Alexandros El Sachat, Peng Xiao, Davide Donadio, Frédéric Bonell, Marianna Sledzinska, Alain Marty, Céline Vergnaud, Hervé Boukari, Matthieu Jamet, Guillermo Arregui, Zekun Chen, Francesc Alzina, Clivia M. Sotomayor Torres, Emigdio Chavez-Angel, Agencia Estatal de Investigación (España), Generalitat de Catalunya, Ministerio de Ciencia e Innovación (España), European Commission, ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), Département de physique [Departament de Física, Universitat Autònoma de Barcelona], University of California [Davis] (UC Davis), University of California (UC), SPINtronique et TEchnologie des Composants (SPINTEC), Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Nanophysique et Semiconducteurs (NEEL - NPSC), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Institució Catalana de Recerca i Estudis Avançats (ICREA), and ANR-10-LABX-0051,LANEF,Laboratory of Alliances on Nanosciences - Energy for the Future(2010)
We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of layered PtSe films of varying thickness (1–40 layers) using frequency-domain thermo-reflectance, low-frequency Raman, and pump-probe coherent phonon spectroscopy. We find ballistic cross-plane heat transport up to ~30 layers PtSe and a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 20 layers compared to the crystalline films of the same thickness. First-principles calculations further reveal a high degree of thermal conductivity anisotropy and a remarkable large contribution of the optical phonons to the thermal conductivity in bulk (~20%) and thin PtSe films (~30%). Moreover, we show strong interlayer interactions in PtSe, short acoustic phonon lifetimes in the range of picoseconds, an out-of-plane elastic constant of 31.8 GPa, and a layer-dependent group velocity ranging from 1340 ms in bilayer to 1873 ms in eight layers of PtSe. The potential of tuning the lattice thermal conductivity of layered materials with the level of crystallinity and the real-time observation of coherent phonon dynamics open a new playground for research in 2D thermoelectric devices and provides guidelines for thermal management in 2D electronics., This work has been supported by the Severo Ochoa program, the Spanish Research Agency (AEI, grant no. SEV-2017-0706), and the CERCA Program/Generalitat de Catalunya. The authors acknowledge support from the Spanish MICINN project SIP (PGC2018-101743-B-I00), and the EU project NANOPOLY (GA 289061). The LANEF framework (ANR-10-LABX-51-01) is acknowledged for its support of mutualized infrastructure. PX acknowledges support for the Ph.D. fellowship from the EU Marie Sklodowska-Curie COFUND PREBIST (Grant Agreement 754558). AES acknowledges support by the H2020-MSCA-IF project THERMIC-GA No. 101029727. The authors acknowledge Dr. John Cuffe for his critical comments.