Establishing Self‐Dopant Design Principles from Structure–Function Relationships in Self‐n‐Doped Perylene Diimide Organic Semiconductors
Year: 2022
Type: article
Abstract: Self-doping is a particular doping method that has been applied to a wide range of organic semiconductors. However, there is a lack of understanding regarding the relationship between dopant structure and function. A structurally diverse series of self-n-doped perylene diimides (PDIs) is investigated to study the impact of steric encumbrance, counterion selection, and dopant/PDI tether distance on functional parameters such as doping, stability, morphology, and charge-carrier mobility. The studies show that self-n-doping is best enabled by the use of sterically encumbered ammoniums with short tethers and Lewis basic counterions. Additionally, water is found to inhibit doping, which concludes that thermal degradation is merely a phenomenological feature of certain dopants, and that residual solvent evaporation is the primary driver of thermally activated doping. In situ grazing-incidence wide-angle X-ray scattering studies show that sample annealing increases the π-π stacking distance and shrinks grain boundaries for improved long-range ordering. These features are then correlated to contactless carrier-mobility measurements with time-resolved microwave conductivity before and after thermal annealing. The collective relationships between structural features and functionality are finally used to establish explicit self-n-dopant design principles for the future design of materials with improved functionality.
Source: Advanced Materials
Institutions: University of Utah, Oregon State University
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, U.S. Department of Energy, Alfred P. Sloan Foundation, Camille and Henry Dreyfus Foundation, Office of Science, Division of Materials Research, Division of Chemical, Bioengineering, Environmental, and Transport Systems, Division of Electrical, Communications and Cyber Systems, Brookhaven National Laboratory
Awards: G1229526393, G1285306620, G2371548206, G241279073, G303061748, G3262563802, G3312677199, G357145406, Developing in operando structure-property-function guidelines for small molecule organic electron acceptors and its implication on device performance and charge carrier mobility, G4654690619, G4751775515, G495301720, G498139845, EAGER: manipulating spin dynamics in thionated perylene diimide organic semiconductors: towards organic spin caloritronic devices, G5570207115, G5765906131, CAS: Magnetic moment-induced adaptability of vertically-oriented 1D electrochemical systems, G7463374569, G7562191352, G7904176522, G8382000481, CAREER:Electro-Optical Logic Gates Based on Perovskite Phototransistors, G872144517, G969889393
OpenAlex ID: W4293696597