发表机构
Simons Center for Computational Physical Chemistry at New York University; Department of Chemistry, New York University; Department of Physics, New York University（纽约大学西蒙计算物理化学中心; 纽约大学化学系; 纽约大学物理系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过半经典映射方法，发现单分子结的稳态电流可直接反映强光-物质耦合特征，并验证其对多种环境因素的鲁棒性，为纳米尺度光-物质相互作用提供新的探测与控制工具。
AI 中文摘要
强光-物质耦合为控制分子性质提供了令人兴奋的机会，但从集体效应中分辨单分子行为仍然是一个挑战。最近在扫描隧道显微镜断裂结（STM-BJs）中的实验已经证明了单分子水平的强光-物质耦合。由于STM-BJs能够直接获取分子结电流，我们研究了强耦合是否在输运中留下可测量的指纹，从而可能超越光学光谱来探测极化激元态。使用一种用于非平衡量子输运的半经典映射方法，我们发现稳态电流确实携带了单分子强耦合的直接特征。我们测试了该特征对电极连接性、核运动、空间结构的电磁模式和溶剂效应的鲁棒性。虽然环境因素和核运动重塑了该特征，但电流不是被动响应，而是受到耦合分子动力学的主动影响。我们的工作确立了电流作为解释和控制纳米尺度结中强光-物质相互作用的工具。
英文摘要
Strong light-matter coupling offers exciting opportunities for controlling molecular properties, yet resolving single-molecule behavior from collective effects remains a challenge. Recent experiments in scanning tunneling microscope break junctions (STM-BJs) have demonstrated strong light-matter coupling at the single-molecule level. Because STM-BJs provide direct access to molecular-junction currents, we investigate whether strong coupling leaves a measurable fingerprint in transport, potentially probing polaritonic states beyond optical spectroscopy. Using a semiclassical mapping approach for nonequilibrium quantum transport, we find that steady-state current indeed carries a direct signature of single-molecule strong coupling. We test the robustness of this signature against electrode connectivity, nuclear motion, spatially structured electromagnetic modes, and solvent effects. While environmental factors and nuclear motion reshape the signature, the current is not a passive response but is actively influenced by coupled molecular dynamics. Our work establishes current as a tool to interpret and control strong light-matter interactions in nanoscale junctions.
Comments19 pages, 8 figures
