Molecular Donor--Bridge--Acceptor Strategies for High-Capacitance Organic Dielectric Materials.
Donor-bridge-acceptor (DBA) systems occupy a rich history in molecular electronics and photonics. A key property of DBA materials is their typically large and tunable (hyper)polarizabilities. While traditionally, classical descriptions such as the Clausius--Mossotti formalism have been used to relat...
| Published in: | Journal of the American Chemical Society Vol. 137; no. 22; pp. 7189 - 7197 |
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| Main Authors: | , , |
| Format: | Article |
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American Chemical Society
6/10/2015
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| Subjects: | |
| Online Access: | View this record in EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=103423835&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 103423835 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 6/10/2015 vid: 137 iid: 22 pid: 997 pub: American Chemical Society artinfo: ui: 103423835 10.1021/jacs.5b03301 ppf: 7189 ppct: 8 formats: tig: atl: Molecular Donor--Bridge--Acceptor Strategies for High-Capacitance Organic Dielectric Materials. aug: au: Heitzer, Henry M. Marks, Tobin J. Ratner, Mark A. affil: Department of Chemistry, Materials Research Center, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States su: Dielectric materials Photonics Imaging systems Condensed matter Thin films sug: subj: Dielectric materials Photonics Imaging systems Condensed matter Thin films ab: Donor-bridge-acceptor (DBA) systems occupy a rich history in molecular electronics and photonics. A key property of DBA materials is their typically large and tunable (hyper)polarizabilities. While traditionally, classical descriptions such as the Clausius--Mossotti formalism have been used to relate molecular polarizabilities to bulk dielectric response, recent work has shown that these classical equations are inadequate for numerous materials classes. Creating high-dielectric organic materials is critically important for utilizing unconventional semiconductors in electronic circuitry. Employing a plane-wave density functional theory formalism, we investigate the dielectric response of highly polarizable DBA molecule-based thin films. Such films are found to have large dielectric response arising from cooperative effects between donor and acceptor units when mediated by a conjugated bridge. Moreover, the dielectric response can be systematically tuned by altering the building block donor, acceptor, or bridge structures and is found to be nonlinearly dependent on electric field strength. The computed dielectric constants are largely independent of the density functional employed, and qualitative trends are readily evident. Remarkably large computed dielectric constants >15.0 and capacitances >6.0 µF/cm² are achieved for squaraine monolayers, significantly higher than in traditional organic dielectrics. Such calculations should provide a guide for designing high-capacitance organic dielectrics that should greatly enhance transistor performance. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2015 holdings: @attributes: islocal: N |
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