11,670 research outputs found
Spin-dependent electron-hole capture kinetics in conjugated polymers
The recombination of electron-hole pairs injected in extended conjugated
systems is modeled as a multi-pathway vibron-driven relaxation in monoexcited
state-space. The computed triplet-to-singlet ratio of exciton formation times
increases from 0.9 for a model dimer to 2.5 for a 32-unit
chain, in excellent agreement with experiments. Therewith we rationalize
recombination efficiency in terms of spin-dependent interstate vibronic
coupling and spin- and conjugation-length-dependent exciton binding
energies.Our model calculations for various length polymers indicate that the
ratio of the singlet to triplet formation ratios, , is
inversely related to the ratio of the singlet and triplet binding energies,
Correlated interaction fluctuations in photosynthetic complexes
The functioning and efficiency of natural photosynthetic complexes is
strongly influenced by their embedding in a noisy protein environment, which
can even serve to enhance the transport efficiency. Interactions with the
environment induce fluctuations of the transition energies of and interactions
between the chlorophyll molecules, and due to the fact that different
fluctuations will partially be caused by the same environmental factors,
correlations between the various fluctuations will occur. We argue that
fluctuations of the interactions should in general not be neglected, as these
have a considerable impact on population transfer rates, decoherence rates and
the efficiency of photosynthetic complexes. Furthermore, while correlations
between transition energy fluctuations have been studied, we provide the first
quantitative study of the effect of correlations between interaction
fluctuations and transition energy fluctuations, and of correlations between
the various interaction fluctuations. It is shown that these additional
correlations typically lead to changes in interchromophore transfer rates,
population oscillations and can lead to a limited enhancement of the light
harvesting efficiency
Electron Transfer in Donor-Acceptor Systems: Many-Particle Effects and Influence of Electronic Correlations
We investigate electron transfer processes in donor-acceptor systems with a
coupling of the electronic degrees of freedom to a common bosonic bath. The
model allows to study many-particle effects and the influence of the local
Coulomb interaction U between electrons on donor and acceptor sites. Using the
non-perturbative numerical renormalization group approach we find distinct
differences between the electron transfer characteristics in the single- and
two-particle subspaces. We calculate the critical electron-boson coupling
alpha_c as a function of and show results for density-density correlation
functions in the whole parameter space. The possibility of many-particle
(bipolaronic) and Coulomb-assisted transfer is discussed.Comment: 4 pages, 4 figure
Subband Engineering Even-Denominator Quantum Hall States
Proposed even-denominator fractional quantum Hall effect (FQHE) states
suggest the possibility of excitations with non-Abelian braid statistics.
Recent experiments on wide square quantum wells observe even-denominator FQHE
even under electrostatic tilt. We theoretically analyze these structures and
develop a procedure to accurately test proposed quantum Hall wavefunctions. We
find that tilted wells favor partial subband polarization to yield Abelian
even-denominator states. Our results show that tilting quantum wells
effectively engineers different interaction potentials allowing exploration of
a wide variety of even-denominator states
Chalk cliff retreat in East Sussex and Kent 1870s to 2001
The retreat of chalk cliffs fringing the eastern English Channel contributes shingle to the beaches which helps to protect the cliffs and slow down erosion. Conversely, cliff retreat endangers settlements and infrastructure on the clifftop. Rates of retreat have been calculated by a variety of methods over the past century, but no attempt has been made to provide a complete coverage that allows for a true comparison of retreat rates over the entire coastline. Using historic maps and recent orthophotos, cliff retreat rates have been calculated for consecutive 50 m sections of chalk cliff along the English side of the entire eastern English Channel for a period of 125 years. The chalk cliffs of East Sussex erode at an average rate of 0.25 - 0.3 m y−1 while those in Kent at a rate of 0.1 m y−1
Benchmarking calculations of excitonic couplings between bacteriochlorophylls
Excitonic couplings between (bacterio)chlorophyll molecules are necessary for
simulating energy transport in photosynthetic complexes. Many techniques for
calculating the couplings are in use, from the simple (but inaccurate)
point-dipole approximation to fully quantum-chemical methods. We compared
several approximations to determine their range of applicability, noting that
the propagation of experimental uncertainties poses a fundamental limit on the
achievable accuracy. In particular, the uncertainty in crystallographic
coordinates yields an uncertainty of about 20% in the calculated couplings.
Because quantum-chemical corrections are smaller than 20% in most biologically
relevant cases, their considerable computational cost is rarely justified. We
therefore recommend the electrostatic TrEsp method across the entire range of
molecular separations and orientations because its cost is minimal and it
generally agrees with quantum-chemical calculations to better than the
geometric uncertainty. We also caution against computationally optimizing a
crystal structure before calculating couplings, as it can lead to large,
uncontrollable errors. Understanding the unavoidable uncertainties can guard
against striving for unrealistic precision; at the same time, detailed
benchmarks can allow important qualitative questions--which do not depend on
the precise values of the simulation parameters--to be addressed with greater
confidence about the conclusions
Emergence of diversity in a model ecosystem
The biological requirements for an ecosystem to develop and maintain species
diversity are in general unknown. Here we consider a model ecosystem of sessile
and mutually excluding organisms competing for space [Mathiesen et al. Phys.
Rev. Lett. 107, 188101 (2011)]. The competition is controlled by an interaction
network with fixed links chosen by a Bernoulli process. New species are
introduced in the system at a predefined rate. In the limit of small
introduction rates, the system becomes bistable and can undergo a phase
transition from a state of low diversity to high diversity. We suggest that
patches of isolated meta-populations formed by the collapse of cyclic relations
are essential for the transition to the state of high diversity.Comment: 7 pages, 6 figures. Accepted for publication in PRE. Typos corrected,
Fig.3A and Fig.6 update
Exciton coherence lifetimes from electronic structure
We model the coherent energy transfer of an electronic excitation within
covalently linked aromatic homodimers from first-principles, to answer whether
the usual models of the bath calculated via detailed electronic structure
calculations can reproduce the key dynamics. For these systems the timescales
of coherent transport are experimentally known from time-dependent polarization
anisotropy measurements, and so we can directly assess the whether current
techniques might be predictive for this phenomenon. Two choices of electronic
basis states are investigated, and their relative merits discussed regarding
the predictions of the perturbative model. The coupling of the electronic
degrees of freedom to the nuclear degrees of freedom is calculated rather than
assumed, and the fluorescence anisotropy decay is directly reproduced.
Surprisingly we find that although TDDFT absolute energies are routinely in
error by orders of magnitude more than the coupling energy, the coherent
transport properties of these dimers can be semi-quantitatively reproduced from
first-principles. The directions which must be pursued to yield predictive and
reliable prediction of coherent transport are suggested.Comment: 22 pages, 7 figure
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