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Herein, we successfully design and fabricate the first example of MNC\u2010based spin valves (SVs) that exhibit remarkable magnetoresistance (MR) value up to 1.6\u2009% even at room temperature (300\u2005K). The concomitant photoresponse of MNC\u2010based SVs unambiguously confirms that the spin\u2010polarized electron transmission takes place across the MNC interlayer. Furthermore, the spin\u2010dependent transport property of MNC\u2010based SVs is largely varied by changing the atomic structure of MNCs. Both experimental proofs and quantum chemistry calculations reveal that the atomic structure\u2010discriminative spin transport behavior is attributed to the distinct spin\u2010orbit coupling (SOC) effect of MNCs.<\/jats:p>","DOI":"10.1002\/anie.202213208","type":"journal-article","created":{"date-parts":[[2022,11,29]],"date-time":"2022-11-29T17:44:46Z","timestamp":1669743886000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Room\u2010Temperature Spin Transport in Metal Nanocluster\u2010Based Spin Valves"],"prefix":"10.1002","volume":"62","author":[{"given":"Yanfei","family":"Zhu","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology  Beijing 100190 P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 P. R. 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