A detailed understanding of the vibrational heat transfer mechanisms between solids is essential for the efficient thermal engineering and control of nanomaterials. We investigate the frequency dependence of anharmonic scattering and interfacial thermal conduction between two acoustically mismatched solids in planar contact by calculating the spectral decomposition of the heat current flowing through an interface between two materials. The calculations are based on analyzing the correlations of atomic vibrations using the data extracted from nonequilibrium molecular dynamics simulations. Inelastic effects arising from anharmonic interactions are shown to significantly facilitate heat transfer between two mass-mismatched face-centered-cubic lattices even at frequencies exceeding the cutoff frequency of the heavier material due to (i) enhanced dissipation of evanescent vibrational modes and (ii) frequency-doubling and frequency-halving three-phonon energy transfer processes at the interface. The results provide substantial insight into interfacial energy transfer mechanisms, especially at high temperatures, where inelastic effects become important and other computational methods are ineffective.

Conventional theories of electromagnetic waves in a medium assume that the energy propagating with the light pulse in the medium is entirely carried by the field. Thus, the possibility that the optical force field of the light pulse would drive forward an atomic mass density wave (MDW) and the related kinetic and elastic energies is neglected. In this work, we present foundations of a covariant theory of light propagation in a medium by considering a light wave simultaneously with the dynamics of the medium atoms driven by optoelastic forces between the induced dipoles and the electromagnetic field. We show that a light pulse having a total electromagnetic energy ω propagating in a nondispersive medium transfers a mass equal to δm = (n 2 −1) ω/c 2 , where n is the refractive index. MDW, which carries this mass, consists of atoms, which are more densely spaced inside the light pulse as a result of the field-dipole interaction. We also prove that the transfer of mass with the light pulse, the photon mass drag effect, gives an essential contribution to the total momentum of the light pulse, which becomes equal to the Minkowski momentum pM = n ω/c. The field's share of the momentum is the Abraham momentum pA = ω/(nc), while the difference pM − pA is carried by MDW. Due to the coupling of the field and matter, only the total momentum of the light pulse and the transferred mass δm can be directly measured. Thus, our theory gives an unambiguous physical meaning to the Abraham and Minkowski momenta. We also show that to solve the centenary Abraham-Minkowski controversy of the momentum of light in a nondispersive medium in a way that is consistent with Newton's first law, one must account for the mass transfer effect. We derive the photon mass drag effect using two independent but complementary covariant models. In the mass-polariton (MP) quasiparticle approach, we consider the light pulse as a coupled state between the photon and matter, isolated from the rest of the medium. The momentum and the transferred mass of MP follow unambiguously from the Lorentz invariance and the fundamental conservation laws of nature. To enable the calculation of the mass and momentum distribution of a light pulse, we have also generalized the electrodynamics of continuous media to account for the space-and time-dependent optoelastic dynamics of the medium driven by the field-dipole forces. In this optoelastic continuum dynamics (OCD) approach, we obtain with an appropriate space-time discretization a numerically accurate solution of the Newtonian continuum dynamics of the medium when the light pulse is propagating in it. The OCD simulations of a Gaussian light pulse propagating in a diamond crystal give the same momentum pM and the transferred mass δm for the light pulse as the MP quasiparticle approach. Our simulations also show that, after photon transmission, some nonequilibrium of the mass distribution is left in the medium. Since the elastic forces are included in our simulations on equal footing with the optical forces, our simulatio...

Owing to their long phonon mean free paths (MFPs) and high thermal conductivity, carbon nanotubes (CNTs) are ideal candidates for, e.g., removing heat from electronic devices. It is unknown, however, how the intrinsic phonon MFPs depend on vibrational frequency in non-equilibrium. We determine the spectrally resolved phonon MFPs in isotopically pure CNTs from the spectral phonon transmission function calculated using non-equilibrium molecular dynamics, fully accounting for the resistive phonon-phonon scattering processes through the anharmonic terms of the interatomic potential energy function. Our results show that the effective room temperature MFPs of low-frequency phonons (f < 0.5 THz) exceeds 10 µm, while the MFP of high-frequency phonons (f 20 THz) is in the range 10-100 nm. Because the determined MFPs directly reflect the resistance to energy flow, they can be used to accurately predict the thermal conductivity for arbitrary tube lengths by calculating a single frequency integral. The presented results and methods are expected to significantly improve the understanding of non-equilibrium thermal transport in low-dimensional nanostructures.

Thermal transport through liquid-solid interfaces plays an important role in many chemical and biological processes, and better understanding of liquid-solid energy transfer is expected to enable improving the efficiency of thermally driven applications. We determine the spectral distribution of thermal current at liquid-solid interfaces from nonequilibrium molecular dynamics, delivering a detailed picture of the contributions of different vibrational modes to liquid-solid energy transfer. Our results show that surface modes located at the Brillouin zone edge and polarized along the liquidsolid surface normal play a crucial role in liquid-solid energy transfer. Strong liquid-solid adhesion allows also for the coupling of in-plane polarized modes in the solid with the liquid, enhancing the heat transfer rate and enabling efficient energy transfer up to the cut-off frequency of the solid. Our results provide fundamental understanding of the energy transfer mechanisms in liquid-solid systems and enable detailed investigations of energy transfer between, e.g., water and organic molecules.

Modeling of thermal transport in practical nanostructures requires making trade-offs between the size of the system and the completeness of the model. We study quantum heat transfer in a selfconsistent thermal bath setup consisting of two lead regions connected by a center region. Atoms both in the leads and in the center region are coupled to quantum Langevin heat baths that mimic the damping and dephasing of phonon waves by anharmonic scattering. This approach treats the leads and the center region on same footing and thereby allows for a simple and physically transparent thermalization of the system, enabling also perfect acoustic matching between the leads and the center region. Increasing the strength of the coupling reduces the mean free path of phonons and gradually shifts phonon transport from ballistic regime to diffusive regime. In the center region, the bath temperatures are determined self-consistently from the requirement of zero net energy exchange between the local heat bath and each atom. By solving the stochastic equations of motion in frequency space and averaging over noise using the general fluctuation-dissipation relation derived by Dhar and Roy [J. Stat. Phys. 125, 801 (2006)], we derive the formula for thermal current, which contains the Caroli formula for phonon transmission function and reduces to the Landauer-Büttiker formula in the limit of vanishing coupling to local heat baths. We prove that the bath temperatures measure local kinetic energy and can, therefore, be interpreted as true atomic temperatures. In a setup where phonon reflections are eliminated, Boltzmann transport equation under gray approximation with full phonon dispersion is shown to be equivalent to the self-consistent heat bath model. We also study thermal transport through two-dimensional constrictions in square lattice and graphene and discuss the differences between the exact solution and linear approximations.

We discuss the ultimate limit of performance of semiconductor light-emitting diodes (LEDs) and its dependence on temperature. It is known that in high quality semiconductor materials it is, in principle, possible to reach wall plug efficiencies exceeding unity, which allows electroluminescent cooling in addition of very high efficiency light emission. Our simulation results suggest a few fairly simple measures that may further improve the external quantum efficiency (EQE) of LEDs toward the electroluminescent cooling limit. These include reducing the current density, modifying the LED structure by making thicker active regions and barrier layers, and doping of the active material. Our calculations also indicate that, contrary to the present understanding, operating LEDs at relatively high temperatures of 400–600 K may, in fact, improve the performance.

The quantization of the electromagnetic field in lossy and dispersive dielectric media has been widely studied during the last few decades. However, several aspects of energy transfer and its relation to consistently defining position-dependent ladder operators for the electromagnetic field in nonequilibrium conditions have partly escaped the attention. In this work we define the position-dependent ladder operators and an effective local photon-number operator that are consistent with the canonical commutation relations and use these concepts to describe the energy transfer and thermal balance in layered geometries. This approach results in a position-dependent photon-number concept that is simple and consistent with classical energy conservation arguments. The operators are formed by first calculating the vector potential operator using Green's function formalism and Langevin noise source operators related to the medium and its temperature, and then defining the corresponding position-dependent annihilation operator that is required to satisfy the canonical commutation relations in arbitrary geometry. Our results suggest that the effective photon number associated with the electric field is generally position dependent and enables a straightforward method to calculate the energy transfer rate between the field and the local medium. In particular, our results predict that the effective photon number in a vacuum cavity formed between two lossy material layers can oscillate as a function of the position suggesting that also the local field temperature oscillates. These oscillations are expected to be directly observable using relatively straightforward experimental setups in which the field-matter interaction is dominated by the coupling to the electric field

Harnessing the power of low-dimensional materials in thermal applications calls for a solid understanding of the anomalous thermal properties of such systems. We analyze thermal conduction in one-dimensional systems by determining the frequency-dependent phonon mean free paths (MFPs) for an anharmonic chain, delivering insight into the diverging thermal conductivity observed in computer simulations. In our approach, the MFPs are extracted from the length dependence of the spectral heat current obtained from nonequilibrium molecular dynamics simulations. At low frequencies, the results reveal a power-law dependence of the MFPs on frequency, in agreement with the diverging conductivity and the recently determined equilibrium MFPs. At higher frequencies, however, the nonequilibrium MFPs consistently exceed the equilibrium MFPs, highlighting the differences between the two quantities. Exerting pressure on the chain is shown to suppress the mean free paths and to generate a weaker divergence of MFPs at low frequencies. The results deliver important insight into the anomalous thermal conduction in low-dimensional systems and also reveal differences between the MFPs obtained from equilibrium and nonequilibrium simulations.