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However, their high intralayer lattice thermal conductivity presents an obstacle for thermoelectric applications. This work proposes a rattling\u2010scatter strategy to reduce intralayer lattice thermal conductivity through the intercalation of organic molecules, as demonstrated with ethylenediamine (EDA) intercalated into black phosphorus (BP). Theoretical calculations reveal that this mechanism significantly enhances lattice anharmonicity and reduces group velocity, achieving a more than one order of magnitude decrease in intralayer lattice thermal conductivity. Experimental results validate these findings, revealing a significantly reduced thermal conductivity of 0.13 Wm\n                    <jats:sup>\u22121<\/jats:sup>\n                    K\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 300 K in BP\/EDA composites, which is only 1.45% of that in polycrystalline BP. Additionally, EDA intercalation distorts the BP structure, causing conduction band convergence around the Fermi level and enhancing electrical performance. The BP\/EDA is predicted to have an impressive\n                    <jats:italic>zT<\/jats:italic>\n                    value of 0.53 at 300 K, a staggering 19 fold increase over pristine BP. This study demonstrates that organic\u2010molecule intercalation effectively induces rattling motion, providing a promising strategy to suppress lattice thermal conductivity and improve thermoelectric performance in layered materials, thereby offering valuable insights for thermoelectric material design.\n                  <\/jats:p>","DOI":"10.1002\/smll.202505129","type":"journal-article","created":{"date-parts":[[2025,6,17]],"date-time":"2025-06-17T08:37:57Z","timestamp":1750149477000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Rattling\u2010Induced Ultralow Thermal Conductivity in Black Phosphorus Through Organic\u2010Molecule Intercalation"],"prefix":"10.1002","volume":"21","author":[{"given":"Shuai","family":"Duan","sequence":"first","affiliation":[{"name":"Laboratory of High Pressure Physics and Material Science (HPPMS) School of Physics and Physical Engineering Qufu Normal University  Qufu Shandong 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