arXiv subjects

Paul Desmarchelier

Publications and source records attributed to Paul Desmarchelier.

7 recordsLinked to original sources

arXiv2026

Dynamics of charge fluctuations in nanocapacitors: effects of salt concentration and electrode metallicity from Brownian dynamics

Electric double-layer capacitors (EDLCs) rely on the dynamical response of confined electrolytes to store and release charge, yet the interplay between ion transport, electrostatic interactions, and electrode metallicity remains poorly understood at the nanoscale. We develop a comprehensive Brownian dynamics framework to compute the frequency-dependent admittance of nanocapacitors, explicitly accounting for salt concentration and the finite screening length of electrodes (modeled via Thomas-Fermi theory). We derive the fluctuation-dissipation relation connecting the dynamics of equilibrium charge fluctuations to the linear response of the system quantified by the frequency-dependent admittance. Specifically, we obtain two estimators for the admittance, based on ionic positions and forces, and combine them via a control variate method to reduce uncertainty across all frequencies. We show that the admittance exhibits a low-frequency regime dominated by capacitive effects, and a high-frequency one governed by the ideal Nernst-Einstein conductivity. The crossover between these regimes is characterized by a timescale that depends on both the electrode metallicity and salt concentration, highlighting the role of ion-wall collisions and electrostatic interactions. Comparisons with analytical models show that while mean-field theories capture qualitative trends, they systematically overestimate low-frequency admittance and underestimate high-frequency behavior, underscoring the necessity of explicit ion-ion and ion-wall interactions. This work connects microscopic dynamics to macroscopic electrochemical observables, offering a tool to interpret impedance spectra in nanoscale systems. Beyond charge storage in EDLCs, our framework provides insights for sensing applications in nanofluidic devices, where charge/current fluctuations enable the detection of electrochemically active species.

physics.chem-ph↗

arXiv2026

Quantifying the Features of an Amorphous Solid's Local Yield Surface

In two-dimensional Lennard-Jones glasses, mechanical probing reveals that local yield surfaces are dominated by regions with a positive second derivative of the yield stress with respect to the loading angle. Each feature corresponds to a shear transformation zone and a characteristic non-affine displacement field at yield. Most features are well described by a combined Schmid-Mohr-Coulomb criterion parameterized by a weak-plane orientation, a critical stress, and a pressure sensitivity. The resulting parameter statistics clarify how the onset of plastic flow is governed by the population of discrete yielding features encoded in the amorphous structure.

cond-mat.soft↗

arXiv2026

Brownian dynamics simulations of electric double-layer capacitors with tunable metallicity

We introduce an efficient description of electrodes, characterized by their Thomas-Fermi screening length lTF inside the metal, for Brownian dynamics (BD) simulations of capacitors. Within a Born-Oppenheimer approximation for the electron charge density inside the electrodes, we derive the effective many-body potential for ions in an implicit solvent between Thomas-Fermi electrodes, taking into account the constraints of applied voltage and of global electro-neutrality of the system, as well as the 2D periodic boundary conditions along the electrode surfaces. We derive the average charge and the fluctuation-dissipation relation for the differential capacitance, highlighting the contribution of the fluctuations of the net ionic dipole moment, as well as those from the solvent polarization and of the electron density, whose fluctuations are suppressed within the Born-Oppenheimer description. We demonstrate the relevance of this model by validating its predictions against known results for the force on ions as a function of the ion-surface distance in simple geometries. The equilibrium ionic density profiles from BD simulations are in excellent agreement with those from an explicit electrode model for perfect metals, and are obtained at a significantly lower computational cost. Finally, we discuss with the present model the effect of the Thomas-Fermi screening length on the equilibrium ionic density profiles and the capacitance. While limited to parallel plate capacitors, the present simulation method allows to consider larger systems, lower concentrations, and longer time scales concentrations than molecular simulations in order to predict the electrochemical properties of Thomas-Fermi capacitors and correlate them with the ion dynamics.

physics.chem-ph↗

arXiv2024

Resonant phonons: Localization in a structurally ordered crystal

Phonon localization is a phenomenon that influences numerous material properties in condensed matter physics. Anderson localization brings rise to localized atomic-scale phonon interferences in disordered lattices with an influence limited to high-frequency phonons having wavelengths comparable to the size of a randomly perturbed unit cell. Here we theoretically reveal a new form of phonon localization induced by augmenting a crystalline material with intrinsic phonon nanoresonators with feature sizes that can be smaller or larger than the phonon wavelengths but must be relatively small compared to the phonon mean free paths. This mechanism is deterministic and takes place within numerous discrete narrow-frequency bands spread throughout the full spectrum with central frequencies controlled by design. For demonstration, we run molecular dynamics simulations of all-silicon nanopillared membranes at room temperature, and apply to the underlying thermalized environment narrowband wave packets as an excitation at precisely the frequencies where resonant hybridizations are evident in the anharmonic phonon band structure. Upon comparison to other frequency ranges where the nanostructure does not exhibit local resonances, significant intrinsic spatial phonon localization along the direction of transport is explicitly observed. Furthermore, the energy exchange with external sources is minimized at the resonant frequencies. We conclude by making a direct comparison with Anderson localization highlighting the superiority of the resonant phonons across both sides of the interference frequency limit.

cond-mat.mes-hall↗

arXiv2024

Topological characterization of rearrangements in amorphous solids

In amorphous materials, plasticity is localized and occurs as shear transformations. It was recently shown by Wu et al. that these shear transformations can be predicted by applying topological defect concepts developed for liquid crystals to an analysis of vibrational eigenmodes [Wu et al.; Nat. Com.,2023]. This study relates the -1 topological defects to the displacement fields expected of an Eshelby inclusion, which are characterized by an orientation and the magnitude of the eigenstrain. A corresponding orientation and magnitude can be defined for each defect using the local displacement field around each defect. These parameters characterize the plastic stress relaxation associated with the local structural rearrangement and can be extracted using the fit to either the global displacement field or the local field. Both methods provide a reasonable estimation of the MD-measured stress drop, confirming the localized nature of the displacements that control both long-range deformation and stress relaxation.

cond-mat.mes-hall↗

arXiv2022

Phonon Interference at the Atomic Scale

Phonons diffraction and interference patterns are observed at the atomic scale, using molecular dynamics simulations in systems containing crystalline silicon and nanometric obstacles as voids or amorphous-inclusions. The diffraction patterns caused by these nano-architectured systems of the same order as the phonon wavelengths are similar to the ones predicted by a simple Fresnel-Kirchhoff integral, with a few differences due to the nature of the obstacle and the anisotropy of crystalline silicon. These findings give evidence of the wave nature of phonons, can help to a better comprehension of the interaction of phonons with nanoobjects and at long term can be useful for intelligent thermal management and phonon frequency filtering at the nanoscale.

cond-mat.mes-hall↗

arXiv2021

Ballistic Heat Transport in Nanocomposite: the Role of the Shape and Interconnection of Nanoinclusions

The effect on the vibrational and thermal properties of gradually interconnected nanoinclusions embedded in an amorphous silicon matrix is studied using MD simulations. The nanoinclusion arrangement ranges from an aligned sphere array to an interconnected mesh of nanowires. Wave-packet simulations scanning different polarizations and frequencies reveal that the interconnection of the nanoinclusions at constant volume fraction induces a strong increase of the mean free path of high frequency phonons, but does not affect the energy diffusivity. The mean free path and energy diffusivity are then used to estimate the thermal conductivity, showing an enhancement of the effective thermal the effective thermal conductivity due to the existence of crystalline structural interconnections. This enhancement is dominated by the ballistic transport of phonons. Equilibrium molecular dynamics simulations confirm the tendency although less markedly. This leads to the observation that coherent energy propagation with a moderate increase of the thermal conductivity is possible.

cond-mat.mes-hall↗