Yueh-Lin Loo

Electrical Stress Influences the Efficiency of CH3NH3PbI3 Perovskite Light Emitting Devices

Organic-inorganic hybrid perovskite materials are emerging as semiconductors with potential application in optoelectronic devices. In particular, perovskites are very promising for light-emitting devices (LEDs) due to their high color purity, low nonradiative recombination rates, and tunable bandgap. Here, using pure CH3 NH3 PbI3 perovskite LEDs with an external quantum efficiency (EQE) of 5.9% as a platform, it is shown that electrical stress can influence device performance significantly, increasing the EQE from an initial 5.9% to as high as 7.4%. Consistent with the enhanced device performance, both the steady-state photoluminescence (PL) intensity and the time-resolved PL decay lifetime increase after electrical stress, indicating a reduction in nonradiative recombination in the perovskite film. By investigating the temperature-dependent characteristics of the perovskite LEDs and the cross-sectional elemental depth profile, it is proposed that trap reduction and resulting device-performance enhancement is due to local ionic motion of excess ions, likely excess mobile iodide, in the perovskite film that fills vacancies and reduces interstitial defects. On the other hand, it is found that overstressed LEDs show irreversibly degraded device performance, possibly because ions initially on the perovskite lattice are displaced during extended electrical stress and create defects such as vacancies.

Solution-processable, crystalline material for quantitative singlet fission

Amorphous nanoparticles of the singlet fission chromophore 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pn) are fully crystallized through co-precipitation with a chemical additive. Time-resolved measurements indicate that singlet fission in the crystalline nanoparticles is quantitative, or lossless, whereas losses are evident in the amorphous nanoparticles as a result of frustrated triplet pair separation. Because triplet pairs form rapidly and separate slowly in amorphous material, mixed-phase samples are unable to compensate for these losses.

Time-Dependent Mechanical Response of APbX3 (A = Cs, CH3NH3; X = I, Br) Single Crystals

The ease of processing hybrid organic-inorganic perovskite (HOIPs) films, belonging to a material class with composition ABX3 , from solution and at mild temperatures promises their use in deformable technologies, including flexible photovoltaic devices, sensors, and displays. To successfully apply these materials in deformable devices, knowledge of their mechanical response to dynamic strain is necessary. The authors elucidate the time- and rate-dependent mechanical properties of HOIPs and an inorganic perovskite (IP) single crystal by measuring nanoindentation creep and stress relaxation. The observation of pop-in events and slip bands on the surface of the indented crystals demonstrate dislocation-mediated plastic deformation. The magnitudes of creep and relaxation of both HOIPs and IPs are similar, negating prior hypothesis that the presence of organic A-site cations alters the mechanical response of these materials. Moreover, these samples exhibit a pronounced increase in creep, and stress relaxation as a function of indentation rate whose magnitudes reflect differences in the rates of nucleation and propagation of dislocations within the crystal structures of HOIPs and IP. This contribution provides understanding that is critical for designing perovskite devices capable of withstanding mechanical deformations.

Beyond Doping and Charge Balancing: How Polymer Acid Templates Impact the Properties of Conducting Polymer Complexes

Polymer acids are increasingly used as dopants/counterions to access and stabilize the electrically conducting states of conducting polymers. Beyond doping and/or charge balancing, these polymer acids also serve as active components that impact the macroscopic properties of the conducting polymer complexes. Judicious selection of the polymer acid at the onset of synthesis or manipulation of the interactions between the polymer acid and the conducting polymer through processing significantly impacts the electrical conductivity, piezoresistivity, electrochromism, mechanical properties, and thermoelectric efficiency of conducting polymers. As polyelectrolytes, these polymer acids enable conducting polymer complexes to transport ions in addition to electrons/holes. Understanding the role of the polymer acid and its interactions with the conducting polymer generates processing-structure-function relationships for conducting polymer/polymer acid complexes, which can help overcome challenges that were associated with these materials, such as low electrical conductivity and sensitivity to humidity, and enable the design of conducting polymer complexes with desired functionalities.

Nanoscale electrical properties of epitaxial Cu3Ge film

Cu3Ge has been pursued as next-generation interconnection/contact material due to its high thermal stability, low bulk resistivity and diffusion barrier property. Improvements in electrical performance and structure of Cu3Ge have attracted great attention in the past decades. Despite the remarkable progress in Cu3Ge fabrication on various substrates by different deposition methods, polycrystalline films with excess Ge were frequently obtained. Moreover, the characterization of nanoscale electrical properties remains challenging. Here we show the fabrication of epitaxial Cu3Ge thin film and its nanoscale electrical properties, which are directly correlated with localized film microstructures and supported by HRTEM observations. The average resistivity and work function of epitaxial Cu3Ge thin film are measured to be 6 ± 1 μΩ cm and ~4.47 ± 0.02 eV respectively, qualifying it as a good alternative to Cu.

Understanding the Crystal Packing and Organic Thin-Film Transistor Performance in Isomeric Guest–Host Systems

In order to understand how additives influence the structure and electrical properties of active layers in thin-film devices, a compositionally identical but structurally different guest-host system based on the syn and anti isomers of triethylsilylethynyl anthradithiophene (TES ADT) is systematically explored. The mobility of organic thin-film transistors (OTFTs) comprising anti TES ADT drops with the addition of only 0.01% of the syn isomer and is pinned at the mobility of OTFTs having pure syn isomer after the addition of only 10% of the isomer. As the syn isomer fraction increases, intermolecular repulsion increases, resulting in a decrease in the unit-cell density and concomitant disordering of the charge-transport pathway. This molecular disorder leads to an increase in charge trapping, causing the mobility of OTFTs to drop with increasing syn-isomer concentration. Since charge transport is sensitive to even minute fractions of molecular disorder, this work emphasizes the importance of prioritizing structural compatibility when choosing material pairs for guest-host systems.

Polar‐Electrode‐Bridged Electroluminescent Displays: 2D Sensors Remotely Communicating Optically

A novel geometry for electroluminescent devices, which does not require transparent electrodes for electrical input, is demonstrated, theoretically analyzed, and experimentally characterized. Instead of emitting light through a conventional electrode, light emission occurs through a polar liquid or solid and input electrical electrodes are coplanar, rather than stacked in a sandwich configuration. This new device concept is scalable and easily deployed for a range of modular alternating-current-powered electroluminescent light sources and light-emitting sensing devices. The polar-electrode-bridged electroluminescent displays can be used as remotely readable, spatially responsive sensors that emit light in response to the accumulation and distribution of materials on the device surface. Using this device structure, various types of alternating current devices are demonstrated. These include an umbrella that automatically lights up when it rains, a display that emits light from regions touched by human fingers (or painted upon using a mixture of oil and water), and a sensor that lights up differently in different areas to indicate the presence of water and its freezing. This study extends the dual-stack, coplanar-electrode device geometry to provide displays that emit light from a figure drawn on an electroluminescent panel using a graphite pencil.

Tuning the Magnitude and the Polarity of the Piezoresistive Response of Polyaniline through Structural Control

We demonstrate the tunability of both the polarity and the magnitude of the piezoresistive response of polyaniline that is template-synthesized on poly(2-acrylamido-2-methyl-1-propanesulfonic acid), PANI-PAAMPSA, by altering the template molecular weight. Piezoresistivity is quantified by gauge factor, a unitless parameter that relates changes in electrical resistance to applied strain. The gauge factor of PANI-PAAMPSA decreases linearly and becomes negative with decreasing PAAMPSA molecular weight. The polarity of PANI-PAAMPSAs gauge factor is determined by macroscopic connectivity across thin films. PANI-PAAMPSA thin films comprise electrostatically stabilized particles whose size is determined at the onset of synthesis. An increase in the interparticle spacing with applied strain results in a positive gauge factor. The presence of PANI crystallites increases connectivity between particles; these samples instead exhibit a negative gauge factor whereby the resistance decreases with increasing strain. The tunability of the piezoresistive response of these conducting polymers allows their utilization in a broad range of flexible electronics applications, including thermo- and chemoresistive sensors and strain gauges.

Presence of Short Intermolecular Contacts Screens for Kinetic Stability in Packing Polymorphs

Polymorphism is pervasive in molecular solids. While computational predictions of the molecular polymorphic landscape have improved significantly, identifying which polymorphs are preferentially accessed and experimentally stable remains a challenge. We report a framework that correlates short intermolecular contacts with polymorphic stability. The presence of short contacts between neighboring molecules prevents structural rearrangement and stabilizes the packing arrangement, even when the stabilized polymorph is not enthalpically favored. In the absence of such intermolecular short contacts, the molecules have added degrees of freedom for structural rearrangement, and solid-solid polymorphic transformations occur readily. Starting with a series of core-halogenated naphthalene tetracarboxylic diimides, we establish this framework with the packing polymorphs of more than 20 compounds, ranging from molecular semiconductors to pharmaceutics and biological building blocks. This framework, widely applicable across molecular solids, can help refine computational predictions by identifying the polymorphs that are kinetically stable.

Semiconducting SWNTs sorted by polymer wrapping: How pure are they?

Short-channel field-effect transistors (FETs) prepared from semiconducting single-walled carbon nanotube (s-SWNT) dispersions sorted with poly(2,5-dimethylidynenitrilo-3,4-didodecylthienylene) are demonstrated. Electrical analysis of the FETs shows no evidence of metallic tubes out of a total number of 646 SWNTs tested, implying an estimated purity of our semiconducting SWNT solution higher than 99.85%. These findings confirm the effectiveness of the polymer-wrapping technique in selecting semiconducting SWNTs, as well as the potential of sorted nanotubes for the fabrication of short channel FETs comprising from 1 to up to 15 nanotubes without inter-nanotube junctions.