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Ferroelectricity and a variety of other intriguing physical characteristics. These arise from its van der Waals (vdW) layered structure, interlayer coupling, and intralayer interactions. The vibrational modes of 2D InSe are highly sensitive to thickness. The phase transitions in 2D materials, which are critical to their properties and applications, are closely related to interlayer and intralayer vibrations. However, the effect of the thickness on these vibrational behaviors during phase transitions remains insufficiently understood. In this study, we investigate the Raman spectra of\n                    <jats:italic>\u03b2<\/jats:italic>\n                    \u2010InSe with layer numbers (LN) ranging from 4 to 33 under high pressure and construct a pressure LN phase diagram. Unexpectedly, due to the quantum confinement and defect effects, InSe flakes with fewer layers require more energy to undergo phase transitions which is confirmed by PL experiments and DFT calculations, irrespective of whether pressure is being increased or decreased. This research establishes a solid foundation for exploring and characterizing interlayer and intralayer lattice dynamics through pressure engineering in vdW materials.\n                  <\/jats:p>","DOI":"10.1002\/adma.73416","type":"journal-article","created":{"date-parts":[[2026,5,16]],"date-time":"2026-05-16T13:19:23Z","timestamp":1778937563000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Unveiling Layer\u2010Dependent Phase Transition and Lattice Dynamics in Two\u2010Dimensional InSe"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-8279-4278","authenticated-orcid":false,"given":"Wenqian","family":"Shen","sequence":"first","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; Advanced Films (COSDAF) City University of Hong Kong  Kowloon China"},{"name":"City University of Hong Kong Shenzhen Research Institute  Shenzhen China"},{"name":"Department of Chemistry and State Key Laboratory of Marine Environmental Health City University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lok Wing","family":"Wong","sequence":"additional","affiliation":[{"name":"Department of Applied Physics The Hong Kong Polytechnic University  Kowloon China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huizhong","family":"Bai","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; Advanced Films (COSDAF) City University of Hong Kong  Kowloon China"},{"name":"Department of Applied Physics The Hong Kong Polytechnic University  Kowloon China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ka Ho","family":"Leung","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; Advanced Films (COSDAF) City University of Hong Kong  Kowloon China"},{"name":"City University of Hong Kong Shenzhen Research Institute  Shenzhen China"},{"name":"Department of Chemistry and State Key Laboratory of Marine Environmental Health City University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianren","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Applied Physics The Hong Kong Polytechnic University  Kowloon China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ping","family":"Man","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; Advanced Films (COSDAF) City University of Hong Kong  Kowloon China"},{"name":"City University of Hong Kong Shenzhen Research Institute  Shenzhen China"},{"name":"Department of Chemistry and State Key Laboratory of Marine Environmental Health City University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shan","family":"Gao","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; Advanced Films (COSDAF) City University of Hong Kong  Kowloon China"},{"name":"City University of Hong Kong Shenzhen Research Institute  Shenzhen China"},{"name":"Department of Chemistry and State Key Laboratory of Marine Environmental Health City University of Hong Kong  Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7411-0734","authenticated-orcid":false,"given":"Jiong","family":"Zhao","sequence":"additional","affiliation":[{"name":"Department of Applied Physics The Hong Kong Polytechnic University  Kowloon China"},{"name":"The Research Institute for Advanced Manufacturing The Hong Kong Polytechnic University  Kowloon Hong Kong China"},{"name":"The Hong Kong Polytechnic University Shenzhen Research Institute  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7852-3811","authenticated-orcid":false,"given":"Thuc Hue","family":"Ly","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Center of Super\u2010Diamond &amp; 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