arXiv subjects

Alexandra Olaya-Castro

Publications and source records attributed to Alexandra Olaya-Castro.

36 records · Page 2Linked to original sources

arXiv2017

Non-Perturbative Electron Counting Statistics

The theory of full counting statistics allows complete characterization of charge transport processes through nanoscale systems. The majority of existing theoretical treatments used to obtain the current cumulants rely on perturbative approximations with respect to either the system-bath coupling or the electronic tunnelling coupling within the system. This is not generally well suited to electron transfer through organic molecules where these couplings can be on the same order of magnitude. Here we present a non-perturbative approach that uses the formalism of the hierarchical equations of motion to describe the system-bath dynamics while retaining a weak coupling with respect to source and drain leads. The scope of this new framework is demonstrated by comparisons with a perturbative approach for a dimer system coupled to a thermal bath. The inadequacy of the perturbative approach to describe current fluctuations in a variety of regimes is shown.

cond-mat.mes-hall↗

arXiv2017

Isolating the chiral contribution in optical two-dimensional chiral spectroscopy using linearly polarized light

The full development of mono- or multi-dimensional time-resolved spectroscopy techniques incorporating optical activity signals has been strongly hampered by the challenge of identifying the small chiral signals over the large achiral background. Here we propose a new methodology to isolate chiral signals removing the achiral background from two commonly used configurations for performing two dimensional optical spectroscopy, known as BOXCARS and GRadient Assisted Photon Echo Spectroscopy (GRAPES). It is found that in both cases an achiral signal from an isotropic system can be completely eliminated by small manipulations of the relative angles between the linear polarizations of the four input laser pulses. Starting from the formulation of a perturbative expansion of the signal in the angle between the beams and the propagation axis, we derive analytic expressions that can be used to estimate how to change the polarization angles of the four pulses to minimize achiral contributions in the studied configurations. The generalization to any other possible experimental configurations has also been discussed. %We derive analytic expressions to changes required to the polarizations in terms of a perturbative expansion in the angle between the beams and the colinear axis. We also numerically estimate higher order coefficients which cover arbitrarily large angles and thus any experimental configuration.

physics.optics↗

arXiv2016

Coherence specific signal detection via chiral pump-probe spectroscopy

We examine transient circular dichroism spectroscopy (TRCD) as a technique to investigate signatures of exciton coherence dynamics under the influence of structured vibrational environments. We consider a pump-probe configuration with a linearly polarized pump and a circularly polarized probe, with a variable angle $θ$ between the two directions of propagation. In our theoretical formalism the signal is decomposed in chiral and achiral doorway and window functions. Using this formalism, we show that the chiral doorway component, which beats during the population time, can be isolated by comparing signals with different values of $θ$. As in the majority of time-resolved pump-probe spectroscopy, the overall TRCD response shows signatures of both excited and ground state dynamics. However, we demonstrate that the chiral doorway function has only a weak ground state contribution, which can generally be neglected if an impulsive pump pulse is used. These findings suggest that the pump-probe configuration of optical TRCD in the impulsive limit has the potential to unambiguously probe quantum coherence beating in the excited state. We present numerical results for theoretical signals in an example dimer system.

physics.chem-ph↗

arXiv2015

Work, heat and entropy production in bipartite quantum systems

In bipartite quantum systems commutation relations between the Hamiltonian of each subsystem and the interaction impose fundamental constraints on the dynamics of each partition. Here we investigate work, heat and entropy production in bipartite systems characterized by particular commutators between their local Hamiltonians and the interaction operator. We consider the formalism of [Weimer, EPL, 83:30008, 2008], in which heat (work) is identified with energy changes that (do not) alter the local von Neumann entropy, as observed in an effective local measurement basis. We demonstrate the consequences of the commutation relations on the work and heat fluxes into each partition, and extend the formalism to open quantum systems where one, or both, partitions are subject to a Markovian thermal bath. We also discuss the relation between heat and entropy in bipartite quantum systems out of thermal equilibrium, and reconcile the aforementioned approach with the second law of thermodynamics.

quant-ph↗

arXiv2014

Comment on "Excitons in Molecular Aggregates with Levy Disorder: Anomalous Localization and Exchange Broadening of Optical Spectra"

In their Letter [Phys. Rev. Lett. 105, 137402 (2010)], Eisfeld et al. predicted the exchange broadening and blue-shift of the absorption band as well as a nonuniversal disorder scaling of the localization length of excitons in J-aggregates with Levy disorder, which they contrasted with the previously analyzed Gaussian and Lorentzian case [Phys. Rev. B, 79, 1 (2009)]. The observations were explained by chain segmentation due to outliers, and its interplay with localization of states in effective potential wells created by typical random site energies. We argue that the previously known theory does not break down and thus anticipates the properties of absorption band investigated in the commented work.

cond-mat.dis-nn↗

arXiv2014

Non-classicality of the molecular vibrations assisting exciton energy transfer at room temperature

Advancing the debate on quantum effects in light-initiated reactions in biology requires clear identification of non-classical features that these processes can exhibit and utilise. Here we show that in prototype dimers present in a variety of photosynthetic antennae, efficient vibration-assisted energy transfer in the subpicosecond timescale and at room temperature can manifest and benefit from non-classical fluctuations of collective pigment motions. Non-classicality of initially thermalised vibrations is induced via coherent exciton-vibration interactions and is unambiguously indicated by negativities in the phase-space quasi-probability distribution of the effective collective mode coupled to the electronic dynamics. These quantum effects can be prompted upon incoherent input of excitation. Our results therefore suggest that investigation of the non-classical properties of vibrational motions assisting excitation and charge transport, photoreception and chemical sensing processes could be a touchstone for revealing a role for non-trivial quantum phenomena in biology.

quant-ph↗

arXiv2013

Dynamical transitions in Markovian exciton transport

The large deviation theory has recently been applied to open quantum systems to uncover dynamical crossovers in the space of quantum trajectories associated to Markovian evolutions. Such dynamical crossovers are characterized by qualitative changes in the fluctuations of rare quantum jump trajectories, and have been observed in the statistics of coherently driven quantum systems. In this article we investigate the counting statistics of rare quantum trajectories of an undriven system undergoing a pure relaxation process, namely, Markovian exciton transport. We find that dynamical crossovers occur in systems with a minimum of three interacting molecules, and are strongly activated by exciton delocalization and interference. Our results illustrate how quantum features of the underlying system Hamiltonian can influence the statistical properties of energy transfer processes in a non-trivial manner.

quant-ph↗

arXiv2012

The fundamental role of quantized vibrations in coherent light harvesting by cryptophyte algae

The influence of fast vibrations on energy transfer and conversion in natural molecular aggregates is an issue of central interest. This article shows the important role of high-energy quantized vibrations and their non-equilibrium dynamics for energy transfer in photosynthetic systems with highly localized excitonic states. We consider the cryptophyte antennae protein phycoerythrin 545 and show that coupling to quantized vibrations which are quasi-resonant with excitonic transitions is fundamental for biological function as it generates non-cascaded transport with rapid and wider spatial distribution of excitation energy. Our work also indicates that the non-equilibrium dynamics of such vibrations can manifest itself in ultrafast beating of both excitonic populations and coherences at room temperature, with time scales in agreement with those reported in experiments. Moreover, we show that mechanisms supporting coherent excitonic dynamics assist coupling to selected modes that channel energy to preferential sites in the complex. We therefore argue that, in the presence of strong coupling between electronic excitations and quantized vibrations, a concrete and important advantage of quantum coherent dynamics is precisely to tune resonances that promote fast and effective energy distribution.

physics.bio-ph↗

arXiv2011

Electronic excitation dynamics in multichromophoric systems described via a polaron-representation master equation

We derive a many-site version of the non-Markovian time-convolutionless polaron master equation [S. Jang et al., J. Chem Phys. 129, 101104 (2008)] to describe electronic excitation dynamics in multichromophoric systems. By treating electronic and vibrational degrees of freedom in a combined frame (polaron frame), this theory is capable of interpolating between weak and strong exciton-phonon coupling and is able to account for initial non-equilibrium bath states and spatially correlated environments. Besides outlining a general expression for the expected value of any electronic system observable in the original frame, we also discuss implications of the Markovian and secular approximations highlighting that they need not hold in the untransformed frame despite being strictly satisfied in the polaron frame. The key features of the theory are illustrated using as an example a four-site subsystem of the Fenna-Mathew-Olson light-harvesting complex. For a spectral density including a localised high-energy mode, we show that oscillations of site populations may only be observed when non-equilibrium bath effects are taken into account. Furthermore, we illustrate how this formalism allows us to identify the electronic or vibrational origin of the oscillatory dynamics.

quant-ph↗

arXiv2010

Quantum State Tuning of Energy Transfer in a Correlated Environment

We investigate multichromophoric energy transfer allowing for bath-induced fluctuations at different sites to be correlated. As a prototype system we consider a light-harvesting antenna surrounding a reaction center. We show that the interplay between quantum coherence and correlated fluctuations can generate a room temperature transfer process featuring a marked dependence on the degree of symmetry and delocalization of the initial exciton state. Our work illustrates how these quantum features could support fine tuning of energy transfer efficiencies in closely-packed natural and artificial light-harvesting complexes

quant-ph↗

arXiv2010

Distribution of entanglement in light-harvesting complexes and their quantum efficiency

Recent evidence of electronic coherence during energy transfer in photosynthetic antenna complexes has reinvigorated the discussion of whether coherence and/or entanglement has any practical functionality for these molecular systems. Here we investigate quantitative relationships between the quantum yield of a light-harvesting complex and the distribution of entanglement among its components. Our study focusses on the entanglement yield or average entanglement surviving a time scale comparable to the average excitation trapping time. As a prototype system we consider the Fenna-Matthews-Olson (FMO) protein of green sulphur bacteria and show that there is an inverse relationship between the quantum efficiency and the average entanglement between distant donor sites. Our results suggest that longlasting electronic coherence among distant donors might help modulation of the lightharvesting function.

quant-ph↗

arXiv2008

Efficiency of energy transfer in a light-harvesting system under quantum coherence

We investigate the role of quantum coherence in the efficiency of excitation transfer in a ring-hub arrangement of interacting two-level systems, mimicking a light-harvesting antenna connected to a reaction center as it is found in natural photosynthetic systems. By using a quantum jump approach, we demonstrate that in the presence of quantum coherent energy transfer and energetic disorder, the efficiency of excitation transfer from the antenna to the reaction center depends intimately on the quantum superposition properties of the initial state. In particular, we find that efficiency is sensitive to symmetric and asymmetric superposition of states in the basis of localized excitations, indicating that initial state properties can be used as a efficiency control parameter at low temperatures.

quant-ph↗

arXiv2006

Optical signatures of quantum phase transitions in a light-matter system

Information about quantum phase transitions in conventional condensed matter systems, must be sought by probing the matter system itself. By contrast, we show that mixed matter-light systems offer a distinct advantage in that the photon field carries clear signatures of the associated quantum critical phenomena. Having derived an accurate, size-consistent Hamiltonian for the photonic field in the well-known Dicke model, we predict striking behavior of the optical squeezing and photon statistics near the phase transition. The corresponding dynamics resemble those of a degenerate parametric amplifier. Our findings boost the motivation for exploring exotic quantum phase transition phenomena in atom-cavity, nanostructure-cavity, and nanostructure-photonic-band-gap systems.

quant-ph↗

arXiv2005

Renormalization scheme for a multi-qubit-network

We present a renormalization scheme which simplifies the dynamics of an important class of interacting multi-qubit systems. We show that a wide class of M+1 qubit systems can be reduced to an equivalent n+1 qubit system with n equal to, or greater than, 2, for any M. Our renormalization scheme faithfully reproduces the overall dynamics of the original system including the entanglement properties. In addition to its direct application to atom-cavity and nanostructure systems, the formalism offers insight into a variety of situations ranging from decoherence due to a spin-bath with its own internal entanglement, through to energy transfer processes in organic systems such as biological photosynthetic units.

quant-ph↗

arXiv2004

A robust one-step catalytic machine for high fidelity anti-cloning and W-state generation in a multi-qubit system

We propose a physically realizable machine which can either generate multiparticle W-like states, or implement high fidelity $1 \to M$ ($M=1,2,... \infty$) anti-cloning of an arbitrary qubit state, in a single step. Moreover this universal machine acts as a catalyst in that it is unchanged after either procedure, effectively resetting itself for its next operation. It also possesses an inherent {\em immunity} to decoherence. Most importantly in terms of practical multi-party quantum communication, the machine's robustness in the presence of decoherence actually {\em increases} as the number of qubits $M$ increases.

quant-ph↗

arXiv2004

Quantum Information Processing in Nanostructures

Semiconductor quantum dots integrated with ultrafast spectroscopy technology are prime candidates for building scalable architectures for Quantum Information Processing. In this review paper we survey the current state of theoretical proposals concerning all-optical control of nanostructure qubits and their interactions. These schemes offer potential for ultrafast optical manipulation of quantum information in time scales within the coherence time.

quant-ph↗

arXiv2004

Dynamics of quantum correlations and linear entropy in a multi-qubit-cavity system

We present a theoretical study of the relationship between entanglement and entropy in multi-qubit quantum optical systems. Specifically we investigate quantitative relations between the concurrence and linear entropy for a two-qubit mixed system, implemented as two two-level atoms interacting with a single-mode cavity field. The dynamical evolutions of the entanglement and entropy, are controlled via time-dependent cavity-atom couplings. Our theoretical findings lead us to propose an alternative measure of entanglement, which could be used to develop a much needed correlation measure for more general multi-partite quantum systems.

quant-ph↗

arXiv2003

Ultrafast deterministic generation of entanglement in a time-dependent asymmetric two-qubit-cavity system

We present an efficient scheme for the controlled generation of pure two-qubit states possessing {\em any} desired degree of entanglement and a {\em prescribed} symmetry in two cavity QED based systems, namely, cold trapped ions and flying atoms. This is achieved via on-resonance ion/atom-cavity couplings which are time-dependent and asymmetric, leading to a trapping vacuum state condition which does not arise for identical couplings. A duality in the role of the coupling ratio yields states with a given concurrence but opposing symmetries. The experimental feasibility of the proposed scheme is also discussed.

quant-ph↗