Fundamental Gaps of Condensed-Phase Organic Semiconductors from Single-Molecule Calculations using Polarization-Consistent Optimally Tuned Screened Range-Separated Hybrid Functionals

Srijana Bhandari, Margaret S. Cheung, Eitan Geva, Leeor Kronik, Barry D. Dunietz

Research output: Contribution to journalArticlepeer-review

Abstract

Range-separated hybrid (RSH) functionals have been shown to overcome the tendency of traditional density functional theory to underestimate the fundamental orbital gap. More recently, the screened RSH (SRSH) approach has been developed as a means to extend these functionals to address the effect of the electrostatic environment on the fundamental gap. Here, we report a scheme that combines the SRSH formulation with the polarized continuum model (PCM) within a consistent framework for addressing long-range screened electrostatic interactions, which is further improved by optimal tuning (OT). The quantitative predictive power of the new OT-SRSH-PCM scheme by addressing fundamental gaps in thin films of organic semiconducting materials. This is especially impressive as the approach is based on single molecule calculations. We also discuss the advantages of this approach over alternative schemes combining PCM with RSH. In particular, we show that it avoids the well-documented tendency of standard OT to collapse the range separation parameter when performed within a dielectric continuum.

Original languageEnglish
Pages (from-to)6287-6294
Number of pages8
JournalJournal of Chemical Theory and Computation
Volume14
Issue number12
DOIs
StatePublished - 11 Dec 2018

All Science Journal Classification (ASJC) codes

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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