Michael Verhage, Pantelis Bampoulis, Marco D. Preuss, Ivo Filot, Rick R. M. Joosten, Heiner Friedrich, E. W. Meijer, Kees Flipse
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引用次数: 0
摘要
手性诱导的自旋选择性(CISS)效应是一种迷人的现象,它将分子结构与电子自旋极化(SP)联系在一起。量化自旋过滤幅度的实验程序广泛使用了磁场依赖性导电原子力显微镜。本文研究了酰亚胺取代冠烯双酰亚胺((S)-CBI-GCH)的手性晶体,以解释电流-电压 I - V 光谱的动态,并探究叠加峰的起源。一种动态的电压-扫描速率相关现象会产生复杂的 I - V 曲线。具有电荷局部化能力的氧化还原基团作为局部状态干扰了 π - π 堆积的连续性,从而产生了法诺共振。该研究引入了一种新的动态传输机制,让我们深入了解了瞬时电荷极化引导下,结晶的 CBI-GCH 分子在金属基底上吸收后产生自旋极化电荷的原因。最重要的是,传输过程中电荷局部化和脱局部化之间的干扰可能是理解静电力显微镜观察到的磁旋现象的重要特性。最后,我们观察到电荷捕获灵敏地改变了注入屏障,从直接隧道传输变为福勒-诺德海姆隧道传输,从而支持了该类分子在 CISS 中的非线性。
Chirality-Induced Magnetic Polarization by Charge Localization in a Chiral Supramolecular Crystal
The chirality-induced spin selectivity (CISS) effect is a fascinating phenomenon that correlates the molecular structure with electron spin-polarization (SP). Experimental procedures to quantify the spin-filtering magnitude have extensively used magnetic-field-dependent conductive AFM. In this work chiral crystals of imide-substituted coronene bisimide ((S)-CBI-GCH) are studied to explain the dynamics of the current–voltage I − V spectra and the origin of superimposed peaks are investigated. A dynamic voltage-sweep rate-dependent phenomenon can give rise to complex I − V curves. The redox group, capable of localization of charge, acts as a localized state that interferes with the continuum of the π – π stacking, giving rise to Fano resonances. A novel mechanism for dynamic transport is introduced, which provides insight into the origin of spin-polarized charge in crystallized CBI-GCH molecules after absorption on a metallic substrate, guided by transient charge polarization. Crucially, interference between charge localization and delocalization during transport may be important properties in understanding the magnetochiral phenomena observed by electrostatic force microscopy. Finally, it is observed that charge trapping sensitively modifies the injection barrier from direct tunneling to Fowler–Nordheim tunneling transport supporting nonlinearity in CISS for this class of molecules.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.