Plasmon-Driven Charge Transfer Aids Selective Nonthermal Vibrational Excitation in Nitrobenzenethiol on Silver Nanoparticles: Insights from Embedded Correlated Wavefunction Calculations
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Doped antiferromagnets host a vast array of physical properties and learning how to control them is one of the biggest challenges of condensed matter physics. La 1.67 Sr 0.33 NiO 4 (LSNO) is a classic example of such a material. At low temperatures holes introduced via substitution of La by Sr segregate into lines to form boundaries between magnetically ordered domains in the form of stripes. The stripes become dynamic at high temperatures, but LSNO remains insulating presumably because an interplay between magnetic correlations and electron–phonon coupling localizes charge carriers. Magnetic degrees of freedom have been extensively investigated in this system, but phonons are almost completely unexplored. We searched for electron–phonon anomalies in LSNO by inelastic neutron scattering. Giant renormalization of plane Ni–O bond-stretching modes that modulate the volume around Ni appears on entering the dynamic charge stripe phase. Other phonons are a lot less sensitive to stripe melting. Dramatic overdamping of the breathing modes indicates that dynamic stripe phase may host small polarons. We argue that this feature sets electron–phonon coupling in nickelates apart from that in cuprates where breathing phonons are not overdamped and point out remarkable similarities with the colossal magnetoresistance manganites.
Liquid/liquid extraction is one of the most widely used separation and purification methods, where a forefront of research is the study of transport mechanisms for solute partitioning and the relationships that these have to solution structure at the phase boundary. To date, organized surface features that include protrusions, water-fingers, and molecular hinges have been reported. Many of these equilibrium studies have focused upon small-molecule transport – yet the extent to which the complexity of the solute, and the competition between different solutes, influence transport mechanisms have not been explored. Here we report molecular dynamics simulations that demonstrate that a metal salt (LiNO 3 ) can be transported via a protrusion mechanism that is remarkably similar to that reported for H 2 O by tri-butyl phosphate (TBP), a process that involves dimeric assemblies. Yet the LiNO 3 out-competes H 2 O for a bridging position between the extracting TBP dimer, which in-turn changes the preferred transport pathway of H 2 O. Examining the electrolyte concentration dependence on ion-pair transport unexpectedly reveals an inverse correlation with the extracting surfactant concentration. As [LiNO 3 ] increases, surface adsorbed TBP becomes a limiting reactant in correlation with an increased negative surface charge induced by excess interfacial NO 3 – , however the rate of transport is enhanced. Within the highly dynamic interfacial environment, we hypothesize that this unique cooperative effect may be due to perturbed surface organization that either decreases the energy of formation of transporting protrusion motifs or makes it easier for these self-assembled species to disengage from the surface.
It is widely accepted that micro- and nanoscale inhomogeneities govern the performance of many thin-film solar cell absorbers. These inhomogeneities yield material properties (e.g., composition, structure, and charge collection) that are challenging to correlate across length scales and measurement modalities. The challenge is compounded if a correlation is sought during device operation or in conditions that mimic aging under particular stressors (e.g., heat and electrical bias). Correlative approaches, particularly those based on synchrotron x-ray sources, are powerful since they can access several material properties in different modes (e.g., fluorescence, diffraction, and absorption) with minimal sample preparation. Small-scale laboratory x-ray instruments have begun to offer multi-modality but are typically limited by low x-ray photon flux, low spatial resolution, or specific sample sizes. To overcome these limitations, a characterization stage was developed to enable multi-scale, multi-modal operando measurements of industrially relevant photovoltaic devices. The stage offers compatibility across synchrotron x-ray facilities, enabling correlation between nanoscale x-ray fluorescence microscopy, microscale x-ray diffraction microscopy, and x-ray beam induced current microscopy, among others. Furthermore, the stage can accommodate device sizes up to 25 × 25 mm 2 , offering access to multiple regions of interest and increasing the statistical significance of correlated properties. The stage materials can sustain humid and non-oxidizing atmospheres, and temperature ranges encountered by photovoltaic devices in operational environments (e.g., from 25 to 100 °C). As a case study, we discuss the functionality of the stage by studying Se-alloyed CdTe photovoltaic devices aged in the stage between 25 and 100 °C.
The chiral magnetic effect (CME) is a phenomenon in which electric charge is separated by a strong magnetic field from local domains of chirality imbalance and parity violation in quantum chromodynamics. The CME-sensitive observable, the charge-dependent three-point azimuthal correlator Δ𝛾 , is contaminated by a major physics background proportional to the particle's elliptic flow anisotropy 𝑣 2 . Event-shape engineering (ESE) binning events in dynamical fluctuations of 𝑣 2 and event-shape selection (ESS) binning events in statistical fluctuations of 𝑣 2 are two methods to search for the CME by projecting Δ𝛾 to the measured anisotropy 𝑣 2 = 0 intercept. Here, we conduct a systematic study of these two methods using physics models as well as toy model simulations. It is observed that the ESE method fulfills the general premise of measuring the CME but is statistically hungry. It is found that the intercept from the ESS method depends on the details of the event content, such as the mixtures of background-contributing sources, because of statistical fluctuations of intertwining variables used in the method, and is thus not practically useful to measure the CME.
Searching for the $p + ip$ superconducting (SC) state has become a fascinating subject in condensed matter physics recently, as a dream application awaiting in topological quantum computation. Unfortunately, so far there is no universal principle for realizing $p + ip$ in generic solid-state systems. Here we report a theoretical discovery of a $p + ip$ SC ground state (coexisting with ferromagnetic order) in the honeycomb lattice Hubbard model in the extremely strong-coupling limit (e.g., infinite U) at low doping $(δ < 0.2)$, by using both the state-of-art Grassmann tensor product state approach and a continuum quantum field theory approach. Our discovery suggests a mechanism for the $p + ip$ SC state in generic strongly correlated systems based on spin-charge separation and the charge current–current coupling scenario, which opens a door towards experimental realization. The $p + ip$ SC state has an instability towards a potential non-Fermi liquid with a large but finite U . Nevertheless, by applying an in-plane Zeeman field, such a $p + ip$ SC state can be stabilized with finite U in a very wide range of doping. Relevant realistic materials are also proposed.
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Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5$\textit{d}$ electrons. Iin this work, we engineer a well-known triangular lattice 2D Mott insulator 1$\textit{T}$ – TaS 2 into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired $\textit{d}$ electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow $Z_2$ topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.
The MIDNA application specific integrated circuit (ASIC) is a skipper-CCD readout chip fabricated in a 65 nm LP-CMOS process that is capable of working at cryogenic temperatures. The chip integrates four front-end channels that process the skipper-CCD signal and performs differential averaging using a dual slope integration (DSI) circuit. Each readout channel contains a pre-amplifier, a DC restorer, and a dual-slope integrator with chopping capability. The integrator chopping is a key system design element in order to mitigate the effect of low-frequency noise produced by the integrator itself, and it is not often required with standard CCDs. Each channel consumes 4.5 mW of power, occupies 0.156 mm${^2}$ area and has an input referred noise of 2.7${\mu\nu}_{rms}$. It is demonstrated experimentally to achieve sub-electron noise when coupled with a skipper-CCD by means of averaging samples of each pixel. Here, sub-electron noise is shown in three different acquisition approaches. The signal range is 6000 electrons. The readout system achieves 0.2${e^{-}}$ RMS by averaging 1000 samples with MIDNA both at room temperature and at 180 Kelvin.
The ICARUS Liquid Argon Time Projection Chamber (LArTPC) is used to investigate short-baseline neutrino oscillations and the possible existence of sterile neutrinos. To aid in identifying and rejecting cosmic ray backgrounds, the system is outfitted with external Cosmic Ray Taggers (CRTs). The CRT is able to measure more tracks and at a wider range of angles, useful in further detailing future calibrations. This project compared the most probable values (MPVs) of charge deposition between CRT tagged and TPC tagged tracks. The Y-Z maps of charge scale for both datasets show a strong correlation, not just in their overall structure, but also in how they reflect known detector effects. Both reconstruction paths showed similar structures in their charge distribution, such as less effective wire section or mechanical support, confirming that CRT-tagged tracks, despite being external, respond to the same calibration landscape as Pandora tracks, validating previous Pandora reconstructions and values. Overall, the analysis supports the idea that the CRT tags are a useful addition to ICARUS calibration efforts. Their broad angular range and independence from Pandora reconstruction make them a helpful secondary tool and a potential asset in extending calibration across the detector volume.
A family of heterometallic metal-organic frameworks (MOFs) (CPM200s) harmoniously coexisting as Lewis acids and base (azo) sites were prepared. Seven CPM200s were employed as multifunctional heterogeneous cascade catalysts for the one-pot deacetalization-Knoevenagel reaction in a solvent-free system. Benefiting from the cooperation between Lewis acids from the open metal sites and base sites from the ligands, the CPM200s showed high activity and selectivity for the tandem reaction. The heterometallic 3D porous framework reported here not only offers a combination of two opposite active sites in the same framework of materials but also increases mass transfer of the substrate, thus maximizing the efficiency and substrate selectivity of the bifunctional catalysts. The CPM200s showed the highest turnover frequency (TOF), outperforming that of the reported MOFs in tandem with the deacetalization-Knoevenagel reaction. A strong correlation between the TOF and charge-to-radius ratio (z/r) of metal ions in the CPM200s was observed for the first time. The bifunctional CPM200s catalysts can be reused five times without significant loss of activity.
Calcium H and K line anomaly in faint meteor spectra, discussing brightness correlation with aerodynamic flow and resonant charge exchange with ionized nitrogen
The use of statistical analysis (regression analysis) to determine the data correlation between eight voltage parameters is discussed. The eight parameters correlated include: temperature, depth of discharge; charge rate; discharge rate; percent recharge; concentration of KOH; amount of KOH; and precharge. Graphs are presented which show: (1) starpoint/centerpoint cycles to failure vs. parameters; (2) cycles to failure vs. temperature; and (3) positive and negative plate thickness and weight vs. cycles. An empirical equation derived from cycles to failure vs. temperature graph for cells cycled at 1C charge, 2C discharge, and 14 percent recharge is also presented.
A number of phenomena observed on the first orbiting Meteosat satellite attributed to spacecraft charging effects are considered. Design analysis, correlation of anomalies with space environmental data, on ground tests with an engineering model spacecraft, tests on the validity of improvements, and installation of suitable monitors for the second improved flight satellite are discussed.
The generated flow rates of gaseous hydrogen and gaseous oxygen from an electrical vehicle nickel-iron battery system were determined and used to evaluate the flame quenching capabilities of several candidate devices to prevent flame propagation within batteries having central watering/venting systems. The battery generated hydrogen and oxygen gases were measured for a complete charge and discharge cycle. The data correlates well with accepted theory during strong overcharge conditions indicating that the measurements are valid for other portions of the cycle. Tests confirm that the gas mixture in the cells is always flammable regardless of the battery status. The literature indicated that a conventional flame arrestor would not be effective over the broad spectrum of gassing conditions presented by a nickel-iron battery. Four different types of protective devices were evaluated. A foam-metal arrestor design was successful in quenching gaseous hydrogen and gaseous oxygen flames, however; the application of this flame arrestor to individual cell or module protection in a battery is problematic. A possible rearrangement of the watering/venting system to accept the partial protection of simple one-way valves is presented which, in combination with the successful foam-metal arrestor as main vent protection, could result in a significant improvement in battery protection.
An experiment to investigate the spatial homogeneity of large-grain polycrystalline silicon shows a number of performance-loss mechanisms. Arrays of up to 400 small (about 0.2 sq cm in area) photodiodes were fabricated on a selection of 10 cm x 10 cm polycrystalline silicon wafers. Measurements of the illuminated current-voltage (J-V) characteristics were used to generate maps of Voc, Jsc, and FF as a function of position; and dark J-V and LBIC analysis were used to determine the cause of low performance in areas with significantly degraded J-V characteristics. In addition to the presence of inclusions, which act as resistive shunts, the performance of many of the cells is limited by quasineutral recombination current, which may vary by up to an order of magnitude across a wafer. The increase is the result of either electrically-active grain boundaries or numerous subgrain boundaries within the grain bulk. In other isolated instances, the open-circuit voltage is reduced by excess space-charge recombination current that is not correlated with either grain or subgrain boundary activity.
We use JWST NIRCam short-wavelength photometry to capture a transit lightcurve of the exoplanet HAT-P-14 b to assess performance as part of instrument commissioning. The short-wavelength precision is 152 ppm per 27 s integration as measured over the full time series compared to a theoretical limit of 107 ppm, after corrections to spatially correlated 1/f noise. Persistence effects from charge trapping are well fit by an exponential function with short characteristic timescales, settling on the order of 5–15 minutes. The short-wavelength defocused photometry is also uniquely well suited to measure the real-time wave-front error of JWST. Analysis of the images and reconstructed wave-front maps indicates that two different hexagonal primary mirror segments exhibited “tilt events,” where they changed orientation rapidly in less than ∼1.4 s. In some cases, the magnitude and timing of the flux jumps caused by tilt events can be accurately predicted with a telescope model. These tilt events can be sensed by simultaneous longer-wavelength NIRCam grism spectral images alone in the form of changes to the point-spread function, diagnosed from the full width at half maximum. They can also be sensed with the fine guidance sensor instrument from difference images. Tilt events possibly from sudden releases of stress in the backplane structure behind the mirrors were expected during the commissioning period because they were found in ground-based testing. Tilt events have shown signs of decreasing in frequency but have not disappeared completely. The detectors exhibit some minor (less than 1%) deviations from linear behavior in the first few groups of each integration, potentially impacting absolute fluxes and transit depths on bright targets, where only a handful of groups are possible. Overall, the noise is within 50% of the theoretical photon noise and read noise. This bodes well for high-precision measurements of transiting exoplanets and other time variable targets.
The ICARUS Liquid Argon Time Projection Chamber (LArTPC) is used to investigate short-baseline neutrino oscillations and the possible existence of sterile neutrinos. To aid in identifying and rejecting cosmic ray backgrounds, the system is outfitted with external Cosmic Ray Taggers (CRTs). The CRT is able to measure more tracks and at a wider range of angles, useful in further detailing future calibrations. This project compared the most probable values (MPVs) of charge deposition between CRT tagged and TPC tagged tracks. The Y-Z maps of charge scale for both datasets show a strong correlation, not just in their overall structure, but also in how they reflect known detector effects. Both reconstruction paths showed similar structures in their charge distribution, such as less effective wire section or mechanical support, confirming that CRT-tagged tracks, despite being external, respond to the same calibration landscape as Pandora tracks, validating previous Pandora reconstructions and values. Overall, the analysis supports the idea that the CRT tags are a useful addition to ICARUS calibration efforts. Their broad angular range and independence from Pandora reconstruction make them a helpful secondary tool and a potential asset in extending calibration across the detector volume.