Abstract The densification of integrated circuits requires thermal management strategies and high thermal conductivity materials 1–3 . Recent innovations include the development of materials with thermal conduction anisotropy, which can remove hotspots along the fast-axis direction and provide thermal insulation along the slow axis 4,5 . However, most artificially engineered thermal conductors have anisotropy ratios much smaller than those seen in naturally anisotropic materials. Here we report extremely anisotropic thermal conductors based on large-area van der Waals thin films with random interlayer rotations, which produce a room-temperature thermal anisotropy ratio close to 900 in MoS 2 , one of the highest ever reported. This is enabled by the interlayer rotations that impede the through-plane thermal transport, while the long-range intralayer crystallinity maintains high in-plane thermal conductivity. We measure ultralow thermal conductivities in the through-plane direction for MoS 2 (57 ± 3 mW m −1 K −1 ) and WS 2 (41 ± 3 mW m −1 K −1 ) films, and we quantitatively explain these values using molecular dynamics simulations that reveal one-dimensional glass-like thermal transport. Conversely, the in-plane thermal conductivity in these MoS 2 films is close to the single-crystal value. Covering nanofabricated gold electrodes with our anisotropic films prevents overheating of the electrodes and blocks heat from reaching the device surface. Our work establishes interlayer rotation in crystalline layered materials as a new degree of freedom for engineering-directed heat transport in solid-state systems.
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Modeling the tunable thermal conductivity of intercalated layered materials with three-directional anisotropic phonon dispersion and relaxation times
An analytical model using three-directional anisotropic (TDA) dispersion and a novel anisotropic relaxation time (RT) relation for modeling the thermal conductivity ( k ) of intercalated layered materials is developed. The TDA dispersion eliminates the restriction of in-plane isotropy and is suitable for TDA materials such as black phosphorous. We compare calculations of k of bulk intercalated layered materials using the isotropic Debye dispersion and BvK dispersion with our TDA dispersion model, paired with both isotropic and anisotropic RTs. We find that calculated k values by the TDA dispersion model agree best with the experimental data. Furthermore, anisotropic RTs largely improve the performance of the Debye and BvK dispersion models whose average relative deviations for the in-plane k are reduced from 17.3% and 23.0% to 4.4% and 8.5%, respectively. Finally, thermal conductivity accumulation functions of intercalated MoS 2 and graphite are numerically calculated based on the TDA dispersion with anisotropic RTs. These models predict that intercalants cause increased contributions from phonons with shorter mean free paths, especially for in-plane thermal conductivity.
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- Award ID(s):
- 1901972
- PAR ID:
- 10390639
- Date Published:
- Journal Name:
- Journal of Materials Chemistry C
- Volume:
- 10
- Issue:
- 32
- ISSN:
- 2050-7526
- Page Range / eLocation ID:
- 11686 to 11696
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Boundary scattering of thermal phonons in thin solid films is typically analyzed using Fuchs-Sondheimer theory, which provides a simple equation to calculate the reduction of thermal conductivity as a function of the film thickness. However, this widely used equation is not applicable to highly anisotropic solids like graphite because it assumes the phonon dispersion is isotropic. Here, we derive a generalization of the Fuchs-Sondheimer equation for solids with arbitrary dispersion relations and examine its predictions for graphite. We find that the isotropic equation vastly overestimates the boundary scattering that occurs in thin graphite films due to the highly anisotropic group velocity, and that graphite can maintain its high in-plane thermal conductivity even in thin films with thicknesses as small as 10 nm.
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Abstract Heat transport in nanoscale carbon materials such as carbon nanotubes and graphene is normally dominated by phonons. Here, measurements of in‐plane thermal conductivity, electrical conductivity, and thermopower are presented from 77–350 K on two films with thickness <100 nm formed from semiconducting single‐walled carbon nanotubes. These measurements are made with silicon–nitride membrane thermal isolation platforms. The two films, formed from disordered networks of tubes with differing tube and bundle size, have very different thermal conductivity. One film matches a simple model of heat conduction assuming constant phonon velocity and mean free path, and 3D Debye heat capacity with a Debye temperature of 770 K. The second film shows a more complicated temperature dependence, with a dramatic drop in a relatively narrow window near 200 K where phonon contributions to thermal conductivity essentially vanish. This causes a corresponding large increase in thermoelectric figure‐of‐merit at the same temperature. A better understanding of this behavior can allow significant improvement in thermoelectric efficiency of these low‐cost earth‐abundant, organic electronic materials. Heat and charge conductivity near room temperature is also presented as a function of doping, which provides further information on the interaction of dopant molecules and phonon transport in disordered nanotube films.
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Low-dimensional materials with chain-like (one-dimensional) or layered (two-dimensional) structures are of significant interest due to their anisotropic electrical, optical, and thermal properties. One material with a chain-like structure, BaTiS3 (BTS), was recently shown to possess giant in-plane optical anisotropy and glass-like thermal conductivity. To understand the origin of these effects, it is necessary to fully characterize the optical, thermal, and electronic anisotropy of BTS. To this end, BTS crystals with different orientations (a- and c-axis orientations) were grown by chemical vapor transport. X-ray absorption spectroscopy was used to characterize the local structure and electronic anisotropy of BTS. Fourier transform infrared reflection/transmission spectra show a large in-plane optical anisotropy in the a-oriented crystals, while the c-axis oriented crystals were nearly isotropic in-plane. BTS platelet crystals are promising uniaxial materials for infrared optics with their optic axis parallel to the c-axis. The thermal conductivity measurements revealed a thermal anisotropy of ∼4.5 between the c- and a-axis. Time-domain Brillouin scattering showed that the longitudinal sound speed along the two axes is nearly the same, suggesting that the thermal anisotropy is a result of different phonon scattering rates.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/D1TC05369H
