arXiv subjects

Joshua D. Elliott

Publications and source records attributed to Joshua D. Elliott.

4 recordsLinked to original sources

arXiv2025

Symmetry-protected electronic metastability in an optically driven cuprate ladder

Optically excited quantum materials exhibit nonequilibrium states with remarkable emergent properties, but these phenomena are usually transient, decaying on picosecond timescales and limiting practical applications. Advancing the design and control of nonequilibrium phases requires the development of targeted strategies to achieve long-lived, metastable phases. Here, we report the discovery of symmetry-protected electronic metastability in the model cuprate ladder Sr$_{14}$Cu$_{24}$O$_{41}$. Using femtosecond resonant x-ray scattering and spectroscopy, we show that this metastability is driven by a transfer of holes from chain-like charge reservoirs into the ladders. This ultrafast charge redistribution arises from the optical dressing and activation of a hopping pathway that is forbidden by symmetry at equilibrium. Relaxation back to the ground state is hence suppressed after the pump coherence dissipates. Our findings highlight how dressing materials with electromagnetic fields can dynamically activate terms in the electronic Hamiltonian, and provide a rational design strategy for nonequilibrium phases of matter.

cond-mat.str-el↗

arXiv2022

Do specific ion effects influence the physical chemistry of aqueous graphene-based supercapacitors? Perspectives from multiscale QMMD simulations

Whether or not specific ion effects determine the charge storage properties of aqueous graphene and graphite-based supercapacitors remains a highly debated topic. In this work we present a multiscale quantum mechanics classical molecular dynamics investigation of aqueous mono- and divalent salt electrolytes in contact with fully polarizable charged graphene sheets. By computing both the electrochemical double layer and quantum capacitance we observe a constant electrode specific capacitance with cationic radii and charge. Counterintuitively, we determine that a switch in the cation adsorption mechanism from inner to outer Helmholtz layers leads to negligible changes to the EDL capacitance, this appears to be due to the robust electronic structure of the graphene electrodes. However, the ability of ions (such as K+) with a relatively low hydration free energy to penetrate the inner Helmholtz plane and adsorb directly on the electrode surface is found to slow their diffusion parallel to the interface. Ions in the outer Helmholtz layer are found to have higher diffusivity at the surface due to their position in ion channels between water layers. Our results show that surface effects such as the surface polarization and the partial dehydration and local structuring of ions on the surface underpin the behaviour of cations at the interface and add a vital new perspective on trends in ion mobilities seen under confinement.

cond-mat.mtrl-sci↗

arXiv2022

Wettability of graphite under 2D confinement

The thermodynamics of solid/liquid interfaces under nanoconfinement has tremendous implications for liquid transport properties. Here using molecular dynamics, we investigate graphite nanoslits and study how the water/graphite interfacial tension changes with the degree of confinement. We found that, for nanochannel heights between 0.7nm and 2.6nm, graphite becomes more hydrophobic than in bulk, and that the value of the surface tension oscillates before eventually converging towards a constant value for larger slits. The value of the surface tension is correlated with the slip length of the fluid and explained in terms of the effective and interfacial density, hydration pressure and friction coefficient. The study clearly indicates that there is a critical channel height of 0.9nm (achievable experimentally1) at which the surface tension reaches its highest value, but the water diffusion across the channel is at its minimum. The structural analysis shows that for this pore size a transition between a 2D and 3D hydrogen bond network is accompanied by an abrupt increase in conformational entropy. Our results show that the wettability of solid surfaces can change under nanoconfinement and the data can be used to interpret the experimental permeability data.

physics.flu-dyn↗

arXiv2021

Dynamically polarisable force-fields for surface simulations via multi-output classification Neural Networks

We present a general procedure to introduce electronic polarization into classical Molecular Dynamics (MD) force-fields using a Neural Network (NN) model. We apply this framework to the simulation of a solid-liquid interface where the polarization of the surface is essential to correctly capture the main features of the system. By introducing a multi-input, multi-output NN and treating the surface polarization as a discrete classification problem, for which NNs are known to excel, we are able to obtain very good accuracy in terms of quality of predictions. Through the definition of a custom loss function we are able to impose a physically motivated constraint within the NN itself making this model extremely versatile, especially in the modelling of different surface charge states. The NN is validated considering the redistribution of electronic charge density within a graphene based electrode in contact with aqueous electrolyte solution, a system highly relevant to the development of next generation low-cost supercapacitors. We compare the performances of our NN/MD model against Quantum Mechanics/Molecular dynamics simulations where we obtain a most satisfactorily agreement.

physics.comp-ph↗