Extreme near-field heat transfer between metallic surfaces is a subject of debate as the state-of-the-art theory and experiments are in disagreement on the energy carriers driving heat transport. In an effort to elucidate the physics of extreme near-field heat transfer between metallic surfaces, this Letter presents a comprehensive model combining radiation, acoustic phonon and electron transport across sub-10-nm vacuum gaps. The results obtained for gold surfaces show that in the absence of bias voltage, acoustic phonon transport is dominant for vacuum gaps smaller than ~2 nm. The application of a bias voltage significantly affects the dominant energy carriers as it increases the phonon contribution mediated by the long-range Coulomb force and the electron contribution due to a lower potential barrier. For a bias voltage of 0.6 V, acoustic phonon transport becomes dominant at a vacuum gap of 5 nm, whereas electron tunneling dominates at sub-1-nm vacuum gaps. The comparison of the theory against experimental data from the literature suggests that well-controlled measurements between metallic surfaces are needed to quantify the contributions of acoustic phonon and electron as a function of the bias voltage.
The radiative heat transfer between gold nanoparticle layers is presented using the coupled dipole method. Gold nanoparticles are modelled as effective electric and magnetic dipoles interacting via electromagnetic fluctuations. The effect of higher-order multipoles is implemented in the expression of electric polarizability to calculate the interactions at short distances. Our findings show that the near-field radiation reduces as the radius of the nanoparticles is increased. Also, the magnetic dipole contribution to the heat exchange becomes more important for larger particles. When one layer…
There is a great interest in the scientific community to perform calorimetry on samples having mass in the nanogram range. A detailed knowledge of the energy (heat) exchange in the fast growing family of micro- and nano-systems could provide valuable information about the chemistry and physics at the nano-scale. The possibility to have an atomically flat thermal probe represents an added value, because it provides the unique opportunity to perform Scanning Probe Microscopy (SPM) together with calorimetry. Here we report the fabrication, characterization, and calibration of atomically flat, sin…
Radiative heat transfer in systems with core-shell nanoparticles may exhibit not only a combination of disparate physical properties of its components but also further enhanced properties that arise from the synergistic properties of the core and shell components. We study the thermal conductance between two core-shell nanoparticles (CSNPs). The contribution of electric and magnetic dipole moments to the thermal conductance depend sensitively on the core and shell materials, and adjustable by core size and shell thickness. We predict that the radiative heat transfer in a dimer of Au@SiO2 CSNPs…
We show in this paper that the heat generated by the optical excitation of resonant plasmonic antennas and diffusing along a simple glass/air interface disturbs the electron transport of a nearby conductive element. By probing the temperature-dependent resistance of a gold nanowire $R_{\rm nw}(T)$, we quantitatively analyze the impact of a resonant absorption of the laser by the antennas. We find that the temperature rise at the nanowire induced by the laser absorption of a distant nanoparticle may exceed that of a direct illumination of the nanowire itself. We also find that a global temperat…
The understanding and modeling of the heat transport across nanometer and sub-nanometer gaps where the distinction between thermal radiation and conduction become blurred remains an open question. In this work, we present a three-dimensional atomistic simulation framework by combining the molecular dynamics (MD) and phonon non-equilibrium Green's function (NEGF) methods. The relaxed atomic configuration and interaction force constants of metallic nanogaps are generated from MD as inputs into harmonic phonon NEGF. Phonon tunneling across gold-gold and copper-copper nanogaps is quantified, and i…
We present here a theoretical method to determine the phononic contribution to the thermal conductance of nanoscale systems in the phase-coherent regime. Our approach makes use of classical molecular dynamics (MD) simulations to calculate the temperature-dependent dynamical matrix, and the phononic heat conductance is subsequently computed within the Landauer-Büttiker formalism with the help of nonequilibrium Green's function techniques. Tailored to nanostructures, crucial steps of force constant and heat transport calculations are performed directly in real space. As compared to conventional …
In this Letter, we report on quantitative measurements of the absolute near-field mediated heat flux between a gold coated near-field scanning thermal microscope (NSThM) tip and a planar gold sample at nanometer distances of 0.2 nm- 7 nm. We find an extraordinary large heat flux which is more than five orders of magnitude larger than black-body radiation and four orders of magnitude larger than the values predicted by conventional theory of fluctuational electrodynamics. Additionally, we compare our data with different theories of phonon tunneling which might explain a drastically increased he…
We investigate the full counting statistics of extreme-near-field radiative heat transfer using nonequilibrium Green's function formalism. In the extreme near field, the electron-electron interactions between two metallic bodies dominate the heat transfer process. We start from a general tight-binding electron Hamiltonian and obtain a Levitov-Lesovik like scaled cumulant generating function (SCGF) using random phase approximation to deal with electron-electron interaction. The expressions of heat current and its fluctuation (second cumulant) are obtained from the SCGF. The fluctuation symmetry…
Calculations of heat transfer between two plates of gold in an extreme near field is performed taking into account the existence of the electric double layer on metal surfaces. For d < 3nm the double layer contribution exceeds the predictions of the conversional theory of the heat transfer by several orders of magnitudes. This effect is due to a coupling between the radiation electric field and the double layer dipole moment. The results obtained can be used for the heat management at the nanoscale by intentionally changing the parameters of surface dipoles with the help of engineering.
It is suggested that in gold nanoparticles (GNPs) of about 5 nm sizes used in the radiofrequency (RF) hyperthermia, an absorption of the RF photon by the Fermi electron occurs with involvement of the longitudinal acoustic vibrational mode (LAVM), the dominating one in the distribution of vibrational density of states (VDOS). This physical mechanism helps to explain two observed phenomena: the size dependence of the heating rate (HR) in GNPs and reduced heat production in aggregated GNPs. The argumentation proceeds within the one-electron approximation, taking into account the discretenesses of…
We report first-principles calculations of local heating in nanoscale junctions formed by a single molecule and a gold point contact. Due to a larger heat dissipation, the single molecule heats up less than the gold point contact. We also find, at zero temperature, a threshold bias $V_{onset}$ of about 6 mV and 11 mV for the molecule and the point contact, respectively, is required to excite the smallest vibrational mode and generate heat. The latter estimate is in very good agreement with recent experimental results on the same system. At a given external bias $V$ below $V_{onset}$, heating b…
We analyze the heat transfer between two metals separated by a vacuum gap in the extreme near-field regime. In this cross-over regime between conduction and radiation, heat exchanges are mediated by photon, phonon and electron tunneling. We quantify the relative contribution of these carriers with respect to both the separation distance between the two bodies and the applied bias voltage. In the presence of a weak bias ($V_{\rm b}<100$~mV), electrons and phonons can contribute equally to the heat transfer near contact, while the contribution of photons becomes negligible. On the other hand, fo…
Heat transfer from irradiated metallic nanoparticles is relevant to a broad array of applications ranging from water desalination to photoacoustics. The efficacy of such processes relies on the ability of these nanoparticles to absorb the pulsed illuminating light and to quickly transfer energy to the environment. Here we show that compared to homogeneous gold nanoparticles having the same size, gold-silica core-shell nanoparticles enable heat transfers to liquid water that are faster. We reach this conclusion by considering both analytical and numerical calculations. The key factor explaining…
Metallization of Schottky surface gates by sputtering Au on strained Si/SiGe heterojunctions enables the depletion of the two dimensional electron gas (2DEG) at a relatively small voltage while maintaining an extremely low level of leakage current. A fabrication process has been developed to enable the formation of sub-micron Au electrodes sputtered onto Si/SiGe without the need of a wetting layer.
With the objective to understand microscopic principles governing thermal energy flow in nanojunctions, we study phononic heat transport through metal-molecule-metal junctions using classical molecular dynamics (MD) simulations. Considering a single-molecule gold-alkanedithiol-gold junction, we first focus on aspects of method development and compare two techniques for calculating thermal conductance: (i) The Reverse Nonequilibrium MD (RNEMD) method, where heat is inputted and extracted at a constant rate from opposite metals. In this case, the thermal conductance is calculated from the nonequ…
To develop next-generation electronics and high efficiency energy-harvesting devices, it is crucial to understand how charge and heat are transported at the nanoscale. Metallic atomic-size contacts are ideal systems to probe the quantum limits of transport. The thermal and electrical conductance of gold atomic contacts has been recently proven to be quantized at room temperature. However, a big experimental challenge in such measurements is represented by the fast breaking dynamics of metallic junctions at room temperature, which can exceed the typical response time of the thermal measurement.…
Crystal Orientation Dependence of Extreme Near-Field Heat Transfer between Polar Materials Governed by Surface Phonon Modes
School of Energy Science and Engineering, Harbin Institute of Technology（哈尔滨工业大学能源学院）；Key Laboratory of Aerospace Thermophysics, Ministry of Industry and Information Technology（工业和信息化部航空航天热物理重点实验室）
We explore the thermoelectric properties of gold atomic chains bridging gold electrodes by means of \textit{ab initio} and semi-empirical calculations, and heuristic reasoning. We predict the thermoelectric voltage induced by a temperature difference across such junctions to oscillate, repeatedly changing sign, as a function of the number of atoms $N$ making up the atomic chain. We also predict the amplitude of the oscillations to be proportional to $N$ for long atomic chains. Further we predict the thermoelectric voltage to change sign, in some cases, if the junction is stretched without chan…
We theoretically investigate the heat transfer between two metals across a vacuum gap in extreme near-field regime by quantifying the relative contribution of electrons, phonons and photons. We show that electrons play a dominant role in the heat transfer between two metals at subnanometric distance subject to a temperature gradient. Moreover, we demonstrate that this effect is dramatically amplified in the presence of an applied bias voltage. These results could pave the way to novel strategies for thermal management and energy conversion in extreme near-field regime.
We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical …
We propose a new approach to understand the time-dependent temperature increasing process of gold-silica core-shell nanoparticles injected into chicken tissues under near-infrared laser irradiation. Gold nanoshells strongly absorb near-infrared radiations and efficiently transform absorbed energy into heat. Temperature rise given by experiments and numerical calculations based on bioheat transfer are in good agreement. Our work improves the analysis of a recent study [Richardson et al., Nano Lett. 9, 1139 (2009)] by including effects of the medium perfusion on temperature increase. The theoret…
We have studied the electron-phonon (e-p) interaction in thin Cu and Au films at sub-Kelvin temperatures with the help of the hot electron effect, using symmetric normal metal-insulator-superconductor tunnel junction pairs as thermometers. By Joule heating the electron gas and measuring the electron and the lattice temperatures simultaneously, we show that the electron-phonon scattering rate follows a $T^{4}$ temperature dependence in both metals. The result is in accordance with the theory of e-p scattering in disordered films with vibrating boudaries and impurities, in contrast to the $T^{3}…
Current-voltage characteristics of H2-Au molecular junctions exhibit intriguing steps around a characteristic voltage of 40 mV. Surprisingly, we find that a hysteresis is connected to these steps with a typical time scale > 10 ms. This time constant scales linearly with the power dissipated in the junction beyond an ofset power P_s = IV_s. We propose that the hysteresis is related to vibrational heating of both the molecule in the junction and a set of surrounding hydrogen molecules. Remarkably, we can engineer our junctions such that the hysteresis' characteristic time becomes >days. We demon…
Superlubricity, or alternatively termed structural (super)lubrictiy, is a concept where ultra-low friction is expected at the interface between sliding surfaces if these surfaces are incommensurate and thus unable to interlock. In this work, we now report on sudden, reversible, friction changes that have been observed during AFM based nanomanipulation experiments of gold nanoparticles sliding on highly oriented pyrolythic graphite. These effects are can be explained by rotations of the gold nanoparticles within the concept of structural superlubricity, where the occurrence of ultra-low frictio…
We study the ionization dynamics of Ar clusters exposed to ultrashort near-infrared (NIR) laser pulses for intensities well below the threshold at which tunnel ionization ignites nanoplasma formation. We find that the emission of highly charged ions up to Ar$^{8+}$ can be switched on with unit contrast by generating only a few seed electrons with an ultrashort extreme ultraviolet (XUV) pulse prior to the NIR field. Molecular dynamics simulations can explain the experimental observations and predict a generic scenario where efficient heating via inverse bremsstrahlung and NIR avalanching are fo…
