Realizing nearly-free-electron like conduction band in a molecular film through mediating intermolecular van der Waals interactions

Xingxia Cui, Ding Han, Hongli Guo, Linwei Zhou, Jingsi Qiao, Qing Liu, Zhihao Cui, Yafei Li, Chungwei Lin, Limin Cao, Wei Ji (), Hrvoje Petek () and Min Feng ()
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Xingxia Cui: Wuhan University
Ding Han: Wuhan University
Hongli Guo: Wuhan University
Linwei Zhou: Renmin University of China
Jingsi Qiao: Renmin University of China
Qing Liu: Wuhan University
Zhihao Cui: Wuhan University
Yafei Li: Wuhan University
Chungwei Lin: Mitsubishi Electric Research Laboratories
Limin Cao: Wuhan University
Wei Ji: Renmin University of China
Hrvoje Petek: University of Pittsburgh
Min Feng: Wuhan University

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Collective molecular physical properties can be enhanced from their intrinsic characteristics by templating at material interfaces. Here we report how a black phosphorous (BP) substrate concatenates a nearly-free-electron (NFE) like conduction band of a C60 monolayer. Scanning tunneling microscopy reveals the C60 lowest unoccupied molecular orbital (LUMO) band is strongly delocalized in two-dimensions, which is unprecedented for a molecular semiconductor. Experiment and theory show van der Waals forces between C60 and BP reduce the inter-C60 distance and cause mutual orientation, thereby optimizing the π-π wave function overlap and forming the NFE-like band. Electronic structure and carrier mobility calculations predict that the NFE band of C60 acquires an effective mass of 0.53–0.70 me (me is the mass of free electrons), and has carrier mobility of ~200 to 440 cm2V−1s−1. The substrate-mediated intermolecular van der Waals interactions provide a route to enhance charge delocalization in fullerenes and other organic semiconductors.

Date: 2019
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DOI: 10.1038/s41467-019-11300-y

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