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result(s) for
"Ganapathy, Rajesh"
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Tuning the performance of a micrometer-sized Stirling engine through reservoir engineering
2021
Colloidal heat engines are paradigmatic models to understand the conversion of heat into work in a noisy environment - a domain where biological and synthetic nano/micro machines function. While the operation of these engines across thermal baths is well-understood, how they function across baths with noise statistics that is non-Gaussian and also lacks memory, the simplest departure from the thermal case, remains unclear. Here we quantified the performance of a colloidal Stirling engine operating between an engineered memoryless non-Gaussian bath and a Gaussian one. In the quasistatic limit, the non-Gaussian engine functioned like a thermal one as predicted by theory. On increasing the operating speed, due to the nature of noise statistics, the onset of irreversibility for the non-Gaussian engine preceded its thermal counterpart and thus shifted the operating speed at which power is maximum. The performance of nano/micro machines can be tuned by altering only the nature of reservoir noise statistics.
Micro scale heat engines may be subjected to quite intriguing scenarios. Roy et al superimpose artificial random kicks on an optically trapped colloid, emulating a memoryless non-gaussian reservoir that markedly alters the conditions under which the engine performs at optimum efficiency.
Journal Article
Structure determines where crystallization occurs in a soft colloidal glass
2021
Glass is inherently unstable to crystallization. However, how this transformation occurs while the dynamics in the glass stay frozen at the particle scale is poorly understood. Here, through single-particle-resolved imaging experiments, we show that due to frozen-in density inhomogeneities, a soft colloidal glass crystallizes via two distinct pathways. In the poorly packed regions of the glass, crystallinity grew smoothly due to local particle shuffles, whereas in the well-packed regions, we observed abrupt jumps in crystallinity that were triggered by avalanches—cooperative rearrangements involving many tens of particles. Importantly, we show that softness—a structural-order parameter determined through machine-learning methods—not only predicts where crystallization initiates in a glass but is also sensitive to the crystallization pathway. Such a causal connection between the structure and stability of a glass has so far remained elusive. Devising strategies to manipulate softness may thus prove invaluable in realizing long-lived glassy states.Softness, a machine-learned structural quantity, has been recently identified as a parameter that characterizes glassy dynamics. Here, the authors observe devitrification in 3D soft colloidal glasses and find that softness may indicate regions predisposed to crystallization.
Journal Article
Cooperatively rearranging regions change shape near the mode-coupling crossover for colloidal liquids on a sphere
by
Singh, Navneet
,
Sood, A. K.
,
Ganapathy, Rajesh
in
639/301/923/218
,
639/301/923/916
,
639/766/119
2020
The structure and dynamics of liquids on curved surfaces are often studied through the lens of frustration-based approaches to the glass transition. Competing glass transition theories, however, remain largely untested on such surfaces and moreover, studies hitherto have been entirely theoretical/numerical. Here we carry out single particle-resolved imaging of dynamics of bi-disperse colloidal liquids confined to the surface of a sphere. We find that mode-coupling theory well captures the slowing down of dynamics in the moderate to deeply supercooled regime. Strikingly, the morphology of cooperatively rearranging regions changed from string-like to compact near the mode-coupling crossover—a prediction unique to the random first-order theory of glasses. Further, we find that in the limit of strong curvature, Mermin–Wagner long-wavelength fluctuations are irrelevant and liquids on a sphere behave like three-dimensional liquids. A comparative evaluation of competing mechanisms is thus an essential step towards uncovering the true nature of the glass transition.
The static and dynamic behavior of condensed phases residing on curved surfaces can be fundamentally different from their counterparts in Euclidean space. Singh et al. test several competing glass theories on colloidal liquids confined to the surface of a sphere and show they behave like 3D bulk liquids.
Journal Article
Overcoming power-efficiency tradeoff in a micro heat engine by engineered system-bath interactions
by
Sood, A. K.
,
Krishnamurthy, Sudeesh
,
Ganapathy, Rajesh
in
639/766/530/2804
,
639/766/530/951
,
Colloids
2023
All real heat engines, be it conventional macro engines or colloidal and atomic micro engines, inevitably tradeoff efficiency in their pursuit to maximize power. This basic postulate of finite-time thermodynamics has been the bane of all engine design for over two centuries and all optimal protocols implemented hitherto could at best minimize only the loss in the efficiency. The absence of a protocol that allows engines to overcome this limitation has prompted theoretical studies to suggest universality of the postulate in both passive and active engines. Here, we experimentally overcome the power-efficiency tradeoff in a colloidal Stirling engine by selectively reducing relaxation times over only the isochoric processes using system bath interactions generated by electrophoretic noise. Our approach opens a window of cycle times where the tradeoff is reversed and enables the engine to surpass even their quasistatic efficiency. Our strategies finally cut loose engine design from fundamental restrictions and pave way for the development of more efficient and powerful engines and devices.
The trade-off between power and efficiency in designing heat engines has remained unsolved for the last two centuries. The authors overcome this trade-off in a colloidal Stirling engine by electrophoretically inducing system-reservoir interactions to enhance heat transfer during an isochoric process.
Journal Article
Direct measurements of growing amorphous order and non-monotonic dynamic correlations in a colloidal glass-former
2015
As a liquid relaxes towards the glass transition, its dynamics is thought to become more cooperative. Experiments using holographic optical tweezers support a contested thermodynamic picture, claiming this cooperation involves morphology changes.
The transformation of flowing liquids into rigid glasses is thought to involve increasingly cooperative relaxation dynamics as the temperature approaches that of the glass transition. However, the precise nature of this motion is unclear, and a complete understanding of vitrification thus remains elusive. Of the numerous theoretical perspectives
1
,
2
,
3
,
4
devised to explain the process, random first-order theory (RFOT; refs
2
,
5
) is a well-developed thermodynamic approach, which predicts a change in the shape of relaxing regions as the temperature is lowered. However, the existence of an underlying ‘ideal’ glass transition predicted by RFOT remains debatable, largely because the key microscopic predictions concerning the growth of amorphous order and the nature of dynamic correlations lack experimental verification. Here, using holographic optical tweezers, we freeze a wall of particles in a two-dimensional colloidal glass-forming liquid and provide direct evidence for growing amorphous order in the form of a static point-to-set length. We uncover the non-monotonic dependence of dynamic correlations on area fraction and show that this non-monotonicity follows directly from the change in morphology and internal structure of cooperatively rearranging regions
6
,
7
. Our findings support RFOT and thereby constitute a crucial step in distinguishing between competing theories of glass formation.
Journal Article
A shape-driven reentrant jamming transition in confluent monolayers of synthetic cell-mimics
2024
Many critical biological processes, like wound healing, require densely packed cell monolayers/tissues to transition from a jammed solid-like to a fluid-like state. Although numerical studies anticipate changes in the cell shape alone can lead to unjamming, experimental support for this prediction is not definitive because, in living systems, fluidization due to density changes cannot be ruled out. Additionally, a cell’s ability to modulate its motility only compounds difficulties since even in assemblies of rigid active particles, changing the nature of self-propulsion has non-trivial effects on the dynamics. Here, we design and assemble a monolayer of synthetic cell-mimics and examine their collective behaviour. By systematically increasing the persistence time of self-propulsion, we discovered a cell shape-driven, density-independent, re-entrant jamming transition. Notably, we observed cell shape and shape variability were mutually constrained in the confluent limit and followed the same universal scaling as that observed in confluent epithelia. Dynamical heterogeneities, however, did not conform to this scaling, with the fast cells showing suppressed shape variability, which our simulations revealed is due to a transient confinement effect of these cells by their slower neighbors. Our experiments unequivocally establish a morphodynamic link, demonstrating that geometric constraints alone can dictate epithelial jamming/unjamming.
Living cell collectives can jam and unjam through many pathways, yet the details remain elusive. Arora et al. design a monolayer of deformable cell-mimics composed of chiral active granular ellipsoids confined in flexible paper rings and show a re-entrant jamming transition mediated solely by cell shape change.
Journal Article
Reentrant melting of scarred odd crystals by self-shear
2026
Spatial confinement can induce geometrical frustration in condensed phases, giving rise to topological defects that confer materials with new and exotic properties. Here, we experimentally uncover the effect of confinement-induced defect strings termed ‘grain boundary scars’ on the behavior of dense two-dimensional assemblies of granular spinners, a canonical odd elastic solid. The spatial arrangement of these scars fundamentally reshapes the flows triggered by chiral activity. Specifically, they cause the topologically protected edge flows - a ubiquitous feature of confined spinner assemblies - to decouple from the bulk. Strikingly, increasing the net chiral activity of the system by tuning the ratio of counterclockwise to clockwise spinners caused spontaneous self-shearing. The resulting odd radial stresses led to a chiral activity-mediated reentrant melting transition at a fixed areal spinner density. Our findings open new avenues for exploiting geometrical frustration to elicit novel responses from odd elastic solids.
Geometrical frustration in confined systems can lead to the emergence of topological defects, which significantly influence the physical properties of materials. This study demonstrates that grain boundary scars in dense assemblies of active spinners can decouple edge flows from the bulk, resulting in spontaneous self-shearing and a chiral activity-mediated reentrant melting transition.
Journal Article
Growing dynamical facilitation on approaching the random pinning colloidal glass transition
by
Gokhale, Shreyas
,
Hima Nagamanasa, K.
,
Sood, A. K.
in
Freezing
,
Humanities and Social Sciences
,
multidisciplinary
2014
Despite decades of research, it remains to be established whether the transformation of a liquid into a glass is fundamentally thermodynamic or dynamic in origin. Although observations of growing length scales are consistent with thermodynamic perspectives, the purely dynamic approach of the Dynamical Facilitation (DF) theory lacks experimental support. Further, for vitrification induced by randomly freezing a subset of particles in the liquid phase, simulations support the existence of an underlying thermodynamic phase transition, whereas the DF theory remains unexplored. Here, using video microscopy and holographic optical tweezers, we show that DF in a colloidal glass-forming liquid grows with density as well as the fraction of pinned particles. In addition, we observe that heterogeneous dynamics in the form of string-like cooperative motion emerges naturally within the framework of facilitation. Our findings suggest that a deeper understanding of the glass transition necessitates an amalgamation of existing theoretical approaches.
It remains a matter of debate whether the glass transition is thermodynamic or dynamic in nature. Here Gokhale
et al.
examine slow dynamics in a binary colloidal liquid and provide support for the dynamical facilitation approach–a purely dynamic theory of the glass transition.
Journal Article
Long-wavelength fluctuations and anomalous dynamics in 2-dimensional liquids
by
Li, Yan-Wei
,
Sun, Zhao-Yan
,
Ciamarra, Massimo Pica
in
Decoupling
,
Diffusion coefficient
,
Divergence
2019
In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature which is the divergence of the vibrational amplitude with the system size also affects disordered solids and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where D ∝ 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 at extremely low densities in colloidal systems.
Journal Article
Confined glassy dynamics at grain boundaries in colloidal crystals
by
Nagamanasa, K. Hima
,
Gokhale, Shreyas
,
Ganapathy, Rajesh
in
Colloids
,
confocal microscopy
,
crystallites
2011
Grain boundary (GB) microstructure and dynamics dictate the macroscopic properties of polycrystalline materials. Although GBs have been investigated extensively in conventional materials, it is only recently that molecular dynamics simulations have shown that GBs exhibit features similar to those of glass-forming liquids. However, current simulation techniques to probe GBs are limited to temperatures and driving forces much higher than those typically encountered in atomic experiments. Further, the short spatial and temporal scales in atomic systems preclude direct experimental access to GB dynamics. Here, we have used confocal microscopy to investigate the dynamics of high misorientation angle GBs in a three-dimensional colloidal polycrystal, with single-particle resolution, in the zero-driving force limit. We show quantitatively that glassy behavior is inherent to GBs as exemplified by the slowing down of particle dynamics due to transient cages formed by their nearest neighbors, non-Gaussian probability distribution of particle displacements and string-like cooperative rearrangements of particles. Remarkably, geometric confinement of the GB region by adjacent crystallites decreases with the misorientation angle and results in an increase in the size of cooperatively rearranging regions and hence the fragility of the glassy GBs.
Journal Article