arXiv subjects

Alex W. Chin

Publications and source records attributed to Alex W. Chin.

48 records · Page 3Linked to original sources

arXiv2014

Phonon-Assisted Ultrafast Charge Separation in a Realistic PCBM Aggregate

Organic solar cells must separate strongly bound electron-hole pairs into free charges. This is achieved at interfaces between electron donor and acceptor organic semiconductors. The most popular electron acceptor is the fullerene derivative PCBM. Electron-hole separation has been observed on femtosecond timescales, which is incompatible with conventional Marcus theories of organic transport. In this work we show that ultrafast charge transport in PCBM arises from its broad range of electronic eigenstates, provided by the presence of three closely spaced delocalised bands near the LUMO level. Vibrational fluctuations enable rapid transitions between these bands, which drives an electron transport of $\sim$3 nm within 100 fs. All this is demonstrated within a realistic tight binding Hamiltonian containing transfer integrals no larger than 8 meV.

cond-mat.mtrl-sci↗

arXiv2014

Stabilizing Spin Coherence Through Environmental Entanglement in Strongly Dissipative Quantum Systems

The key feature of a quantum spin coupled to a harmonic bath---a model dissipative quantum system---is competition between oscillator potential energy and spin tunneling rate. We show that these opposing tendencies cause environmental entanglement through superpositions of adiabatic and antiadiabatic oscillator states, which then stabilizes the spin coherence against strong dissipation. This insight motivates a fast-converging variational coherent-state expansion for the many-body ground state of the spin-boson model, which we substantiate via numerical quantum tomography.

quant-ph↗

arXiv2013

Time-frequency resolved ultrafast spectroscopy techniques using wavelet analysis

New experimental techniques based on non-linear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates, including both natural and artificial light harvesting complexes. Fourier transform-based spectroscopies have been particularly successful, yet 'complete' spectral information normally necessitates the loss of all information on the temporal sequence of events in a signal. This information though is particularly important in transient or multi-stage processes, in which the spectral decomposition of the data evolves in time. By going through several examples of ultrafast quantum dynamics, we demonstrate that the use of wavelets provide an efficient and accurate way to simultaneously acquire both temporal and frequency information about a signal, and argue that this greatly aids the elucidation and interpretation of physical process responsible for non-stationary spectroscopic features, such as those encountered in coherent excitonic energy transport.

quant-ph↗

arXiv2013

Quantum dynamics in photonic crystals

Employing a recently developed method that is numerically accurate within a model space simulating the real-time dynamics of few-body systems interacting with macroscopic environmental quantum fields, we analyze the full dynamics of an atomic system coupled to a continuum light-field with a gapped spectral density. This is a situation encountered, for example, in the radiation field in a photonic crystal, whose analysis has been so far been confined to limiting cases due to the lack of suitable numerical techniques. We show that both atomic population and coherence dynamics can drastically deviate from the results predicted when using the rotating wave approximation, particularly in the strong coupling regime. Experimental conditions required to observe these corrections are also discussed.

quant-ph↗

arXiv2012

Quantum Metrology in Non-Markovian Environments

We analyze precision bounds for a local phase estimation in the presence of general, non-Markovian phase noise. We demonstrate that the metrological equivalence of product and maximally entangled states that holds under strictly Markovian dephasing fails in the non-Markovian case. Using an exactly solvable model of a physically realistic finite bandwidth dephasing environment, we demonstrate that the ensuing non-Markovian dynamics enables quantum correlated states to outperform metrological strategies based on uncorrelated states using otherwise identical resources. We show that this conclusion is a direct result of the coherent dynamics of the global state of the system and environment and therefore the obtained scaling with the number of particles, which surpasses the standard quantum limit but does not achieve Heisenberg resolution, possesses general validity that goes beyond specific models. This is in marked contrast with the situation encountered under general Markovian noise, where an arbitrarily small amount of noise is enough to restore the scaling dictated by the standard quantum limit.

quant-ph↗

arXiv2012

Ground state and dynamics of the biased dissipative two-state system: Beyond variational polaron theory

We propose a ground-state ansatz for the Ohmic spin-boson model that improves upon the variational treatment of Silbey and Harris for biased systems in the scaling limit. In particular, it correctly captures the smooth crossover behaviour expected for the ground-state magnetisation when moving between the delocalised and localised regimes of the model, a feature that the variational treatment is unable to properly reproduce, while it also provides a lower ground-state energy estimate in the crossover region. We further demonstrate the validity of our intuitive ground-state by showing that it leads to predictions in excellent agreement with those derived from a non-perturbative Bethe-ansatz technique. Finally, recasting our ansatz in the form of a generalised polaron transformation, we are able to explore the dissipative two-state dynamics beyond weak system-environment coupling within an efficient time-local master equation formalism.

cond-mat.mes-hall↗

arXiv2012

The nature of the low energy band of the Fenna-Matthews-Olson complex: vibronic signatures

Based entirely upon actual experimental observations on electron-phonon coupling, we develop a theoretical framework to show that the lowest energy band of the Fenna- Matthews-Olson (FMO) complex exhibits observable features due to the quantum nature of the vibrational manifolds present in its chromophores. The study of linear spectra provides us with the basis to understand the dynamical features arising from the vibronic structure in non-linear spectra in a progressive fashion, starting from a microscopic model to finally performing an inhomogenous average. We show that the discreteness of the vibronic structure can be witnessed by probing the diagonal peaks of the non-linear spectra by means of a relative phase shift in the waiting time resolved signal. Moreover, we demonstrate the photon-echo and non-rephasing paths are sensitive to different harmonics in the vibrational manifold when static disorder is taken into account. Supported by analytical and numerical calculations, we show that nondiagonal resonances in the 2D spectra in the waiting time, further capture the discreteness of vibrations through a modulation of the amplitude without any effect in the signal intrinsic frequency. This fact generates a signal that is highly sensitive to correlations in the static disorder of the excitonic energy albeit protected against dephasing due to inhomogeneities of the vibrational ensemble.

q-bio.BM↗

arXiv2011

Chain representations of open quantum systems and their numerical simulation with time-adapative density matrix renormalisation group methods

This chapter gives a self-contained review of the how standard open quantum system Hamiltonians can be mapped analytically onto representations in which the environments appear as one dimensional harmonic chains with nearest neighbour interactions. This mapping, carried out rigorously using orthogonal polynomial theory, then allows the full evolution of the system and environment to be simulated using time-adaptive density matrix renormalisation group methods. With the combination of these two techniques, numerically-exact results can be obtained for dissipative quantum systems in the presence of arbitrarily complex environmental spectral functions, and the correlations and processes in the environment which drive the effectively irreversible dynamics of the reduced state of the quantum system can be explored in real time. The chain representation also reveals a number of universal features of harmonic environments characterised by a spectral density which are discussed here.

quant-ph↗

arXiv2010

Exact mapping between system-reservoir quantum models and semi-infinite discrete chains using orthogonal polynomials

By using the properties of orthogonal polynomials, we present an exact unitary transformation that maps the Hamiltonian of a quantum system coupled linearly to a continuum of bosonic or fermionic modes to a Hamiltonian that describes a one-dimensional chain with only nearest-neighbour interactions. This analytical transformation predicts a simple set of relations between the parameters of the chain and the recurrence coefficients of the orthogonal polynomials used in the transformation, and allows the chain parameters to be computed using numerically stable algorithms that have been developed to compute recurrence coefficients. We then prove some general properties of this chain system for a wide range of spectral functions, and give examples drawn from physical systems where exact analytic expressions for the chain properties can be obtained. Crucially, the short range interactions of the effective chain system permits these open quantum systems to be efficiently simulated by the density matrix renormalization group methods.

quant-ph↗

arXiv2010

Noise-assisted energy transfer in quantum networks and light-harvesting complexes

We provide physically intuitive mechanisms for the effect of noise on excitation energy transfer (EET) in networks. Using these mechanisms of dephasing-assisted transport (DAT) in a hybrid basis of both excitons and sites, we develop a detailed picture of how noise enables energy transfer with efficiencies well above $90%$ across the Fenna-Matthew-Olson (FMO) complex, a type of light harvesting molecule. We demonstrate explicitly how noise alters the pathways of energy transfer across the complex, suppressing ineffective pathways and facilitating direct ones to the reaction centre. We explain that the fundamental mechanisms underpinning DAT are expected to be robust with respect to the considered noise model but show that the specific details of the exciton-phonon coupling, which remain largely unknown in these type of complexes, and in particular the impact of non-Markovian effects, results in variations of dynamical features that should be amenable to experimental verification within current or planned technology. A detailed understanding of DAT in natural compounds should open up a new paradigm of `noise-engineering' by which EET can be optimized in artificial light-harvesting structures.

quant-ph↗

arXiv2010

Entanglement and entangling power of the dynamics in light-harvesting complexes

We study the evolution of quantum entanglement during exciton energy transfer (EET) in a network model of the Fenna-Matthews-Olson (FMO) complex, a biological pigment-protein complex involved in the early steps of photosynthesis in sulphur bacteria. The influence of Markovian, as well as spatially and temporally correlated (non-Markovian) noise on the generation of entanglement across distinct chromophores (site entanglement) and different excitonic eigenstates (mode entanglement) is studied for different injection mechanisms, including thermal and coherent laser excitation. Additionally, we study the entangling power of the FMO complex under natural operating conditions. While quantum information processing tends to favor maximal entanglement, near unit EET is achieved as the result of an intricate interplay between coherent and noisy processes where the initial part of the evolution displays intermediate values of both forms of entanglement.

quant-ph↗

arXiv2009

Highly efficient energy excitation transfer in light-harvesting complexes: The fundamental role of noise-assisted transport

Excitation transfer through interacting systems plays an important role in many areas of physics, chemistry, and biology. The uncontrollable interaction of the transmission network with a noisy environment is usually assumed to deteriorate its transport capacity, especially so when the system is fundamentally quantum mechanical. Here we identify key mechanisms through which noise such as dephasing, perhaps counter intuitively, may actually aid transport through a dissipative network by opening up additional pathways for excitation transfer. We show that these are processes that lead to the inhibition of destructive interference and exploitation of line broadening effects. We illustrate how these mechanisms operate on a fully connected network by developing a powerful analytical technique that identifies the invariant (excitation trapping) subspaces of a given Hamiltonian. Finally, we show how these principles can explain the remarkable efficiency and robustness of excitation energy transfer from the light-harvesting chlorosomes to the bacterial reaction center in photosynthetic complexes and present a numerical analysis of excitation transport across the Fenna-Matthew-Olson (FMO) complex together with a brief analysis of its entanglement properties. Our results show that, in general, it is the careful interplay of quantum mechanical features and the unavoidable environmental noise that will lead to an optimal system performance.

quant-ph↗