Molecular Donor-Bridge-Acceptor Strategies for High-Capacitance Organic Dielectric Materials

Henry M. Heitzer, Tobin J Marks, Mark A Ratner

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

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. (Figure Presented).

Original languageEnglish
Pages (from-to)7189-7196
Number of pages8
JournalJournal of the American Chemical Society
Volume137
Issue number22
DOIs
Publication statusPublished - Jun 10 2015

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Optics and Photonics
Semiconductors
Capacitance
History
Permittivity
Molecular electronics
squaraine
Photonics
Density functional theory
Monolayers
Transistors
Electric fields
Semiconductor materials
Thin films
Molecules

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Molecular Donor-Bridge-Acceptor Strategies for High-Capacitance Organic Dielectric Materials. / Heitzer, Henry M.; Marks, Tobin J; Ratner, Mark A.

In: Journal of the American Chemical Society, Vol. 137, No. 22, 10.06.2015, p. 7189-7196.

Research output: Contribution to journalArticle

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