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At least 1,369 records · Page 76

Local Time Dependence of Jupiter's Polar Auroral Emissions Observed by Juno UVS

Auroral brightness and color ratio imagery, captured using the Juno mission's Ultraviolet Spectrograph, display intense emissions poleward of Jupiter's northern main emission, and these are split into two distinctly different spectral or “color ratio” regimes. The most poleward region, designated the “swirl region” by Grodent et al. (2003), https://doi.org/10.1029/2003ja010017, exhibits a high color ratio, while low color ratio emissions are found within the collar around the swirl region but still poleward of the main emission. We confirm the apparent strong magnetospheric local time control within the polar collar (Grodent et al., 2003, https://doi.org/10.1029/2003ja010017), with the dusk side bright “active region” emissions extending from ∼11 to 22 hr of magnetospheric local time. These bright emissions dim by at least an order of magnitude between ∼0 and 11 hr magnetospheric local time, in the midnight to dawn side “dark region.” This magnetospheric local time structure holds true even when the entire northern oval is located on the night side of the planet (in ionospheric local time), a geometry unstudied prior to Juno, as it is unobservable from Earth. The swirl region brightens at ionospheric dawn (∼5–7 ionospheric local time) and diminishes or completely disappears at ionospheric local times of ∼20–22 hr. Finally, the southern auroral polar emissions appear to share all of the local time dependencies of its northern counterpart, but at a reduced intensity

Thomas Greathouse↗

How Well Do Multisatellite Products Capture the Space–Time Dynamics of Precipitation? Part I: Five Products Assessed via a Wavenumber–Frequency Decomposition

As more global satellite-derived precipitation products become available, it is imperative to evaluate them more carefully for providing guidance as to how well precipitation space–time features are captured for use in hydrologic modeling, climate studies, and other applications. Here we propose a space–time Fourier spectral analysis and define a suite of metrics that evaluate the spatial organization of storm systems, the propagation speed and direction of precipitation features, and the space–time scales at which a satellite product reproduces the variability of a reference “ground-truth” product (“effective resolution”). We demonstrate how the methodology relates to our physical intuition using the case study of a storm system with rich space–time structure. We then evaluate five high-resolution multisatellite products (CMORPH, GSMaP, IMERG-Early, IMERG-Final, and PERSIANN-CCS) over a period of 2 years over the southeastern United States. All five satellite products show generally consistent space–time power spectral density when compared to a reference ground gauge–radar dataset (GV-MRMS), revealing agreement in terms of average morphology and dynamics of precipitation systems. However, a deficit of spectral power at wavelengths shorter than 200 km and periods shorter than 4 h reveals that all satellite products are excessively “smooth.” The products also show low levels of spectral coherence with the gauge–radar reference at these fine scales, revealing discrepancies in capturing the location and timing of precipitation features. From the space–time spectral coherence, the IMERG-Final product shows superior ability in resolving the space–time dynamics of precipitation down to 200-km and 4-h scales compared to the other products.

Clement Guilloteau↗

Assessing the Needs of NASA's Near Real-Time Earth Observation Products

"The 2017-2027 Decadal Survey for Earth Science and Applications from Space stated that NASA's Earth Science with planned implementation of applications provides sustained earth observations for societal benefits [1]. The Decadal Survey indicated that data latency is invaluable for time-sensitive applications including disaster risk reduction, wildland fire carbon emissions quantification, real-time measurements of the state of the hydrologic systems and many more. Data latency refers to the time between earth observation and data products available to users. During the past 13 years, NASA's Land, Atmosphere Near Real-Time Capability for Earth Observing Systems (LANCE) continues to provide free access to earth observation products that are made available much quicker than routine processing allows. The latency of most LANCE data products is Near Real-time (NRT) which is defined as less than three hours from satellite observations [2]. LANCE is managed by the Earth Science Data and Information System (ESDIS) Project at NASA Goddard Space Flight Center [3], and a User Working Group (UWG) is responsible for providing guidance to LANCE. LANCE data are used by direct users and brokers who add value to the data [4]. NASA Earth Applied Sciences Program (ASP) is one of the primary users of LANCE, which collaborates with partner organizations and provides support to scientists to solve problems in applications of earth observations. ASP promotes the use of LANCE NRT data products to demonstrate applications in decision making, facilitates end-user feedback to the science team to improve data products, and provides information on future demands for research. LANCE supports applications that need a rapid response including detecting wildland fires and volcanic eruptions, tracking smoke, ash and dust plumes, monitoring air quality and tracking extreme weather events such as hurricanes, landslides, and floods. To gather feedback regarding the availability, accessibility and actionability of NASA's NRT data products for societal benefit, three surveys and a few discussions with experts involved in the topic within ASP were conducted from the perspective of users. Feedback has been collected from users who are interested in using low latency NASA data within application communities of agriculture, disasters, water resources, health and air quality, ecological conservation, wildland fires and capacity building. Analysis-ready NRT data products in a variety of formats have been mentioned many times in the collected feedback, especially for applied users with little to no experience using research-grade earth observation products. Users prefer to have products that can be easily integrated into their existing workflows and take their analysis to the data. HDF5 is a commonly used data format for research, but typically requires some conversion to a more friendly format for applications and regular use in decision-making. Users prefer the GeoTIFF data format that can be directly ingested into a GIS mapping software and platform for data analysis and visualization. For example, LANCE’s fire, flood, SO2 and Black Marble Nighttime Blue/Yellow Composite data products have been integrated into NASA Disasters Mapping Portal, which is an GIS-based open data portal, for users in the disaster management community. There are 291 LANCE NRT layers available through GIBS and Worldview, where users can download a snapshot in GeoTIFF format. Operational users expect data to be processed as close to the user as possible. The collected feedback indicates that LANCE fire products within 3 hours latency would meet the needs of the wildland fire community. The ideal latency for volcanic application is 10-15 minutes. Users in Volcanic Ash Advisory Centers (VAAC) reported that the first forecast volcanic product should be issued within 75 minutes from the volcano eruption [5]. Overall, for disaster applications, data latency within 3 hours is useful while latency greater than 12 hours is not timely enough for operational use. Capacity building and training are critical for users to be able to access, interpret and use data products and tools for their decision making, especially for applied users with limited experience using earth observation products. LANCE data products have been used in a number of capacity building projects domestically and internationally [6]. As LANCE continues to bring new products into the system, users request training to utilize LANCE new and upcoming data products and capabilities in their applications. Due to the limitation of bandwidth and downstream flow paths, users in some developing countries need tools to select and download data for a specific area of interest instead of bulk downloads. The collected feedback also shows the lack of available SAR satellite low latency data products. The advantages of SAR to monitor conditions and changes on the ground through darkness, clouds, volcanic ash, and other atmospheric conditions, are appealing to low latency users. For example, terabytes of low latency but cloudy optical images are not helpful in rapidly identifying the extent of flood or fire impacts. LANCE could be complemented with low latency measurements via the upcoming NASA-ISRO Synthetic Aperture Radar (NISAR) mission [7]. Requests for higher spatial resolution products are expressed. A user from the wildland fire management community reported that products with 30-m spatial resolution could be used to detect small fires. The 30-m Landsat OLI fire data is now part of NASA’s Fire Information for Resource Management System (FIRMS) US/Canada [8]. Within the open and free NASA resources, LANCE disseminates NRT data products in a manner that allows them to be accessible and understandable to both scientific and applied users. In many application areas, latency plays an important or even decisive role where low latency earth observations help people to observe areas of interest, detect and track changes in the environment and make timely decisions. NASA’s Earth Applied Sciences Program promotes the use of LANCE NRT products and builds a bridge between application users and research teams. The collected feedback indicates data latency within 3 hours is useful for most of the applications, and shows the needs of user-friendly, analysis-ready products, and requests training on LANCE’s new and upcoming data products. User feedback has been provided to LANCE UWG for guidance and recommendations, and for translating findings into something actionable.

Tian Yao↗

A New Scheme of Redundant Timing Crosschecking for Frontend Systems

In high energy physics experiments, frontend digitization modules are usually driven by a common clock. At the frontend electronics and digitization modules of the detector, a precise timing reference must establish in order to make a useful timing measurement. It would be very useful for the frontend digitization system to include a feature of redundant timing crosschecking. The inspiration for the timing crosschecking scheme came from the long-abandoned analog mean-timer schemes. In this scheme, several Front-end modules are connected together through a cable set with taps connected to the digitization modules. Pulses are driven from every FE modules alternately without overlapping. The arrival times of pulses sent from FE modules are digitized at the timing crosschecking module. The mean times will change as temperature changes, but their difference between two FE modules are cancelled mathematically. This feature enables easy achievement of good timing precision without the need for complex hardware.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Method for enhancing a computer to estimate an uncertainty of an onset of a signal of interest in time-series noisy data

A computer-implemented method of enhancing a computer to estimate an uncertainty of an onset of a signal of interest in time-series noisy data. A first mathematical model of first time series data that contains only noise is calculated. A second mathematical model of second time series data that contains the noise and an onset of a signal of interest in the second time series data is calculated. A difference is evaluated between a first combination, being the first mathematical model and the second mathematical model, and a second combination, being the first time series data and the second time series data, wherein evaluating is performed using a generalized entropy metric. A specific time when an onset of the signal of interest occurs is estimated from the difference. An “a posteriori” distribution is derived for an uncertainty of the specific time at which the onset occurs.

Stracuzzi, David John↗

Optimizing Rate of Penetration and Tripping Decision-Making using Real-Time Bit Wear Monitoring While Drilling Geothermal Wells

Understanding bit wear while drilling is critical to minimizing non-productive time (NPT) and optimizing rate of penetration (ROP). Lengthening drilling runs with damaged bits does not only lower the ROP, but also elevates the risk of inducing severe bit damage, which could potentially lead to time-consuming fishing operations. When drillers believe the bit has worn off substantially, the bit is tripped out to be replaced. On geothermal wells, tripping can take up to 20% of the overall well construction time, and this is generally acknowledged as an opportunity for improvement. Ideally, a bit run should be terminated before the bit is damaged beyond repair. At the same time, premature bit pulls are to be avoided as well. This study aims to leverage bit and tooth wear metrics that can be obtained in real time to characterize bit condition in order to optimize ROP and determine the optimal time to pull the bit. Two metrics were explored in this study: a bit wear metric that incorporated depth-of-cut, and a tooth wear metric developed by Bourgoyne & Young characterizing the state of bit teeth dull. Both metrics were computed using recorded data from 12¼ inches roller cone insert bit runs in five geothermal wells targeting a granodiorite formation in the western United States. Together with the actual dull grades, determined after the bits were pulled to surface, the metric trends were interpreted to characterize the downhole bit condition and identify the point at which the bit should have optimally been tripped out. The insights from studying the actual dull grades and how they relate to the two metrics were used to establish a reliable bit pull criterion. The bit wear metric trend correctly showed a noticeable departure from baseline for bits experiencing major dulling behavior. Additionally, the tooth wear model predicted the cutter dull within two dull grades for most runs, with better performance in predicting the inner teeth dull. Moreover, the combination of the bit wear and tooth wear metrics was effective in revealing the cause of the bit performance impairment. Proactive tracking of these two metrics in real-time can facilitate geothermal drilling ROP optimization and better-informed tripping decision-making, thereby avoiding wasted time and cost.

Ashari, Rahmat↗

Weighted relaxation for multigrid reduction in time

Current trends in computer architectures now mean that faster computation speed must come primarily from increased concurrency, not faster clock speeds, which are stagnating. Thus, this situation creates bottlenecks for serial algorithms, including the well-known bottleneck for sequential time-integration, where each individual time-value (i.e., time-step) is computed sequentially. One approach to alleviate this and achieve parallelism in time is with multigrid. Here, in this work, we consider multigrid-reduction-in-time (MGRIT), a multilevel method applied to the time dimension that computes multiple time-steps in parallel. Like all multigrid methods, MGRIT relies on the complementary relationship between relaxation on a fine-grid and a correction from the coarse grid to solve the problem. All current MGRIT implementations are based on unweighted-Jacobi relaxation; here we introduce the concept of weighted relaxation to MGRIT. We derive new convergence bounds for weighted relaxation, and use this analysis to guide the selection of relaxation weights. Numerical results then demonstrate that by choosing appropriate non-unitary relaxation weights, one can achieve faster convergence rates and lower iteration counts for MGRIT when compared with unweighted relaxation. In most cases, weighted relaxation yields a 10%–20% saving in iterations, which is significant when using large high-performance computers. For A-stable integration schemes, results also illustrate that under-relaxation can restore convergence in some cases where unweighted relaxation is not convergent.

97 MATHEMATICS AND COMPUTING↗

Developing a Consistent Travel-Time Framework for Comparing Three-Dimensional Velocity Models for Seismic Location Accuracy

Abstract Location algorithms have historically relied on simple, one-dimensional (1D) velocity models for fast seismic event locations. 1D models are generally used as travel-time lookup tables, one for each seismic phase, with travel-times pre-calculated for event distance and depth. These travel-time lookup tables are extremely fast to use and this fast computational speed makes them the preferred type of velocity model for operational needs. Higher-dimensional (i.e., three-dimensional—3D) seismic velocity models are becoming readily available and provide more accurate event locations over 1D models. The computational requirements of these 3D models tend to make their operational use prohibitive. Additionally, comparing location accuracy for 3D seismic velocity models tends to be problematic, as each model is determined using different ray-tracing algorithms. Attempting to use a different algorithm than the one used to develop a model usually results in poor travel-time prediction. We demonstrate and test a framework to create first-P and first-S 3D travel-time correction surfaces using an open-source framework ( PCalc + GeoTess , https://www.sandia.gov/salsa3d/software/geotess ) that easily stores 3D travel-time and uncertainty data. This framework produces fast travel-time and uncertainty predictions and overcomes the ray-tracing algorithm hurdle because the lookup tables can be generated using the exact ray-tracing algorithm that is preferred for a model.

3D velocity models↗

Isobar Separation in a Multiple-Reflection Time-of-Flight Mass Spectrometer by Mass-Selective Re-Trapping

A novel method for (ultra-)high-resolution spatial mass separation in time-of-flight mass spectrometers is presented. Ions are injected into a time-of-flight analyzer from a radio frequency (rf) trap, dispersed in time-of-flight according to their mass-to-charge ratios and then re-trapped dynamically in the same rf trap. This re-trapping technique is highly mass-selective and after sufficiently long flight times can provide even isobaric separation. A theoretical treatment of the method is presented and the conditions for optimum performance of the method are derived. The method has been implemented in a multiple-reflection time-of-flight mass spectrometer and mass separation powers (FWHM) in excess of 70,000, and re-trapping efficiencies of up to 35% have been obtained for the protonated molecular ion of caffeine. The isobars glutamine and lysine (relative mass difference of 1/4000) have been separated after a flight time of 0.2 ms only. Higher mass separation powers can be achieved using longer flight times. The method will have important applications, including isobar separation in nuclear physics and (ultra-)high-resolution precursor ion selection in multiple-stage tandem mass spectrometry. .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Effect of surface viscosity, anchoring energy, and cell gap on the response time of nematic liquid crystals

An analytical expression for the relaxation time of a nematic liquid crystal is obtained for the first time by considering the influence of surface viscosity, anchoring energy strength and cell gap, validated numerically by using the so-called relaxation method. This general equation for the molecular response time (τ{sub 0}) was derived for a vertical aligned cell and by solving an eigenvalue equation coming from the usual balance of torque equation in the Derzhanskii and Petrov formulation, recovering the usual equations in the appropriate limit. The results show that τ∼d{sup b}, where b=2 is observed only for strongly anchored cells, while for moderate to weak anchored cells, the exponent lies between 1 and 2, depending on both, surface viscosity and anchoring strength. We found that the surface viscosity is important when calculating the response time, specially for thin cells, critical for liquid crystal devices. The surface viscosity’s effect on the optical response time with pretilt is also explored. Our results bring new insights about the role of surface viscosity and its effects in applied physics. - Highlights: • The relaxation of nematic liquid crystals is calculated by taking the surface viscosity into account. • An analytical expression for the relaxation time depending on surface viscosity, anchoring strength and cell gap is obtained. • The results are numerically verified. • Surface viscosity is crucial for thin and weak anchored cells. • The effect on optical time and pretilt angle is also studied.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

New perspectives on materials and device dynamics using time-resolved full-field diffraction X-ray imaging

Understanding how materials evolve during synthesis, processing, or device operation requires experimental access to structural dynamics across wide ranges of length and time scales, often in bulk samples or even within packaged devices. Time-resolved full-field diffraction X-ray microscopy has recently emerged as a powerful way to meet this need by combining the penetration and structural sensitivity of X-ray diffraction with objective-lens-based magnification, sensitive high-resolution X-ray imaging detectors, and pump-probe and real-time imaging strategies. Advances in full-field X-ray diffraction microscopy, often termed dark-field X-ray microscopy (DFXM), enable simultaneous imaging of extended fields of view while retaining crystallographic selectivity. Time-resolved DFXM promises to enable advances in materials processing and dynamics, electrochemical and photochemical processes, and the design of electronic devices. This Perspective summarizes the key instrumental concepts that define the performance of these methods, including the choice of imaging optics, detector considerations, and the impact of source time structure at synchrotron light sources and X-ray free-electron lasers (XFELs). We discuss the simultaneous use of complementary imaging modes that are increasingly used in practice. The early demonstrations of the potential of time-resolved DFXM include real-time defect and grain-boundary dynamics during metal annealing, stroboscopic imaging of functional devices with high strain sensitivity, and ultrafast pump-probe implementations at XFELs that directly visualize acoustic-wave propagation and energy dissipation in bulk crystals.

Dark-field X-ray microscopy↗

FITEVT: A FORTRAN program for arrival-time analysis of nuclear-decay events

FITEVT is a FORTRAN program designed to analyze recorded arrival times of nuclear-decay events affected by dead-time. Here, the primary goal of the program is precise and accurate determination of half-lives. Its method involves imposition of a known sufficiently long extending dead-time to the recorded event sequence, so that the original dead-time effects are completely obliterated and the remaining live-times of the survived events are known exactly. Upon completion of the analysis, the arrival-time spectrum and the live-time spectrum are predicted and compared to those constructed from the survived events.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Explicit quantification of residence and flushing times in the Salish Sea using a sub-basin scale shoreline resolving model

The Salish Sea, located in the Pacific Northwest region of North America has complex currents and circulation features distributed over numerous interconnected deep basins with islands. Increased risk of exposure to oil spills and untreated wastewater from maritime emergencies and treatment plant failures have led to a need for quantifying residence and flushing characteristics at a sub-basin scale using a shoreline resolving hydrodynamic model. An unstructured grid model of the Salish Sea was developed using FVCOM with a ≈75-100m shoreline resolution. In addition to 7 tides and 23 salinity and temperature monitoring stations, an extensive currents data set from 135 stations collected over a span of three years was used for skill assessment and validation. Explicit forward computations were then conducted to define and quantify residence and flushing times in various sub-basins of interest using (a) Lagrangian particles and (b) Numerical/virtual dye experiments. The results in most basins show expected seasonal variability with longer flushing time associated with summer lower tides and lower freshwater inflows. However, contrary to expectation, flushing time is significantly longer in wintertime in large fjord-like basins such as Hood Canal (≈138 days), likely due to increased stratification and reduced mixing. The flushing time for the Puget Sound region of the Salish Sea is ≈115 days, while Georgia Basin is 240 days when analyzed as stand-alone basins with zero background concentrations. When examined as part of the flushing of the entire Puget Sound filled with virtual dye, the compounded flushing times for embedded sub-basins can be significantly longer in order of magnitudes and largely dictated by the flushing time of Puget Sound. The computed residence and flushing time scales tabulated over 36 sub-basins provide an improved understanding of water renewal in the system, informing pollution management actions.

54 ENVIRONMENTAL SCIENCES↗

A new time calibration method for switched-capacitor-array-based waveform samplers

Here we have developed a new time calibration method for the DRS4 waveform sampler that enables us to precisely measure the non-uniform sampling interval inherent in the switched-capacitor cells of the DRS4. The method uses the proportionality between the differential amplitude and sampling interval of adjacent switched-capacitor cells responding to a sawtooth-shape pulse. In the experiment, a sawtooth-shape pulse with a 40 ns period generated by a Tektronix AWG7102 is fed to a DRS4 evaluation board for calibrating the sampling intervals of all 1024 cells individually. The electronic time resolution of the DRS4 evaluation board with the new time calibration is measured to be ~2.4 ps RMS by using two simultaneous Gaussian pulses with 2.35 ns full-width at half-maximum and applying a Gaussian fit. The time resolution dependencies on the time difference with the new time calibration are measured and compared to results obtained by another method. Ultimately, the new method could be applicable for other switched-capacitor-array technology-based waveform samplers for precise time calibration.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Do parcel lockers reduce delivery times? Evidence from the field

Common-carrier parcel lockers have emerged as a secure, automated, self-service means of delivery consolidation in congested urban areas, which are believed to mitigate last-mile delivery challenges through reducing out-of-vehicle delivery times and consequently vehicle dwell times at the curb. However, little research exists to empirically demonstrate the environmental and efficiency gains from this technology. In this study, we designed a nonequivalent groups pre-test/post-test control experiment to estimate the causal effects of a parcel locker on delivery times in a residential building in downtown Seattle, WA. Here, the causal effects are measured in terms of vehicle dwell time and the time delivery couriers spend inside the building, through the difference-in-difference method and using a similar nearby residential building as a control. The results showed a statistically significant decrease in time spent inside the building, and small yet insignificant reduction in delivery vehicle dwell time at the curb. The locker was also well received by the building managers and residents.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets

Ultrafast time-resolved x-ray scattering is an emerging approach to image the dynamical evolution of the electronic charge distribution during complex chemical and biological processes in real-space and real-time. Recently, the differences between semiclassical and quantum-electrodynamical (QED) theory of light-matter interaction for scattering of ultrashort x-ray pulses from the electronic wavepacket were formally demonstrated and visually illustrated by scattering patterns calculated for an electronic wavepacket in atomic hydrogen [G. Dixit, O. Vendrell, and R. Santra, Proc. Natl. Acad. Sci. U.S.A. 109, 11636 (2012)]. In this work, we present a detailed analysis of time-resolved x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons within both the theories. In a many-electron system, the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is investigated. In general, QED and semiclassical theory provide different results for the contribution from the scattering interference, which depends on the energy resolution of the detector and the x-ray pulse duration. The present findings are demonstrated by means of a numerical example of x-ray time-resolved imaging for an electronic wavepacket in helium. It is shown that the time-dependent scattering interference vanishes within semiclassical theory and the corresponding patterns are dominated by the scattering contribution from the time-independent interference, whereas the time-dependent scattering interference contribution do not vanish in the QED theory and the patterns are dominated by the scattering contribution from the non-stationary electron scattering.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Detection of nonlinear picosecond acoustic pulses by time-resolved Brillouin scattering

In time-resolved Brillouin scattering (also called picosecond ultrasonic interferometry), the time evolution of the spatial Fourier component of an optically excited acoustic strain distribution is monitored. The wave number is determined by the momentum conservation in photon-phonon interaction. For linear acoustic waves propagating in a homogeneous medium, the detected time-domain signal of the optical probe transient reflectivity shows a sinusoidal oscillation at a constant frequency known as the Brillouin frequency. This oscillation is a result of heterodyning the constant reflection from the sample surface with the Brillouin-scattered field. Here, we present an analytical theory for the nonlinear reshaping of a propagating, finite amplitude picosecond acoustic pulse, which results in a time-dependence of the observed frequency. In particular, we examine the conditions under which this information can be used to study the time-evolution of the weak-shock front speed. Depending on the initial strain pulse parameters and the time interval of its nonlinear transformation, our theory predicts the detected frequency to either be monotonically decreasing or oscillating in time. We support these theoretical predictions by comparison with available experimental data. In general, we find that picosecond ultrasonic interferometry of nonlinear acoustic pulses provides access to the nonlinear acoustic properties of a medium spanning most of the GHz frequency range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump–probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump–probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗