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G. Andrew D. Briggs

Publications and source records attributed to G. Andrew D. Briggs.

At least 19 recordsLinked to original sources

Experimental Nanoscale Thermodynamics

Modern fabrication techniques have allowed artificial systems to be constructed on a nanometre length scale. The ideas underlying thermodynamics, a field invented to describe large macroscopic systems, need to be modified to describe much smaller systems. There are implications for our understanding of entropy, cooling, the arrow of time, heat flow, engines, erasure, and mutual information. The theoretical concepts have been implemented and tested in a wide range of experiments, many of which are at low temperatures. Nanoscale thermodynamics is not only a descriptive tool of nanoscale systems, but a design principle that helps us to build new architectures, processors and learning machines.

quant-ph↗

Quantum computing and artificial intelligence: status and perspectives

This white paper discusses and explores the various points of intersection between quantum computing and artificial intelligence (AI). It describes how quantum computing could support the development of innovative AI solutions. It also examines use cases of classical AI that can empower research and development in quantum technologies, with a focus on quantum computing and quantum sensing. The purpose of this white paper is to provide a long-term research agenda aimed at addressing foundational questions about how AI and quantum computing interact and benefit one another. It concludes with a set of recommendations and challenges, including how to orchestrate the proposed theoretical work, align quantum AI developments with quantum hardware roadmaps, estimate both classical and quantum resources - especially with the goal of mitigating and optimizing energy consumption - advance this emerging hybrid software engineering discipline, and enhance European industrial competitiveness while considering societal implications.

quant-ph↗

Identifying Pauli spin blockade using deep learning

Pauli spin blockade (PSB) can be employed as a great resource for spin qubit initialisation and readout even at elevated temperatures but it can be difficult to identify. We present a machine learning algorithm capable of automatically identifying PSB using charge transport measurements. The scarcity of PSB data is circumvented by training the algorithm with simulated data and by using cross-device validation. We demonstrate our approach on a silicon field-effect transistor device and report an accuracy of 96% on different test devices, giving evidence that the approach is robust to device variability. The approach is expected to be employable across all types of quantum dot devices.

cond-mat.mes-hall↗

Quantum Interference Enhances the Performance of Single-Molecule Transistors

An unresolved challenge facing electronics at a few-nm scale is that resistive channels start leaking due to quantum tunneling. This affects the performance of nanoscale transistors, with single-molecule devices displaying particularly low switching ratios and operating frequencies, combined with large subthreshold swings.1 The usual strategy to mitigate quantum effects has been to increase device complexity, but theory shows that if quantum effects are exploited correctly, they can simultaneously lower energy consumption and boost device performance.2-6 Here, we demonstrate experimentally how the performance of molecular transistors can be improved when the resistive channel contains two destructively-interfering waves. We use a zinc-porphyrin coupled to graphene electrodes in a three-terminal transistor device to demonstrate a >104 conductance-switching ratio, a subthreshold swing at the thermionic limit, a > 7 kHz operating frequency, and stability over >105 cycles. This performance is competitive with the best nanoelectronic transistors. We fully map the antiresonance interference features in conductance, reproduce the behaviour by density functional theory calculations, and trace back this high performance to the coupling between molecular orbitals and graphene edge states. These results demonstrate how the quantum nature of electron transmission at the nanoscale can enhance, rather than degrade, device performance, and highlight directions for future development of miniaturised electronics.

physics.chem-ph↗

Phase-Coherent Charge Transport through a Porphyrin Nanoribbon

Quantum interference in nano-electronic devices could lead to reduced-energy computing and efficient thermoelectric energy harvesting. When devices are shrunk down to the molecular level it is still unclear to what extent electron transmission is phase coherent, as molecules usually act as scattering centres, without the possibility of showing particle-wave duality. Here we show electron transmission remains phase coherent in molecular porphyrin nanoribbons, synthesized with perfectly defined geometry, connected to graphene electrodes. The device acts as a graphene Fabry-Pérot interferometer, allowing direct probing of the transport mechanisms throughout several regimes, including the Kondo one. Electrostatic gating allows measurement of the molecular conductance in multiple molecular oxidation states, demonstrating a thousand-fold increase of the current by interference, and unravelling molecular and graphene transport pathways. These results demonstrate a platform for the use of interferometric effects in single-molecule junctions, opening up new avenues for studying quantum coherence in molecular electronic and spintronic devices.

cond-mat.mes-hall↗

Charge-state dependent vibrational relaxation in a single-molecule junction

The interplay between nuclear and electronic degrees of freedom strongly influences molecular charge transport. Herein, we report on transport through a porphyrin dimer molecule, weakly coupled to graphene electrodes, that displays sequential tunneling within the Coulomb-blockade regime. The sequential transport is initiated by current-induced phonon absorption and proceeds by rapid sequential transport via a non-equilibrium vibrational distribution. We demonstrate this is possible only when the vibrational dissipation is slow relative to sequential tunneling rates, and obtain a lower bound for the vibrational relaxation time of 8 ns, a value that is dependent on the molecular charge state.

cond-mat.mes-hall↗

Single-electron transport in a molecular Hubbard dimer

Many-body electron interactions are at the heart of chemistry and solid-state physics. Understanding these interactions is crucial for the development of molecular-scale quantum and nanoelectronic devices. Here, we investigate single-electron tunneling through an edge-fused porphyrin oligomer and demonstrate that its transport behavior is well described by the Hubbard dimer model. This allows us to study the role of electron-electron interactions in the transport setting. In particular, we empirically determine the molecule's on-site and inter-site electron-electron repulsion energies, which are in good agreement with density functional calculations, and establish the molecular electronic structure within various charge states. The gate-dependent rectification behavior is used to further confirm the selection rules and state degeneracies resulting from the Hubbard model. We therefore demonstrate that current flow through the molecule is governed by a non-trivial set of vibrationally coupled electronic transitions between various many-body states, and experimentally confirm the importance of electron-electron interactions in single-molecule devices.

cond-mat.mes-hall↗

Understanding resonant charge transport through weakly coupled single-molecule junctions

Off-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and it is now well understood within the framework of the non-interacting Landauer approach. Conversely, gaining a qualitative and quantitative understanding of the resonant transport regime has proven more elusive. Here, we study resonant charge transport through graphene-based zinc-porphyrin junctions. We experimentally demonstrate an inadequacy of the non-interacting Landauer theory as well as the conventional single-mode Franck-Condon model. Instead, we model the overall charge transport as a sequence of non-adiabatic electron transfers, the rates of which depend on both outer and inner-sphere vibrational interactions. We show that the transport properties of our molecular junctions are determined by a combination of electron-electron and electron-vibrational coupling, and are sensitive to the interactions with the wider local environment. Furthermore, we assess the importance of nuclear tunnelling and examine the suitability of semi-classical Marcus theory as a description of charge transport in molecular devices.

cond-mat.mes-hall↗

The role of metallic leads and electronic degeneracies in thermoelectric power generation in quantum dots

The power factor of a thermoelectric device is a measure of the heat-to-energy conversion efficiency in nanoscopic devices. Yet, even as interest in low-dimensional thermoelectric materials has increased, experimental research on what influences the power factor in these systems is scarce. Here, we present a detailed thermoelectric study of graphene quantum dot devices. We show that spin-degeneracy of the quantum dot states has a significant impact on the zero-bias conductance of the device and leads to an increase of the power factor. Conversely, we demonstrate that non-ideal heat exchange within the leads can suppress the power factor near the charge degeneracy point and non-trivially influences its temperature dependence.

cond-mat.mes-hall↗

Realization of a Carbon-Nanotube-Based Superconducting Qubit

Hybrid circuit quantum electrodynamics (QED) involves the study of coherent quantum physics in solid state systems via their interactions with superconducting microwave circuits. Here we present an implementation of a hybrid superconducting qubit that employs a carbon nanotube as a Josephson junction. We realize the junction by contacting a carbon nanotube with a superconducting Pd/Al bi-layer, and implement voltage tunability of the qubit frequency using a local electrostatic gate. We demonstrate strong dispersive coupling to a coplanar waveguide resonator via observation of a resonator frequency shift dependent on applied gate voltage. We extract qubit parameters from spectroscopy using dispersive readout and find qubit relaxation and coherence times in the range of $10-200~\rm{ns}$.

quant-ph↗

Geometrically Enhanced Thermoelectric Effects in Graphene Nanoconstrictions

The influence of nanostructuring and quantum confinement on the thermoelectric properties of materials has been extensively studied. While this has made possible multiple breakthroughs in the achievable figure of merit, classical confinement, and its effect on the local Seebeck coefficient has mostly been neglected, as has the Peltier effect in general due to the complexity of measuring small temperature gradients locally. Here we report that reducing the width of a graphene channel to 100 nm changes the Seebeck coefficient by orders of magnitude. Using a scanning thermal microscope allows us to probe the local temperature of electrically contacted graphene two-terminal devices or to locally heat the sample. We show that constrictions in mono- and bilayer graphene facilitate a spatially correlated gradient in the Seebeck and Peltier coefficient, as evidenced by the pronounced thermovoltage $V_{th}$ and heating/cooling response $ΔT_{Peltier}$, respectively. This geometry dependent effect, which has not been reported previously in 2D materials, has important implications for measurements of patterned nanostructures in graphene and points to novel solutions for effective thermal management in electronic graphene devices or concepts for single material thermocouples.

cond-mat.mes-hall↗

Beyond Marcus theory and the Landauer-Büttiker approach in molecular junctions: A unified framework

Charge transport through molecular junctions is often described either as a purely coherent or a purely classical phenomenon, and described using the Landauer-Büttiker formalism or Marcus theory, respectively. Using a generalised quantum master equation, we here derive an expression for current through a molecular junction modelled as a single electronic level coupled to a collection of thermalised vibrational modes. We demonstrate that the aforementioned theoretical approaches can be viewed as two limiting cases of this more general expression, and present a series of approximations of this result valid at higher temperatures. We find that Marcus theory is often insufficient in describing the molecular charge transport characteristics and gives rise to a number of artefacts, especially at lower temperatures. Alternative expressions, retaining its mathematical simplicity but rectifying those shortcomings, are suggested. In particular, we show how lifetime broadening can be consistently incorporated into Marcus theory, and we derive a low-temperature correction to the semi-classical Marcus hopping rates. Our results are applied to examples building on phenomenological as well as microscopically-motivated electron-vibrational coupling. We expect them to be particularly useful in experimental studies of charge transport through single-molecule junctions as well as self-assembled monolayers.

cond-mat.mes-hall↗

Seeing opportunity in every difficulty: protecting information with weak value techniques

A weak value is an effective description of the influence of a pre and post-selected 'principal' system on another 'meter' system to which it is weakly coupled. Weak values can describe anomalously large deflections of the meter, and deflections in otherwise unperturbed variables: this motivates investigation of the potential benefits of the protocol in precision metrology. We present a visual interpretation of weak value experiments in phase space, enabling an evaluation of the effects of three types of detector noise as 'Fisher information efficiency' functions. These functions depend on the marginal distribution of the Wigner function of the meter, and give a unified view of the weak value protocol as a way of protecting Fisher information from detector imperfections. This approach explains why weak value techniques are more effective for avoiding detector saturation than for mitigating detector jitter or pixelation.

quant-ph↗

Quantum Interference in Silicon 1D Quasi-Ballistic Junctionless Nanowire Field Effect Transistors

We investigate the low temperature transport in 8 nm diameter Si junctionless nanowire field effect transistors fabricated by top down techniques with a wrap-around gate and two different activated doping densities. First we extract the intrinsic gate capacitance of the device geometry from a device that shows Coulomb blockade at 13 mK with over 500 Coulomb peaks across a gate voltage range of 6 V indicating the formation of a single island in the entire nanowire channel. In two other devices, doped Si:P $4\times10^{19}\,\text{cm}^{-3}$ and $2\times10^{20}\,\text{cm}^{-3}$, we observe quantum interference and use the extracted gate coupling to determine the dominant energy scale and the corresponding mean-free paths. For the higher doped device the analysis yields a mean free path of $4\pm2\,\text{nm}$, which is on the order of the average dopant spacing and suggests scattering on unactivated or activated dopants. For the device with an activated dopant density of $4\times10^{19}\,\text{cm}^{-3}$ the quantum interference effects suggest a mean free path of $10\pm2\,\text{nm}$, which is comparable to the nanowire width, and thus quasi-ballistic transport. A temperature dependent analysis of Universal Conductance Fluctuations suggests a coherence length above the nanowire length for temperatures below 1.9 K and decoherence from 1D electron-electron interactions for higher temperatures. The mobility is limited by scattering on impurities rather than the expected surface roughness scattering for nanowires with diameters larger or comparable to the Fermi wavelength. Our measurements therefore provide insight into the performance limitations from dominant scattering and dephasing mechanisms in technologically relevant silicon device geometries.

cond-mat.mes-hall↗

Spiro-Conjugated Molecular Junctions: between Jahn-Teller Distortion and Destructive Quantum Interference

The quest for molecular structures exhibiting strong quantum interference effects in the transport setting has long been on the forefront of chemical research. Here, we establish theoretically that the unusual geometry of spiro-conjugated systems gives rise to complete destructive interference in the resonant-transport regime. This results in a current blockade of the type not present in meta-connected benzene or similar molecular structures. We further show that these systems can undergo a transport-driven Jahn-Teller distortion which can lift the aforementioned destructive-interference effects. The overall transport characteristics is determined by the interplay between the two phenomena. Spiro-conjugated systems may therefore serve as a novel platform for investigations of quantum interference and vibronic effects in the charge transport setting. The potential to control quantum interference in these systems can also turn them into attractive components in designing functional molecular circuits.

cond-mat.mes-hall↗

Field-Effect Control of Graphene-Fullerene Thermoelectric Nanodevices

Although it was demonstrated that discrete molecular levels determine the sign and magnitude of the thermoelectric effect in single-molecule junctions, full electrostatic control of these levels has not been achieved to date. Here, we show that graphene nanogaps combined with gold microheaters serve as a testbed for studying single-molecule thermoelectricity. Reduced screening of the gate electric field compared to conventional metal electrodes allows control of the position of the dominant transport orbital by hundreds of meV. We find that the power factor of graphene-fullerene junctions can be tuned over several orders of magnitude to a value close to the theoretical limit of an isolated Breit-Wigner resonance. Furthermore, our data suggest that the power factor of an isolated level is only given by the tunnel coupling to the leads and temperature. These results open up new avenues for exploring thermoelectricity and charge transport in individual molecules and highlight the importance of level alignment and coupling to the electrodes for optimum energy conversion in organic thermoelectric materials.

cond-mat.mes-hall↗

Environment-Assisted Quantum Transport through Single-Molecule Junctions

Single-molecule electronics has been envisioned as the ultimate goal in the miniaturisation of electronic circuits. While the aim of incorporating single-molecule junctions into modern technology still proves elusive, recent developments in this field have begun to enable experimental investigation fundamental concepts within the area of chemical physics. One such phenomenon is the concept of Environment-Assisted Quantum Transport which has emerged from the investigation of exciton transport in photosynthetic complexes. Here, we study charge transport through a two-site molecular junction coupled to a vibrational environment. We demonstrate that vibrational interactions can also significantly enhance the current through specific molecular orbitals. Our study offers a clear pathway towards finding and identifying environment-assisted transport phenomena in charge transport settings.

cond-mat.mes-hall↗

A double quantum dot memristor

Memristive systems are generalisations of memristors, which are resistors with memory. In this paper, we present a quantum description of memristive systems. Using this model we propose and experimentally demonstrate a simple and practical scheme for realising memristive systems with quantum dots. The approach harnesses a phenomenon that is commonly seen as a bane of nanoelectronics, i.e. switching of a trapped charge in the vicinity of the device. We show that quantum-dot memristive systems have hysteresis current-voltage characteristics and quantum jump induced stochastic behaviour. Realising such a quantum memristor completes the menu of components for quantum circuit design.

cond-mat.mes-hall↗