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Rozylowicz, Kalee

Publications and source records attributed to Rozylowicz, Kalee.

Using Molecular Structure to Tune Intrachain and Interchain Charge Transport in Indacenodithiophene-Based Copolymers

Here, in this work, we compare two structurally near-amorphous rigid-rod polymers-poly(indacenodithiophene-co-benzothiadiazole), p(IDT-BT), and poly(indacenodithiophene-co-benzopyrollodione), p(IDT-BPD)-with orders of magnitude different mobilities to understand the effect charge carrier intrachain delocalization has on electronic transport. Quantum chemical calculations show that p(IDT-BPD) has a barrier to torsion that is significantly lower than that of p(IDT-BT) and is thus more likely to have reduced conjugation lengths. We utilize absorption and photoluminescence spectroscopy to characterize energetic disorder and show that p(IDT-BPD) has higher energetic disorder. Charge modulation spectroscopy (CMS) and model calculations are used to show that charge carriers are substantially delocalized in p(IDT-BT) and occupy near-uniform energetic environments. We find that mobility activated hopping barriers are similar in these two materials. Electronic structure calculations show that both intrachain and interchain couplings of monomer units are poor enough in p(IDT-BPD) that charge carriers collapse to single IDT units and transport via a through-space tunneling mechanism. This work highlights the remarkable charge transport properties of p(IDT-BT) by showing that high mobilities are achievable on device-relevant length scales with only 1D carrier delocalization.

36 MATERIALS SCIENCE↗

Tuning Organic Electrochemical Transistor Threshold Voltage using Chemically Doped Polymer Gates

Organic electrochemical transistors (OECTs) have shown promise as transducers and amplifiers of minute electronic potentials due to their large transconductances. Tuning the OECT threshold voltage is important to achieve low-powered devices with amplification properties within the desired operational voltage range. However, traditional design approaches have struggled to decouple channel and materials properties from threshold voltage, thereby compromising on several other OECT performance metrics, such as electrochemical stability, transconductance, and dynamic range. In this work, simple solution-processing methods are utilized to chemically dope polymer gate electrodes, thereby controlling their work function, which in turn tunes the operation voltage range of the OECTs without perturbing their channel properties. Chemical doping of initially air-sensitive polymer electrodes further improves their electrochemical stability in ambient conditions. Thus, OECTs that are simultaneously low-powered and electrochemically resistant to oxidative side reactions under ambient conditions are demonstrated. Furthermore, this approach shows that threshold voltage, which is once interwoven with other OECT properties, can in fact be an independent design parameter, expanding the design space of OECTs.

chemical doping↗