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At least 199 records · Page 11

Direct Laser Writing Crystal Polymorphs of Organic Semiconductors for Phase Change Electronics

The many diverse polymorphic behaviors observed in organic electronic materials offer opportunities to modulate electronic properties through reversibly switching crystal structures. Here, we access the prolific polymorphism observed in two-dimensional quinoidal terthiophene via laser writing to locally heat and direct the phase transitions. We access a metastable polymorph IV through rapid cooling and observe distinct symmetry as well as packing through grazing incidence X-ray diffraction (GIXD). Using our open-source PolyChemPrint patterning platform, we direct laser heating to initiate the IV-I transition, switching the conductance by >2 orders of magnitude. Here, this is confirmed via a combination of GIXD and Raman spectroscopy. Finally, we demonstrate switching of transistor devices as well as discrete tuning of conductance via laser writing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rotary Table Design for the Modular In-Chamber Electron Beam Welding System

The Modular In-Chamber Electron Beam Welding (MIC-EBW) system which is being designed and assembled under DOE Projects DE-NE0008846 (Phase 1--completed) and DE-NE0009039 (Phase 2—in progress) includes several major components: four modules (the lower vacuum module, electron beam module, a spacer module, and a lid), a robust rotary table, large vacuum pumps/system, electron beam welding system controls/power supply, and an electron beam generator/gun. Many of these components and their functions were described in the earlier EPRI-DOE report 3002018146. This report provides an overview of one of the primary components, the rotary table, that has been designed and will be manufactured by Rusach International in Phase 2 of the project.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Dynamic-pressure measurements using an electronically scanned pressure module

Frequency response was measured for different lengths and diameters of tubing between a sinusoidal pressure source and a pressure sensing module from an electronically scanned pressure measuring system. Measurements were made for straight runs of both steel and vinyl tubing. For steel tubing, measured results are compared with results calculated by using equations developed by Tijdeman and Bergh. Measurements were also made with a bend in the vinyl tubing at the module. In addition, measurements were made with two coils placed in the tubing near the middle of the run.

Chapin, W. G.↗

Electrochemistry at Back-Gated, Ultrathin ZnO Electrodes: Field-Effect Modulation of Heterogeneous Electron Transfer Rate Constants by 30× with Enhanced Gate Capacitance

We report steady-state voltammetry of outer-sphere redox species at back-gated ultrathin ZnO working electrodes in order to determine electron transfer rate constants k ET as a function of independently-controlled gate bias, V G . We demonstrate that k ET can be modulated as much as 30-fold by application of V G ≤ 8 V. Key to this demonstration was integrating the ultrathin (5 nm) ZnO on a high dielectric constant (k) insulator, HfO 2 (30 nm), which was grown on a Pd metal gate. The high-k HfO 2 dramatically decreased the required V G values and increased the gate-induced charge in ZnO compared to previous studies. Importantly, the enhanced gating power of the Pd/HfO 2 /ZnO stack meant it was possible to observe a non-monotonic dependence of k ET on V G , which reflects the inherent density of redox acceptor states in solution. Furthermore, this work adds to the growing body of literature demonstrating that electrochemical kinetics (i.e., rate constants and overpotentials) at ultrathin working electrodes can be tuned by V G , independent of the conventional electrochemical working electrode potential.

36 MATERIALS SCIENCE↗

Scalable solution-phase epitaxial growth of symmetry-mismatched heterostructures on two-dimensional crystal soft template

Epitaxial heterostructures with precisely controlled composition and electronic modulation are of central importance for electronics, optoelectronics, thermoelectrics, and catalysis. In general, epitaxial material growth requires identical or nearly identical crystal structures with small misfit in lattice symmetry and parameters and is typically achieved by vapor-phase depositions in vacuum. We report a scalable solution-phase growth of symmetry-mismatched PbSe/Bi 2 Se 3 epitaxial heterostructures by using two-dimensional (2D) Bi 2 Se 3 nanoplates as soft templates. The dangling bond–free surface of 2D Bi 2 Se 3 nanoplates guides the growth of PbSe crystal without requiring a one-to-one match in the atomic structure, which exerts minimal restriction on the epitaxial layer. With a layered structure and weak van der Waals interlayer interaction, the interface layer in the 2D Bi 2 Se 3 nanoplates can deform to accommodate incoming layer, thus functioning as a soft template for symmetry-mismatched epitaxial growth of cubic PbSe crystal on rhombohedral Bi 2 Se 3 nanoplates. We show that a solution chemistry approach can be readily used for the synthesis of gram-scale PbSe/Bi 2 Se 3 epitaxial heterostructures, in which the square PbSe (001) layer forms on the trigonal/hexagonal (0001) plane of Bi 2 Se 3 nanoplates. We further show that the resulted PbSe/Bi 2 Se 3 heterostructures can be readily processed into bulk pellet with considerably suppressed thermal conductivity (0.30 W/m·K at room temperature) while retaining respectable electrical conductivity, together delivering a thermoelectric figure of merit ZT three times higher than that of the pristine Bi 2 Se 3 nanoplates at 575 K. Our study demonstrates a unique epitaxy mode enabled by the 2D nanocrystal soft template via an affordable and scalable solution chemistry approach. It opens up new opportunities for the creation of diverse epitaxial heterostructures with highly disparate structures and functions.

2D crystals↗

DE-FE0031180 Final Report - LGFCS Prototype System Testing - R0

In the project, LGFCS assembled and tested its modular SOFC Power System that incorporates all critical technology improvements identified for its “product-like” demonstration. This product demonstrator is expected to meet customer and LGFCS performance expectations for operation, availability, durability and serviceability. The principal technology improvements are aimed at increasing the fuel cell power output and reducing the stack degradation rate. Improvements were also made for added system robustness and increased reliability. The objective of this program is to test a 250kWe thermally self-sustaining modular solid oxide fuel cell (SOFC) Power System for a minimum of 5,000 hours while advancing this commercial prototype product demonstrator to a Technical Readiness Level (TRL) 7. The SOFC system was tested on a site provided by Stark State College in North Canton, Ohio. System performance and degradation as well as cost estimates were compared to established SOFC Program performance metrics to assess progress. The major achievements were to assemble, and QA qualify 70 fuel cell strips for 12 integrated blocks into a fuel cell vessel and install it into a generator module with the fuel and power electronics modules on the test site. Performance to date included over 1800 hours on load at 250 KW-AC to the grid with a DC efficiency of 61% and AC efficiency of 55%. Power degradation was less than 0.4% per 1000 hours and NOx emissions met standards. The LGFCS SOFC Prototype System (GEN0) was demonstrated in an operational environment and therefore achieving Technical Readiness Level 7. The work presented here represents the efforts of all the employees of LG Fuel Cell Systems. Their dedication and hard work made GEN0 possible and successful.

03 NATURAL GAS↗

LGFCS Prototype System Testing (Final Report)

In the project, LGFCS assembled and tested its modular SOFC Power System that incorporates all critical technology improvements identified for its “product-like” demonstration. This product demonstrator is expected to meet customer and LGFCS performance expectations for operation, availability, durability and serviceability. The principal technology improvements are aimed at increasing the fuel cell power output and reducing the stack degradation rate. Improvements were also made for added system robustness and increased reliability. The objective of this program is to test a 250kWe thermally self-sustaining modular solid oxide fuel cell (SOFC) Power System for a minimum of 5,000 hours while advancing this commercial prototype product demonstrator to a Technical Readiness Level (TRL) 7. The SOFC system was tested on a site provided by Stark State College in North Canton, Ohio. System performance and degradation as well as cost estimates were compared to established SOFC Program performance metrics to assess progress. The major achievements were to assemble, and QA qualify 70 fuel cell strips for 12 integrated blocks into a fuel cell vessel and install it into a generator module with the fuel and power electronics modules on the test site. Performance to date included over 1800 hours on load at 250 KWAC to the grid with a DC efficiency of 61% and AC efficiency of 55%. Power degradation was less than 0.4% per 1000 hours and NOx emissions met standards. The LGFCS SOFC Prototype System (GEN0) was demonstrated in an operational environment and therefore achieving Technical Readiness Level 7. The work presented here represents the efforts of all the employees of LG Fuel Cell Systems. Their dedication and hard work made GEN0 possible and successful.

03 NATURAL GAS↗

Design and Operation of the Planetary In-Situ Capillary Electrophoresis System (PISCES)

The PISCES instrument is a portable, miniature, modular instrument designed to analyze organic molecular signatures of life. PISCES uses microcapillary electrophoresis (μCE) with laser-induced fluorescence detection (LIFD) to analyze fluorescently-labeled analytes prepared on a multi-layer microfluidic chip. As a modular instrument composed of five independently functioning units, each module can be easily detached from the system and used for subsystem testing in different environments, e.g. low temperature. The pneumatic module contains mechanical and electrical components necessary to control pneumatically-actuated valves for on-chip sample processing. A prototype LabVIEW program and two custom printed circuit boards (PCBs) operate the pneumatics module using an Arduino microcontroller, and a tentative design for the module’s housing has been developed. The high-voltage module contains circuitry required to apply varying electrical potentials to the electrophoretic channel of the microdevice. Work is currently being done to design the circuit and PCB for this module in collaboration with our SBIR partners at Los Gatos Research. The optical electronics module contains the spectrometer, laser, and laser power supply. The mounting components for the electronics and housing for the module have been designed, assembled, and tested. The optical module contains optical components to focus the laser to a 20μm spot in the center of the electrophoretic channel.The housing for this module has been designed and assembled with the aligned optical components inside.

Willis, Peter A.↗

The generation of rapid solar flare hard X-ray and microwave fluctuations in current sheets

The generation of rapid fluctuations, or spikes, in hard X-ray and microwave bursts via the disruption of electron heating and acceleration in current sheets is studied. It is found that 20 msec hard X-ray fluctuations can be thermally generated in a current sheet if the resistivity in the sheet is highly anomalous, the plasma density in the emitting region is relatively high, and the volume of the emitting region is greater than that of the current sheet. A specific mechanism for producing the fluctuations, involving heating in the presence of ion acoustic turbulence and a constant driving electric field, and interruption of the heating by a strong two-stream instability, is discussed. Variations upon this mechanism are also discussed. This mechanism also modulates electron acceleration, as required for the microwave spike emission. If the hard X-ray emission at energies less than approx. 1000 keV is nonthermal bremsstrahlung, the coherent modulation of electron acceleration in a large number of current sheets is required.

Holman, Gordon D.↗

Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO 2 via introducing strong electronic metal-support interaction for efficient CO 2 photoreduction

This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO 2 -V O (V O : oxygen vacancy) for gas-phase CO 2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO 2 -V O in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO 2 -V O resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO 2 -V O . The optimized Pt/TiO 2 -V O demonstrated a high quantum yield of 1.49% with high CH 4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO 2 -V O and Pt/TiO 2 . More importantly, the EMSI also played a critical role in preserving the surface metallic Pt 0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO 2 -V O , whereas rapid catalytic deactivation are observed for both TiO 2 -V O and Pt/TiO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interplay between Ultrafast Electronic and Librational Dynamics in Liquid Nitrobenzene Probed with Two-Color Four-Wave Mixing

Here, we present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near-infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal measured in the Optical Kerr Effect geometry. The signal is measured to be nonzero only at negative time delays, corresponding to the near-infrared pulses arriving before the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations with classical libration to simulate the experiment. The simulations support the conclusion that the near-infrared pulses launch librational motion while creating electronic coherences resulting in a libration-modulated electronic nonlinear response. The analysis of the phase-matched four-wave mixing signals suggests a nonparametric process leaving the molecules in an excited electronic state, providing new insight into ultrafast nonlinear optical interactions in liquids and advancing toward probing ultrafast electronic coherences in complex molecular liquids.

Shivaram, Niranjan [Lawrence Berkeley National Lab↗

P-Type Doping of Mixed Tin–Lead Halide Perovskites Using Electron Transfer to Mo(tfd-COCF3) 3 and F 4 TCNQ

Mixed tin-lead halide perovskites are emerging as promising candidates to address the toxicity issues of lead-based perovskites and to provide additional bandgap tunability for optoelectronic applications. Electron-transfer doping offers a prospective pathway to modulate electronic properties of metal-halide perovskites, while not disturbing the underlying crystal structure. However, limited research exists comparing molecular dopants for these systems. Here, our study investigates the p-type electron-transfer doping of the mixed tin-lead halide perovskite MAPb 0.5 Sn 0.5 I 3 (MA = methylammonium) using a sequential deposition approach (perovskite film followed by dopant incorporation) and the molecular dopants F 4 TCNQ and Mo(tfd-COCF 3 ) 3 . Up to 3 orders of magnitude higher carrier density and up to 2 orders of magnitude greater conductivity are achieved relative to the undoped samples, with F 4 TCNQ and Mo(tfd-COCF 3 ) 3 demonstrating similar doping efficiencies (associated with the ratio of mobile charges added to the number of dopant molecules incorporated) of 0.031(3) % and 0.024(3) %, respectively. Differences in the doping effectiveness for a given molarity doping solution likely follow from variations in dopant incorporation within the film during the spin coating deposition step.

14 SOLAR ENERGY↗

Kinetic interpretation of resonance phenomena in low pressure capacitively coupled radio frequency plasmas

Low pressure capacitive radio frequency (RF) plasmas are often described by equivalent circuit models based on fluid approaches that predict the self-excitation of resonances, e.g., high frequency oscillations of the total current in asymmetric discharges, but do not provide a kinetic interpretation of these effects. In fact, they leave important questions open: How is current continuity ensured in the presence of energetic electron beams generated by the expanding sheaths that lead to a local enhancement of the conduction current propagating through the bulk? How do the beam electrons interact with cold bulk electrons? What is the kinetic origin of resonance phenomena? Based on kinetic simulations, we find that the energetic beam electrons interact with cold bulk electrons (modulated on a timescale of the inverse local electron plasma frequency) via a time dependent electric field outside the sheaths. This electric field is caused by the electron beam itself, which leaves behind a positive space charge, that attracts cold bulk electrons towards the expanding sheath. The resulting displacement current ensures current continuity by locally compensating the enhancement of the conduction current. The backflow of cold electrons and their interaction with the nonlinear plasma sheath cause the generation of multiple electron beams during one phase of sheath expansion and contribute to a strongly non-sinusoidal RF current. These kinetic mechanisms are the basis for a fundamental understanding of the electron power absorption dynamics and resonance phenomena in such plasmas, which are found to occur in discharges of different symmetries including perfectly symmetric plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Passive Ballistic Microbunching of Non-Ultrarelativistic Electron Bunches using Electromagnetic Wakefields in Dielectric-Lined Waveguides

Temporally-modulated electron beams have a wide array of applications ranging from the generation of coherently-enhanced electromagnetic radiation to the resonant excitation of electromagnetic wakefields in advanced-accelerator concepts. Likewise producing low-energy ultrashort microbunches could be useful for ultra-fast electron diffraction and new accelerator-based light-source concepts. In this Letter we propose and experimentally demonstrate a passive microbunching technique capable of forming a picosecond bunch train at $\sim 6$~MeV. The method relies on the excitation of electromagnetic wakefields as the beam propagates through a dielectric-lined waveguide. Owing to the non-ultrarelativistic nature of the beam, the induced energy modulation eventually converts into a density modulation as the beam travels in a following free-space drift. The modulated beam is further accelerated to $\sim20$~MeV while preserving the imparted density modulation.

43 PARTICLE ACCELERATORS↗