542 research outputs found
Tuning nonradiative lifetimes via molecular aggregation
We show that molecular aggregation can strongly influence the nonradiative
decay (NRD) lifetime of an electronic excitation. As a demonstrative example,
we consider a transition-dipole-dipole-interacting dimer whose monomers have
harmonic potential energy surfaces (PESs). Depending on the position of the NRD
channel (), we find that the NRD lifetime () can exhibit a completely different dependence on the
intermolecular-interaction strength. We observe that (i) for near
the Franck-Condon region, increases with the
interaction strength; (ii) for near the minimum of the monomer
excited PES, the intermolecular interaction has little influence on ; (iii) for near the classical turning point of the
monomer nuclear dynamics, on the other side of the minimum, decreases with the interaction strength. Our findings suggest design
principles for molecular systems where a specific fluorescence quantum yield is
desired
Anomalous strong exchange narrowing in excitonic systems
We investigate theoretically the phenomenon of exchange narrowing in the
absorption spectrum of a chain of monomers, which are coupled via resonant
dipole-dipole interaction. The individual (uncoupled) monomers exhibit a broad
absorption line shape due to the coupling to an environment consisting of a
continuum of vibrational modes. Upon increasing the interaction between the
monomers, the absorption spectrum of the chain narrows. For a non-Markovian
environment with a Lorentzian spectral density, we find a narrowing of the peak
width (full width at half maximum (FWHM)) by a factor 1/N, where N is the
number of monomers. This is much stronger than the usual 1/sqrt{N} narrowing.
Furthermore it turns out that for a Markovian environment no exchange narrowing
at all occurs. The relation of different measures of the width (FWHM, standard
deviation) is discussed
The J- and H-bands of dye aggregate spectra: Analysis of the coherent exciton scattering (CES) approximation
The validity of the CES approximation is investigated by comparison with
direct diagonalisation of a model vibronic Hamiltonian of identical
monomers interacting electronically. Even for quite short aggregates (N\gtrsim
6) the CES approximation is shown to give results in agreement with direct
diagonalisation, for all coupling strengths, except that of intermediate
positive coupling (the H-band region). However, previously excellent agreement
of CES calculations and measured spectra in the H-band region was obtained [A.
Eisfeld, J. S. Briggs, Chem. Phys. 324, 376]. This is shown to arise from use
of the measured monomer spectrum which includes implicitly dissipative effects
not present in the model calculation
Quantum Dynamics Simulation with Classical Oscillators
In a previous paper [J.S.Briggs and A.Eisfeld, Phys.Rev.A 85, 052111] we
showed that the time-development of the complex amplitudes of N coupled quantum
states can be mapped by the time development of positions and velocities of N
coupled classical oscillators. Here we examine to what extent this mapping can
be realised to simulate the "quantum" properties of entanglement and qubit
manipulation. By working through specific examples, e.g. of quantum gate
operation, we seek to illuminate quantum/classical differences which hitherto
have been treated more mathematically. In addition we show that important
quantum coupled phenomena, such as the Landau-Zener transition and the
occurrence of Fano resonances can be simulated by classical oscillators
On the Equivalence of Quantum and Classical Coherence in Electronic Energy Transfer
To investigate the effect of quantum coherence on electronic energy transfer,
which is the subject of current interest in photosynthesis, we solve the
problem of transport for the simplest model of an aggregate of monomers
interacting through dipole-dipole forces using both quantum and classical
dynamics. We conclude that for realistic coupling strengths quantum and
classical coherent transport are identical. This is demonstrated by numerical
calculations for a linear chain and for the photosynthetic Fenna-Matthews-Olson
(FMO) comple
Gaussian processes for choosing laser parameters for driven, dissipative Rydberg aggregates
To facilitate quantum simulation of open quantum systems at finite
temperatures, an important ingredient is to achieve thermalization on a given
time-scale. We consider a Rydberg aggregate (an arrangement of Rydberg atoms
that interact via long-range interactions) embedded in a laser-driven atomic
environment. For the smallest aggregate (two atoms), suitable laser parameters
can be found by brute force scanning of the four tunable laser parameters. For
more atoms, however, such parameter scans are too computationally costly. Here
we apply Gaussian processes to predict the thermalization performance as a
function of the laser parameters for two-atom and four-atom aggregates. These
predictions perform remarkably well using just 1000 simulations, demonstrating
the utility of Gaussian processes in an atomic physics setting. Using this
approach, we find and present effective laser parameters for generating
thermalization, the robustness of these parameters to variation, as well as
different thermalization dynamics
Hierarchy of stochastic pure states for open quantum system dynamics
We derive a hierarchy of stochastic evolution equations for pure states
(quantum trajectories) to efficiently solve open quantum system dynamics with
non-Markovian structured environments. From this hierarchy of pure states
(HOPS) the exact reduced density operator is obtained as an ensemble average.
We demonstrate the power of HOPS by applying it to the Spin-Boson model, the
calculation of absorption spectra of molecular aggregates and energy transfer
in a photosynthetic pigment-protein complex
Excitons in Molecular Aggregates with L\'evy Disorder: Anomalous Localization and Exchange Broadening of Optical Spectra
We predict the existence of exchange broadening of optical lineshapes in
disordered molecular aggregates and a nonuniversal disorder scaling of the
localization characteristics of the collective electronic excitations
(excitons). These phenomena occur for heavy-tailed L\'evy disorder
distributions with divergent second moments - distributions that play a role in
many branches of physics. Our results sharply contrast with aggregate models
commonly analyzed, where the second moment is finite. They bear a relevance for
other types of collective excitations as well
Conical intersections in an ultracold gas
We find that energy surfaces of more than two atoms or molecules interacting
via dipole-dipole po- tentials generically possess conical intersections (CIs).
Typically only few atoms participate strongly in such an intersection. For the
fundamental case, a circular trimer, we show how the CI affects adiabatic
excitation transport via electronic decoherence or geometric phase
interference. These phe- nomena may be experimentally accessible if the trimer
is realized by light alkali atoms in a ring trap, whose dipole-dipole
interactions are induced by off-resonant dressing with Rydberg states. Such a
setup promises a direct probe of the full many-body density dynamics near a
conical intersection.Comment: 4 pages, 4 figures, replacement to add archive referenc
Non-Markovian Dynamics in Ultracold Rydberg Aggregates
We propose a setup of an open quantum system in which the environment can be
tuned such that either Markovian or non-Markovian system dynamics can be
achieved. The implementation uses ultracold Rydberg atoms, relying on their
strong long-range interactions. Our suggestion extends the features available
for quantum simulators of molecular systems employing Rydberg aggregates and
presents a new test bench for fundamental studies of the classification of
system-environment interactions and the resulting system dynamics in open
quantum systems.Comment: 13 pages, 4 figure
- …