arXiv subjects

Alice L. Thorneywork

Publications and source records attributed to Alice L. Thorneywork.

9 recordsLinked to original sources

arXiv2026

Orientational bistability and field-controlled switching of a superparamagnetic dimer

We study the orientational dynamics of superparamagnetic colloidal dimers that carry both an induced magnetic moment, proportional to the applied field, and an effective permanent moment. In a static, uniform magnetic field, dimers that are permanently fixed together hop between two preferred in-plane angles, developing a bimodal steady-state orientation distribution. When the same field is periodically reversed, we observe a sharp, field-controlled change in the dynamical response from small hopping events with $Δθ\ll π$ to full $Δθ\approx π$ rotations on each field flip. We show that both the static bistability and the switching bifurcation can be rationalised by a magnetic response in the dimer that consists of both a strong induced and weak body-fixed component. This leads to a complex orientational energy/potential landscape, with coupled roll-yaw rotations of the dimer responsible for the bistable dynamics. By combining the misorientation between dimer axis and field, bifurcation field strength and short-time orientational variance, we determine the magnitude and orientation of the net permanent dipole, thereby characterising details of the internal magnetic structure of the particles via microscopy.

cond-mat.soft↗

arXiv2025

Collective Hard Core Interactions Leave Multiscale Signatures in Number Fluctuation Spectra

A full understanding of transport in dense, interacting suspensions requires analysis frameworks sensitive to self and collective dynamics across all relevant spatial and temporal scales. Here we introduce a trajectory-free approach to address this problem based on the power spectral density of particle number fluctuations (N-PSD). By combining colloidal experiments and theory we show that the N-PSD naturally probes behaviour across multiple important dynamic regimes and we fully uncover the mechanistic origins of characteristic spectral scalings and timescales. In particular, we demonstrate that while high-frequency scalings link to self-diffusion, low-frequency scalings sensitively capture long-lived correlations and collective dynamics. In this regime, interactions lead to non-trivial spectral signatures, governed by pairwise particle exchange at small length scales and collective rearrangements over large scales. Our findings thus provide important insight into the effect of interactions on microscopic dynamics and fluctuation phenomena and establish a powerful new tool with which to probe dynamics in complex systems.

cond-mat.soft↗

arXiv2025

Decoding Noise in Nanofluidic Systems: Adsorption versus Diffusion Signatures in Power Spectra

Adsorption processes play a fundamental role in molecular transport through nanofluidic systems, but their signatures in measured signals are often hard to distinguish from other processes like diffusion. In this paper, we derive an expression for the power spectral density (PSD) of particle number fluctuations in a channel, accounting for diffusion and adsorption/desorption to a wall. Our model, validated by Brownian dynamics simulations, is set in a minimal but adaptable geometry, allowing us to eliminate the effects of specific geometries. We identify distinct signatures in the PSD as a function of frequency $f$, including a $1/f^{3/2}$ scaling related to diffusive entrance/exit effects, and a $1/f^2$ scaling associated with adsorption. These scalings appear in key predicted quantities -- the total number of particles in the channel and the number of adsorbed or unadsorbed particles -- and can dominate or combine in non-trivial ways depending on parameter values. Notably, when there is a separation of timescales between diffusion inside the channel and adsorption/desorption times, the PSD can exhibit two distinct corners with well-separated slopes in some of the predicted quantities. We provide a strategy to identify adsorption and diffusion mechanisms in the shape of the PSD of experimental systems on the nano- and micro-scale, such as ion channels, nanopores, and electrochemical sensors, potentially offering insights into noisy experimental data.

cond-mat.soft↗

arXiv2025

Measuring collective diffusion properties by counting particles in boxes

The collective diffusion coefficient $D_\mathrm{coll}$ is a key quantity for describing the macroscopic transport properties of soft matter systems. However, measuring $D_\mathrm{coll}$ is a fundamental experimental and numerical challenge, as it either relies on nonequilibrium techniques that are hard to interpret or, at equilibrium, on Fourier-based approaches which are fraught with difficulties associated with Fourier transforms. In this work, we investigate the equilibrium diffusive dynamics of a 2D colloidal suspension experimentally and numerically. We use a "Countoscope" technique, which analyses the statistics of particle number counts $N(t)$ in virtual observation boxes of a series of microscopy images at equilibrium, to measure $D_\mathrm{coll}$ for the first time. We validate our results against Fourier-based approaches and establish best practices for measuring $D_\mathrm{coll}$ using fluctuating counts. We show that Fourier techniques yield inaccurate long-range collective measurements because of the non-periodic nature of an experimental image, yet counting exploits this property by using finite observation windows. Finally, we discuss the potential of our method to advance our understanding of collective properties in suspensions, particularly the role of hydrodynamic interactions.

cond-mat.soft↗

arXiv2024

Interpreting the power spectral density of a fluctuating colloidal current

The transport of molecules through biological and synthetic nanopores is governed by multiple stochastic processes that lead to noisy, fluctuating currents. Disentangling the characteristics of different noise-generating mechanisms is central to better understanding molecular transport at a fundamental level but is extremely challenging in molecular systems, due to their complexity and relative experimental inaccessibility. Here, we construct a colloidal model microfluidic system for the experimental measurement of particle currents, where the governing physical properties are directly controllable and particle dynamics directly observable, unlike in the molecular case. Currents of hard spheres fluctuate due to the random arrival times of particles into the channel and the distribution of particle speeds within the channel, which results in characteristic scalings in the power spectral density. We rationalise these scalings by quantitatively comparing to a model for shot noise with a finite transit time, extended to include the distribution of particle speeds. Particle velocity distributions sensitively reflect the confining geometry and we interpret and model these in terms of the underlying fluid flow profiles. Finally, we explore the extent to which details of these distributions govern the form of the resulting power spectral density, thereby establishing concrete links between the power spectral density and underlying mechanisms for this experimental system. This paves the way for establishing a more systematic understanding of the links between characteristics of transport fluctuations and underlying molecular mechanisms in driven systems such as nanopores.

cond-mat.soft↗

arXiv2024

The Countoscope: Measuring Self and Collective Dynamics without Trajectories

Driven by physical questions pertaining to quantifying particle dynamics, microscopy can now resolve complex systems at the single particle level, from cellular organisms to individual ions. Yet, available analysis techniques face challenges reconstructing trajectories in dense and heterogeneous systems where accurately labelling particles is difficult. Furthermore, the inescapable finite field of view of experiments hinders the measurement of collective effects. Inspired by Smoluchowski, we introduce a broadly applicable analysis technique that probes dynamics of interacting particle suspensions based on a remarkably simple principle: counting particles in finite observation boxes. Using colloidal experiments, advanced simulations and theory, we first demonstrate that statistical properties of fluctuating counts can be used to determine self-diffusion coefficients, so alleviating the hurdles associated with trajectory reconstruction. We also provide a recipe for practically extracting the diffusion coefficient from experimental data at variable particle densities, which is sensitive to steric and hydrodynamic interactions. Remarkably, by increasing the observation box size, counting naturally enables the study of collective dynamics in dense suspensions. Using our novel analysis of particle counts, we uncover a surprising enhancement of collective behaviour, as well as a new length scale associated with hyperuniform-like structure. Our counting framework, the Countoscope, thus enables efficient measurements of self and collective dynamics in dense suspensions and opens the way to quantifying dynamics and identifying novel physical mechanisms in diverse complex systems where single particles can be resolved.

cond-mat.soft↗

arXiv2024

Resolution dependence of most probable pathways with state-dependent diffusivity

Recent experiments have probed the relative likelihoods of trajectories in stochastic systems by observing survival probabilities within a tube of radius $R$ in spacetime. We measure such probabilities here for a colloidal particle in a corrugated channel, corresponding to a bistable potential with state-dependent diffusivity. In contrast to previous findings for state-independent noise, we find that the most probable pathway changes qualitatively as the tube radius $R$ is altered. We explain this by computing the survival probabilities predicted by overdamped Langevin dynamics. At high enough resolution (small enough $R$), survival probabilities depend solely on diffusivity variations, independent of deterministic forces; finite $R$ corrections yield a generalization of the Onsager-Machlup action. As corollary, ratios of survival probabilities are singular as $R \to 0$, but become regular, and described by the classical Onsager-Machlup action, only in the special case of state-independent noise.

cond-mat.stat-mech↗

arXiv2021

3D Flow Field Measurements Outside Nanopores

We demonstrate a non-stereoscopic, video-based particle tracking system with optical tweezers to study fluid flow in 3D in the vicinity of glass nanopores. In particular, we used the Quadrant Interpolation algorithm to extend our video-based particle tracking to displacements out of the trapping plane of the tweezers. This permitted the study of flow from nanopores oriented at an angle to the trapping plane, enabling the mounting of nanopores on a micromanipulator with which it was then possible to automate the mapping procedure. Mapping of voltage driven flow in 3D volumes outside nanopores revealed polarity dependent flow fields. This is in agreement with the model of voltage driven flow in conical nanopores depending on the interaction of distinct flows within the nanopore and along the outer walls.

physics.flu-dyn↗

arXiv2016

Dynamic heterogeneities and non-Gaussian behavior in two-dimensional randomly confined colloidal fluids

A binary mixture of super-paramagnetic colloidal particles is confined between glass plates such that the large particles become fixed and provide a two-dimensional disordered matrix for the still mobile small particles, which form a fluid. By varying fluid and matrix area fractions and tuning the interactions between the super-paramagnetic particles via an external magnetic field, different regions of the state diagram are explored. The mobile particles exhibit delocalized dynamics at small matrix area fractions and localised motion at high matrix area fractions, and the localization transition is rounded by the soft interactions [T. O. E. Skinner et al, Phys. Rev. Lett. {\bf 111}, 128301 (2013)]. Expanding on previous work, we find the dynamics of the tracers to be strongly heterogeneous and show that molecular dynamics simulations of an ideal gas confined in a fixed matrix exhibit similar behavior. The simulations show how these soft interactions make the dynamics more heterogenous compared to the disordered Lorentz gas and lead to strong non-Gaussian fluctuations.

cond-mat.soft↗