Radiative transfer of energy at the nanometre length scale is of great importance to a variety of technologies including heat-assisted magnetic recording, near-field thermophotovoltaics and lithography. Although experimental advances have enabled elucidation of near-field radiative heat transfer in gaps as small as 20-30 nanometres (refs 4-6), quantitative analysis in the extreme near field (less than 10 nanometres) has been greatly limited by experimental challenges. Moreover, the results of pioneering measurements differed from theoretical predictions by orders of magnitude. Here we use custom-fabricated scanning probes with embedded thermocouples, in conjunction with new microdevices capable of periodic temperature modulation, to measure radiative heat transfer down to gaps as small as two nanometres. For our experiments we deposited suitably chosen metal or dielectric layers on the scanning probes and microdevices, enabling direct study of extreme near-field radiation between silica-silica, silicon nitride-silicon nitride and gold-gold surfaces to reveal marked, gap-size-dependent enhancements of radiative heat transfer. Furthermore, our state-of-the-art calculations of radiative heat transfer, performed within the theoretical framework of fluctuational electrodynamics, are in excellent agreement with our experimental results, providing unambiguous evidence that confirms the validity of this theory for modelling radiative heat transfer in gaps as small as a few nanometres. This work lays the foundations required for the rational design of novel technologies that leverage nanoscale radiative heat transfer.
Thermal transport in individual atomic junctions and chains is of great fundamental interest because of the distinctive quantum effects expected to arise in them. By using novel, custom-fabricated, picowatt-resolution calorimetric scanning probes, we measured the thermal conductance of gold and platinum metallic wires down to singleatom junctions. Our work reveals that the thermal conductance of gold single-atom junctions is quantized at room temperature and shows that the Wiedemann-Franz law relating thermal and electrical conductance is satisfied even in single-atom contacts. Furthermore, we quantitatively explain our experimental results within the Landauer framework for quantum thermal transport. The experimental techniques reported here will enable thermal transport studies in atomic and molecular chains, which will be key to investigating numerous fundamental issues that thus far have remained experimentally inaccessible.T he study of thermal transport at the nanoscale is of critical importance for the development of novel nanoelectronic devices and holds promise to unravel quantum phenomena that have no classical analogs (1-3). In the context of nanoscale devices, metallic atomic-size contacts (4) and single-molecule junctions (5) represent the ultimate limit of miniaturization and have emerged as paradigmatic systems revealing previously unknown quantum effects related to charge and energy transport. For instance, transport properties of atomic-scale systems-such as electrical conductance (6), shot noise (7, 8), thermopower (9-11), and Joule heating (12)-are completely dominated by quantum effects, even at room temperature. Therefore, they drastically differ from those of macroscale devices. Unfortunately, the experimental study of thermal transport in these systems constitutes a formidable challenge and has remained elusive to date, in spite of its fundamental interest (13).Probing thermal transport in junctions of atomic dimensions is crucial for understanding the ultimate quantum limits of energy transport. These limits have been explored in a variety of microdevices (14-18), where it has been shown that, irrespective of the nature of the carriers (phonons, photons, or electrons), heat is ultimately transported via discrete channels. The maximum contribution per channel to the thermal conductance is equal to the universal thermal conduct-T/3h, where k B is the Boltzmann constant, T is the absolute temperature, and h is the Planck's constant. However, observations of quantum thermal transport in microscale devices have only been possible at sub-Kelvin temperatures, and other attempts at higher-temperature regimes have yielded inconclusive results (19).The energy-level spacing in metallic contacts of atomic size is of the order of electron volts (i.e., much larger than thermal energy); therefore, these junctions offer an opportunity to explore whether thermal transport can still be quantized at room temperature. However, probing thermal transport in atomic junctions is challenging because of the technic...
Single-molecule junctions have been extensively used to probe properties as diverse as electrical conduction 1-3 , light emission 4 , thermoelectric energy conversion 5,6 , quantum interference 7,8 , heat dissipation 9,10 and electronic noise 11 at atomic and molecular scales. However, a key quantity of current interest-the thermal conductance of single-molecule junctions-has not yet been directly experimentally determined, owing to the challenge of detecting minute heat currents at the picowatt level. Here we show that picowatt-resolution scanning probes previously developed to study the thermal conductance of single-metal-atom junctions 12 , when used in conjunction with a time-averaging measurement scheme to increase the signal-to-noise ratio, also allow quantification of the much lower thermal conductance of single-molecule junctions. Our experiments on prototypical Au-alkanedithiol-Au junctions containing two to ten carbon atoms confirm that thermal conductance is to a first approximation independent of molecular length, consistent with detailed ab initio simulations. We anticipate that our approach will enable systematic exploration of thermal transport in many other one-dimensional systems, such as short molecules and polymer chains, for which computational predictions of thermal conductance 13-16 have remained experimentally inaccessible.Studies of charge and heat transport in molecules are of great fundamental interest, and are of critical importance for the development of a variety of technologies, including molecular electronics 17 , thermally conductive polymers 18 and thermoelectric energy-conversion devices 19 . Given this overall importance and the daunting experimental challenges, a number of initial studies explored charge transport in ensembles of molecules 20,21 . Although such measurements provided important insights, researchers gradually began to realize that it was
Radiative heat transfer in Ångström- and nanometre-sized gaps is of great interest because of both its technological importance and open questions regarding the physics of energy transfer in this regime. Here we report studies of radiative heat transfer in few Å to 5 nm gap sizes, performed under ultrahigh vacuum conditions between a Au-coated probe featuring embedded nanoscale thermocouples and a heated planar Au substrate that were both subjected to various surface-cleaning procedures. By drawing on the apparent tunnelling barrier height as a signature of cleanliness, we found that upon systematically cleaning via a plasma or locally pushing the tip into the substrate by a few nanometres, the observed radiative conductances decreased from unexpectedly large values to extremely small ones—below the detection limit of our probe—as expected from our computational results. Our results show that it is possible to avoid the confounding effects of surface contamination and systematically study thermal radiation in Ångström- and nanometre-sized gaps.
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