Publications
14 results found
Bresme F, Olarte-Plata JD, Chapman A, et al., 2022, Thermophoresis and thermal orientation of Janus nanoparticles in thermal fields, The European Physical Journal E: soft Matter and Biological Physics, Vol: 45, ISSN: 1292-8941
Thermal fields provide a route to control the motion of nanoparticles and molecules and potentially modify the behaviour of soft matter systems. Janus nanoparticles have emerged as versatile building blocks for the self-assembly of materials with novel properties. Here we investigate using non-equilibrium molecular dynamics simulations the behaviour of coarse-grained models of Janus nanoparticles under thermal fields. We examine the role of the heterogeneous structure of the particle on the Soret coefficient and thermal orientation by studying particles with different internal structures, mass distribution, and particle–solvent interactions. We also examine the thermophoretic response with temperature, targeting liquid and supercritical states and near-critical conditions. We find evidence for a significant enhancement of the Soret coefficient near the critical point, leading to the complete alignment of a Janus particle in the thermal field. This behaviour can be modelled and rationalized using a theory that describes the thermal orientation with the nanoparticle Soret coefficient, the mass and interaction anisotropy of the Janus nanoparticle, and the thermal field’s strength. Our simulations show that the mass anisotropy plays a crucial role in driving the thermal orientation of the Janus nanoparticles.
González-Colsa J, Olarte-Plata JD, Bresme F, et al., 2022, Enhanced thermo-optical response by means of anapole excitation., Journal of Physical Chemistry Letters, Vol: 13, Pages: 6230-6235, ISSN: 1948-7185
High refractive index (HRI) dielectric nanostructures offer a versatile platform to control the light-matter interaction at the nanoscale as they can easily support electric and magnetic modes with low losses. An additional property that makes them extraordinary is that they can support low radiative modes, so-called anapole modes. In this work, we propose a spectrally tunable anapole nanoheater based on the use of a dielectric anapole resonator. We show that a gold ring nanostructure, a priori nonresonant, can be turned into a resonant unit by just filling its hole with an HRI material supporting anapole modes, resulting in a more efficient nanoheater able to amplify the photothermal response of the bare nanoring. As proof of concept, we perform a detailed study of the thermoplasmonic response of a gold nanoring used as heating source and a silicon disk, designed to support anapole modes, located in its center acting as an anapolar resonator. Furthermore, we utilize the anapole excitation to easily shift the thermal response of these structures from the shortwave infrared range to the near-infrared range.
Olarte-Plata JD, Bresme F, 2022, Thermal conductance of the water-gold interface: the impact of the treatment of surface polarization in non-equilibrium molecular simulations., Journal of Chemical Physics, Vol: 156, Pages: 204701-204701, ISSN: 0021-9606
Interfacial thermal conductance (ITC) quantifies heat transport across material-fluid interfaces. It is a property of crucial importance to study heat transfer processes at both macro- and nanoscales. Therefore, it is essential to accurately model the specific interactions between solids and liquids. Here, we investigate the thermal conductance of gold-water interfaces using polarizable and non-polarizable models. Both models have been fitted to reproduce the interfacial tension of the gold-water interface, but they predict significantly different ITCs. We demonstrate that the treatment of polarization using Drude-like models, widely employed in molecular simulations, leads to a coupling of the solid and liquid vibrational modes that give rise to a significant overestimation of the ITCs. We analyze the dependence of the vibrational coupling with the mass of the Drude particle and propose a solution to the artificial enhancement of the ITC, preserving at the same time the polarization response of the solid. Based on our calculations, we estimate ITCs of 200 MW/(m2 K) for the water-gold interface. This magnitude is comparable to that reported recently for gold-water interfaces [279 ± 16 MW/(m2 K)] using atomic fluctuating charges to account for the polarization contribution.
Jiang M, Olarte-Plata JD, Bresme F, 2022, Heterogeneous thermal conductance of nanoparticle-fluid interfaces: An atomistic nodal approach, Journal of Chemical Physics, Vol: 156, ISSN: 0021-9606
The Interfacial Thermal Conductance (ITC) is a fundamental property of materials and has particular relevance at the nanoscale. The ITC quantifies the thermal resistance between materials of different compositions or between fluids in contact with materials. Furthermore, the ITC determines the rate of cooling/heating of the materials and the temperature drop across the interface. Here, we propose a method to compute local ITCs and temperature drops of nanoparticle–fluid interfaces. Our approach resolves the ITC at the atomic level using the atomic coordinates of the nanomaterial as nodes to compute local thermal transport properties. We obtain high-resolution descriptions of the interfacial thermal transport by combining the atomistic nodal approach, computational geometry techniques, and “computational farming” using non-equilibrium molecular dynamics simulations. We use our method to investigate the ITC of nanoparticle–fluid interfaces as a function of the nanoparticle size and geometry, targeting experimentally relevant structures of gold nanoparticles: capped octagonal rods, cuboctahedrons, decahedrons, rhombic dodecahedrons, cubes, icosahedrons, truncated octahedrons, octahedrons, and spheres. We show that the ITC of these very different geometries varies significantly in different regions of the nanoparticle, increasing generally in the order face < edge < vertex. We show that the ITC of these complex geometries can be accurately described in terms of the local coordination number of the atoms in the nanoparticle surface. Nanoparticle geometries with lower surface coordination numbers feature higher ITCs, and the ITC generally increases with the decreasing particle size
Olarte-Plata JD, Bresme F, 2022, The impact of the thermostats on the non-equilibrium computer simulations of the interfacial thermal conductance, Molecular Simulation, Vol: 48, Pages: 87-98, ISSN: 0892-7022
Non-equilibrium molecular dynamics simulations have expanded our ability to investigate interfacial thermal transport and quantify the interfacial thermal conductance (ITC) across solid and fluid interfaces. NEMD studies have highlighted the importance of interfacial degrees of freedom and the need to include effects beyond traditional theoretical methods that rely on bulk properties. NEMD simulations often use explicit hot and cold thermostats to set up thermal gradients. We analyse here the impact of the thermostat on the calculated ITC of the gold-water interface. We employ a polarisable model for gold based on Drude oscillators. We show that the ‘local’ Langevin thermostat modifies the vibrational density of states of the polarisable solid, resulting in ITCs that depend very strongly on the damping constant of the thermostat. We report an increase of the ITC of up to 40% for short damping times. Damping times longer than the characteristic heat flux relaxation time of the solid lead to converging ITCs. In contrast, the ITCs obtained with global canonical velocity rescale thermostats are independent of the damping time but lead to a break of equipartition for Drude particles. Setting individual thermostats for the core and shell sites in the Drude particle solves this problem.
Olarte-Plata JD, Gabriel J, Albella P, et al., 2021, Spatial control of heat flow at the nanoscale using Janus Particles., ACS Nano, Vol: 16
Janus nanoparticles (JNPs) feature heterogeneous compositions, bringing opportunities in technological and medical applications. We introduce a theoretical approach based on nonequilibrium molecular dynamics simulations and heat transfer continuum theory to investigate the temperature fields generated around heated spherical JNPs covering a wide range of particle sizes, from a few nm to 100 nm. We assess the performance of these nanoparticles to generate anisotropic heating at the nanoscale. We demonstrate that the contrasting interfacial thermal conductances of the fluid-material interfaces arising from the heterogeneous composition of the JNPs can be exploited to control the thermal fields around the nanoparticle, leading to a temperature difference between both sides of the nanoparticle (temperature contrast) that is significant for particles comprising regions with disparate hydrophilicity. We illustrate this idea using coarse-grained and atomistic models of gold nanoparticles with hydrophobic and hydrophilic coatings, in water. Furthermore, we introduce a continuum model to predict the temperature contrast as a function of the interfacial thermal conductance and nanoparticle size. We further show that, unlike homogeneous nanoparticles, the interfacial fluid temperature depends on the interfacial thermal conductance of Janus nanoparticles.
Olarte-Plata JD, Brekke-Svaland G, Bresme F, 2020, The influence of surface roughness on the adhesive interactions and phase behavior of suspensions of calcite nanoparticles, Publisher: ROYAL SOC CHEMISTRY
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Olarte-Plata JD, Bresme F, 2020, Orientation of Janus particles under thermal fields: The role of internal mass anisotropy., Journal of Chemical Physics, Vol: 152, Pages: 204902-204902, ISSN: 0021-9606
Janus particles (JPs) are a special kind of colloids that incorporate two hemispheres with distinct physical properties. These particles feature a complex phase behavior, and they can be propelled with light by heating them anisotropically when one of the hemispheres is metallic. It has been shown that JPs can be oriented by a homogeneous thermal field. We show using multiscale simulations and theory that the internal mass gradient of the JPs can enhance and even reverse the relative orientation of the particle with the thermal field. This effect is due to a coupling of the internal anisotropy of the particle with the heat flux. Our results help rationalize previous experimental observations and open a route to control the behavior of JPs by exploiting the synergy of particle-fluid interactions and particle internal mass composition.
Olarte-Plata JD, Brekke-Svaland G, Bresme F, 2020, The influence of surface roughness on the adhesive interactions and phase behavior of suspensions of calcite nanoparticles., Nanoscale, Vol: 12, Pages: 11165-11173, ISSN: 2040-3364
We investigate the impact of nanoparticle roughness on the phase behaviour of suspensions in models of calcium carbonate nanoparticles. We use a Derjaguin approach that incorporates roughness effects and interactions between the nanoparticles modelled with a combination of DLVO forces and hydration forces, derived using experimental data and atomistic molecular dynamics simulations, respectively. Roughness effects, such as atomic steps or terraces appearing in mineral surfaces result in very different effective inter-nanoparticle potentials. Using stochastic Langevin Dynamics computer simulations and the effective interparticle interactions we demonstrate that relatively small changes in the roughness of the particles modify significantly the stability of the suspensions. We propose that the sensitivity of the phase behavior to the roughness is connected to the short length scale of the adhesive attraction arising from the ordering of water layers confined between calcite surfaces. Particles with smooth surfaces feature strong adhesive forces, and form gel fractal structures, while small surface roughness, of the order of atomic steps in mineral faces, stabilize the suspension. We believe that our work helps to rationalize the contrasting experimental results that have been obtained recently using nanoparticles or extended surfaces, which provide support for the existence of adhesive or repulsive interactions, respectively. We further use our model to analyze the synergistic effects of roughness, pH and ion concentration on the phase behavior of suspensions, connecting with recent experiments using calcium carbonate nanoparticles.
Gittus OR, Olarte-Plata JD, Bresme F, 2019, Thermal orientation and thermophoresis of anisotropic colloids: the role of the internal composition, European Physical Journal E, Vol: 42, ISSN: 1292-8941
The drift motion experienced by colloids immersed in a fluid with an intrinsic temperature gradient is referred to as thermophoresis. An anisotropic mass distribution inside colloidal particles imparts a net orientation with respect to the applied thermal field, and in turn alters the thermophoretic response of the colloids. This rectification of the rotational Brownian motion is called thermal orientation. To explore the sensitivity of the thermal orientation effect with the internal composition of colloids, we investigate the thermophoretic response of rod-like colloids in the dilute regime, targeting different internal mass distributions. We derive phenomenological equations to model the dependence of the Soret coefficient with degree of mass anisotropy and test these equations using non-equilibrium molecular dynamics simulations. Using both theory and simulation, we show that the average orientation and the Soret coefficients of the colloids can depend significantly on the internal mass distribution. This observation suggests an approach to identify internal colloidal compositions using thermal gradients as sensing probes.
Olarte-Plata JD, Bresme F, 2019, Theoretical description of the thermomolecular orientation of anisotropic colloids, Physical Chemistry Chemical Physics, Vol: 21, Pages: 1131-1140, ISSN: 1463-9076
Thermal fields bring new opportunities to manipulate colloidal suspensions. Mass anisotropy inside the colloid leads to the thermal orientation effect and to a non-monotonic dependence of the thermophoretic force with the mass of the colloid. We show here that the thermal orientation of these anisotropic colloids can be described using the von Mises probability distribution. We derive equations that link the orientation to the internal degrees of freedom of the colloid, and test these equations using both atomistic and mesoscopic stochastic rotation dynamics simulations. Our approach can be used to describe the thermophoretic response of anisotropic colloids as a function of their size and composition.
Olarte-Plata J, Rubi JM, Bresme F, 2018, Thermophoretic torque in colloidal particles with mass asymmetry, Physical Review E, Vol: 97, ISSN: 1539-3755
We investigate the response of anisotropic colloids suspended in a fluid under a thermal field. Using nonequilibrium molecular dynamics computer simulations and nonequilibrium thermodynamics theory, we show that an anisotropic mass distribution inside the colloid rectifies the rotational Brownian motion and the colloids experience transient torques that orient the colloid along the direction of the thermal field. This physical effect gives rise to distinctive changes in the dependence of the Soret coefficient with colloid mass, which features a maximum, unlike the monotonic increase of the thermophoretic force with mass observed in homogeneous colloids.
Olarte-Plata JD, Bresme F, 2018, Microscopic relationship between colloid-colloid interactions and the rheological behaviour of suspensions: a molecular dynamics-stochastic rotation dynamics investigation, MOLECULAR PHYSICS, Vol: 116, Pages: 2032-2040, ISSN: 0026-8976
We investigate the dependence of the shear viscosity of suspensions of spherical colloids as a function of the volume fraction of the suspension, the colloid–colloid interactions and the shear rate. We couple molecular dynamics to describe the motion of the colloids with stochastic rotation dynamics (MD–SRD) for the fluid environment by means of stochastic collisions, in order to incorporate hydrodynamics effects leading to non-newtonian responses. The shear viscosity is computed using non-equilibrium simulations by imposing explicit velocity gradients. The impact of the colloid–colloid interactions is examined by modelling the inter-colloid pair potential with a repulsive power law, that allows interpolating different degrees of colloidal softness. The general rheological behaviour of our suspensions can be described with a Krieger–Dougherty like equation, which must be corrected to account for the variations in the maximum packing fraction and non-equilibrium effects arising from the flux of momentum imposed to the suspension, which appear when varying the softness of the inter-colloidal interactions. We further show evidence for non-newtonian behaviour at high Péclet numbers, characterised both by shear thinning and shear thickening, and thus demonstrate these effects can be successfully captured using MD–SRD methods.
Olarte-Plata JD, Haddad N, Vaillant C, et al., 2016, The folding landscape of the epigenome, PHYSICAL BIOLOGY, Vol: 13, ISSN: 1478-3967
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- Citations: 20
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