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Abstract Determining the relative energies of transport states in organic semiconductors is critical to understanding the properties of electronic devices and in designing device stacks. Futhermore, defect states are also highly important and can greatly impact material properties and device performance. Recently, energy‐resolved electrochemical impedance spectroscopy (ER‐EIS) is developed to probe both the ionization energy (IE) and electron affinity (EA) as well as sub‐bandgap defect states in organic semiconductors. Herein, ER‐EIS is compared to cyclic voltammetry (CV) and photoemission spectroscopies for extracting IE and EA values, and to photothermal deflection spectroscopy (PDS) for probing defect states in both polymer and molecular organic semiconductors. The results show that ER‐EIS determined IE and EA are in better agreement with photoemission spectroscopy measurements as compared to CV for both polymer and molecular materials. Furthermore, the defect states detected by ER‐EIS agree with sub‐bandgap features detected by PDS. Surprisingly, ER‐EIS measurements of regiorandom and regioregular poly(3‐hexylthiophene) (P3HT) show clear defect bands that occur at significantly different energies. In regioregular P3HT the defect band is near the edge of the occupied states while it is near the edge of the unoccupied states in regiorandom P3HT. 

Abstract Radiation therapy is one of the most prevalent procedures for cancer treatment, but the risks of malignancies induced by peripheral beam in healthy tissues surrounding the target is high. Therefore, being able to accurately measure the exposure dose is a critical aspect of patient care. Here a radiation detector based on an organic field‐effect transistor (RAD‐OFET) is introduced, an in vivo dosimeter that can be placed directly on a patient's skin to validate in real time the dose being delivered and ensure that for nearby regions an acceptable level of low dose is being received. This device reduces the errors faced by current technologies in approximating the dose profile in a patient's body, is sensitive for doses relevant to radiation treatment procedures, and robust when incorporated into conformal large‐area electronics. A model is proposed to describe the operation of RAD‐OFETs, based on the interplay between charge photogeneration and trapping. 

Abstract Optoelectronic properties of anisotropic crystals vary with direction requiring that the orientation of molecular organic semiconductor crystals is controlled in optoelectronic device active layers to achieve optimal performance. Here, a generalizable strategy to introduce periodic variations in the out‐of‐plane orientations of 5,11‐bis(triisopropylsilylethynyl)anthradithiophene (TIPS ADT) crystals is presented. TIPS ADT crystallized from the melt in the presence of 16 wt.% polyethylene (PE) forms banded spherulites of crystalline fibrils that twist in concert about the radial growth direction. These spherulites exhibit band‐dependent light absorption, photoluminescence, and Raman scattering depending on the local orientation of crystals. Mueller matrix imaging reveals strong circular extinction (CE), with TIPS ADT banded spherulites exhibiting domains of positive or negative CE signal depending on the crystal twisting sense. Furthermore, orientation‐dependent enhancement in charge injection and extraction in films of twisted TIPS ADT crystals compared to films of straight crystals is visualized in local conductive atomic force microscopy maps. This enhancement leads to 3.3‐ and 6.2‐times larger photocurrents and external quantum efficiencies, respectively, in photodetectors comprising twisted crystals than those comprising straight crystals. 

Abstract Polymer ferroelectrics are playing an increasingly active role in flexible memory application and wearable electronics. The relaxor ferroelectric dielectric, poly(vinylidene fluoride trifluorethylene (PVDF‐TrFE), although vastly used in organic field‐effect transistors (FETs), has issues with gate leakage current especially when the film thickness is below 500 nm. This work demonstrates a novel method of selective poling the dielectric layer. By using solution‐processed 6,13‐bis(triisopropylsilylethynyl)pentacene (TIPS‐pentacene) as the organic semiconductor, it is shown that textured poling of the PVDF‐TrFE layer dramatically improves FET properties compared to unpoled or uniformly poled ferroelectric films. The texturing is achieved by first vertically poling the PVDF‐TrFE film and then laterally poling the dielectric layer close to the gate electrode. TIPS‐pentacene FETs show on/off ratios of 10⁵and hole mobilities of 1 cm²Vs⁻¹under ambient conditions with operating voltages well below −5 V. The electric field distribution in the dielectric layer is simulated by using finite difference time domain methods.