Non-additivity of van der Waals forces on liquid surfaces

We present an approach for modeling nanoscale wetting and dewetting of liquid surfaces that exploits recently developed, sophisticated techniques for computing van der Waals (vdW) or (more generally) Casimir forces in arbitrary geometries. We solve the variational formulation of the Young--Laplace equation to predict the equilibrium shapes of fluid--vacuum interfaces near solid gratings and show that the non-additivity of vdW interactions can have a significant impact on the shape and wetting properties of the liquid surface, leading to very different surface profiles and wetting transitions compared to predictions based on commonly employed additive approximations, such as Hamaker or Derjaguin approximations.Comment: 5 pages (including abstract, acknowledgments, and references), 3 figure

Fluctuational Electrodynamics in Atomic and Macroscopic Systems: van der Waals Interactions and Radiative Heat Transfer

We present an approach to describing fluctuational electrodynamic (FED) interactions, particularly van der Waals (vdW) interactions as well as radiative heat transfer (RHT), between material bodies of vastly different length scales, allowing for going between atomistic and continuum treatments of the response of each of these bodies as desired. Any local continuum description of electromagnetic (EM) response is compatible with our approach, while atomistic descriptions in our approach are based on effective electronic and nuclear oscillator degrees of freedom, encapsulating dissipation, short-range electronic correlations, and collective nuclear vibrations (phonons). While our previous works using this approach have focused on presenting novel results, this work focuses on the derivations underlying these methods. First, we show how the distinction between "atomic" and "macroscopic" bodies is ultimately somewhat arbitrary, as formulas for vdW free energies and RHT look very similar regardless of how the distinction is drawn. Next, we demonstrate that the atomistic description of material response in our approach yields EM interaction matrix elements which are expressed in terms of analytical formulas for compact bodies or semianalytical formulas based on Ewald summation for periodic media; we use this to compute vdW interaction free energies as well as RHT powers among small biological molecules in the presence of a metallic plate as well as between parallel graphene sheets in vacuum, showing strong deviations from conventional macroscopic theories due to the confluence of geometry, phonons, and EM retardation effects. Finally, we propose formulas for efficient computation of FED interactions among material bodies in which those that are treated atomistically as well as those treated through continuum methods may have arbitrary shapes, extending previous surface-integral techniques.Comment: 25 pages, 5 figures, 2 appendice

Impact of nuclear vibrations on van der Waals and Casimir interactions at zero and finite temperature

Van der Waals (vdW) and Casimir interactions depend crucially on material properties and geometry, especially at molecular scales, and temperature can produce noticeable relative shifts in interaction characteristics. Despite this, common treatments of these interactions ignore electromagnetic retardation, atomism, or contributions of collective mechanical vibrations (phonons) to the infrared response, which can interplay with temperature in nontrivial ways. We present a theoretical framework for computing electromagnetic interactions among molecular structures, accounting for their geometry, electronic delocalization, short-range interatomic correlations, dissipation, and phonons at atomic scales, along with long-range electromagnetic interactions among themselves or in the vicinity of continuous macroscopic bodies. We find that in carbon allotropes, particularly fullerenes, carbyne wires, and graphene sheets, phonons can couple strongly with long-range electromagnetic fields, especially at mesoscopic scales (nanometers), to create delocalized phonon polaritons that significantly modify the infrared molecular response. These polaritons especially depend on the molecular dimensionality and dissipation, and in turn affect the vdW interaction free energies of these bodies above a macroscopic gold surface, producing nonmonotonic power laws and nontrivial temperature variations at nanometer separations that are within the reach of current Casimir force experiments.Comment: 11 pages, 4 figures (3 single-column, 1 double-column), 2 appendice

Mechanical relations between conductive and radiative heat transfer

We present a general nonequilibrium Green's function formalism for modeling heat transfer in systems characterized by linear response that establishes the formal algebraic relationships between phonon and radiative conduction, and reveals how upper bounds for the former can also be applied to the latter. We also propose an extension of this formalism to treat systems susceptible to the interplay of conductive and radiative heat transfer, which becomes relevant in atomic systems and at nanometric and smaller separations where theoretical descriptions which treat each phenomenon separately may be insufficient. We illustrate the need for such coupled descriptions by providing predictions for a low-dimensional system of carbyne wires in which the total heat transfer can differ from the sum of its radiative and conductive contributions. Our framework has ramifications for understanding heat transfer between large bodies that may approach direct contact with each other or that may be coupled by atomic, molecular, or interfacial film junctions.Comment: 16 pages, 2 figures, 1 table, 2 appendice

T\mathbb{T}-operator bounds on angle-integrated absorption and thermal radiation for arbitrary objects

We derive fundamental per-channel bounds on angle-integrated absorption and thermal radiation for arbitrary bodies---for any given material susceptibility and bounding region---that simultaneously encode both the per-volume limit on polarization set by passivity and geometric constraints on radiative efficiencies set by finite object sizes through the scattering $\mathbb{T}$-operator. We then analyze these bounds in two practical settings, comparing against prior limits as well as near optimal structures discovered through topology optimization. Principally, we show that the bounds properly capture the physically observed transition from the volume scaling of absorptivity seen in deeply subwavelength objects (nanoparticle radius or thin film thickness) to the area scaling of absorptivity seen in ray optics (blackbody limits).Comment: 9 pages including appendices, 2 figures, 1 tabl

Fundamental limits to attractive and repulsive Casimir--Polder forces

We derive upper and lower bounds on the Casimir--Polder force between an anisotropic dipolar body and a macroscopic body separated by vacuum via algebraic properties of Maxwell's equations. These bounds require only a coarse characterization of the system---the material composition of the macroscopic object, the polarizability of the dipole, and any convenient partition between the two objects---to encompass all structuring possibilities. We find that the attractive Casimir--Polder force between a polarizable dipole and a uniform planar semi-infinite bulk medium always comes within 10% of the lower bound, implying that nanostructuring is of limited use for increasing attraction. In contrast, the possibility of repulsion is observed even for isotropic dipoles, and is routinely found to be several orders of magnitude larger than any known design, including recently predicted geometries involving conductors with sharp edges. Our results have ramifications for the design of surfaces to trap, suspend, or adsorb ultracold gases.Comment: 6 pages, 3 figure

Fundamental limits to radiative heat transfer: theory

Near-field radiative heat transfer between bodies at the nanoscale can surpass blackbody limits on thermal radiation by orders of magnitude due to contributions from evanescent electromagnetic fields, which carry no energy to the far-field. Thus far, principles guiding explorations of larger heat transfer beyond planar structures have assumed utility in surface nanostructuring, which can enhance the density of states, and further assumed that such design paradigms can approach Landauer limits, in analogy to conduction. We derive fundamental shape-independent limits to radiative heat transfer, applicable in near- through far-field regimes, that incorporate material and geometric constraints such as intrinsic dissipation and finite object sizes, and show that these preclude reaching the Landauer limits in all but a few restrictive scenarios. Additionally, we show that the interplay of material response and electromagnetic scattering among proximate bodies means that bodies which maximize radiative heat transfer actually maximize scattering rather than absorption. Finally, we compare our new bounds to existing Landauer limits, as well as limits involving bodies maximizing far-field absorption, and show that these lead to overly optimistic predictions. Our results have ramifications for the ultimate performance of thermophotovoltaics and nanoscale cooling, as well as related incandescent and luminescent devices.Comment: 12 pages including appendices, 1 figure; SM and PSV contributed equall

Phonon-polariton mediated thermal radiation and heat transfer among molecules and macroscopic bodies: nonlocal electromagnetic response at mesoscopic scales

Thermal radiative phenomena can be strongly influenced by the coupling of phonons and long-range electromagnetic fields at infrared frequencies. Typically employed macroscopic descriptions of thermal fluctuations tend to ignore atomistic effects that become relevant at nanometric scales, whereas purely microscopic treatments ignore long-range, geometry-dependent electromagnetic effects. We describe a mesoscopic framework for modeling thermal fluctuation phenomena among molecules in the vicinity of macroscopic bodies, conjoining atomistic treatments of electronic and vibrational fluctuations obtained from ab-initio density functional theory in the former with continuum descriptions of electromagnetic scattering in the latter. The interplay of these effects becomes particularly important at mesoscopic scales, where phonon polaritons can be strongly influenced by the finite sizes, shapes, and non-local/many-body response of the bodies to electromagnetic fluctuations. We show that even in small but especially in elongated low-dimensional molecular systems, such effects can modify thermal emission and heat transfer by orders of magnitude and produce qualitatively different behavior compared to predictions based on local, dipolar, or pairwise approximations valid only in dilute media.Comment: 7 pages, 2 figures, includes supplement as appendi

Channel-based algebraic limits to conductive heat transfer

Recent experimental advances probing coherent phonon and electron transport in nanoscale devices at contact have motivated theoretical channel-based analyses of conduction based on the nonequilibrium Green's function formalism. The transmission through each channel has been known to be bounded above by unity, yet actual transmissions in typical systems often fall far below these limits. Building upon recently derived radiative heat transfer limits and a unified formalism characterizing heat transport for arbitrary bosonic systems in the linear regime, we propose new bounds on conductive heat transfer. In particular, we demonstrate that our limits are typically far tighter than the Landauer limits per channel and are close to actual transmission eigenvalues by examining a model of phonon conduction in a 1-dimensional chain. Our limits have ramifications for designing molecular junctions to optimize conduction.Comment: 10 pages, 2 figures, 2 appendice

Ayurveda and Epilepsy

This article does not have an abstract