Unraveling Heat Transport and Dissipation in Suspended MoSe2 from Bulk to Monolayer

David Saleta Reig; Sebin Varghese; Roberta Farris; Alexander Block; Jake D. Mehew; Olle Hellman; Paweł Woźniak; Marianna Sledzinska; Alexandros El Sachat; Emigdio Chávez-Ángel; Sergio O. Valenzuela; Niek F. van Hulst; Pablo Ordejón; Zeila Zanolli; Clivia M. Sotomayor Torres; Matthieu J. Verstraete; Klaas-Jan Tielrooij

doi:10.1002/adma.202108352

Unraveling Heat Transport and Dissipation in Suspended MoSe₂ from Bulk to Monolayer

David Saleta Reig, Sebin Varghese, Roberta Farris, Alexander Block, Jake D. Mehew, Olle Hellman, Paweł Woźniak, Marianna Sledzinska, Alexandros El Sachat, Emigdio Chávez-Ángel, Sergio O. Valenzuela, Niek F. van Hulst, Pablo Ordejón, Zeila Zanolli, Clivia M. Sotomayor Torres, Matthieu J. Verstraete, Klaas-Jan Tielrooij (Corresponding author)

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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 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.

Original language	English
Article number	2108352
Number of pages	9
Journal	Advanced Materials
Volume	34
Issue number	10
DOIs	https://doi.org/10.1002/adma.202108352
Publication status	Published - 10 Mar 2022
Externally published	Yes

Funding

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). 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).

Keywords

2D materials
ab initio
heat transport
Raman thermometry
transition metal dichalcogenides

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Saleta Reig, D., Varghese, S., Farris, R., Block, A., Mehew, J. D., Hellman, O., Woźniak, P., Sledzinska, M., El Sachat, A., Chávez-Ángel, E., Valenzuela, S. O., van Hulst, N. F., Ordejón, P., Zanolli, Z., Sotomayor Torres, C. M., Verstraete, M. J., & Tielrooij, K.-J. (2022). Unraveling Heat Transport and Dissipation in Suspended MoSe₂ from Bulk to Monolayer. Advanced Materials, 34(10), Article 2108352. https://doi.org/10.1002/adma.202108352

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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 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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author = "{Saleta Reig}, David and Sebin Varghese and Roberta Farris and Alexander Block and Mehew, {Jake D.} and Olle Hellman and Pawe{\l} Wo{\'z}niak and Marianna Sledzinska and {El Sachat}, Alexandros and Emigdio Ch{\'a}vez-{\'A}ngel and Valenzuela, {Sergio O.} and {van Hulst}, {Niek F.} and Pablo Ordej{\'o}n and Zeila Zanolli and {Sotomayor Torres}, {Clivia M.} and Verstraete, {Matthieu J.} and Klaas-Jan Tielrooij",

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Saleta Reig, D, Varghese, S, Farris, R, Block, A, Mehew, JD, Hellman, O, Woźniak, P, Sledzinska, M, El Sachat, A, Chávez-Ángel, E, Valenzuela, SO, van Hulst, NF, Ordejón, P, Zanolli, Z, Sotomayor Torres, CM, Verstraete, MJ & Tielrooij, K-J 2022, 'Unraveling Heat Transport and Dissipation in Suspended MoSe₂ from Bulk to Monolayer', Advanced Materials, vol. 34, no. 10, 2108352. https://doi.org/10.1002/adma.202108352

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AU - Saleta Reig, David

AU - Varghese, Sebin

AU - Farris, Roberta

AU - Block, Alexander

AU - Mehew, Jake D.

AU - Hellman, Olle

AU - Woźniak, Paweł

AU - Sledzinska, Marianna

AU - El Sachat, Alexandros

AU - Chávez-Ángel, Emigdio

AU - Valenzuela, Sergio O.

AU - van Hulst, Niek F.

AU - Ordejón, Pablo

AU - Zanolli, Zeila

AU - Sotomayor Torres, Clivia M.

AU - Verstraete, Matthieu J.

AU - Tielrooij, Klaas-Jan

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