Charge transport properties of open-shell graphene fragments: a computational study of the phenalenyl tilings

Literature Information

Publication Date 2020-11-23
DOI 10.1039/D0CP03140B
Impact Factor 3.676
Authors

Wei-Chih Chen, Ito Chao


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Abstract

Thinking outside the box of the phenalenyl radical: a systematic structure design strategy, phenalenyl tiling, is found to benefit the electron transport properties of open-shell graphene fragments with one free radical. Compared with the closed-shell species, phenalenyl-based π-radicals exhibit smaller intramolecular reorganization energies and larger intermolecular electronic couplings. However, the on-site Coulomb repulsion can be too strong and impedes the charge transport efficiency of such materials. The repulsion can be weakened in radical species by spin delocalization. In this paper, the extended π-radicals we studied are categorized into three types of open-shell structures: the zigzag, the armchair and the discotic odd alternant hydrocarbons. The latter two belong to phenalenyl tilings. We found that the phenalenyl tilings fully inherit the desirable features of the singly occupied molecular orbital of the phenalenyl radical in a predictable and delocalized fashion, and their on-site Coulomb repulsion is effectively reduced. The zigzag π-radicals are less satisfactory. Therefore, the phenalenyl tilings are favorable candidates for charge transporting materials.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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