Sangmoo Choi

Stable organic field-effect transistors for continuous and nondestructive sensing of chemical and biologically relevant molecules in aqueous environment.

The use of organic field-effect transistors (OFETs) as sensors in aqueous media has gained increased attention for environmental monitoring and medical diagnostics. However, stable operation of OFETs in aqueous media is particularly challenging because of electrolytic hydrolysis of water, high ionic conduction through the analyte, and irreversible damage of organic semiconductors when exposed to water. To date, OFET sensors have shown the capability of label-free sensing of various chemical/biological species, but they could only be used once because their operational stability and lifetime while operating in aqueous environments has been poor, and their response times typically slow. Here, we report on OFETs with unprecedented water stability. These OFETs are suitable for the implementation of reusable chemical/biological sensors because they primarily respond to charged species diluted in an aqueous media by rapidly shifting their threshold voltage. These OFET sensors present stable current baselines and saturated signals which are ideal for detection of low concentration of small or large molecules that alter the pH of an aqueous environment. The overall response of these OFET sensors paves the way for the development of continuous chemical/biological nondestructive sensor applications in aqueous media.

Stable low-voltage operation top-gate organic field-effect transistors on cellulose nanocrystal substrates.

We report on the performance and the characterization of top-gate organic field-effect transistors (OFETs), comprising a bilayer gate dielectric of CYTOP/Al2O3 and a solution-processed semiconductor layer made of a blend of TIPS-pentacene:PTAA, fabricated on recyclable cellulose nanocrystal-glycerol (CNC/glycerol) substrates. These OFETs exhibit low operating voltage, low threshold voltage, an average field-effect mobility of 0.11 cm(2)/(V s), and good shelf and operational stability in ambient conditions. To improve the operational stability in ambient a passivation layer of Al2O3 is grown by atomic layer deposition (ALD) directly onto the CNC/glycerol substrates. This layer protects the organic semiconductor layer from moisture and other chemicals that can either permeate through or diffuse out of the substrate.

Solution-based electrical doping of semiconducting polymer films over a limited depth

Solution-based electrical doping protocols may allow more versatility in the design of organic electronic devices; yet, controlling the diffusion of dopants in organic semiconductors and their stability has proven challenging. Here we present a solution-based approach for electrical p-doping of films of donor conjugated organic semiconductors and their blends with acceptors over a limited depth with a decay constant of 10-20 nm by post-process immersion into a polyoxometalate solution (phosphomolybdic acid, PMA) in nitromethane. PMA-doped films show increased electrical conductivity and work function, reduced solubility in the processing solvent, and improved photo-oxidative stability in air. This approach is applicable to a variety of organic semiconductors used in photovoltaics and field-effect transistors. PMA doping over a limited depth of bulk heterojunction polymeric films, in which amine-containing polymers were mixed in the solution used for film formation, enables single-layer organic photovoltaic devices, processed at room temperature, with power conversion efficiencies up to 5.9 ± 0.2% and stable performance on shelf-lifetime studies at 60 °C for at least 280 h.

A Study on Reducing Contact Resistance in Solution-Processed Organic Field-Effect Transistors

We report on the reduction of contact resistance in solution-processed TIPS-pentacene (6,13-bis(triisopropylsilylethynyl)pentacene) and PTAA (poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine]) top-gate bottom-contact organic field-effect transistors (OFETs) by using different contact-modification strategies. The study compares the contact resistance values in devices that comprise Au source/drain electrodes either treated with 2,3,4,5,6-pentafluorothiophenol (PFBT), or modified with an evaporated thin layer of the metal-organic molecular dopant molybdenum tris-[1,2-bis(trifluoromethyl)ethane-1,2-dithiolene] (Mo(tfd)3), or modified with a thin layer of the oxide MoO3. An improved performance is observed in devices modified with Mo(tfd)3 or MoO3 as compared to devices in which Au electrodes are modified with PFBT. We discuss the origin of the decrease in contact resistance in terms of increase of the work function of the modified Au electrodes, Fermi-level pinning effects, and decrease of bulk resistance by electrically doping the organic semiconductor films in the vicinity of the source/drain electrodes.

Self-forming electrode modification in organic field-effect transistors

We report on self-forming electrode modification by mixing 2,3,4,5,6-pentafluorothiophenol (PFBT) directly into the solution of the organic semiconductor prior to film formation on top of existing metal electrodes. During the formation of the semiconductor layer from the mixed solution, PFBT chemisorbs on the underlying source/drain electrodes and modifies their electronic properties. The modification of evaporated silver, gold, or printed silver electrodes with PFBT is analyzed by X-ray photoelectron spectroscopy. The use of this self-forming electrode modification is applied to solution-processed p-channel top-gate 6,13-bis(triisopropylsilylethynyl)pentacene/poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] organic field-effect transistors (OFETs) that comprise bare silver or gold source/drain electrodes. The proposed new method simplifies device fabrication while yielding OFETs with a performance level that is comparable to that of reference devices in which the metal electrodes are modified with PFBT prior to the fabrication of the semiconductor layer.

Recent advances in the science and engineering of organic light-emitting diodes(Conference Presentation)

In this talk, we will discuss recent advances in the science and engineering of organic light-emitting diodes (OLEDs). First, we will focus on materials in which light emission involves the process of thermally activated delayed fluorescence (TADF). In these materials, triplet excited states can convert into optically emissive singlet excited states by reverse intersystem crossing, allowing for nearly 100% internal quantum efficiency. This process can be used to design a new class of materials that are all organic, offering a lower cost alternative to conventional electrophosphorescent materials that contain heavy and expensive elements such as Pt and Ir. We will discuss molecular design strategies and present examples of materials that can be used as emitters or hosts in the emissive layer. In a second part of this talk, we will review recent progress in fabricating OLEDs on shape memory polymer substrates (SMPs). SMPs are mechanically active, smart materials that can exhibit a significant drop in modulus once an external stimulus such as temperature is applied. In their rubbery state upon heating, the SMP can be easily deformed by external stresses into a temporary geometric configuration that can be retained even after the stress is removed by cooling the SMP to below the glass transition temperature. Reheating the SMP causes strain relaxation within the polymer network and induces recovery of its original shape. We will discuss how these unique mechanical properties can also be extended to a new class of OLEDs.

Highly stable organic field-effect transistors with engineered gate dielectrics(Conference Presentation)

Organic field-effect transistors (OFETs) have the potential to lead to low-cost flexible displays, wearable electronics, and sensors. While recent efforts have focused greatly on improving the maximum charge mobility that can be achieved in such devices, studies about the stability and reliability of such high performance devices are relatively scarce. In this talk, we will discuss the results of recent studies aimed at improving the stability of OFETs under operation and their shelf lifetime. In particular, we will focus on device architectures where the gate dielectric is engineered to act simultaneously as an environmental barrier layer. In the past, our group had demonstrated solution-processed top-gate OFETs using TIPS-pentacene and PTAA blends as a semiconductor layer with a bilayer gate dielectric layer of CYTOP/Al2O3, where the oxide layer was fabricated by atomic layer deposition, ALD. Such devices displayed high operational stability with little degradation after 20,000 on/off scan cycles or continuous operation (24 h), and high environmental stability when kept in air for more than 2 years, with unchanged carrier mobility. Using this stable device geometry, simple circuits and sensors operating in aqueous conditions were demonstrated. However, the Al2O3 layer was found to degrade due to corrosion under prolonged exposure in aqueous solutions. In this talk, we will report on the use of a nanolaminate (NL) composed of Al2O3 and HfO2 by ALD to replace the Al2O3 single layer in the bilayer gate dielectric use in top-gate OFETs. Such OFETs were found to operate under harsh condition such as immersion in water at 95 °C. This work was funded by the Department of Energy (DOE) through the Bay Area Photovoltaics Consortium (BAPVC) under Award Number DE-EE0004946.

Top-gate organic field-effect transistors fabricated on shape-memory polymer substrates

We demonstrate top-gate organic field-effect transistors (OFETs) with a bilayer gate dielectric and doped contacts fabricated on shape-memory polymer (SMP) substrates. SMPs exhibit large variations in Young’s modulus dependent on temperature and have the ability to fix two or more geometric configurations when a proper stimulus is applied. These unique properties make SMPs desirable for three-dimensional shape applications of OFETs. The electrical properties of OFETs on SMP substrates are presented and compared to those of OFETs on traditional glass substrates.

Organic field-effect transistor circuits with electrode interconnections using reverse stamping

We discuss a non-vacuum low-cost reverse stamping method for the realization of circuits based on top-gate organic field-effect transistors (OFETs) with a bi-layer gate dielectric. This method allows for patterning of high-k inorganic dielectric films produced by atomic layer deposition and consequently of the bilayer gate dielectric layers used in our top-gate OFETs. We demonstrate the fabrication and operation of logic inverters and ring oscillators following this approach.