Thermal expansion and transport in van der Waals solids from first-principles calculations

Abstract

The lattice thermal expansion and conductivity in bulk Mo and W-based transition metal dichalcogenides are investigated by means of density functional and Boltzmann transport theory calculations. To this end, a recent van der Waals density functional (vdW-DF-CX) is employed, which is shown to yield excellent agreement with reference data for the structural parameters. The calculated in-plane thermal conductivity compares well with experimental room temperature values, when phonon-phonon and isotopic scattering are included. To explain the behavior over the entire available temperature range one must, however, include additional (temperature independent) scattering mechanisms that limit the mean free path. Generally, the primary heat carrying modes have mean free paths of $1\mu \text{m}$ or more, which makes these materials very susceptible to structural defects. The conductivity of Mo and W-based TMDs is primarily determined by the chalcogenide species and increases in the order Te-Se-S. While for the tellurides and selenides the transition metal element has a negligible effect, the conductivity of WS${}_2$ is notably higher than for MoS${}_2$, which can be traced to the much larger phonon band gap of the former. Overall the present study provides a consistent set of thermal conductivities that reveal chemical trends and constitute the basis for future investigations of van der Waals solids.

10 pages, 11 figures, 2 tables

References in corpus (9)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Ultrafast Charge Transfer in Atomically Thin MoS2/WS2 Heterostructures
• Distribution of phonon lifetime in Brillouin zone
• van der Waals forces in density functional theory: The vdW-DF method
• Phonon Transport in Single-Layer Transition Metal Dichalcogenides: a First-Principles Study
• Testing several recent van der Waals density functionals for layered structures
• van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions
• The Role of Transport Agents in MoS2 Single Crystals

Cited by in corpus (29)

• The hiphive package for the extraction of high-order force constants by machine learning
• Anisotropic thermal transport in bulk hexagonal boron nitride
• Time-domain thermoreflectance (TDTR) measurements of anisotropic thermal conductivity using a variable spot size approach
• Relating chemical bonding to physical properties: The origin of unexpected isotropic properties in layered materials
• Elastic properties of bulk and low-dimensional materials using Van der Waals density functional
• Quasi-ballistic thermal transport across MoS${}_2$ thin films
• Thermal Transport in MoS${}_2$ from Molecular Dynamics using Different Empirical Potentials
• Ab initio study on lattice thermal conductivity of Cu${}_2$O using GGA and hybrid density functional methods
• Assessment of two hybrid van der Waals density functionals for covalent and non-covalent binding of molecules
• Screening nature of the van der Waals density functional method: A review and analysis of the many-body physics foundation
• Strongly Tunable Anisotropic Thermal Transport in MoS2 by Strain and Lithium Intercalation: First--Principles Calculations
• Anisotropic Thermal Transport in Phase-Transition Layered 2D Alloys WSe2(1-x)Te2x
• Finite-temperature properties of non-magnetic transition metals: Comparison of the performance of constraint-based semi and nonlocal functionals
• libvdwxc: A library for exchange-correlation functionals in the vdW-DF family
• Moiré-Driven Interfacial Thermal Transport in Twisted Transition Metal Dichalcogenides
• Simultaneous measurement of anisotropic thermal conductivity and thermal boundary conductance of 2-dimensional materials
• Picosecond Transient Thermoreflectance for Thermal Conductivity Characterization
• Signatures of van der Waals binding: a coupling-constant scaling analysis
• Extent of Fock-exchange mixing for a hybrid van der Waals density functional?
• Energy scaling law for nanostructured materials
• Thermal conductivity in intermetallic clathrates: A first principles perspective
• Glass-like Cross-plane Thermal Conductivity of Kagome Metals RbV3Sb5 and CsV3Sb5
• A pre-time-zero spatiotemporal microscopy technique for the ultrasensitive determination of the thermal diffusivity of thin films
• High-throughput characterization of transition metal dichalcogenide alloys: Thermodynamic stability and electronic band alignment
• Quantitative predictions of the thermal conductivity in transition metal dichalcogenides: The impact of point defects in MoS${}_2$ and WS${}_2$ monolayers
• Generation and detection of coherent longitudinal acoustic waves in ultrathin 1T'-MoTe2
• Improved proton-transfer barriers with van der Waals density functionals: Role of repulsive non-local correlation
• Ab Initio Modeling of Thermal Transport through van der Waals Materials
• Discarded gems: Thermoelectric performance of materials with band gap emerging at the hybrid-functional level