arXiv subjects

Tristan Farrow

Publications and source records attributed to Tristan Farrow.

12 recordsLinked to original sources

arXiv2023

Boosting Biomolecular Switch Efficiency With Quantum Coherence

The resource theory of quantum thermodynamics has emerged as a powerful tool for exploring the out-of-equilibrium dynamics of microscopic and highly correlated systems. Recently, it has been employed in photoisomerization, a mechanism facilitating vision through the isomerism of the photo receptor protein rhodopsin, to elucidate the fundamental limits of efficiency inherent in this physical process. Limited attention has been given to the impact of energetic quantum coherences in this process, as these coherences do not influence the energy level populations within an individual molecule subjected to thermal operations. However, a specific type of energetic quantum coherences can impact the energy level populations in the scenario involving two or more molecules. In this study, we examine the case of two molecules undergoing photoisomerization to show that energetic quantum coherence can function as a resource that amplifies the efficiency of photoisomerization. These insights offer evidence for the role of energetic quantum coherence as a key resource in the realm of quantum thermodynamics at mesoscopic scales.

quant-ph↗

arXiv2023

Ultranarrow linewidth room-temperature single-photon source from perovskite quantum dot embedded in optical microcavity

Ultranarrow bandwidth single-photon sources operating at room-temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud based quantum information processing networks, and quantum metrology. Here we show a room-temperature ultranarrow bandwidth single-photon source generating polarised photons at a rate of 5MHz based on an inorganic CsPbI3 perovskite quantum dot embedded in a tunable open-access optical microcavity. When coupled to an optical cavity mode, the quantum dot room-temperature emission becomes single-mode and the spectrum narrows down to just 1 nm. The low numerical aperture of the optical cavities enables efficient collection of high-purity single-mode single-photon emission at room-temperature, offering promising performance for photonic and quantum technology applications. We measure 94% pure single-photon emission into a single-mode under pulsed and continuous-wave (CW) excitation.

physics.optics↗

arXiv2022

A precision method for integrating shock sensors in the lining of sports helmets by additive manufacturing

An additive manufacturing method is presented for embedding optical fibre-based pressure sensors into the lining of sports helmets to monitor head impact in contact sports. Proof-of-concept thermoplastic polyurethane (TPU) helmet padding segments with embedded sensors are demonstrated for their sensitive shock-monitoring capabilities. The system offers a cost-effective solution for manufacturing consumer products at scale, is unobtrusive, and can be powered by medical-grade cell batteries requiring low maintenance.

physics.ins-det↗

arXiv2021

Resonantly pumped bright-triplet exciton lasing in caesium lead bromide perovskites

The surprising recent observation of highly emissive triplet-states in lead halide perovskites accounts for their orders-of-magnitude brighter optical signals and high quantum efficiencies compared to other semiconductors. This makes them attractive for future optoelectronic applications, especially in bright low-threshold nano-lasers. Whilst non-resonantly pumped lasing from all-inorganic lead-halide perovskites is now well-established as an attractive pathway to scalable low-power laser sources for nano-optoelectronics, here we showcase a resonant optical pumping scheme on a fast triplet-state in CsPbBr3 nanocrystals. The scheme allows us to realize a polarized triplet-laser source that dramatically enhances the coherent signal by one order of magnitude whilst suppressing non-coherent contributions. The result is a source with highly attractive technological characteristics including a bright and polarized signal, and a high stimulated-to-spontaneous emission signal contrast that can be filtered to enhance spectral purity. The emission is generated by pumping selectively on a weakly-confined excitonic state with a Bohr radius ~10 nm in the nanocrystals. The exciton fine-structure is revealed by the energy-splitting resulting from confinement in nanocrystals with tetragonal symmetry. We use a linear polarizer to resolve two-fold non-degenerate sub-levels in the triplet exciton and use photoluminescence excitation spectroscopy to determine the energy of the state before pumping it resonantly.

physics.optics↗

arXiv2019

Emergence of correlated proton tunneling in water ice

Several experimental and theoretical studies report instances of concerted or correlated multiple proton tunneling in solid phases of water. Here, we construct a pseudo-spin model for the quantum motion of protons in a hexameric H$_2$O ring and extend it to open system dynamics that takes environmental effects into account in the form of O$-$H stretch vibrations. We approach the problem of correlations in tunneling using quantum information theory in a departure from previous studies. Our formalism enables us to quantify the coherent proton mobility around the hexagonal ring by one of the principal measures of coherence, the $l_1$ norm of coherence. The nature of the pairwise pseudo-spin correlations underlying the overall mobility is further investigated within this formalism. We show that the classical correlations of the individual quantum tunneling events in long-time limit is sufficient to capture the behaviour of coherent proton mobility observed in low-temperature experiments. We conclude that long-range intra-ring interactions do not appear to be a necessary condition for correlated proton tunneling in water ice.

quant-ph↗

arXiv2018

Proton tunneling in hydrogen bonds and its implications in an induced-fit model of enzyme catalysis

The role of proton tunneling in biological catalysis is investigated here within the frameworks of quantum information theory and thermodynamics. We consider the quantum correlations generated through two hydrogen bonds between a substrate and a prototypical enzyme that first catalyzes the tautomerization of the substrate to move on to a subsequent catalysis, and discuss how the enzyme can derive its catalytic potency from these correlations. In particular, we show that classical changes induced in the binding site of the enzyme spreads the quantum correlations among all of the four hydrogen-bonded atoms thanks to the directionality of hydrogen bonds. If the enzyme rapidly returns to its initial state after the binding stage, the substrate ends in a new transition state corresponding to a quantum superposition. Open quantum system dynamics can then naturally drive the reaction in the forward direction from the major tautomeric form to the minor tautomeric form without needing any additional catalytic activity. We find that in this scenario the enzyme lowers the activation energy so much that there is no energy barrier left in the tautomerization, even if the quantum correlations quickly decay.

physics.chem-ph↗

arXiv2016

Organic molecule fluorescence as an experimental test-bed for quantum jumps in thermodynamics

We demonstrate with an experiment how molecules are a natural test-bed for probing fundamental quantum thermodynamics. Single-molecule spectroscopy has undergone transformative change in the past decade with the advent of techniques permitting individual molecules to be distinguished and probed. By considering the time-resolved emission spectrum of organic molecules as arising from quantum jumps between states, we demonstrate that the quantum Jarzynski equality is satisfied in this set-up. This relates the heat dissipated into the environment to the free energy difference between the initial and final state. We demonstrate also how utilizing the quantum Jarzynski equality allows for the detection of energy shifts within a molecule, beyond the relative shift.

quant-ph↗

arXiv2014

Scale-estimation of quantum coherent energy transport in multiple-minima systems

A generic and intuitive model for coherent energy transport in multiple minima systems coupled to a quantum mechanical bath is shown. Using a simple spin-boson system, we illustrate how a generic donor-acceptor system can be brought into resonance using a narrow band of vibrational modes, such that the transfer efficiency of an electron-hole pair (exciton) is made arbitrarily high. Coherent transport phenomena in nature are of renewed interest since the discovery that a photon captured by the light-harvesting complex (LHC) in photosynthetic organisms can be conveyed to a chemical reaction centre with near-perfect efficiency. Classical explanations of the transfer use stochastic diffusion to model the hopping motion of a photo-excited exciton. This accounts inadequately for the speed and efficiency of the energy transfer measured in a series of recent landmark experiments. Taking a quantum mechanical perspective can help capture the salient features of the efficient part of that transfer. To show the versatility of the model, we extend it to a multiple minima system comprising seven-sites, reminiscent of the widely studied Fenna-Matthews-Olson (FMO) light-harvesting complex. We show that an idealised transport model for multiple minima coupled to a narrow-band phonon can transport energy with arbitrarily high efficiency.

physics.bio-ph↗

arXiv2014

Classification of macroscopic quantum effects

We review canonical experiments on systems that have pushed the boundary between the quantum and classical worlds towards much larger scales, and discuss their unique features that enable quantum coherence to survive. Because the types of systems differ so widely, we use a case by case approach to identifying the different parameters and criteria that capture their behaviour in a quantum mechanical framework. We find it helpful to categorise systems into three broad classes defined by mass, spatio-temporal coherence, and number of particles. The classes are not mutually exclusive and in fact the properties of some systems fit into several classes. We discuss experiments by turn, starting with interference of massive objects like macromolecules and micro-mechanical resonators, followed by self-interference of single particles in complex molecules, before examining the striking advances made with superconducting qubits. Finally, we propose a theoretical basis for quantifying the macroscopic features of a system to lay the ground for a more systematic comparison of the quantum properties in disparate systems.

quant-ph↗

arXiv2014

Optimized entropic uncertainty relation for successive measurement

In the history of quantum mechanics, various types of uncertainty relationships have been introduced to accommodate different operational meanings of Heisenberg uncertainty principle. We derive an optimized entropic uncertainty relation (EUR) that quantifies an amount of quantum uncertainty in the scenario of successive measurements. The EUR characterizes the limitation in the measurability of two different quantities of a quantum state when they are measured through successive measurements. We find that the bound quantifies the information between the two measurements and imposes a condition that is consistent with the recently-derived error-disturbance relationship.

quant-ph↗

arXiv2011

Quantum coherent contributions in biological electron transfer

Many biological electron transfer (ET) reactions are mediated by metal centres in proteins. NADH:ubiquinone oxidoreductase (complex I) contains an intramolecular chain of seven iron-sulphur (FeS) clusters, one of the longest chains of metal centres in biology and a test case for physical models of intramolecular ET. In biology, intramolecular ET is commonly described as a diffusive hopping process, according to the semi-classical theories of Marcus and Hopfield. However, recent studies have raised the possibility that non-trivial quantum mechanical effects play a functioning role in certain biomolecular processes. Here, we extend the semi-classical model for biological ET to incorporate both semi-classical and coherent quantum phenomena using a quantum master equation based on the Holstein Hamiltonian. We test our model on the structurally-defined chain of FeS clusters in complex I. By exploring a wide range of realistic parameters we find that, when the energy profile for ET along the chain is relatively flat, just a small coherent contribution can provide a robust and significant increase in ET rate (above the semi-classical diffusive-hopping rate), even at physiologically-relevant temperatures. Conversely, when the on-site energies vary significantly along the chain the coherent contribution is negligible. For complex I, a crucial respiratory enzyme that is linked to many neuromuscular and degenerative diseases, our results suggest a new contribution towards ensuring that intramolecular ET does not limit the rate of catalysis. For the emerging field of quantum biology, our model is intended as a basis for elucidating the general role of coherent ET in biological ET reactions.

q-bio.BM↗

arXiv2010

Vibration-enhanced energy transfer in living molecules

The conversion of an absorbed photon from the exciton energy into the reaction centre in the photosynthetic complex has a near unit efficiency. It is becoming clear that any classical model, where the exciton hopping is modeled by a classical stochastic diffusion equation, cannot explain such a high degree of efficiency. A number of different quantum models have been proposed, ranging from a purely unitary model with long range exciton interactions to a noise-aided stochastic resonance models. Here we propose a very simple spin-boson model that captures all the features of the efficient part of energy transfer. We show how this model describes a scenario where a donor-acceptor system can be brought into resonance by a narrow band of vibrational modes so that the excitation transfer between the two can be made arbitrarily high. This is then extended to a seven exciton system such as the widely-studied FMO photosynthetic complex to show that a high efficiency is also achievable therein. Our model encodes a number of readily testable predictions and we discuss its generalisations to include the localisation in the reaction centre.

quant-ph↗