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However, comparative studies of charge transport in these two junction types are limited. Here, a highly conjugated pyrene derivative has been engineered to construct both single\u2010molecule and monolayer junctions. The charge transport within these junctions has been examined systematically through theoretical simulations and electrical measurements. These studies demonstrate a distinct transition in a single molecule from temperature\u2010independent coherent tunneling to temperature\u2010dependent incoherent transport, indicating vibration\u2010mediated transport, while vibration\u2010suppressed coherent transport is observed in a densely packed monolayer. Additionally, anisotropic gating experiments reveal that parallel fields relative to the molecular connection modulate energy levels more efficiently in comparison with perpendicular fields. These findings enrich our understanding of molecular electronic transport and pave the way for diverse developments in the field of molecular electronic devices.<\/jats:p>","DOI":"10.1002\/anie.202508708","type":"journal-article","created":{"date-parts":[[2025,7,30]],"date-time":"2025-07-30T07:13:58Z","timestamp":1753859638000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Distinct Charge Transport and its Regulation in Single\u2010Molecule and Monolayer Junctions"],"prefix":"10.1002","volume":"64","author":[{"given":"Lan","family":"Yang","sequence":"first","affiliation":[{"name":"Center of Single\u2010Molecule Sciences Institute of Modern Optics Frontiers Science Center for New Organic Matter Tianjin Key Laboratory of Microscale Optical Information Science and Technology College of Electronic Information and Optical Engineering Nankai University  38 Tongyan Road Jinnan District Tianjin 300350 P.R. 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