Unraveling Heat Transport and Dissipation in Suspended MoSe2 from Bulk to Monolayer
Reig, David Saleta; Varghese, Sebin; Farris, Roberta; Block, Alexander; Mehew, Jake D; Hellman, Olle; Woźniak, Pawełl; Sledzinska, Marianna; Sachat, Alexandros El; Chávez-Ángel, Emigdio; Valenzuela, Sergio O; van Hulst, Niek F; Ordejón, Pablo; Zanolli, Zeila; Torres, Clivia M Sotomayor; Verstraete, Matthieu J; Tielrooij, Klaas-Jan
(2022) Advanced Materials, volume 34, issue 10, pp. 1 - 9
(Article)
Abstract
Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental–theoretical study establishes
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a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe2. Thermal conductivity measurements using Raman thermometry on a large set of clean, crystalline, suspended crystals with systematically varied thickness are combined with ab initio simulations with phonons at finite temperature. The results show that phonon dispersions and lifetimes change strongly with thickness, yet the thinnest TMD films exhibit an in-plane thermal conductivity that is only marginally smaller than that of bulk crystals. This is the result of compensating phonon contributions, in particular heat-carrying modes around ≈0.1 THz in (sub)nanometer thin films, with a surprisingly long mean free path of several micrometers. This behavior arises directly from the layered nature of the material. Furthermore, out-of-plane heat dissipation to air molecules is remarkably efficient, in particular for the thinnest crystals, increasing the apparent thermal conductivity of monolayer MoSe2 by an order of magnitude. These results are crucial for the design of (flexible) TMD-based (opto-)electronic applications.
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Keywords: 2D materials, Raman thermometry, ab initio, heat transport, transition metal dichalcogenides, General Materials Science, Mechanics of Materials, Mechanical Engineering
ISSN: 0935-9648
Publisher: Wiley-VCH Verlag
Note: Funding Information: The authors thank Andrea Pitillas Martínez for the graphics shown in the ToC and Figure 1a,b. D.S.R. and S.V. would like to acknowledge the support of the Spanish Ministry of Economy through FPI-SO2019 and FPI-SO2018, respectively. R.F., P.O., and Z.Z. acknowledge support by the EU H2020-NMBP-TO-IND-2018 project “INTERSECT” (Grant No. 814487), the EC H2020-INFRAEDI-2018-2020 MaX “Materials Design at the Exascale” CoE (Grant No. 824143), and Spanish MCI/AEI/FEDER-UE (Grant No. PGC2018-096955-B-C43). O.H. acknowledges support from the Swedish Research Council (VR) program 2020-04630. P.W. acknowledges funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłlodowska-Curie Grant Agreement No. 754510 (PROBIST). M.S., A.E.S., E.C.A., and C.M.S.T. acknowledge support of the Spanish MICIN project SIP (PGC2018-101743-B-I00). S.O.V. acknowledges support from MINECO under contract numbers PID2019-111773RB-I00/AEI/10.13039/501100011033. Z.Z. acknowledges financial support by the Netherlands Sector Plan program 2019-2023. M.J.V. acknowledges support from FRS-FNRS Belgium PdR Grant No. T.0103.19—ALPS, and contributions from the Melodica flag-era.net project. K.J.T., M.S., C.M.S.T., S.O.V., and N.F.v.H. acknowledge funding from BIST Ignite project 2DNanoHeat. K.J.T. acknowledges funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 804349 (ERC StG CUHL), RYC fellowship No. RYC-2017-22330, and IAE project PID2019-111673GB-I00. ICN2 was supported by the Severo Ochoa program from Spanish MINECO Grant No. SEV-2017-0706 and Generalitat de Catalunya (CERCA program and Grant 201756R1506). Funding Information: The authors thank Andrea Pitillas Martínez for the graphics shown in the ToC and Figure 1a,b . D.S.R. and S.V. would like to acknowledge the support of the Spanish Ministry of Economy through FPI‐SO2019 and FPI‐SO2018, respectively. R.F., P.O., and Z.Z. acknowledge support by the EU H2020‐NMBP‐TO‐IND‐2018 project “INTERSECT” (Grant No. 814487), the EC H2020‐INFRAEDI‐2018‐2020 MaX “Materials Design at the Exascale” CoE (Grant No. 824143), and Spanish MCI/AEI/FEDER‐UE (Grant No. PGC2018‐096955‐B‐C43). O.H. acknowledges support from the Swedish Research Council (VR) program 2020‐04630. P.W. acknowledges funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłlodowska‐Curie Grant Agreement No. 754510 (PROBIST). M.S., A.E.S., E.C.A., and C.M.S.T. acknowledge support of the Spanish MICIN project SIP (PGC2018‐101743‐B‐I00). S.O.V. acknowledges support from MINECO under contract numbers PID2019‐111773RB‐I00/AEI/10.13039/501100011033. Z.Z. acknowledges financial support by the Netherlands Sector Plan program 2019‐2023. M.J.V. acknowledges support from FRS‐FNRS Belgium PdR Grant No. T.0103.19—ALPS, and contributions from the Melodica flag‐era.net project. K.J.T., M.S., C.M.S.T., S.O.V., and N.F.v.H. acknowledge funding from BIST Ignite project 2DNanoHeat. K.J.T. acknowledges funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 804349 (ERC StG CUHL), RYC fellowship No. RYC‐2017‐22330, and IAE project PID2019‐111673GB‐I00. ICN2 was supported by the Severo Ochoa program from Spanish MINECO Grant No. SEV‐2017‐0706 and Generalitat de Catalunya (CERCA program and Grant 201756R1506). Publisher Copyright: © 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH
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