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  1. Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response

    Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We also explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picturemore » that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. Our simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.« less
  2. Group- and phase-velocity-mismatch fringes in triple sum-frequency spectroscopy

  3. Quasilinear diffusion coefficients in a finite Larmor radius expansion for ion cyclotron heated plasmas

    In this study, a reduced model of quasilinear velocity diffusion by a small Larmor radius approximation is derived to couple the Maxwell’s equations and the Fokker Planck equation self-consistently for the ion cyclotron range of frequency waves in a tokamak. The reduced model ensures the important properties of the full model by Kennel-Engelmann diffusion, such as diffusion directions, wave polarizations, and H-theorem. The kinetic energy change (Wdot ) is used to derive the reduced model diffusion coefficients for the fundamental damping (n = 1) and the second harmonic damping (n = 2) to the lowest order of the finite Larmormore » radius expansion. The quasilinear diffusion coefficients are implemented in a coupled code (TORIC-CQL3D) with the equivalent reduced model of the dielectric tensor. We also present the simulations of the ITER minority heating scenario, in which the reduced model is verified within the allowable errors from the full model results.« less
  4. Single-Crystal Thin Films of Cesium Lead Bromide Perovskite Epitaxially Grown on Metal Oxide Perovskite (SrTiO 3)

    High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr 3) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO 3(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcomingmore » the limitation of island-forming Volmer–Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr 3 epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (10 4 cm s –1), and low defect density of 10 12 cm –3, which are comparable to those of CsPbBr 3 single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. Furthermore, the high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunities for a variety of high-performance optoelectronics devices.« less
    Cited by 4
  5. Complex and noncentrosymmetric stacking of layered metal dichalcogenide materials created by screw dislocations

    The interesting and tunable properties of layered metal dichalcogenides heavily depend on their phase and layer stacking. Here, we show and explain how the layer stacking and physical properties of WSe 2 are influenced by screw dislocations. A one-to-one correlation of atomic force microscopy and high- and low-frequency Raman spectroscopy of many dislocated WSe 2 nanoplates reveals variations in the number and shapes of dislocation spirals and different layer stackings that are determined by the number, rotation, and location of the dislocations. Plates with triangular dislocation spirals form noncentrosymmetric stacking that gives rise to strong second-harmonic generation and enhanced photoluminescence,more » plates with hexagonal dislocation spirals form the bulk 2H layer stacking commonly observed, and plates containing mixed dislocation shapes have intermediate noncentrosymmetric stackings with mixed properties. Multiple dislocation cores and other complexities can lead to more complex stackings and properties. Finally, these previously unobserved properties and layer stackings in WSe 2 will be interesting for spintronics and valleytronics.« less
    Cited by 5
  6. Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways

    Hybrid organic-inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We also collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3), with excitation over a range of fluences and repetition rates, to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion ofmore » spatially-correlated pairs, along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and non-geminate pathways shows geminate processes are dominant at high carrier densities and early times. This combination of data and simulation provides a detailed picture of perovskite photophysics across multiple excitation regimes that was not previously available.« less
  7. Fusion Energy Sciences Exascale Requirements Review. An Office of Science review sponsored jointly by Advanced Scientific Computing Research and Fusion Energy Sciences, January 27-29, 2016, Gaithersburg, Maryland

    The additional computing power offered by the planned exascale facilities could be transformational across the spectrum of plasma and fusion research — provided that the new architectures can be efficiently applied to our problem space. The collaboration that will be required to succeed should be viewed as an opportunity to identify and exploit cross-disciplinary synergies. To assess the opportunities and requirements as part of the development of an overall strategy for computing in the exascale era, the Exascale Requirements Review meeting of the Fusion Energy Sciences (FES) community was convened January 27–29, 2016, with participation from a broad range ofmore » fusion and plasma scientists, specialists in applied mathematics and computer science, and representatives from the U.S. Department of Energy (DOE) and its major computing facilities. This report is a summary of that meeting and the preparatory activities for it and includes a wealth of detail to support the findings. Technical opportunities, requirements, and challenges are detailed in this report (and in the recent report on the Workshop on Integrated Simulation). Science applications are described, along with mathematical and computational enabling technologies. Also see http://exascaleage.org/fes/ for more information.« less
  8. The re-introduction of the 40 mm powder gun at the pRad facility

  9. Propagation And Damping Of High Harmonic Fast Waves And Electron Cyclotron Waves In The Nstx-U-Device

    For the spherical torus and for conventional tokamaks to be viable means of producing fusion energy there are two important requirements. The first is to heat the plasma in the experimental devices to high temperatures; preferably, to fusion relevant temperatures. The second is to drive a current in the plasma so that the fusion device operates in a steady-state mode. A pulsed fusion reactor for energy production is not desirable. A favored means to achieve both of these requirements is through the use of microwaves, commonly referred to as radio frequency waves. This proposal was to understand observations from themore » National Spherical Torus Experiment Upgrade (NSTX-U) device on radio frequency wave heating of the confined plasma during operations with high harmonic fast waves. The proposed research was also directed toward assisting in the optimization of the experimental modes of operation so as to maximize the heating efficiency. A detailed analysis of the experiments has shown that about one-third of the input radio frequency power does not make it into the core region of the plasma where heating is required. The losses are believed to occur primarily in the edge region where the radio frequency power is initially coupled into the plasma. Using sophisticated computational codes and theoretical models, that have been developed for the NSTX-U experimental program, this research quantified the physical processes which occur in the edge plasma and lead to a decrease in the heating efficiency. The effect of edge turbulence on the scattering of radio frequency waves was studied for waves in the ion cyclotron and electron cyclotron range of frequencies. For high harmonic fast waves in the ion cyclotron range of frequencies, simulations were carried out using a full-wave solver that was extended to the vacuum vessel wall. These simulations successfully reproduced trends that were observed experimentally. This simulation capability was also used to study the interaction of high harmonic fast waves with the scrape-off layer plasma. More recently, a new technique has been developed for the calculation of radio frequency waves in toroidal geometry that enables the simultaneous incorporation of antenna geometry, plasma facing components, the scrape off-layer, and core propagation in the high harmonic fast wave regime. The effect of turbulent plasmas on the mode conversion of extraordinary electromagnetic waves in the electron cyclotron range of frequencies in the NSTX-U plasma has been studied theoretically. In the over-dense plasmas of NSTX-U, the traditional electromagnetic waves are not effective for delivering energy and momentum to the core plasma. However, electron Bernstein waves generated by mode conversion are efficient carriers of wave energy and momentum to the core. The mode conversion occurs in the turbulent edge region. A theory for mode conversion in such plasmas has been developed. The parameters that can optimize the mode conversion can be readily determined. Also, the model is useful for experimentalists to analyze observation on a shot-to-shot basis.« less
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