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The realization of single-molecule thermal conductance measurements has driven the need for theoretical tools to describe conduction processes that occur over atomistic length scales. In macroscale systems, the principle that is typically used to understand thermal conductivity is Fourier’s law. At molecular length scales, however, deviations from Fourier’s law are common in part because microscale thermal transport properties typically depend on the complex interplay between multiple heat conduction mechanisms. Here, the thermal transport properties that arise from electron transfer across a thermal gradient in a molecular conduction junction are examined theoretically. We illustrate how transport in a model junction is affected by varying the electronic structure and length of the molecular bridge in the junction as well as the strength of the coupling between the bridge and its surrounding environment. Three findings are of note: First, the transport properties can vary significantly depending on the characteristics of the molecular bridge and its environment; second, the system’s thermal conductance commonly deviates from Fourier’s law; and third, in properly engineered systems, the magnitude of electron hopping thermal conductance is similar to what has been measured in single-molecule devices.
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Nondiffusive thermal transport and prediction of the breakdown of Fourier’s law in nanograting experiments
An appropriate heat conduction model is indispensable for experimental data analysis in nanothermometry in order to extract parameters of interests and to achieve a fundamental understanding of phonon-mediated heat transfer in nanostructures and across interfaces. Recently, nanoscale periodic metallic gratings are used as a group of distributed heaters as well as transducers in nanothermometry. However, in this technique, there are coupled hotspot-size-dependent effective thermal conductivity (ETC) and hotspot-size-dependent thermal interface resistivity, which posts a challenge for experimental data analysis using Fourier’s law that fails to extract both ETC and thermal interface resistivity simultaneously. To overcome this challenge, a novel two-parameter nondiffusive heat conduction (TPHC) model, which has been successfully applied to data analysis in different types of pump-probe experiments, is applied to analyze laser-induced nondiffusive heat transfer in nanoscale metallic grating experiments. Since the hotspot-size-dependent ETC is automatically captured by the TPHC model, the hotspot-size-dependent interface resistivity becomes the only parameter to be determined from experiments through data fitting. Thus, the hotspot-size-dependent thermal interface resistivity can be determined from experiments without the impact from the hotspot-size-dependent ETC. Currently, there is a lack of a criterion to predict when Fourier’s law breaks down in nanoscale heat transfer. To fill this gap, a criterion based the TPHC model is identified to predict the valid range of Fourier’s law, which is validated in both theoretical analyses and nanoscale metallic grating experiments.
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- Award ID(s):
- 1637370
- PAR ID:
- 10597430
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- AIP Advances
- Volume:
- 7
- Issue:
- 1
- ISSN:
- 2158-3226
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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