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Beyond the most apparent anisotropy in 2D materials, due to distinct in-plane and out-of-plane (intralayer and interlayer) thermal transport, certain systems also present in-plane thermal anisotropy, whose origin may be more subtle. Here, we report on the vibrational and thermal properties of PdSe<jats:sub>2<\/jats:sub> crystals, obtaining the complete (diagonal) elements of the thermal conductivity tensor (\u03ba<jats:italic>\n                     <jats:sub>ij<\/jats:sub>\n                  <\/jats:italic>), and their low-frequency (GHz, Brillouin) and high-frequency (THz, Raman) lattice vibrations. Remarkably, we observe substantial anisotropy for the in-plane directions with <jats:inline-formula>\n                     <jats:tex-math\/>\n                     <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" overflow=\"scroll\">\n                        <mml:mrow>\n                           <mml:msubsup>\n                              <mml:mi>\u03b7<\/mml:mi>\n                              <mml:mrow>\n                                 <mml:mi>y<\/mml:mi>\n                                 <mml:mi>x<\/mml:mi>\n                              <\/mml:mrow>\n                              <mml:mrow>\n                                 <mml:mrow>\n                                    <mml:mtext>exp<\/mml:mtext>\n                                 <\/mml:mrow>\n                              <\/mml:mrow>\n                           <\/mml:msubsup>\n                           <mml:mo>=<\/mml:mo>\n                           <mml:mrow>\n                              <mml:msub>\n                                 <mml:mi>\u03ba<\/mml:mi>\n                                 <mml:mi>y<\/mml:mi>\n                              <\/mml:msub>\n                           <\/mml:mrow>\n                           <mml:mrow>\n                              <mml:mo>\/<\/mml:mo>\n                           <\/mml:mrow>\n                           <mml:mrow>\n                              <mml:msub>\n                                 <mml:mi>\u03ba<\/mml:mi>\n                                 <mml:mi>x<\/mml:mi>\n                              <\/mml:msub>\n                           <\/mml:mrow>\n                           <mml:mo>=<\/mml:mo>\n                           <mml:mn>1.38<\/mml:mn>\n                        <\/mml:mrow>\n                     <\/mml:math>\n                  <\/jats:inline-formula>. By performing <jats:italic>ab initio<\/jats:italic> calculations of the vibrational modes, we demonstrate that this anisotropy arises from the strong lattice anharmonicity. This is reflected by the enhanced coupling between acoustic and low-energy optical branches along the [100] crystallographic direction (<jats:italic>x<\/jats:italic>-axis), where vibrational anharmonicity is larger than in the [010] direction (<jats:italic>y<\/jats:italic>-axis).<\/jats:p>","DOI":"10.1088\/2053-1583\/ad64e3","type":"journal-article","created":{"date-parts":[[2024,7,18]],"date-time":"2024-07-18T22:49:36Z","timestamp":1721342976000},"page":"045006","update-policy":"https:\/\/doi.org\/10.1088\/crossmark-policy","source":"Crossref","is-referenced-by-count":7,"title":["Unravelling the origin of thermal anisotropy in PdSe<sub>2<\/sub>"],"prefix":"10.1088","volume":"11","author":[{"given":"Kai","family":"Xu","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luis Mart\u00ednez","family":"Armesto","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Josef","family":"Sv\u011btl\u00edk","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5438-0534","authenticated-orcid":true,"given":"Juan F","family":"Sierra","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vera","family":"Marinova","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dimitre","family":"Dimitrov","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alejandro R","family":"Go\u00f1i","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Adam","family":"Krysztofik","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bartlomiej","family":"Graczykowski","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4086-4191","authenticated-orcid":true,"given":"Riccardo","family":"Rurali","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sergio O","family":"Valenzuela","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9679-0075","authenticated-orcid":true,"given":"Juan Sebasti\u00e1n","family":"Reparaz","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"266","published-online":{"date-parts":[[2024,7,29]]},"reference":[{"key":"tdmad64e3bib1","doi-asserted-by":"publisher","first-page":"11803","DOI":"10.1021\/acsnano.7b07436","article-title":"Van der Waals layered materials: opportunities and challenges","volume":"11","author":"Duong","year":"2017","journal-title":"ACS Nano"},{"key":"tdmad64e3bib2","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtadv.2020.100076","article-title":"2D layered noble metal dichalcogenides (Pt, Pd, Se, S) for electronics and energy applications","volume":"7","author":"Chen","year":"2020","journal-title":"Mater. 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