arXiv subjects

Chandan K. Mishra

Publications and source records attributed to Chandan K. Mishra.

5 recordsLinked to original sources

arXiv2024

Pinned Ad-colloids Disfavors Nucleation in Colloidal Vapor Deposition

Crystallization through vapor deposition is ubiquitous, and is inevitably influenced by impurities, which often impact the local structure. Interestingly, the effect of immobilizing some of the depositing particles themselves, which would still preserve local structural symmetry, remains largely unexplored. Herein, we perform colloidal vapor deposition on a substrate with a few pinned ad-colloids, termed "mobility impurities". Through thermodynamic and kinematic measurements, we demonstrate that these pinned ad-colloids, even though they share identical geometry and interaction with depositing particles, are disfavored as nucleation centers. We reveal that entropic contributions, rather than energetic ones, govern nucleation physics in the presence of mobility impurities. Moreover, tuning the mobility of colloids on the substrate adjusts the nucleation likelihood at pinned sites. In later stages of growth, pinning induces mode localization and alters the thin film's vibrational spectrum. Our work, thus, underscores the potential of strategically incorporating mobility impurities to engineer material properties.

cond-mat.soft↗

arXiv2024

Anisotropic Cage Evolution in Quasi-two-dimensional Colloidal Fluids

We experimentally explore the morphological evolution of cages in quasi-two-dimensional suspensions of colloidal fluids, uncovering a complex dynamic restructuring in the fluid. Although cages display isotropic evolution in the laboratory frame, we observe a striking anisotropy when analyzed in the displacement frame of the caged particles. Moreover, our findings reveal that particles in specific but distinct regions of the cage predominantly contribute to either its persistence or relaxation. Thus, our study provides a coarse-grained microscopic picture of the structural relaxation of these fluids through cage evolution, which has broader implications for the flow and phase behavior of complex fluids in confined geometry.

cond-mat.soft↗

arXiv2023

Direction-dependent Dynamics of Colloidal Particle Pairs and the Stokes-Einstein Relation in Quasi-Two-Dimensional Fluids

Hydrodynamic interactions are important for diverse fluids especially those with low Reynold's number such as microbial and particle-laden suspensions, and proteins diffusing in membranes. Unfortunately, while far-field (asymptotic) hydrodynamic interactions are fully understood in two- and three-dimensions, near-field interactions are not, and thus our understanding of motions in dense fluid suspensions is still lacking. In this contribution, we experimentally explore the hydrodynamic correlations between particles in quasi-two-dimensional colloidal fluids in the near-field. Surprisingly, the measured displacement and relaxation of particle pairs in the body frame exhibit direction-dependent dynamics that can be connected quantitatively to the measured near-field hydrodynamic interactions. These findings, in turn, suggest a mechanism for how and when hydrodynamics can lead to a breakdown of the ubiquitous Stokes-Einstein relation (SER). We observe this breakdown, and interestingly, we show that the direction-dependent breakdown of the SER is ameliorated along directions where hydrodynamic correlations are smallest. In total, the work uncovers significant ramifications of near-field hydrodynamics on transport and dynamic restructuring of fluids in two-dimensions.

cond-mat.soft↗

arXiv2019

Long-wavelength fluctuations and anomalous dynamics in two-dimensional liquids

Long-wavelength Mermin-Wagner fluctuations prevent the existence of translational long-range order, in two-dimensional systems at finite temperature. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids and washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperature. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics does not reveal a transient solid-like response. In this regime, they induce an unusual but ubiquitous decoupling between long-time diffusion coefficient $D$ and structural relaxation time $τ$, where $D\propto τ^{-κ}$, with $κ> 1$. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures, in molecular liquids, or extremely low densities, in colloidal systems.

cond-mat.soft↗

arXiv2014

Dynamical facilitation governs glassy dynamics in suspensions of colloidal ellipsoids

One of the greatest challenges in contemporary condensed matter physics is to ascertain whether the formation of glasses from liquids is fundamentally thermodynamic or dynamic in origin. While the thermodynamic paradigm has dominated theoretical research for decades, the purely kinetic perspective of the dynamical facilitation (DF) theory has attained prominence in recent times. In particular, recent experiments and simulations have highlighted the importance of facilitation using simple model systems composed of spherical particles. However, an overwhelming majority of liquids possess anisotropy in particle shape and interactions and it is therefore imperative to examine facilitation in complex glass-formers. Here, we apply the DF theory to systems with orientational degrees of freedom as well as anisotropic attractive interactions. By analyzing data from experiments on colloidal ellipsoids, we show that facilitation plays a pivotal role in translational as well as orientational relaxation. Further, we demonstrate that the introduction of attractive interactions leads to spatial decoupling of translational and rotational facilitation, which subsequently results in the decoupling of dynamical heterogeneities. Most strikingly, the DF theory can predict the existence of reentrant glass transitions based on the statistics of localized dynamical events, called excitations, whose duration is substantially smaller than the structural relaxation time. Our findings pave the way for systematically testing the DF approach in complex glass-formers and also establish the significance of facilitation in governing structural relaxation in supercooled liquids.

cond-mat.soft↗