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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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133 records · Page 8

Ultrafast Charge Transfer Dynamics at the Origin of Photoconductivity in Doped Organic Solids

In spite of their growing importance for optoelectronic devices, the fundamental properties and photophysics of molecularly doped organic solids remain poorly understood. Such doping typically leads to a small fraction of free conductive charges, with most electronic carriers remaining Coulombically bound to the ionized dopant. Recently, we have reported photocurrent for devices containing vacuum-deposited TAPC (1,1-bis(4-bis(4- methylphenyl)aminophenyl)cyclohexane) doped with MoO 3 , showing that photoexcitation of charged TAPC molecules increases the concentration of free holes that contribute to conduction. Here, we elucidate the excited-state dynamics of such doped TAPC films to unravel the key mechanisms responsible for this effect. We demonstrate that excitation of different electronic transitions in charged and neutral TAPC molecules allows bound holes to overcome the Coulombic attraction to their MoO 3 counterions, resulting in an enhanced yield of long-lived free carriers. This is caused by ultrafast back-and-forth shuffling of charges and excitation energy between adjacent cations and neutral molecules, competing with relatively slow nonradiative decay from higher excited states of TAPC •+ . The light-induced generation of conductive carriers requires the coexistence of cationic and neutral TAPC, a favorable energy level alignment, and intermolecular interactions in the solid state.

36 MATERIALS SCIENCE↗

High-Density Polyethylene Custom Focusing Lenses for High-Resolution Transient Terahertz Biomedical Imaging Sensors

Transient terahertz time-domain spectroscopy (THz-TDS) imaging has emerged as a novel non-ionizing and noninvasive biomedical imaging modality, designed for the detection and characterization of a variety of tissue malignancies due to their high signal-to-noise ratio and submillimeter resolution. We report our design of a pair of aspheric focusing lenses using a commercially available lens-design software that resulted in about 200 × 200-μm2 focal spot size corresponding to the 1-THz frequency. The lenses are made of high-density polyethylene (HDPE) obtained using a lathe fabrication and are integrated into a THz-TDS system that includes low-temperature GaAs photoconductive antennae as both a THz emitter and detector. The system is used to generate high-resolution, two-dimensional (2D) images of formalin-fixed, paraffin-embedded murine pancreas tissue blocks. The performance of these focusing lenses is compared to the older system based on a pair of short-focal-length, hemispherical polytetrafluoroethylene (TeflonTM) lenses and is characterized using THz-domain measurements, resulting in 2D maps of the tissue refractive index and absorption coefficient as imaging markers. For a quantitative evaluation of the lens effect on the image resolution, we formulated a lateral resolution parameter, R2080, defined as the distance required for a 20–80% transition of the imaging marker from the bare paraffin region to the tissue region in the same image frame. The R2080 parameter clearly demonstrates the advantage of the HDPE lenses over TeflonTM lenses. The lens-design approach presented here can be successfully implemented in other THz-TDS setups with known THz emitter and detector specifications.

47 OTHER INSTRUMENTATION↗

Growth of Crystallographically Aligned PbSe Films of Controlled Thickness on Amorphous Substrates

Lead selenide (PbSe) has extensively been investigated due to its thermoelectric and photoconductive properties. More recently, predictions of emergent properties have focused synthetic efforts on preparing ultra-smooth layers of crystallographically aligned PbSe layers with a thickness equal to an integer number of monolayers. While rough films are typically formed through Volmer-Weber growth on heated substrates, we report the data presented herein indicates that a crystallographically aligned, ultrathin layer with a defined number of PbSe layers forms on mostly amorphous Mo-Se and V-Se coated Si substrates during nominally room temperature deposition. Since the films are uniform in thickness, the number of PbSe bilayers formed depends on the amount of Pb (or Se) deposited. If the amount of Pb deposited is close to that required for an integral number of unit cells and there is sufficient Se, Laue oscillations are present in the as-deposited samples. The Laue oscillations reflect the quality and uniformity of the crystalline PbSe domains. This study demonstrates that the substrate does not need to be crystalline to form uniform, crystallographically aligned, integer monolayer thick PbSe films. These results suggest that tuning the strength of interactions be-tween substrate and growing film is necessary to form smooth, crystallographically aligned layers. The substrate does not need to be crystalline for these interactions to be strong enough to enable growth of crystallographically aligned films.

36 MATERIALS SCIENCE↗

Light-driven permanent transition from insulator to conductor

The transition from insulator to conductor can be realized in some materials but requires modification of both the arrangement of atoms and their electronic configurations. This is often achieved by doping. Here we reveal a different mechanism the lattice may adopt to induce such a transition. Experiments showed the surprising finding that limited exposure to subband-gap light caused a permanent transition from an insulator state to a conductor state in the insulating oxide Ga 2 O 3 , with a nine orders of magnitude increase in electronic conduction. Furthermore, annealing up to 400 °C did not suppress or decrease the induced conductivity. Photoexcitation by light-induced modification in the charge state of defects and subsequent lattice distortion around them was suggested to be the underlying mechanism behind this transition. Density functional theory calculations confirmed that modifying the charge state of defects leads to redistribution of the localized electrons and massive structural distortion in the surrounding lattice, causing large shifts in the density of states and introducing new states with shallower energy levels. Both experimental and theoretical results revealed the introduction of stable shallow energy levels, explaining the mechanism behind the transition from an insulator to a conductor state by light. We suggest that this mechanism may occur in other wide band-gap metal oxides leading to drastic modification in their electronic properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Sensitivity and Detection Limit of Spectroscopic-Grade Perovskite CsPbBr 3 Crystal for Hard X-Ray Detection

We report spectroscopic-grade single crystal detectors can register the energies of individual X-ray interactions enabling photon-counting systems with superior resolution over traditional photoconductive X-ray detection systems. Current technical challenges have limited the preparation of perovskite semiconductors for energy-discrimination X-ray photon-counting detection. Here, this work reports the deployment of a spectroscopic-grade CsPbBr 3 Schottky detector under reverse bias for continuum hard X-ray detection in both the photocurrent and spectroscopic schemes. High surface barriers of approximate to ≈ 1 eV are formed by depositing solid bismuth and gold contacts. The spectroscopic response under a hard X-ray source is assessed in resolving the characteristic X-ray peak. The methodology in enhancing X-ray sensitivity by controlling the X-ray energies and flux, and voltage, is described. The X-ray sensitivity varies between a few tens to over 8000 μC Gy air -1 cm -2 . The detectable dose rate of the CsPbBr 3 detectors is as low as 0.02 nGy air s -1 in the energy discrimination configuration. Finally, the unbiased CsPbBr 3 device forms a spontaneous contact potential difference of about 0.7 V enabling high quality of the CsPbBr 3 single crystals to operate in "passive" self-powered X-ray detection mode and the X-ray sensitivity is estimated as 14 μC Gy air -1 cm -2 . The great potential of spectroscopic-grade CsPbBr 3 devices for X-ray photon-counting systems is anticipated in this work.

36 MATERIALS SCIENCE↗

High broadband photoconductivity of few-layered MoS 2 field-effect transistors measured using multi-terminal methods: effects of contact resistance

Among the layered two dimensional semiconductors, molybdenum disulfide (MoS 2 ) is considered to be an excellent candidate for applications in optoelectronics and integrated circuits due to its layer-dependent tunable bandgap in the visible region, high ON/OFF current ratio in field-effect transistors (FET) and strong light–matter interaction properties. In this study, using multi-terminal measurements, we report high broadband photocurrent response ( R ) and external quantum efficiency (EQE) of few-atomic layered MoS 2 phototransistors fabricated on a SiO 2 dielectric substrate and encapsulated with a thin transparent polymer film of Cytop. The photocurrent response was measured using a white light source as well as a monochromatic light of wavelength λ = 400 nm–900 nm. We measured responsivity using a 2-terminal configuration as high as R = 1 × 10 3 A W -1 under white light illumination with an optical power P opt = 0.02 nW. The R value increased to 3.5 × 10 3 A W -1 when measured using a 4-terminal configuration. Using monochromatic light on the same device, the measured values of R were 10 3 and 6 × 10 3 A W -1 under illumination of λ = 400 nm when measured using 2- and 4-terminal methods, respectively. The highest EQE values obtained using λ = 400 nm were 10 5 % and 10 6 % measured using 2- and 4-terminal configurations, respectively. The wavelength dependent responsivity decreased from 400 nm to the near-IR region at 900 nm. The observed photoresponse, photocurrent–dark current ratio (PDCR), detectivity as a function of applied gate voltage, optical power, contact resistances and wavelength were measured and are discussed in detail. The observed responsivity is also thoroughly studied as a function of contact resistance of the device.

36 MATERIALS SCIENCE↗

Purely electronic insulator-metal transition in rutile VO 2

Volatile resistive switching in neuromorphic computing can be tuned by external stimuli such as temperature or electric-field. However, this type of switching is generally coupled to structural changes, resulting in slower reaction speed and higher energy consumption when incorporated into an electronic device. The vanadium dioxide (VO 2 ), which has near room temperature metal-insulator transition (MIT), is an archetypical volatile resistive switching system. Here, we demonstrate an isostructural MIT in an ultrathin VO 2 film capped with a photoconductive cadmium sulfide (CdS) layer. Transmission electron microscopy, resistivity experiments, and first-principles calculations show that the hole carriers induced by CdS photovoltaic effect are driving the MIT in rutile VO 2 . The insulating-rutile VO 2 phase has been proved and can remain stable for hours. Our finding provides a new approach to produce purely electronically driven MIT in VO 2 , and widens its applications in fast-response, low-energy neuromorphic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗