Chandan Kumar Mishra - Academia.edu (original) (raw)
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Papers by Chandan Kumar Mishra
Nature Communications
Hydrodynamic interactions are important for diverse fluids, especially those with low Reynolds nu... more Hydrodynamic interactions are important for diverse fluids, especially those with low Reynolds 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 we show that t...
Physical Review E, 2019
Spatiotemporal dynamics of short-and long-time structural relaxation are measured experimentally ... more Spatiotemporal dynamics of short-and long-time structural relaxation are measured experimentally as a function of packing fraction, φ, in quasi-two-dimensional colloidal supercooled liquids and glasses. The relaxation times associated with long-time dynamic heterogeneity and short-time intracage motion are found to be strongly correlated and to grow by orders of magnitude with increasing φ towards dynamic arrest. We find that clusters of fast particles on the two timescales often overlap, and, interestingly, the distribution of minimum-spatial-separation between closest non-overlapping clusters across the two timescales is revealed to be exponential with a decay length that increases with φ. In total, the experimental observations suggest short-time relaxation events are very often precursors to heterogeneous relaxation at longer timescales in glassy materials.
Physical Review Letters, 2015
We examine the role of shape of dynamical heterogeneities on the validity of the Stokes-Einstein ... more We examine the role of shape of dynamical heterogeneities on the validity of the Stokes-Einstein (SE) and Stokes-Einstein-Debye (SED) relations in quasi-two-dimensional suspensions of colloidal ellipsoids. For ellipsoids with repulsive interactions, although the orientational relaxation time remains coupled to the structural one, the SED relation by the Einstein formalism shows a breakdown. Strikingly, we find that it is the change in the shape of the dynamical heterogeneities from string-like to compact and not just their presence that results in the breakdown of both the SE and SED relations. On introducing a short-range depletion attraction between the ellipsoids, associated with the lack of morphological evolution of dynamical heterogeneities, the SE and SED relations remain valid even for deep supercooling. Our observations are consistent with numerical predictions.
Proceedings of the National Academy of Sciences of the United States of America, Jan 28, 2014
One of the greatest challenges in contemporary condensed matter physics is to ascertain whether t... more 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. Although 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 orientationa...
Physical Review Letters, 2013
We study experimentally the glass transition dynamics in quasi-two-dimensional suspensions of col... more We study experimentally the glass transition dynamics in quasi-two-dimensional suspensions of colloidal ellipsoids, aspect ratio ¼ 2:1, with repulsive as well as attractive interactions. For the purely repulsive case, we find that the orientational and translational glass transitions occur at the same area fraction. Strikingly, for intermediate depletion attraction strengths, we find that the orientational glass transition precedes the translational one. By quantifying structure and dynamics, we show that quasi-longrange ordering is promoted at these attraction strengths, which subsequently results in a two-step glass transition. Most interestingly, within experimental certainty, we observe reentrant glass dynamics only in the translational degrees of freedom.
Proceedings of the National Academy of Sciences of the United States of America, Oct 25, 2016
The monomer surface mobility is the single most important parameter that decides the nucleation d... more The monomer surface mobility is the single most important parameter that decides the nucleation density and morphology of islands during thin-film growth. During template-assisted surface growth in particular, low surface mobilities can prevent monomers from reaching target sites and this results in a partial to complete loss of nucleation control. Whereas in atomic systems a broad range of surface mobilities can be readily accessed, for colloids, owing to their large size, this window is substantially narrow and therefore imposes severe restrictions in extending template-assisted growth techniques to steer their self-assembly. Here, we circumvented this fundamental limitation by designing templates with spatially varying feature sizes, in this case moiré patterns, which in the presence of short-range depletion attraction presented surface energy gradients for the diffusing colloids. The templates serve a dual purpose: first, directing the particles to target sites by enhancing thei...
Nature Communications
Hydrodynamic interactions are important for diverse fluids, especially those with low Reynolds nu... more Hydrodynamic interactions are important for diverse fluids, especially those with low Reynolds 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 we show that t...
Physical Review E, 2019
Spatiotemporal dynamics of short-and long-time structural relaxation are measured experimentally ... more Spatiotemporal dynamics of short-and long-time structural relaxation are measured experimentally as a function of packing fraction, φ, in quasi-two-dimensional colloidal supercooled liquids and glasses. The relaxation times associated with long-time dynamic heterogeneity and short-time intracage motion are found to be strongly correlated and to grow by orders of magnitude with increasing φ towards dynamic arrest. We find that clusters of fast particles on the two timescales often overlap, and, interestingly, the distribution of minimum-spatial-separation between closest non-overlapping clusters across the two timescales is revealed to be exponential with a decay length that increases with φ. In total, the experimental observations suggest short-time relaxation events are very often precursors to heterogeneous relaxation at longer timescales in glassy materials.
Physical Review Letters, 2015
We examine the role of shape of dynamical heterogeneities on the validity of the Stokes-Einstein ... more We examine the role of shape of dynamical heterogeneities on the validity of the Stokes-Einstein (SE) and Stokes-Einstein-Debye (SED) relations in quasi-two-dimensional suspensions of colloidal ellipsoids. For ellipsoids with repulsive interactions, although the orientational relaxation time remains coupled to the structural one, the SED relation by the Einstein formalism shows a breakdown. Strikingly, we find that it is the change in the shape of the dynamical heterogeneities from string-like to compact and not just their presence that results in the breakdown of both the SE and SED relations. On introducing a short-range depletion attraction between the ellipsoids, associated with the lack of morphological evolution of dynamical heterogeneities, the SE and SED relations remain valid even for deep supercooling. Our observations are consistent with numerical predictions.
Proceedings of the National Academy of Sciences of the United States of America, Jan 28, 2014
One of the greatest challenges in contemporary condensed matter physics is to ascertain whether t... more 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. Although 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 orientationa...
Physical Review Letters, 2013
We study experimentally the glass transition dynamics in quasi-two-dimensional suspensions of col... more We study experimentally the glass transition dynamics in quasi-two-dimensional suspensions of colloidal ellipsoids, aspect ratio ¼ 2:1, with repulsive as well as attractive interactions. For the purely repulsive case, we find that the orientational and translational glass transitions occur at the same area fraction. Strikingly, for intermediate depletion attraction strengths, we find that the orientational glass transition precedes the translational one. By quantifying structure and dynamics, we show that quasi-longrange ordering is promoted at these attraction strengths, which subsequently results in a two-step glass transition. Most interestingly, within experimental certainty, we observe reentrant glass dynamics only in the translational degrees of freedom.
Proceedings of the National Academy of Sciences of the United States of America, Oct 25, 2016
The monomer surface mobility is the single most important parameter that decides the nucleation d... more The monomer surface mobility is the single most important parameter that decides the nucleation density and morphology of islands during thin-film growth. During template-assisted surface growth in particular, low surface mobilities can prevent monomers from reaching target sites and this results in a partial to complete loss of nucleation control. Whereas in atomic systems a broad range of surface mobilities can be readily accessed, for colloids, owing to their large size, this window is substantially narrow and therefore imposes severe restrictions in extending template-assisted growth techniques to steer their self-assembly. Here, we circumvented this fundamental limitation by designing templates with spatially varying feature sizes, in this case moiré patterns, which in the presence of short-range depletion attraction presented surface energy gradients for the diffusing colloids. The templates serve a dual purpose: first, directing the particles to target sites by enhancing thei...