
Oligomers of the organic semiconductor PTCDA are studied by means of helium
nanodroplet isolation (HENDI) spectroscopy. In contrast to the monomer
absorption spectrum, which exhibits clearly separated, very sharp absorption
lines, it is found that the oligomer spectrum consists of three main peaks
having an apparent width orders of magnitude larger than the width of the
monomer lines. Using a simple theoretical model for the oligomer, in which a
Frenkel exciton couples to internal vibrational modes of the monomers, these
experimental findings are nicely reproduced. The three peaks present in the
oligomer spectrum can already be obtained taking only one effective vibrational
mode of the PTCDA molecule into account. The inclusion of more vibrational
modes leads to quasi continuous spectra, resembling the broad oligomer spectra
Break-up of Rydberg superatoms via dipole-dipole interactions
We investigate resonant dipole-dipole interactions between two "superatoms"
of different angular momentum, consisting of two Rydberg-blockaded atom clouds
where each of them carries initially a coherently shared single excitation. We
demonstrate that the dipole-dipole interaction breaks up the superatoms by
removing the excitations from the clouds. The dynamics is akin to an ensemble
average over systems where only one atom per cloud participates in entangled
motion and excitation transfer. Our findings should thus facilitate the
experimental realization of adiabatic exciton transport in Rydberg systems by
replacing single sites with atom clouds.Comment: 10 pages, 5 figure
Non-Markovian Quantum State Diffusion for Temperature-Dependent Linear Spectra of Light Harvesting Aggregates
Non-Markovian Quantum State Diffusion (NMQSD) has turned out to be an
efficient method to calculate excitonic properties of aggregates composed of
organic chromophores, taking into account the coupling of electronic
transitions to vibrational modes of the chromophores. NMQSD is an open quantum
system approach that incorporates environmental degrees of freedom (the
vibrations in our case) in a stochastic way. We show in this paper that for
linear optical spectra (absorption, circular dichroism) no stochastics is
needed, even for finite temperatures. Thus, the spectra can be obtained by
propagating a single trajectory. To this end we map a finite temperature
environment to the zero temperature case using the so-called thermofield
method. The resulting equations can then be solved efficiently by standard
integrators.Comment: 14 pages, 4 figure
Spectral properties of molecular oligomers. A non-Markovian quantum state diffusion approach
Absorption spectra of small molecular aggregates (oligomers) are considered.
The dipole-dipole interaction between the monomers leads to shifts of the
oligomer spectra with respect to the monomer absorption. The line-shapes of
monomer as well as oligomer absorption depend strongly on the coupling to
vibrational modes. Using a recently developed approach [Roden et. al, PRL 103,
058301] we investigate the length dependence of spectra of one-dimensional
aggregates for various values of the interaction strength between the monomers.
It is demonstrated, that the present approach is well suited to describe the
occurrence of the J- and H-bands
Nanoelectromechanical rotary current rectifier
Nanoelectromechanical systems (NEMS) are devices integrating electrical and
mechanical functionality on the nanoscale. Because of individual electron
tunneling, such systems can show rich self-induced, highly non-linear dynamics.
We show theoretically that rotor shuttles, fundamental NEMS without intrinsic
frequencies, are able to rectify an oscillatory bias voltage over a wide range
of external parameters in a highly controlled manner, even if subject to the
stochastic nature of electron tunneling and thermal noise. Supplemented by a
simple analytic model, we identify different operational modes of charge
rectification. Intriguingly, the direction of the current depends sensitively
on the external parameters
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