{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,23]],"date-time":"2026-10-23T19:44:48Z","timestamp":1792784688382,"version":"4.5.0"},"reference-count":44,"publisher":"American Chemical Society (ACS)","issue":"42","license":[{"start":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T00:00:00Z","timestamp":1791504000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T00:00:00Z","timestamp":1791504000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T00:00:00Z","timestamp":1791504000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100002858","name":"China Postdoctoral Science Foundation","doi-asserted-by":"publisher","award":["2024M762729"],"award-info":[{"award-number":["2024M762729"]}],"id":[{"id":"10.13039\/501100002858","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100004608","name":"Natural Science Foundation of Jiangsu Province","doi-asserted-by":"publisher","award":["BK20230555"],"award-info":[{"award-number":["BK20230555"]}],"id":[{"id":"10.13039\/501100004608","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Natural Science Foundation of Jiangsu Higher Education Institutions of China","award":["23KJB140019"],"award-info":[{"award-number":["23KJB140019"]}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["12304300"],"award-info":[{"award-number":["12304300"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["12604427"],"award-info":[{"award-number":["12604427"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,10,22]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Ultrafast optical control of spin states offers a promising route to molecular-scale magnetic manipulation, yet the mechanisms of laser-driven spin dynamics in atomically precise clusters remain poorly understood. Here, we investigate the ultrafast spin dynamics of the endohedral Mn@Sn12 cluster using real-time time-dependent density functional theory simulations. Strong Mn 3d\u2013Sn 5p orbital hybridization couples the localized Mn center to the Sn12 cage. Upon femtosecond laser excitation, the Mn@Sn12 cluster exhibits a pronounced transient magnetic response within several femtoseconds, accompanied by changes in the local magnetic moments of both subsystems. Time-dependent analyses of spin-resolved electronic occupations, spin density, and density of states provide evidence for early time intersite redistribution of spin-polarized electronic populations between the Mn center and Sn12 cage. Excited-state relaxation analysis further shows that spin-conserving relaxation is substantially faster than spin-flip relaxation, reflecting efficient electron\u2013vibration coupling and limited spin\u2013orbit-mediated mixing between opposite-spin states. These results elucidate the microscopic origin of ultrafast spin dynamics in molecular nanoclusters and highlight endohedral metal clusters as promising platforms for atomic-scale optical spin control.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02587","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T14:02:00Z","timestamp":1791554520000},"page":"12118-12124","source":"Crossref","is-referenced-by-count":0,"title":["Ultrafast Core\u2013Shell\nSpin Transfer and Spin-Selective\nRelaxation in an Endohedral Cage Cluster"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6497-9209","authenticated-orcid":true,"given":"Xueke","family":"Yu","sequence":"first","affiliation":[{"name":"Yangzhou University , , ,","place":["Jiangsu, China, 225009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi","family":"Gao","sequence":"additional","affiliation":[{"name":"Yangzhou University , , ,","place":["Jiangsu, China, 225009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Chen","sequence":"additional","affiliation":[{"name":"Yangzhou University , , ,","place":["Jiangsu, China, 225009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7367-4618","authenticated-orcid":true,"given":"Wei","family":"Pei","sequence":"additional","affiliation":[{"name":"Yangzhou University , , ,","place":["Jiangsu, China, 225009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8618-2751","authenticated-orcid":true,"given":"Xiuyun","family":"Zhang","sequence":"additional","affiliation":[{"name":"Yangzhou University , , ,","place":["Jiangsu, China, 225009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5669-9015","authenticated-orcid":true,"given":"Yan","family":"Su","sequence":"additional","affiliation":[{"name":"Ion and Electron Beams (Dalian University of Technology), Ministry of Education , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3263-7159","authenticated-orcid":true,"given":"Jijun","family":"Zhao","sequence":"additional","affiliation":[{"name":"South China Normal University , , ,","place":["Guangzhou, China, 510006"]},{"name":"South China Normal University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,9]]},"reference":[{"issue":"14","key":"2026102208021437800_cit1","doi-asserted-by":"publisher","first-page":"3025","DOI":"10.1103\/PhysRevLett.85.3025","article-title":"Laser-Induced Ultrafast Demagnetization in Ferromagnetic\nMetals","volume":"85","author":"Zhang","year":"2000","journal-title":"Phys. Rev. Lett."},{"issue":"11","key":"2026102208021437800_cit2","doi-asserted-by":"publisher","first-page":"855","DOI":"10.1038\/nphys1092","article-title":"Control of speed and efficiency of\nultrafast demagnetization by direct transfer of spin angular momentum","volume":"4","author":"Malinowski","year":"2008","journal-title":"Nat. Phys."},{"issue":"3","key":"2026102208021437800_cit3","doi-asserted-by":"publisher","first-page":"2731","DOI":"10.1103\/RevModPhys.82.2731","article-title":"Ultrafast\noptical manipulation of\nmagnetic order","volume":"82","author":"Kirilyuk","year":"2010","journal-title":"Rev. Mod. Phys."},{"issue":"26","key":"2026102208021437800_cit4","doi-asserted-by":"publisher","first-page":"27688","DOI":"10.1021\/jacs.6c07842","article-title":"Structure-Induced Spin\nSwitching in Triple-Decker Metal-Ring-Metal\nNanoclusters","volume":"148","author":"Zhou","year":"2026","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026102208021437800_cit5","doi-asserted-by":"publisher","first-page":"748","DOI":"10.1038\/s41467-022-28328-2","article-title":"Optical charge\ninjection and coherent control of a quantum-dot spin-qubit emitting\nat telecom wavelengths","volume":"13","author":"Dusanowski","year":"2022","journal-title":"Nat. Commun."},{"issue":"1","key":"2026102208021437800_cit6","doi-asserted-by":"publisher","first-page":"445","DOI":"10.1038\/s41467-023-36164-1","article-title":"Accelerating ultrafast\nmagnetization reversal by non-local spin transfer","volume":"14","author":"Remy","year":"2023","journal-title":"Nat. Commun."},{"issue":"25","key":"2026102208021437800_cit7","doi-asserted-by":"publisher","first-page":"7094","DOI":"10.1021\/acs.jpclett.6c01548","article-title":"Transient Laser-Induced Magnetic Order and Relaxation\nPathways in\nTiCrCT2 (T = O, F) MXenes","volume":"17","author":"Yu","year":"2026","journal-title":"J. Phys.\nChem. Lett."},{"issue":"18","key":"2026102208021437800_cit8","doi-asserted-by":"publisher","first-page":"11732","DOI":"10.1021\/acsnano.3c12926","article-title":"Laser-Induced Ultrafast\nSpin Injection in All-Semiconductor Magnetic CrI3\/WSe2 Heterobilayer","volume":"18","author":"Guo","year":"2024","journal-title":"ACS Nano"},{"issue":"4","key":"2026102208021437800_cit9","doi-asserted-by":"publisher","first-page":"529","DOI":"10.1038\/s41567-022-01908-1","article-title":"Coupling of terahertz light with\nnanometre-wavelength magnon modes via spin-orbit torque","volume":"19","author":"Salikhov","year":"2023","journal-title":"Nat. Phys."},{"issue":"11","key":"2026102208021437800_cit10","doi-asserted-by":"publisher","first-page":"879","DOI":"10.1038\/nphys1767","article-title":"Thermally\ndriven\nspin injection from a ferromagnet into a non-magnetic metal","volume":"6","author":"Slachter","year":"2010","journal-title":"Nat. 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Mater."},{"issue":"1","key":"2026102208021437800_cit14","doi-asserted-by":"publisher","first-page":"538","DOI":"10.1038\/s41467-023-36166-z","article-title":"The importance\nof the interface for picosecond spin pumping in antiferromagnet-heavy\nmetal heterostructures","volume":"14","author":"Kholid","year":"2023","journal-title":"Nat. Commun."},{"issue":"2","key":"2026102208021437800_cit15","doi-asserted-by":"publisher","first-page":"021006","DOI":"10.1103\/PhysRevX.2.021006","article-title":"Temperature\nDependence of Laser-Induced Demagnetization in Ni: A Key for Identifying\nthe Underlying Mechanism","volume":"2","author":"Roth","year":"2012","journal-title":"Phys. Rev. X"},{"issue":"3","key":"2026102208021437800_cit16","doi-asserted-by":"publisher","first-page":"259","DOI":"10.1038\/nmat2593","article-title":"Explaining\nthe paradoxical diversity of ultrafast laser-induced demagnetization","volume":"9","author":"Koopmans","year":"2010","journal-title":"Nat. Mater."},{"issue":"20","key":"2026102208021437800_cit17","doi-asserted-by":"publisher","first-page":"207201","DOI":"10.1103\/PhysRevLett.107.207201","article-title":"Ab Initio investigation of the Elliott-Yafet\nelectron-phonon mechanism in laser-induced ultrafast demagnetization","volume":"107","author":"Carva","year":"2011","journal-title":"Phys. Rev. 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Electron."},{"issue":"2","key":"2026102208021437800_cit24","doi-asserted-by":"publisher","first-page":"023116","DOI":"10.1103\/PhysRevResearch.3.023116","article-title":"Terahertz\nspin dynamics driven by\nan optical spin-orbit torque","volume":"3","author":"Mondal","year":"2021","journal-title":"Phys. Rev. Res."},{"issue":"50","key":"2026102208021437800_cit25","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adi1618","article-title":"Light-induced\nultrafast spin transport\nin multilayer metallic films originates from sp-d spin exchange coupling","volume":"9","author":"Chen","year":"2023","journal-title":"Sci. Adv."},{"issue":"3","key":"2026102208021437800_cit26","doi-asserted-by":"publisher","first-page":"1842","DOI":"10.1021\/acs.nanolett.7b05118","article-title":"Laser-Induced\nIntersite Spin Transfer","volume":"18","author":"Dewhurst","year":"2018","journal-title":"Nano Lett."},{"issue":"7764","key":"2026102208021437800_cit27","doi-asserted-by":"publisher","first-page":"240","DOI":"10.1038\/s41586-019-1333-x","article-title":"Light-wave dynamic\ncontrol of magnetism","volume":"571","author":"Siegrist","year":"2019","journal-title":"Nature"},{"issue":"7","key":"2026102208021437800_cit28","doi-asserted-by":"publisher","first-page":"3237","DOI":"10.1021\/acs.nanolett.1c00520","article-title":"Unravelling\nPhotoinduced Interlayer Spin Transfer Dynamics in Two-Dimensional\nNonmagnetic-Ferromagnetic van der Waals Heterostructures","volume":"21","author":"He","year":"2021","journal-title":"Nano Lett."},{"issue":"24","key":"2026102208021437800_cit29","doi-asserted-by":"publisher","first-page":"245411","DOI":"10.1103\/PhysRevB.103.245411","article-title":"Ultralong\nlifetime for fully photogenerated spin-polarized\ncurrent in two-dimensional ferromagnetic\/nonmagnetic semiconductor\nheterostructures","volume":"103","author":"Zhou","year":"2021","journal-title":"Phys. Rev. B"},{"issue":"3","key":"2026102208021437800_cit30","doi-asserted-by":"publisher","first-page":"782","DOI":"10.1021\/acs.jpclett.4c03279","article-title":"Ultrafast\nLaser-Induced Spin Dynamics in All-Semiconductor Ferromagnetic CrSBr-Phosphorene\nHeterostructures","volume":"16","author":"Huo","year":"2025","journal-title":"J. Phys. Chem. Lett."},{"issue":"25","key":"2026102208021437800_cit31","doi-asserted-by":"publisher","first-page":"14361","DOI":"10.1021\/acs.inorgchem.6c02063","article-title":"Coupled Electronic and Structural Dynamics Enable Spin Switching\nin Endohedral Fullerenes","volume":"65","author":"Song","year":"2026","journal-title":"Inorg. Chem."},{"issue":"43","key":"2026102208021437800_cit32","doi-asserted-by":"publisher","first-page":"2507144","DOI":"10.1002\/adfm.202507144","article-title":"Heteroatomic Doping Induces High-Low Spin Isomers in Atomically Precise\nAu Nanoclusters","volume":"35","author":"Yang","year":"2025","journal-title":"Adv. Funct. Mater."},{"key":"2026102208021437800_cit33","volume-title":"Gaussian\n16","author":"Frisch","year":"2016"},{"issue":"18","key":"2026102208021437800_cit34","doi-asserted-by":"publisher","first-page":"3865","DOI":"10.1103\/PhysRevLett.77.3865","article-title":"Generalized Gradient Approximation\nMade Simple","volume":"77","author":"Perdew","year":"1996","journal-title":"Phys. Rev. Lett."},{"issue":"34","key":"2026102208021437800_cit35","doi-asserted-by":"publisher","first-page":"8111","DOI":"10.1021\/jp011945l","article-title":"Addition of Polarization and Diffuse Functions to the\nLANL2DZ Basis Set for P-Block Elements","volume":"105","author":"Check","year":"2001","journal-title":"J. Phys.\nChem. A"},{"issue":"5","key":"2026102208021437800_cit36","doi-asserted-by":"publisher","first-page":"580","DOI":"10.1002\/jcc.22885","article-title":"Multiwfn: A multifunctional wavefunction analyzer","volume":"33","author":"Lu","year":"2012","journal-title":"J. Comput. 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Sci."},{"issue":"13","key":"2026102208021437800_cit40","doi-asserted-by":"publisher","first-page":"133401","DOI":"10.1103\/PhysRevLett.111.133401","article-title":"Stern-Gerlach\nExperiments on Mn@Sn12: Identification\nof a Paramagnetic Superatom and Vibrationally Induced Spin Orientation","volume":"111","author":"Rohrmann","year":"2013","journal-title":"Phys. Rev. Lett."},{"issue":"10","key":"2026102208021437800_cit41","doi-asserted-by":"publisher","first-page":"1192","DOI":"10.1039\/D2NH00281G","article-title":"Tuning photoelectron\ndynamic behavior of thiolate-protected\nMAu24 nanoclusters via heteroatom substitution","volume":"7","author":"Yu","year":"2022","journal-title":"Nanoscale Horiz."},{"issue":"49","key":"2026102208021437800_cit42","doi-asserted-by":"publisher","first-page":"20450","DOI":"10.1021\/acs.inorgchem.3c03482","article-title":"Core-Packing-Related\nVibrational Properties of Thiol-Protected Gold Nanoclusters and Their\nExcited-State Behavior","volume":"62","author":"Yu","year":"2023","journal-title":"Inorg. Chem."},{"issue":"1","key":"2026102208021437800_cit43","doi-asserted-by":"publisher","first-page":"5069","DOI":"10.1038\/s41467-026-73780-z","article-title":"Giant magnetic moment increase by\nultrafast laser light","volume":"17","author":"Sharma","year":"2026","journal-title":"Nat. Commun."},{"issue":"20","key":"2026102208021437800_cit44","doi-asserted-by":"publisher","first-page":"205414","DOI":"10.1103\/dr3g-2zrk","article-title":"Ultrafast spin dynamics in magnetic\/nonmagnetic two-dimensional\ninterfaces: Insights from CrX3\/WZ2 heterostructures\n(X = Br, I; Z = S, Se)","volume":"112","author":"Li","year":"2025","journal-title":"Phys. Rev. B"}],"container-title":["The Journal of Physical\nChemistry Letters"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acs.jpclett.6c02587","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/42\/12118\/68799105\/acs.jpclett.6c02587.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/42\/12118\/68799105\/acs.jpclett.6c02587.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T12:49:07Z","timestamp":1792673347000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article\/17\/42\/12118\/5447746\/Ultrafast-Core-Shell-Spin-Transfer-and-Spin"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,10,9]]},"references-count":44,"journal-issue":{"issue":"42","published-online":{"date-parts":[[2026,10,9]]},"published-print":{"date-parts":[[2026,10,22]]}},"URL":"https:\/\/doi.org\/10.1021\/acs.jpclett.6c02587","relation":{},"ISSN":["1948-7185"],"issn-type":[{"value":"1948-7185","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,10,9]]}}}