Issue 33, 2021

Understanding the structural and charge transport property relationships for a variety of merocyanine single-crystals: a bottom up computational investigation

Abstract

Merocyanines consist of electronic donor (D) and acceptor (A) subunits connected via a methine bridge. They are highly polar organic π-conjugated molecules investigated for their self-assembly and optoelectronic properties. The accurate description of their structure–property relationships remains challenging. We report a comprehensive analysis modelling intra- and inter-molecular charge transport parameters for a library of merocyanines featuring different D/A combinations and lateral substituents. We found that constrained DFT correctly assesses the molecular and electronic structure in single crystals. The most effective charge transport pathways were identified and charge carrier mobilities were computed. We analyzed a large variety of single crystals highlighting the impact of alkyl substituents and casting conditions, drawing clear structure vs. charge transport relationships. Our modelling suggests that hole transport is maximized when dipolar molecules are packed in slipped not centrosymmetric pairs, arranged in 2D interconnected architectures. Computed and experimental charge mobilities for single crystals are in good agreement.

Graphical abstract: Understanding the structural and charge transport property relationships for a variety of merocyanine single-crystals: a bottom up computational investigation

Supplementary files

Article information

Article type
Paper
Submitted
01 abr 2021
Accepted
16 jun 2021
First published
16 jun 2021

J. Mater. Chem. C, 2021,9, 10851-10864

Understanding the structural and charge transport property relationships for a variety of merocyanine single-crystals: a bottom up computational investigation

N. Gildemeister, G. Ricci, L. Böhner, J. M. Neudörfl, D. Hertel, F. Würthner, F. Negri, K. Meerholz and D. Fazzi, J. Mater. Chem. C, 2021, 9, 10851 DOI: 10.1039/D1TC01511G

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