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However, implementing this strategy is nontrivial for metal nanocluster building blocks, due to the limited functional modification of nanoclusters and complexity of their emission mechanism. In this report, we demonstrate that a gold nanocluster modified by 4,6\u2010diamino\u20102\u2010pyrimidinethiol (DPT\u2010AuNCs) self\u2010assembles into two distinct aggregation structures in methanol (MeOH)\/water mixed solvent, thus exhibiting pathway complexity. Kinetic studies show that DPT\u2010AuNCs firstly assembles into non\u2010luminescent nanofibers (kinetically controlled), which further transforms into strongly luminescent microflowers (thermodynamically controlled). In\u2010depth analysis of the assembly mechanism reveals that the transformation of aggregation structures involves the disassembly of nanofibers and a subsequent nucleation\u2010growth process. Temperature\u2010dependent photoluminescence (PL) spectroscopy and infrared (IR) measurements reveal that inter\u2010cluster hydrogen bonding bridged by solvent molecules and C\u2212H\u22c5\u22c5\u22c5\u03c0 interaction are the key factors for emission enhancement. The photoluminescent property of DPT\u2010AuNCs can be controlled by varying the cosolvent in water, enabling DPT\u2010AuNCs to distinguish different kind of alcohols, particularly the isomerism n\u2010propanol (NPA) and isopropanol (IPA). Additionally, the addition of seeds effectively regulate the assembly kinetics of DPT\u2010AuNCs. This study advances our understanding of assembly pathways and improves the luminescent performance of nanoclusters (NCs).<\/jats:p>","DOI":"10.1002\/chem.202401909","type":"journal-article","created":{"date-parts":[[2024,7,7]],"date-time":"2024-07-07T22:40:11Z","timestamp":1720392011000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Gold Nanoclusters Whose Photoluminescent Properties are Dynamically Tunable by Modulating the Assembly Pathway Complexity"],"prefix":"10.1002","volume":"30","author":[{"given":"Jinglin","family":"Shen","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Laboratory of Catalytic Conversion and Clean Energy in Universities of Shandong Province Qufu Normal University  Qufu, Shandong 273165 P. R. 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