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Solid State Dilution Controls Marcus Inverted Transport in Rectifying Molecular Junctions

Authors
Kang, HunguKong, Gyu DonYoon, Hyo Jae
Issue Date
28-1월-2021
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.12, no.3, pp.982 - 988
Indexed
SCIE
SCOPUS
Journal Title
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume
12
Number
3
Start Page
982
End Page
988
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/50056
DOI
10.1021/acs.jpclett.0c03251
ISSN
1948-7185
Abstract
Traditional Marcus theory accounts for electron transfer reactions in solutions, and the polarity of solvent molecule matters for them. How such an environment polarity affects electron transfer reactions in solid-state devices, however, remains uncertain. This paper describes how the Marcus inverted charge transport is influenced by solid-state molecular dilution in large-area tunneling junctions. A monolayer of 2,2'-bipyridyl terminated n-alkanethiolate (SC11BIPY), which rectifies currents via electron hopping within the inverted regime, is diluted with n-alkanethiolate (SCn) of different lengths (n = 8, 10, or 18) or at different surface mole fractions. The dilution introduces nonpolar environments within the monolayer, hinders stabilization of charged BIPY species upon electron hopping, and pushes the equilibrium of BIPY reversible arrow BIPY center dot- process toward the reverse direction. Our work demonstrates that solid-state molecular dilution permits systematic control of the environment polarity of active component in nanoscale devices, much like solvent polarity control in solution, and their performances.
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