arXiv subjects

Liesbeth M. C. Janssen

Publications and source records attributed to Liesbeth M. C. Janssen.

At least 55 records · Page 3Linked to original sources

arXiv2020

Enhanced persistence and collective migration in cooperatively aligning cell clusters

Most cells possess the capacity to locomote. Alone or collectively, this allows them to adapt, to rearrange, and to explore their surroundings. The biophysical characterization of such motile processes, in health and disease, has so far focused mostly on two limiting cases: single-cell motility on the one hand, and the dynamics of confluent tissues such as the epithelium on the other. The in-between regime of clusters, composed of relatively few cells, moving as a coherent unit has received less attention. Such small clusters are, however, deeply relevant in development but also in cancer metastasis. In this work, we use cellular Potts models and analytical active matter theory to understand how the motility of small cell clusters changes with N, the number of cells in the cluster. Modeling and theory reveal our two main findings: Cluster persistence time increases with N while the intrinsic diffusivity decreases with N. We discuss a number of settings in which the motile properties of more complex clusters can be analytically understood, revealing that the focusing effects of small-scale cooperation and cell-cell alignment can overcome the increased bulkiness and internal disorder of multicellular clusters to enhance overall migrational efficacy. We demonstrate this enhancement for small-cluster collective durotaxis, which is shown to proceed more effectively than for single cells. Our results may provide some novel insights into the connection between single-cell and large-scale collective motion and may point the way to the biophysical origins of the enhanced metastatic potential of small tumor cell clusters.

physics.bio-ph↗

arXiv2020

Generalized mode-coupling theory of the glass transition. II. Analytical scaling laws

Generalized mode-coupling theory (GMCT) constitutes a systematically correctable, first-principles theory to study the dynamics of supercooled liquids and the glass transition. It is a hierarchical framework that, through the incorporation of increasingly many particle density correlations, can remedy some of the inherent limitations of the ideal mode-coupling theory (MCT). However, despite MCT's limitations, the ideal theory also enjoys several remarkable successes, notably including the analytical scaling laws for the $α$- and $β$-relaxation dynamics. Here we mathematically derive similar scaling laws for arbitrary-order multi-point density correlation functions obtained from GMCT under arbitrary mean-field closure levels. More specifically, we analytically derive the asymptotic and preasymptotic solutions for the long-time limits of multi-point density correlators, the critical dynamics with two power-law decays, the factorization scaling laws in the $β$-relaxation regime, and the time-density superposition principle in the $α$-relaxation regime. The two characteristic power-law-divergent relaxation times for the two-step decay and the non-trivial relation between their exponents are also obtained. The validity ranges of the leading-order scaling laws are also provided by considering the leading preasymptotic corrections. Furthermore, we test these solutions for the Percus-Yevick hard-sphere system. We demonstrate that GMCT preserves all the celebrated scaling laws of MCT while quantitatively improving the exponents, rendering the theory a promising candidate for an ultimately quantitative first-principles theory of glassy dynamics.

cond-mat.stat-mech↗

arXiv2020

Glassy dynamics from generalized mode-coupling theory: existence and uniqueness of solutions for hierarchically coupled integro-differential equations

Generalized mode-coupling theory (GMCT) is a first-principles-based and systematically correctable framework to predict the complex relaxation dynamics of glass-forming materials. The formal theory amounts to a hierarchy of infinitely many coupled integro-differential equations, which may be approximated using a suitable finite-order closure relation. Although previous studies have suggested that finite-order GMCT leads to well-defined solutions, and that the hierarchy converges as the closure level increases, no rigorous and general result in this direction is known. Here we unambiguously establish the existence and uniqueness of solutions to generic, schematic GMCT hierarchies that are closed at arbitrary order. We consider two types of commonly invoked closure approximations, namely mean-field and exponential closures. We also distinguish explicitly between overdamped and underdamped glassy dynamics, corresponding to hierarchies of first-order and second-order integro-differential equations, respectively. We find that truncated GMCT hierarchies closed under an exponential closure conform to previously developed mathematical theories, such that the existence of a unique solution can be readily inferred. Self-consistent mean-field closures, however, of which the well-known standard-MCT closure approximation is a special case, warrant additional arguments for mathematical rigour. We demonstrate that the existence of a priori bounds on the solution is sufficient to also prove that unique solutions exist for such self-consistent hierarchies. To complete our analysis, we present simple arguments to show that these a priori bounds must exist, motivated by the physical interpretation of the GMCT solutions as density correlation functions. Overall, our work contributes to the theoretical justification of GMCT for studies of the glass transition, placing GMCT on a firmer mathematical footing.

cond-mat.stat-mech↗

arXiv2020

Glassy dynamics of a binary Voronoi fluid: A mode-coupling analysis

The binary Voronoi mixture is a fluid model whose interactions are local and many-body. Here we perform molecular-dynamics (MD) simulations of an equimolar mixture that is weakly polydisperse and additive. For the first time we study the structural relaxation of this mixture in the supercooled-liquid regime. From the simulations we determine the time- and temperature-dependent scattering functions for a large range of wave vectors, as well as the mean-square displacements of both particle species. We perform a detailed analysis of the dynamics by comparing the MD results with the first-principles-based idealized mode-coupling theory (MCT). To this end, we employ two approaches: fits to the asymptotic predictions of the theory, and fit-parameter-free binary MCT calculations based on static-structure-factor input from the simulations. We find that many-body interactions of the Voronoi mixture do not lead to strong qualitative differences relative to similar analyses carried out for simple liquids with pair-wise interactions. For instance, the fits give an exponent parameter $λ\approx 0.746$ comparable to typical values found for simple liquids, the wavevector dependence of the Kohlrausch relaxation time is in good agreement with literature results for polydisperse hard spheres, and the MCT calculations based on static input overestimate the critical temperature, albeit only by a factor of about 1.2. This overestimation appears to be weak relative to other well-studied supercooled-liquid models such as the binary Kob--Andersen Lennard-Jones mixture. Overall, the agreement between MCT and simulation suggests that it is possible to predict several microscopic dynamic properties with qualitative, and in some cases near-quantitative, accuracy based solely on static two-point structural correlations, even though the system itself is inherently governed by many-body interactions.

cond-mat.dis-nn↗

arXiv2019

Understanding, predicting, and tuning the fragility of vitrimeric polymers

Fragility is an empirical property that describes how abruptly a glass-forming material solidifies upon supercooling. The degree of fragility carries important implications for the functionality and processability of a material, as well as for our fundamental understanding of the glass transition. However, the microstructural properties underlying fragility still remain poorly understood. Here, we explain the microstructure-fragility link in vitrimeric networks, a novel type of high-performance polymers with unique bond-swapping functionality and unusual glass-forming behavior. Our results are gained from coarse-grained computer simulations and first-principles Mode-Coupling Theory (MCT) of star-polymer vitrimers. We first demonstrate that the vitrimer fragility can be tuned over an unprecedentedly broad range, from fragile to strong and even superstrong behavior, by decreasing the bulk density. Remarkably, this entire phenomenology can be reproduced by microscopic MCT, thus challenging the conventional belief that existing first-principles theories cannot account for non-fragile behaviors. Our MCT analysis allows us to rationally identify the microstructural origin of the fragile-to-superstrong crossover, which is rooted in the sensitivity of the static structure factor to temperature variations. On the molecular scale, this behavior stems from a change in dominant length scales, switching from repulsive excluded-volume interactions to intrachain attractions as the vitrimer density decreases. Finally, we develop a simplified schematic MCT model which corroborates our microscopically-founded conclusions and which unites our findings with earlier MCT studies. Our work sheds new light on the elusive structure-fragility link in glass-forming matter, and provides a first-principles-based platform for designing novel amorphous materials with an on-demand dynamic response.

cond-mat.soft↗

arXiv2019

Generalized mode-coupling theory of the glass transition. I. Numerical results for Percus-Yevick hard spheres

Mode-coupling theory (MCT) constitutes one of the few first-principles-based approaches to describe the physics of the glass transition, but the theory's inherent approximations compromise its accuracy in the activated glassy regime. Here we show that microscopic generalized mode-coupling theory (GMCT), a recently proposed hierarchical framework to systematically improve upon standard MCT, provides a promising pathway toward a more accurate first-principles description of glassy dynamics. We present a comprehensive numerical analysis for Percus-Yevick hard spheres by performing explicitly wavenumber- and time-dependent GMCT calculations up to sixth order. Specifically, we calculate the location of the critical point, the associated non-ergodicity parameters, the time-dependent dynamics of the density correlators at both absolute and reduced packing fractions, and we test several universal scaling relations in the $α$- and $β$-relaxation regimes. It is found that higher-order GMCT can successfully remedy some of standard MCT's pathologies, including an underestimation of the critical glass transition density and an overestimation of the hard-sphere fragility. Furthermore, we numerically demonstrate that the celebrated scaling laws of standard MCT are preserved in GMCT at all closure levels, and that the predicted critical exponents manifestly improve as more levels are incorporated in the GMCT hierarchy. Although formally the GMCT equations should be solved up to infinite order to reach full convergence, our finite-order GMCT calculations unambiguously reveal a uniform convergence pattern for the dynamics. We thus argue that GMCT can provide a feasible and controlled means to bypass MCT's main uncontrolled approximation, offering hope for the future development of a quantitative first-principles theory of the glass transition.

cond-mat.stat-mech↗

arXiv2019

Stimuli-responsive behavior of PNiPAm microgels under interfacial confinement

The volume phase transition of microgels is one of the most paradigmatic examples of stimuli-responsiveness, enabling a collapse from a highly swollen microgel state into a densely coiled state by an external stimulus. Although well characterized in bulk, it remains unclear how the phase transition is affected by the presence of a confining interface. Here, we demonstrate that the temperature-induced volume phase transition of poly(N-isopropylacrylamide) microgels, conventionally considered an intrinsic molecular property of the polymer, is in fact largely suppressed when the microgel is adsorbed to an air/liquid interface. We further observe a hysteresis in core morphology and interfacial pressure between heating and cooling cycles. Our results, supported by molecular dynamics simulations, reveal that the dangling polymer chains of microgel particles, spread at the interface under the influence of surface tension, do not undergo any volume phase transition, demonstrating that the balance in free energy responsible for the volume phase transition is fundamentally altered by interfacial confinement. These results imply that important technological properties of such systems, including the temperature-induced destabilization of emulsions does not occur via a decrease in interfacial coverage of the microgels.

cond-mat.soft↗

arXiv2019

Active glasses

Active glassy matter has recently emerged as a novel class of non-equilibrium soft matter, combining energy-driven, active particle movement with dense and disordered glass-like behavior. Here we review the state-of-the-art in this field from an experimental, numerical, and theoretical perspective. We consider both non-living and living active glassy systems, and discuss how several hallmarks of glassy dynamics (dynamical slowdown, fragility, dynamical heterogeneity, violation of the Stokes-Einstein relation, and aging) are manifested in such materials. We start by reviewing the recent experimental evidence in this area of research, followed by an overview of the main numerical simulation studies and physical theories of active glassy matter. We conclude by outlining several open questions and possible directions for future work.

cond-mat.soft↗

arXiv2018

Aging and rejuvenation of active matter under topological constraints

The coupling of active, self-motile particles to topological constraints can give rise to novel non-equilibrium dynamical patterns that lack any passive counterpart. Here we study the behavior of self-propelled rods confined to a compact spherical manifold by means of Brownian dynamics simulations. We establish the state diagram and find that short active rods at sufficiently high density exhibit a glass transition toward a disordered state characterized by persistent self-spinning motion. By periodically melting and revitrifying the spherical spinning glass, we observe clear signatures of time-dependent aging and rejuvenation physics. We quantify the crucial role of activity in these non-equilibrium processes, and rationalize the aging dynamics in terms of an absorbing-state transition toward a more stable active glassy state. Our results demonstrate both how concepts of passive glass phenomenology can carry over into the realm of active matter, and how topology can enrich the collective spatiotemporal dynamics in inherently non-equilibrium systems.

cond-mat.stat-mech↗

arXiv2018

Mode-Coupling Theory of the Glass Transition: A Primer

Understanding the physics of glass formation remains one of the major unsolved challenges of condensed matter science. As a material solidifies into a glass, it exhibits a spectacular slowdown of the dynamics upon cooling or compression, but at the same time undergoes only minute structural changes. Among the numerous theories put forward to rationalize this complex behavior, Mode-Coupling Theory (MCT) stands out as the only framework that provides a fully first-principles-based description of glass phenomenology. This review outlines the key physical ingredients of MCT, its predictions, successes, and failures, as well as recent improvements of the theory. We also discuss the extension and application of MCT to the emerging field of non-equilibrium active soft matter

cond-mat.stat-mech↗

arXiv2018

Spontaneous membrane formation and self-encapsulation of active rods in an inhomogeneous motility field

We study the collective dynamics of self-propelled rods in an inhomogeneous motility field. At the interface between two regions of constant but different motility, a smectic rod layer is spontaneously created through aligning interactions between the active rods, reminiscent of an artificial, semi-permeable membrane. This "active membrane" engulfes rods which are locally trapped in low-motility regions and thereby further enhances the trapping efficiency by self-organization, an effect which we call "self-encapsulation". Our results are gained by computer simulations of self-propelled rod models confined on a two-dimensional planar or spherical surface with a stepwise constant motility field, but the phenomenon should be observable in any geometry with sufficiently large spatial inhomogeneity. We also discuss possibilities to verify our predictions of active-membrane formation in experiments of self-propelled colloidal rods and vibrated granular matter.

cond-mat.soft↗

arXiv2016

Direct probe of anisotropy in atom-molecule collisions via quantum scattering resonances

Anisotropy is a fundamental property of particle interactions. It occupies a central role in cold and ultra-cold molecular processes, where long range forces have been found to significantly depend on orientation in ultra-cold polar molecule collisions. Recent experiments have demonstrated the emergence of quantum phenomena such as scattering resonances in the cold collisions regime due to quantization of the intermolecular degrees of freedom. Although these states have been shown to be sensitive to interaction details, the effect of anisotropy on quantum resonances has eluded experimental observation so far. Here, we directly measure the anisotropy in atom-molecule interactions via quantum resonances by changing the quantum state of the internal molecular rotor. We observe that a quantum scattering resonance at a collision energy of $k_B$ x 270 mK appears in the Penning ionization of molecular hydrogen with metastable helium only if the molecule is rotationally excited. We use state of the art ab initio and multichannel quantum molecular dynamics calculations to show that the anisotropy contributes to the effective interaction only for $H_2$ molecules in the first excited rotational state, whereas rotationally ground state $H_2$ interacts purely isotropically with metastable helium. Control over the quantum state of the internal molecular rotation allows us to switch the anisotropy on or off and thus disentangle the isotropic and anisotropic parts of the interaction. These quantum phenomena provide a challenging benchmark for even the most advanced theoretical descriptions, highlighting the advantage of using cold collisions to advance the microscopic understanding of particle interactions.

physics.chem-ph↗

arXiv2015

Microscopic dynamics of supercooled liquids from first principles

Glasses are solid materials whose constituent atoms are arranged in a disordered manner. The transition from a liquid to a glass remains one of the most poorly understood phenomena in condensed matter physics, and still no fully microscopic theory exists that can describe the dynamics of supercooled liquids in a quantitative manner over all relevant time scales. Here we present such a theoretical framework that yields near-quantitative accuracy for the time-dependent correlation functions of a supercooled system over a broad density range. Our approach requires only simple static structural information as input and is based entirely based on first principles. Owing to this first-principles nature, the framework offers a unique platform to study the relation between structure and dynamics in glass-forming matter, and paves the way towards a systematically correctable and ultimately fully quantitative theory of microscopic glassy dynamics.

cond-mat.stat-mech↗

arXiv2015

Generalized mode-coupling theory of the glass transition: schematic results at finite and infinite order

We present an extensive treatment of the generalized mode-coupling theory (GMCT) of the glass transition, which seeks to describe the dynamics of glass-forming liquids using only static structural information as input. This theory amounts to an infinite hierarchy of coupled equations for multi-point density correlations, the lowest-order closure of which is equivalent to standard mode-coupling theory. Here we focus on simplified schematic GMCT hierarchies, which lack any explicit wavevector-dependence and therefore allow for greater analytical and numerical tractability. For one particular schematic model, we derive the unique analytic solution of the infinite hierarchy, and demonstrate that closing the hierarchy at finite order leads to uniform convergence as the closure level increases. We also show numerically that a similarly robust convergence pattern emerges for more generic schematic GMCT models, suggesting that the GMCT framework is generally convergent, even though no small parameter exists in the theory. Finally, we discuss how different effective weights on the high-order contributions ultimately control whether the transition is continuous, discontinuous, or strictly avoided, providing new means to relate structure to dynamics in glass-forming systems.

cond-mat.stat-mech↗

arXiv2014

Relaxation Patterns in Supercooled Liquids from Generalized Mode-Coupling Theory

The mode-coupling theory of the glass transition treats the dynamics of supercooled liquids in terms of two-point density correlation functions. Here we consider a generalized, hierarchical formulation of schematic mode-coupling equations in which the full basis of multipoint density correlations is taken into account. By varying the parameters that control the effective contributions of higher-order correlations, we show that infinite hierarchies can give rise to both sharp and avoided glass transitions. Moreover, small changes in the form of the coefficients result in different scaling behaviors of the structural relaxation time, providing a means to tune the fragility in glass-forming materials. This demonstrates that the infinite-order construct of generalized mode-coupling theory constitutes a powerful and unifying framework for kinetic theories of the glass transition.

cond-mat.stat-mech↗

arXiv2013

Quantum reactive scattering of ultracold NH($X\,^3Σ^-$) radicals in a magnetic trap

We investigate the ultracold reaction dynamics of magnetically trapped NH($X ^3Σ^-$) radicals using rigorous quantum scattering calculations involving three coupled potential energy surfaces. We find that the reactive NH + NH cross section is driven by a short-ranged collisional mechanism, and its magnitude is only weakly dependent on magnetic field strength. Unlike most ultracold reactions observed so far, the NH + NH scattering dynamics is non-universal. Our results indicate that chemical reactions can cause more trap loss than spin-inelastic NH + NH collisions, making molecular evaporative cooling more difficult than previously anticipated.

physics.chem-ph↗

arXiv2012

Quantum-state resolved bimolecular collisions of velocity-controlled OH with NO radicals

Whereas atom-molecule collisions have been studied with complete quantum state resolution, interactions between two state-selected molecules have proven much harder to probe. Here, we report the measurement of state-resolved inelastic scattering cross sections for collisions between two open-shell molecules that are both prepared in a single quantum state. Stark-decelerated OH radicals were scattered with hexapole-focused NO radicals in a crossed beam configuration. Rotationally and spin-orbit inelastic scattering cross sections were measured on an absolute scale for collision energies between 70 and 300 cm$^{-1}$. These cross sections show fair agreement with quantum coupled-channels calculations using a set of coupled model potential energy surfaces based on ab initio calculations for the long-range non-adiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes.

physics.chem-ph↗

arXiv2011

On the role of the magnetic dipolar interaction in cold and ultracold collisions: Numerical and analytical results for NH($^3Σ^-$) + NH($^3Σ^-$)

We present a detailed analysis of the role of the magnetic dipole-dipole interaction in cold and ultracold collisions. We focus on collisions between magnetically trapped NH molecules, but the theory is general for any two paramagnetic species for which the electronic spin and its space-fixed projection are (approximately) good quantum numbers. It is shown that dipolar spin relaxation is directly associated with magnetic-dipole induced avoided crossings that occur between different adiabatic potential curves. For a given collision energy and magnetic field strength, the cross-section contributions from different scattering channels depend strongly on whether or not the corresponding avoided crossings are energetically accessible. We find that the crossings become lower in energy as the magnetic field decreases, so that higher partial-wave scattering becomes increasingly important \textit{below} a certain magnetic field strength. In addition, we derive analytical cross-section expressions for dipolar spin relaxation based on the Born approximation and distorted-wave Born approximation. The validity regions of these analytical expressions are determined by comparison with the NH + NH cross sections obtained from full coupled-channel calculations. We find that the Born approximation is accurate over a wide range of energies and field strengths, but breaks down at high energies and high magnetic fields. The analytical distorted-wave Born approximation gives more accurate results in the case of s-wave scattering, but shows some significant discrepancies for the higher partial-wave channels. We thus conclude that the Born approximation gives generally more meaningful results than the distorted-wave Born approximation at the collision energies and fields considered in this work.

physics.chem-ph↗