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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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47 records · Page 3

Probing nanoparticle substrate interactions with synchrotron infrared nanospectroscopy: Coupling gold nanorod Fabry-Pérot resonances with SiO 2 and $h$-BN phonons

Spectroscopic interrogation of materials in the midinfrared with nanometer spatial resolution is inherently difficult due to the long wavelengths involved, reduced detector efficiencies, and limited availability of spectrally bright, coherent light sources. Technological advances are driving techniques that overcome these challenges, enabling material characterization in this relatively unexplored spectral regime. Synchrotron infrared nanospectroscopy (SINS) is an imaging technique that provides local sample information of nanoscale target specimens in an experimental energy window between 330 and 5000 cm -1 . Here, using SINS, we analyzed a series of individual gold nanorods patterned on a SiO 2 substrate and on a flake of hexagonal boron nitride. The SINS spectra reveal interactions between the nanorod photonic Fabry-Pérot resonances and the surface phonon polaritons of each substrate, which are characterized as avoided crossings. A coupled oscillator model of the hybrid system provides a deeper understanding of the coupling and provides a theoretical framework for future exploration.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optical Processes behind Plasmonic Applications

Plasmonics is a revolutionary concept in nanophotonics that combines the properties of both photonics and electronics by confining light energy to a nanometer-scale oscillating field of free electrons, known as a surface plasmon. Generation, processing, routing, and amplification of optical signals at the nanoscale hold promise for optical communications, biophotonics, sensing, chemistry, and medical applications. Surface plasmons manifest themselves as confined oscillations, allowing for optical nanoantennas, ultra-compact optical detectors, state-of-the-art sensors, data storage, and energy harvesting designs. Surface plasmons facilitate both resonant characteristics of nanostructures and guiding and controlling light at the nanoscale. Plasmonics and metamaterials enable the advancement of many photonic designs with unparalleled capabilities, including subwavelength waveguides, optical nanoresonators, super- and hyper-lenses, and light concentrators. Alternative plasmonic materials have been developed to be incorporated in the nanostructures for low losses and controlled optical characteristics along with semiconductor-process compatibility. This review describes optical processes behind a range of plasmonic applications. It pays special attention to the topics of field enhancement and collective effects in nanostructures. The advances in these research topics are expected to transform the domain of nanoscale photonics, optical metamaterials, and their various applications.

2D materials↗

Charge Delocalization and Vibronic Couplings in Quadrupolar Squaraine Dyes

Squaraines are prototypical quadrupolar charge-transfer chromophores that have recently attracted much attention as building blocks for solution-processed photovoltaics, fluorescent probes with large two-photon absorption cross sections, and aggregates with large circular dichroism. Their optical properties are often rationalized in terms of phenomenological essential state models, considering the coupling of two zwitterionic excited states to a neutral ground state. As a result, optical transitions to the lowest S 1 excited state are one-photon allowed, whereas the next higher S 2 state can only be accessed by two-photon transitions. A further implication of these models is a substantial reduction of vibronic coupling to the ubiquitous high-frequency vinyl-stretching modes of organic materials. Here, in this study, we combine time-resolved vibrational spectroscopy, two-dimensional electronic spectroscopy, and quantum-chemical simulations to test and rationalize these predictions for nonaggregated molecules. We find small Huang–Rhys factors below 0.01 for the high-frequency, 1500 cm –1 modes in particular, as well as a noticeable reduction for those of lower frequency modes in general for the electronic S 0 → S 1 transition. The two-photon allowed state S 2 is well separated energetically from S 1 and has weak vibronic signatures as well. Thus, the resulting pronounced concentration of the oscillator strength in a narrow region relevant to the lowest electronic transition makes squaraines and their aggregates exceptionally interesting for strong and ultrastrong coupling of excitons to localized light modes in external resonators with chiral properties that can largely be controlled by the molecular architecture.

36 MATERIALS SCIENCE↗

Correlation polarimeter-interferometer in the DIII-D tokamak

A correlation polarimeter-interferometer system has been developed for the DIII-D tokamak to detect small amplitude magnetic and density fluctuations. Two collinear, frequency-offset (5–15 MHz), orthogonally polarized (right- and left-handed, circularly polarized) electromagnetic waves at 650 GHz probing the plasma are used to detect the Faraday effect. A third, linearly polarized, electromagnetic wave serves as the local-oscillator to provide a measure of the line-averaged density. Correlation polarimetric measurement is accomplished by correlating the Faraday effect measured along the same line of sight using two independent detectors, whereas simultaneous correlation interferometric measurement is realized by correlating the line-averaged density measured at two different intermediate frequencies. The noise floor of the correlation polarimeter-interferometer has been demonstrated to be more than one order of magnitude lower than that of a standard polarimeter-interferometer measurement. Line-averaged correlation polarimetric-interferometric measurements in DIII-D H-mode plasmas show broadband (up to 750 kHz) magnetic and density fluctuations with amplitudes as low as 0.03 $Gauss$/$\sqrt{kHz}$ and 4 × 10 13 m –3 /$\sqrt{kHz}$, respectively.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Photoinduced Charge Transfer and Vibronic Coherence in CdSe Quantum Dots with Methyl Viologen Acceptors

We show herein that photoinduced charge transfer from CdSe quantum dots (QDs) to surface-bound methyl viologen (MV 2+ ) acceptors is mediated by a vibronically coherent, nonadiabatic mechanism. Broadband multidimensional electronic spectra and an analysis of coherences show that a mixed QD–MV charge-transfer (CT) state is populated on the <50 fs time scale after optical preparation of the X3 (1P 3/2 –1P e ) state, well prior to the appearance of the one-electron photoreduced ground state (MV +• ). A partial redistribution of charge from the core of the QD to the acceptor is revealed by excited-state coherences of an out-of-plane vibrational mode local to MV 2+ and of a low-frequency mode mixing a MV 2+ mode with the longitudinal optical (LO) phonon of the QD core. The ultrafast damping of these coherences indicates that excited-state wavepackets travel from the optically prepared, Franck–Condon structure through a conical intersection to reach the CT state. These results suggest that vibronically coherent processes generating CT intermediates can be exploited to improve the efficiency of QD-based solar cells and photocatalysts.

Cadmium selenide↗

A quadratic programming flux correction method for high-order DG discretizations of S transport

In this work, we present a new flux-fixup approach for arbitrarily high-order discontinuous Galerkin (DG) discretizations of the S N transport equation, and we demonstrate the compatibility of this approach with the Variable Eddington Factor (VEF) method. The new fixup approach is sweep-compatible: during a transport sweep (block Gauss-Seidel iteration in which the scattering source is lagged), a local quadratic programming (QP) problem is solved in each spatial element to ensure that the solution satisfies certain physical constraints, including local particle balance. In this paper, we describe two choices of physical constraints, resulting in two variants of the method: QP Zero (QPZ) and QP Maximum Principle (QPMP). In QPZ, the finite element coefficients of the solution are constrained to be nonnegative. In QPMP, they are constrained to adhere to an approximate discrete maximum principle. There are two primary takeaways in this paper. First, when the positive Bernstein basis is used for DG discretization, the QPMP method eliminates negativities, preserves high-order accuracy for smooth problems, and significantly dampens unphysical oscillations in the solution. The latter feature – the dampening of unphysical oscillations – is an improvement upon standard, simpler fixup approaches such as the approach described in (denoted as the “zero and rescale” (ZR) method in this paper). This improvement comes at a moderate computational cost, but it is not prohibitive. Our results show that, even in an unrealistic worst-case scenario where 83% of the spatial elements require a fixup, the computational cost of performing a transport sweep with fixup is only ~31% greater than performing one without fixup. The second takeaway is that the VEF method can be used to accelerate the convergence of transport sweeps even when a fixup is applied. When optically thick regions are present, transport sweeps converge slowly, regardless of whether a fixup is applied, and acceleration is needed. However, attempting to apply standard diffusion synthetic acceleration (DSA) to fixed-up transport sweeps results in divergence for optically thick problems. Our results show that the same is not true for VEF. When VEF is combined with fixed-up transport sweeps, the result is a scheme that produces a nonnegative solution, converges independently of the mean free path, and, in the case of the QPMP fixup, adheres to an approximate discrete maximum principle.

97 MATHEMATICS AND COMPUTING↗

Phase-controlled improvement of photon lifetime in coupled superconducting cavities

High-quality cavities are crucial for various fundamental physical studies and applications. Here we find that by coupling two cavities directly or via a phase-tunable coupling channel, the photon lifetime of the local field can exceed that of the bare cavities. The cavity photon lifetime is modified by the phases of the initial states and the phase accumulation on the coupling channel, which affect the interference between cavities. In experiments, by coupling superconducting radio-frequency cavities via phase-tunable cables, we realize a factor of 2 improvement in the cavity photon lifetime. The results can bring rich revenue to quantum information science, sensing, and high-energy physics.

43 PARTICLE ACCELERATORS↗

Second Harmonic Generation Electric Field Triplet Interferometry for Absolute Phasing

We report second harmonic generation (SHG) electric field triplet interferometry performed using three mutually coherent ultrafast pulses in a common path with controllable relative phases, namely, the light fields of a sample signal (SI), a reference oscillator (RO), and a local oscillator (LO). The ROLO phase determined from the interference of the light fields produced by two quartz wafers is subtracted from the phase determined from the SIROLO interferogram to yield the signal phase, ϕ SI . The new method also calibrates the measured SHG intensity from a given sample internally by sending the fundamental light field reflected from the sample into one of the quartz wafers in the ROLO element. The approach avoids having to exchange the sample against a reference material with a known χ(2) value or known phase and accounts on-the-fly for situations where the reflected fundamental light field intensity changes with experimental conditions. The new method is successfully benchmarked against z-cut α-quartz, fused silica held at its point of zero charge, and hematite nanolayers in air, across three different interferometers. Furthermore, the approach should be applicable for other second-order nonlinear spectroscopies, such as vibrational or electronic sum-frequency generation.

Interfaces↗

Wide-field microwave magnetic field imaging with nitrogen-vacancy centers in diamond

Non-invasive imaging of microwave (MW) magnetic fields with microscale lateral resolution is pivotal for various applications, such as MW technologies and integrated circuit failure analysis. Diamond nitrogen-vacancy (NV) center magnetometry has emerged as an ideal tool, offering micrometer-scale resolution, millimeter-scale field of view, high sensitivity, and non-invasive imaging compatible with diverse samples. However, up until now, it has been predominantly used for imaging of static or low-frequency magnetic fields or, concerning MW field imaging, to directly characterize the same microwave device used to drive the NV spin transitions. In this work, we leverage an NV center ensemble in diamond for wide-field imaging of MW magnetic fields generated by a test device employing a differential measurement protocol. The microscope is equipped with a MW loop to induce Rabi oscillations between NV spin states, and the MW field from the device-under-test is measured through local deviations in the Rabi frequency. This differential protocol yields magnetic field maps of a 2.57 GHz MW field with a sensitivity of ∼9 μT Hz −1/2 for a total measurement duration of T=357 s, covering a 340 × 340 μm 2 field of view with a micrometer-scale spatial resolution and a device-under-test input power dynamic range of 30 dB. This work demonstrates a novel NV magnetometry protocol, based on differential Rabi frequency measurement, that extends NV wide-field imaging capabilities to imaging of weak MW magnetic fields that would be difficult to measure directly through standard NV Rabi magnetometry.

crystallographic defects↗

Planck 2018 results. VI. Cosmological parameters

In this paper, we present cosmological parameter results from the final full-mission Planck measurements of the cosmic microwave background (CMB) anisotropies, combining information from the temperature and polarization maps and the lensing reconstruction. Compared to the 2015 results, improved measurements of large-scale polarization allow the reionization optical depth to be measured with higher precision, leading to significant gains in the precision of other correlated parameters. Improved modelling of the small-scale polarization leads to more robust constraints on many parameters, with residual modelling uncertainties estimated to affect them only at the 0.5 σ level. We find good consistency with the standard spatially-flat 6-parameter ΛCDM cosmology having a power-law spectrum of adiabatic scalar perturbations (denoted “base ΛCDM” in this paper), from polarization, temperature, and lensing, separately and in combination. A combined analysis gives dark matter density Ω c h 2 = 0.120 ± 0.001, baryon density Ω b h 2 = 0.0224 ± 0.0001, scalar spectral index n s = 0.965 ± 0.004, and optical depth τ = 0.054 ± 0.007 (in this abstract we quote 68% confidence regions on measured parameters and 95% on upper limits). The angular acoustic scale is measured to 0.03% precision, with 100 θ * = 1.0411 ± 0.0003. These results are only weakly dependent on the cosmological model and remain stable, with somewhat increased errors, in many commonly considered extensions. Assuming the base-ΛCDM cosmology, the inferred (model-dependent) late-Universe parameters are: Hubble constant H 0 = (67.4 ± 0.5) km s –1 Mpc –1 ; matter density parameter Ω m = 0.315 ± 0.007; and matter fluctuation amplitude σ 8 = 0.811 ± 0.006. We find no compelling evidence for extensions to the base-ΛCDM model. Combining with baryon acoustic oscillation (BAO) measurements (and considering single-parameter extensions) we constrain the effective extra relativistic degrees of freedom to be N eff = 2.99 ± 0.17, in agreement with the Standard Model prediction N eff = 3.046, and find that the neutrino mass is tightly constrained to Σ m ν < 0.12 eV. The CMB spectra continue to prefer higher lensing amplitudes than predicted in base ΛCDM at over 2 σ , which pulls some parameters that affect the lensing amplitude away from the ΛCDM model; however, this is not supported by the lensing reconstruction or (in models that also change the background geometry) BAO data. The joint constraint with BAO measurements on spatial curvature is consistent with a flat universe, Ω K = 0.001 ± 0.002. Also combining with Type Ia supernovae (SNe), the dark-energy equation of state parameter is measured to be w 0 = –1.03 ± 0.03, consistent with a cosmological constant. We find no evidence for deviations from a purely power-law primordial spectrum, and combining with data from BAO, BICEP2, and Keck Array data, we place a limit on the tensor-to-scalar ratio r 0.002 < 0.06. Standard big-bang nucleosynthesis predictions for the helium and deuterium abundances for the base-ΛCDM cosmology are in excellent agreement with observations. The Planck base-ΛCDM results are in good agreement with BAO, SNe, and some galaxy lensing observations, but in slight tension with the Dark Energy Survey’s combined-probe results including galaxy clustering (which prefers lower fluctuation amplitudes or matter density parameters), and in significant, 3.6 σ , tension with local measurements of the Hubble constant (which prefer a higher value). Simple model extensions that can partially resolve these tensions are not favoured by the Planck data.

79 ASTRONOMY AND ASTROPHYSICS↗