000132272 001__ 132272 000132272 005__ 20250923084417.0 000132272 0247_ $$2doi$$a10.1021/acs.jpcc.3c06820 000132272 0248_ $$2sideral$$a137444 000132272 037__ $$aART-2024-137444 000132272 041__ $$aeng 000132272 100__ $$aMahendran, Srinivasan 000132272 245__ $$aQuantitative Predictions of the Thermal Conductivity in Transition Metal Dichalcogenides: Impact of Point Defects in MoS<sub>2</sub> and WS<sub>2</sub> Monolayers 000132272 260__ $$c2024 000132272 5060_ $$aAccess copy available to the general public$$fUnrestricted 000132272 5203_ $$aTransition metal dichalcogenides are investigated for various applications at the nanoscale because of their unique combination of properties and dimensionality. For many of the anticipated applications, heat conduction plays an important role. At the same time, these materials often contain relatively large amounts of point defects. Here, we provide a systematic analysis of the impact of intrinsic and selected extrinsic defects on the lattice thermal conductivity of MoS2 and WS2 monolayers. We combine Boltzmann transport theory and Green’s function-based T-matrix approach for the calculation of scattering rates. The force constants for the defect configurations are obtained from density functional theory calculations via a regression approach, which allows us to sample a rather large number of defects at a moderate computational cost and to systematically enforce both the translational and rotational acoustic sum rules. The calculated lattice thermal conductivity is in quantitative agreement with the experimental data for heat transport and defect concentrations for both MoS2 and WS2. Crucially, this demonstrates that the strong deviation from a 1/T temperature dependence of the lattice thermal conductivity observed experimentally can be fully explained by the presence of point defects. We furthermore predict the scattering strengths of the intrinsic defects to decrease in the sequence VMo ≈ V2S= > V2S⊥ > VS > Sad in both materials, while the scattering rates for the extrinsic (adatom) defects decrease with increasing mass such that Liad > Naad > Kad. Compared with earlier work, we find that both intrinsic and extrinsic adatoms are relatively weak scatterers. We attribute this difference to the treatment of the translational and rotational acoustic sum rules, which, if not enforced, can lead to spurious contributions in the zero-frequency limit. 000132272 540__ $$9info:eu-repo/semantics/openAccess$$aby$$uhttp://creativecommons.org/licenses/by/3.0/es/ 000132272 590__ $$a3.2$$b2024 000132272 592__ $$a0.914$$b2024 000132272 591__ $$aCHEMISTRY, PHYSICAL$$b95 / 185 = 0.514$$c2024$$dQ3$$eT2 000132272 593__ $$aPhysical and Theoretical Chemistry$$c2024$$dQ1 000132272 591__ $$aNANOSCIENCE & NANOTECHNOLOGY$$b88 / 147 = 0.599$$c2024$$dQ3$$eT2 000132272 593__ $$aElectronic, Optical and Magnetic Materials$$c2024$$dQ1 000132272 591__ $$aMATERIALS SCIENCE, MULTIDISCIPLINARY$$b237 / 460 = 0.515$$c2024$$dQ3$$eT2 000132272 593__ $$aSurfaces, Coatings and Films$$c2024$$dQ1 000132272 593__ $$aEnergy (miscellaneous)$$c2024$$dQ2 000132272 593__ $$aNanoscience and Nanotechnology$$c2024$$dQ2 000132272 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/publishedVersion 000132272 700__ $$0(orcid)0000-0003-0971-1098$$aCarrete, Jesús 000132272 700__ $$aIsacsson, Andreas 000132272 700__ $$aMadsen, Georg K. H. 000132272 700__ $$aErhart, Paul 000132272 773__ $$g128, 4 (2024), 1709-1716$$pJ. phys. chem., C$$tJournal of physical chemistry. C.$$x1932-7447 000132272 8564_ $$s3762345$$uhttps://zaguan.unizar.es/record/132272/files/texto_completo.pdf$$yVersión publicada 000132272 8564_ $$s3271761$$uhttps://zaguan.unizar.es/record/132272/files/texto_completo.jpg?subformat=icon$$xicon$$yVersión publicada 000132272 909CO $$ooai:zaguan.unizar.es:132272$$particulos$$pdriver 000132272 951__ $$a2025-09-22-14:33:39 000132272 980__ $$aARTICLE