Harnessing Quantum Interference in Molecular Dielectric Materials

Bergfield, Justin P.; Heitzer, Henry M.; Van Dyck, Colin; Marks, Tobin J.; Ratner, Mark A.

doi:10.1021/acsnano.5b02042

Title: Harnessing Quantum Interference in Molecular Dielectric Materials

Journal Article · Tue May 26 00:00:00 EDT 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b02042· OSTI ID:1370551

Bergfield, Justin P. ^[1]; Heitzer, Henry M. ^[1]; Van Dyck, Colin ^[1]; Marks, Tobin J. ^[1]; Ratner, Mark A. ^[1]

Northwestern Univ., Evanston, IL (United States)

We investigate the relationship between dielectric response and charge transport in molecule-based materials operating in the quantum coherent regime. We find that quantum interference affects these observables differently, for instance, allowing current passing through certain materials to be reduced by orders of magnitude without affecting dielectric behavior (or band gap). As an example, we utilize ab initio electronic structure theory to calculate conductance and dielectric constants of cross-conjugated anthraquinone (AQ)-based and linearly conjugated anthracene (AC)-based materials. In spite of having nearly equal fundamental gaps, electrode bonding configurations, and molecular dimensions, we find a ~1.7 order of magnitude (~50-fold) reduction in the conductance of the AQ-based material relative to the AC-based material, a value in close agreement with recent measurements, while the calculated dielectric constants of both materials are nearly identical. From these results, we propose two molecular materials in which quantum interference is used to reduce leakage currents across a ~25 Å monolayer gap with dielectric constants larger than 4.5.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Belgian American Educational Foundation (BAEF)

Grant/Contract Number:: SC0000989; DMR-1121262

OSTI ID:: 1370551

Journal Information:: ACS Nano, Vol. 9, Issue 6; Related Information: CBES partners with Northwestern University (lead); Harvard University; New York University; Pennsylvania State University; University of Michigan; University of Pittsburgh; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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Controlling destructive quantum interference in tunneling junctions comprising self-assembled monolayers via bond topology and functional groups Zhang, Yanxi; Ye, Gang; Soni, Saurabh Chemical Science, Vol. 9, Issue 19 https://doi.org/10.1039/c8sc00165k	journal	January 2018
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Title: Harnessing Quantum Interference in Molecular Dielectric Materials

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