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At least 1,513 records · Page 84

Revisiting the Effectiveness Of HCHO/NO2 Ratios for Inferring Ozone Sensitivity to Its Precursors Using High Resolution Airborne Remote Sensing Observations in A High Ozone Episode During the KORUS-AQ Campaign

The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO2) has been widely used for studying O3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO2 on the formation of HCHO is a controlling factor for the transition line between NOx-sensitive and NOx-saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NOx (LNOx) to the chemical loss of HO2+RO2 (LROx) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO2 less than 1 can be safely classified as NOx-saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNOx/LROx~2.7 that accounts for the HCHO-NO2 chemical relationship leading to HCHO = 3.7 × (NO2 – 1.14 × 1016 molec.cm-2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO2 observations form the sensor enhance our understanding of P(O3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly.

KORUS-AQ; formaldehyde; NOx; VOC; OMI; GeoTASO; oz↗

End-to-end Modeling of Lyot Coronagraph for LUVOIR: Sensitivity to Segment-Level Aberrations

Direct imaging and spectroscopic characterization of atmospheres of Earth-like exoplanets require starlight suppression to detect a faint planetary signal at small angular separations. Future space telescopes will require segmentation to survey a statistically significant population of nearby stars systems by increasing aperture size beyond the limits set by traditional monolithic apertures; however, segmentation also represents an additional challenge due to the introduction of temporal pupil discontinuities in terms of both phase and amplitude. For this study, a baseline Lyot coronagraph is used with the Large UV / Optical /Infrared (LUVOIR) mission’s 15-m on-axis, segmented optical telescope assembly (OTA). We present a high-fidelity, end-to-end modeling approach developed as part of the Segmented Coronagraph Design and Analysis (SCDA) group that includes diffractive optical propagations at the 1e-10 contrast level across the entire optical train including the OTA and intermediate re-imaging optics inside the coronagraph instrument. We perform a tolerancing analysis to assess the contrast sensitivity to wavefront perturbations for a set of key telescope terms including segment-level low-order and mid-spatial frequency aberrations. As an input to the end-to-end telescope model, we use two industry-provided segment-level wavefront aberration datasets pertaining: (1) thermal gradients and accelerations (courtesy of Ball-Aerospace and L3-Harris), and (2) telescope dynamics including line-of-sight and segment jitter (courtesy of Lockheed-Martin). Contrast performance outputs of the coronagraph are fed into a mission design reference simulator to assess the scientific yield sensitivity. End-to-end modeling will incorporate performance improvements due to active wavefront sensing and control and/or segment-level metrology to improve system performance.

Optics↗

Application of time-variable process noise in terrestrial reference frames determined from VLBI data

In recent years, Kalman filtering has emerged as a suitable technique to determine terrestrial reference frames (TRFs), a prime example being JTRF2014. The time series approach allows variations of station coordinates that are neither reduced by observational corrections nor considered in the functional model to be taken into account. These variations are primarily due to non-tidal geophysical loading effects that are not reduced according to the current IERS Conventions (2010). It is standard practice that the process noise models applied in Kalman filter TRF solutions are derived from time series of loading displacements and account for station dependent differences. So far, it has been assumed that the parameters of these process noise models are constant over time. However, due to the presence of seasonal and irregular variations, this assumption does not truly reflect reality. In this study, we derive a station coordinate process noise model allowing for such temporal variations. This process noise model and one that is a parameterized version of the former are applied in the computation of TRF solutions based on very long baseline interferometry data. In comparison with a solution based on a constant process noise model, we find that the station coordinates are affected at the millimeter level.

Schuh, Harald↗

Robust Ceramic Coaxial Cable Down-Hole Sensors for Long-Term In Situ Monitoring of Geologic CO 2 Injection and Storage

Energy generation by use of fossil fuels produces large volumes of CO 2 and other greenhouse gases, whose accumulation in the atmosphere is widely seen as undesirable. CO 2 Capture followed by sequestration has been identified as the solution. Subsurface geologic formations offer a potential location for long-term storage of CO 2 because of their requisite size. Unfortunately, the inaccessibility and complexity of the subsurface, the wide range of scales of variability, and the coupled nonlinear processes, impose tremendous challenges to determine the transport and predict the fate of the stored CO 2 . Among the various monitoring approaches, in situ down-hole monitoring of the various state parameters provides critical and direct data points that can be used to validate the models, optimize the injection, detect leakage and track the CO 2 plume. However, down-hole sensors that can withstand the harsh conditions and operate over decades of the project lifecycle remain unavailable. Given that the widespread of carbon capture and storage will be the necessity and reality in the future, fundamental and applied research is required to address the significant challenges and technological gaps in lack of long-term reliable down-hole sensors This project focused on the development and demonstration of a novel, low-cost, distributed, robust ceramic coaxial cable sensor platform for in situ down-hole monitoring of geologic CO 2 injection and storage with high spatial and temporal resolutions. The coaxial cable Fabry-Perot interferometer (CCFPI) has been studied as a general sensor platform for in situ, long-term, measurement of temperature, pressure and strain, which are critical to CO 2 injection and storage. A novel signal processing scheme has been developed and demonstrated for dense multiplexing of the sensors for low-cost distributed sensing with high spatial resolution. The developed temperature, pressure and strain sensors have been extensively tested under laboratory conditions that are similar to the downhole CO 2 storage environment, showing excellent capability for in situ monitoring the various parameters that are important to model, optimize the injection, detect leakage and track the CO 2 plume. In addition, the interactions between the sensor datum and the geological models have been investigated in details for the purposes of model validation, guiding sensor installation/placement, enhancement of model prediction capability and optimization of the injection processes. This project has resulted in the successful development of new ceramic coaxial cable based sensor systems that can monitor directly the changes in pressure, temperature, and strain caused by increased reservoir pressure and reduced reservoir temperature due to the supercritical CO 2 injection. Integrated with geological models, the sensors and measurement data can improve the possibility to identify plume movement and leakage in the cap rock and wells with higher precision and more accuracy. The low cost, ease of deployment, small size and dense multiplexing features of the new sensing technology will allow a large number of sensors to be deployed to address the objective to demonstrate that 99% of the CO 2 remains in the injection zone.

01 COAL, LIGNITE, AND PEAT↗

A Deep Learning Approach for TNC Trip Demand Prediction Considering Spatial-Temporal Features: Preprint

Ride-hailing or transportation network companies (TNCs), such as Uber, Lyft, DiDi Chuxing, or RideAustin, are emerging as a new and disruptive on-demand mobility service in recent years. However, the methods for developing predictive analytics to explore the nature and dynamics of TNCs across cities in the United States are still nascent due to the lack of publicly available data. Recently available public datasets on TNCs by RideAustin offer a unique opportunity to examine spatial, temporal, environmental, and special event factors associated with TNC trip demand. This study explores the use of a deep learning approach - Long Short-Term Memory (LSTM) - to predict TNC trip demand at the ZIP Code level using data from Austin, Texas. The analysis includes key predictive factors such as time of day, day of week, precipitation, and temperature, indicating their corresponding associations with TNC trip demand. Results from initial analysis show that LSTM is able to predict the TNC trip demand for the upcoming hour accurately. LSTM, when compared to other prediction methods, such as historical average and instantaneous trip demand, reduces the mean absolute error (MAE) of the model predictions by 37% and 24%, respectively. This novel method offers significant potential for scaling up and/or replicability across cities where data are available for understanding TNC trip demand to inform emerging mobility system operators. Predicting trip demand can help TNC drivers make informed decisions on how to be more efficient by maximizing passenger pickups and minimizing wait times and deadheading.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Spatially Complete Global Spectral Surface Albedos: Value-Added Datasets Derived from Terra MODIS Land Products

Land surface albedo is an important parameter in describing the radiative properties of the earth s surface as it represents the amount of incoming solar radiation that is reflected from the surface. The amount and type of vegetation of the surface dramatically alters the amount of radiation that is reflected; for example, croplands that contain leafy vegetation will reflect radiation very differently than blacktop associated with urban areas. In addition, since vegetation goes through a growth, or phenological, cycle, the amount of radiation that is reflected changes over the course of a year. As a result, albedo is both temporally and spatially dependant upon global location as there is a distribution of vegetated surface types and growing conditions. Land surface albedo is critical for a wide variety of earth system research projects including but not restricted to remote sensing of atmospheric aerosol and cloud properties from space, ground-based analysis of aerosol optical properties from surface-based sun/sky radiometers, biophysically-based land surface modeling of the exchange of energy, water, momentum, and carbon for various land use categories, and surface energy balance studies. These projects require proper representation of the surface albedo s spatial, spectral, and temporal variations, however, these representations are often lacking in datasets prior to the latest generation of land surface albedo products.

Moody, Eric G.↗

Ultra-Broad-Band Optical Parametric Amplifier or Oscillator

A concept for an ultra-broad-band optical parametric amplifier or oscillator has emerged as a by-product of a theoretical study in fundamental quantum optics. The study was originally intended to address the question of whether the two-photon temporal correlation function of light [in particular, light produced by spontaneous parametric down conversion (SPDC)] can be considerably narrower than the inverse of the spectral width (bandwidth) of the light. The answer to the question was found to be negative. More specifically, on the basis of the universal integral relations between the quantum two-photon temporal correlation and the classical spectrum of light, it was found that the lower limit of two-photon correlation time is set approximately by the inverse of the bandwidth. The mathematical solution for the minimum two-photon correlation time also provides the minimum relative frequency dispersion of the down-converted light components; in turn, the minimum relative frequency dispersion translates to the maximum bandwidth, which is important for the design of an ultra-broad-band optical parametric oscillator or amplifier. In the study, results of an analysis of the general integral relations were applied in the case of an optically nonlinear, frequency-dispersive crystal in which SPDC produces collinear photons. Equations were found for the crystal orientation and pump wavelength, specific for each parametric-down-converting crystal, that eliminate the relative frequency dispersion of collinear degenerate (equal-frequency) signal and idler components up to the fourth order in the frequency-detuning parameter

Strekalov, Dmitry↗

Towards developing an analytical procedure of defining the equatorial electrojet for correcting satellite magnetic anomaly data

Analysis of the total magnetic intensity MAGSAT data has identified and characterized the variability of ionospheric current effects as reflected in the geomagnetic field as a function of longitude, elevation, and time (daily as well as monthly variations). This analysis verifies previous observations in POGO data and provides important boundary conditions for theoretical studies of ionospheric currents. Furthermore, the observations have led to a procedure to remove these temporal perturbations from lithospheric MAGSAT magnetic anomaly data based on 'along-the-dip-latitude' averages from dawn and dusk data sets grouped according to longitudes, time (months), and elevation. Using this method, high-resolution lithospheric magnetic anomaly maps have been prepared of the earth over a plus or minus 50 deg latitude band. These maps have proven useful in the study of the structures, nature, and processes of the lithosphere.

Ravat, Dhananjay↗

Validation of Carbon Flux and Related Products for SIMBIOS: The CARIACO Continental Margin Time Series and the Orinoco River Plume

Between 1997 and 2000, this Sensor Intercomparison and Merger for Biological and Interdisciplinary Oceanic Studies (SIMBIOS) investigation collected bio-optical measurements in the Southeastern Caribbean Sea and the tropical western Atlantic to help understand the color of coastal and continental shelf waters. Specifically, bio-optical data were collected to complement an oceanographic time series maintained within the Cariaco Basin, a site affected by seasonal coastal upwelling. Bio-optical data were also collected within the plume of the Orinoco River during seasonal extremes in discharge. This program focused on providing data to the Sea-Viewing Wide Field-of-view Sensor (SeaWiFS) and SIMBIOS Projects for validating SeaWiFS products. The data are unique in that they provide a substantial number of observations on repeated seasonal cycles for the SeaWIFS Bio-Optical Archive and Storage System (SeaBASS) bio-optical database. An important aspect of this SIMBIOS investigation was a focus on proper interpretation of ocean color remote sensing data from coastal and continental shelf environments. With this goal in mind, ocean color satellite data from a variety and locations and from different satellite sensors were examined to understand spatial and temporal variability in pigment concentrations, and also to conduct an in-depth study of current atmospheric correction and bio-optical algorithms.

Muller-Karger, Frank↗

Separating Spatial and Temporal Variations of the Aurora Using Two Nearly Colocated Satellites

This final report describes the efforts accomplished during the grant's period of performance, covering the period of 1 May 1997 to 30 April 2001, of a NASA Supporting Research and Technology Program grant under the Ionospheric, Thermospheric, and Mesospheric Physics component of the Sun-Earth Connections program. We have met and exceeded the goals set forth in the proposed research objectives. Referred publications have appeared in the scientific literature and several others are in the review process. In addition, numerous invited and contributed presentations of these studies were presented at national and international meetings during the performance period. One graduate student completed his PhD and won two AGU Best Student Paper awards based on research funded by this grant. These studies are summarized below. The science goal delineated in the initial proposal was "to systematically explore the temporal and spatial characteristics of the aurora in a way heretofore impossible, using data from two coplanar DMSP spacecraft." We accomplished this goal through a series of related studies. One study used these unique data to establish the role of Ps6 waves in coupling between the magnetosphere and the auroral ionosphere (omega bands) during the recovery phase of a magnetic storm; the published paper demonstrated the causal relationships between geospace processes occurring in different regions and established a simple conceptual model based on the fortuitous constellation of observations. In the second string of papers, we used these data to explore velocity-dispersed ions (VDIS) in and near the cusp, to test region identification models, and to look at space/time structure of auroral precipitation. On the first topic, the unique DMSP data revealed a remarkable double VDIS with a latitudinal overlap. This could only be explained in terms of a unified reconnection geometry that builds on several earlier unrelated models. The paper outlining this discovery has drawn considerable attention from the community and is currently in press - it adds significantly to the debate over whether reconnection is study state versus bursty and patchy versus global. The second paper develops the model further by incorporating the electron signature - these ionospheric particle precipitation signatures reveal the presence of magnetospheric "fossilized" FTEs, demonstrating the power of ionospheric measurements as a remote diagnostic of magnetospheric processes. Finally, the general nature of aurora] stability and coherence and region identification by particle characteristics were fully explored in a final paper. We identify candidate mechanisms controlling coherence time scales and length scales and refine boundary region identification criteria. We also use the dual-DMSP observations to identify the open and closed LLBL region and related its significance to the generalized bursty, multiple x-line model developed in the first paper. All of these topics are chapters of Dr. Boudouridis' recently completed PhD thesis.

Spence, Harlan E.↗

The Role of Temporal Evolution in Modeling Atmospheric Emissions from Tropical Fires

Fire emissions associated with tropical land use change and maintenance influence atmospheric composition, air quality, and climate. In this study, we explore the effects of representing fire emissions at daily versus monthly resolution in a global composition-climate model. We find that simulations of aerosols are impacted more by the temporal resolution of fire emissions than trace gases such as carbon monoxide or ozone. Daily-resolved datasets concentrate emissions from fire events over shorter time periods and allow them to more realistically interact with model meteorology, reducing how often emissions are concurrently released with precipitation events and in turn increasing peak aerosol concentrations. The magnitude of this effect varies across tropical ecosystem types, ranging from smaller changes in modeling the low intensity, frequent burning typical of savanna ecosystems to larger differences when modeling the short-term, intense fires that characterize deforestation events. The utility of modeling fire emissions at a daily resolution also depends on the application, such as modeling exceedances of particulate matter concentrations over air quality guidelines or simulating regional atmospheric heating patterns.

aerosols↗

The gravity method and interpretive techniques for detecting vertical crustal movements

Observations of temporal variations of gravity can be used as an inexpensive and rapid means of detecting, monitoring, and studying crustal deformation associated with many active geological processes. Such observations can yield qualitative or semiquantitative information on elevation changes and, when combined with independent elevation data, can yield information about changes of the subsurface density field arising from both subsurface displacements and temporal variations of the density of materials in the subsurface. The effectiveness of gravity techniques in specific cases of crustal deformation depends on the configuration of the local gravity field, the physical processes involved in the deformation, and the accuracy with which temporal gravity variations can be measured.

Jachens, R. C.↗

Asymmetric Surface Brightness Structure of Caustic Crossing Arc in SDSS J1226+2152: A Case for Dark Matter Substructure

We study the highly magnified arc SGAS J122651.3+215220 caused by a star-forming galaxy at z s = 2.93 crossing the lensing caustic cast by the galaxy cluster SDSS J1226+2152 (z l = 0.43), using Hubble Space Telescope observations. We report in the arc several asymmetric surface brightness features whose angular separations are a fraction of an arcsecond from the lensing critical curve and appear to be highly but unequally magnified image pairs of underlying compact sources, with one brightest pair having clear asymmetry consistently across four filters. One explanation of unequal magnification is microlensing by intracluster stars, which induces independent flux variations in the images of individual or groups of source stars in the lensed galaxy. For a second possibility, intracluster dark matter subhaloes invisible to telescopes effectively perturb lensing magnifications near the critical curve and give rise to persistently unequal image pairs. Our modelling suggests, at least for the most prominent identified image pair, that the microlensing hypothesis is in tension with the absence of notable asymmetry variation over a six-year baseline, while subhaloes of ∼10 6 –10 8 \Mꙩ anticipated from structure formation with cold dark matter typically produce stationary and sizable asymmetries. We judge that observations at additional times and more precise lens models are necessary to stringently constrain temporal variability and robustly distinguish between the two explanations. The arc under this study is a scheduled target of a Director’s Discretionary Early Release Science program of the James Webb Space Telescope, which will provide deep images and a high-resolution view with integral field spectroscopy.

Liang Dai↗

Multicolor Three-Dimensional Tracking for Single-Molecule Fluorescence Resonance Energy Transfer Measurements

Single-molecule fluorescence resonance energy transfer (smFRET) remains a widely utilized and powerful tool for quantifying heterogeneous interactions and conformational dynamics of biomolecules. However, traditional smFRET experiments either are limited to short observation times (typically less than 1 ms) in the case of “burst” confocal measurements or require surface immobilization which usually has a temporal resolution limited by the camera framing rate. We developed a smFRET 3D tracking microscope that is capable of observing single particles for extended periods of time with high temporal resolution. The confocal tracking microscope utilizes closed-loop feedback to follow the particle in solution by recentering it within two overlapping tetrahedral detection elements, corresponding to donor and acceptor channels. We demonstrated the microscope’s multicolor tracking capability via random walk simulations and experimental tracking of 200 nm fluorescent beads in water with a range of apparent smFRET efficiency values, 0.45-0.69. We also demonstrated the microscope’s capability to track and quantify double-stranded DNA undergoing intramolecular smFRET in a viscous glycerol solution. In future experiments, the smFRET 3D tracking system will be used to study protein conformational dynamics while diffusing in solution and native biological environments with high temporal resolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Long-term soil transplant simulating climate change with latitude significantly alters microbial temporal turnover

To understand soil microbial community stability and temporal turnover in response to climate change, a long-term soil transplant experiment was conducted in three agricultural experiment stations over large transects from a warm temperate zone (Fengqiu station in central China) to a subtropical zone (Yingtan station in southern China) and a cold temperate zone (Hailun station in northern China). Annual soil samples were collected from these three stations from 2005 to 2011, and microbial communities were analyzed by sequencing microbial 16S ribosomal RNA gene amplicons using Illumina MiSeq technology. Our results revealed a distinctly differential pattern of microbial communities in both northward and southward transplantations, along with an increase in microbial richness with climate cooling and a corresponding decrease with climate warming. The microbial succession rate was estimated by the slope (w value) of linear regression of a log-transformed microbial community similarity with time (time–decay relationship). Compared with the low turnover rate of microbial communities in situ (w=0.046, P<0.001), the succession rate at the community level was significantly higher in the northward transplant (w=0.058, P<0.001) and highest in the southward transplant (w=0.094, P<0.001). Climate warming lead to a faster succession rate of microbial communities as well as lower species richness and compositional changes compared with in situ and climate cooling, which may be related to the high metabolic rates and intense competition under higher temperature. This study provides new insights into the impacts of climate change on the fundamental temporal scaling of soil microbial communities and microbial phylogenetic biodiversity.

54 ENVIRONMENTAL SCIENCES↗

Designing an Optimal Sensor Network via Minimizing Information Loss

Optimal experimental design is a classic topic in statistics, with many well-studied problems, applications, and solutions. The design problem we study is the placement of sensors to monitor spatiotemporal processes, explicitly accounting for the temporal dimension in our modeling and optimization. We observe that recent advancements in computational sciences often yield large datasets based on physics-based simulations, which are rarely leveraged in experimental design. We introduce a novel model-based sensor placement criterion, along with a highly-efficient optimization algorithm, which integrates physics-based simulations and Bayesian experimental design principles to identify sensor networks that “minimize information loss” from simulated data. Our technique relies on sparse variational inference and (separable) Gauss-Markov priors, and thus may adapt many techniques from Bayesian experimental design. We validate our method through a case study monitoring air temperature in Phoenix, Arizona, using state-of-the-art physics-based simulations. Our results show our framework to be superior to random or quasi-random sampling, particularly with a limited number of sensors. We conclude by discussing practical considerations and implications of our framework, including more complex modeling tools and real-world deployments.

54 ENVIRONMENTAL SCIENCES↗

Wind Forcing of the North Sea Pole Tide

The Chandler wobble of the earth's rotation has a period near 14 months and sets up the 0.5 cm amplitude pole tide in the deep oceans, However, the pole tide is anomalously large in the North Sea, where the amplitude increases sharply up to 3 cm along the continental coast. It is shown here that the sea levels are well correlated with winds at the pole tide frequency. The Princeton Ocean Model is used to investigate the response of the North Sea to wind forcing. The barotropic numerical ocean model depicts realistic coastlines and bathymetry at 5 ft x 5 ft resolution, with 97 x 73 grid points. The monthly mean wind fields for the 40-year period (1958-1997) from the National Centers for Atmospheric Prediction (NCEP) reanalysis were used to force the model. The winds were converted to stress with a neutral drag coefficient that varied linearly with windspeed (instead of using the NCEP windstress). A 5-day simulation was made for each month until the resulting flow regime came into equilibrium, and model water levels at various station locations were saved for comparison with tidal-gauge observed sea levels from the Permanent Service for Mean Sea Level (PSMSL). The comparison is made for 10 North Sea stations with high quality tide gauge data. We find: (1) good agreement in annual and semi-annual phases and in the trend of amplitude w.r.t. latitude; (2) more importantly for this study, the model-predicted and observed non-seasonal sea level variations show a very significant temporal correlation as well as spectral coherence. However, a large amplitude difference exists between the two sets -- the overall amplitude variability of the observed is generally a factor of 2-3 larger than the model prediction (this same phenomenon has been reported in ocean circulation studies, although the cause is not yet clear.) Our results indicate that the wind forcing is the main cause of the observed large pole tide in the North Sea.

OConnor, W.↗

Environmental Gating and Galvanic Effects in Single Crystals of Organic–Inorganic Halide Perovskites

Understanding the impact of environmental gaseous on the surface of organometal halide perovskites (OMHPs) couples to the electronic and ionic transport is critically important. Here, we explore the transport behavior and origins of the gas sensitivity in MAPbBr 3 single crystals (SCs) devices using impedance spectroscopy and current relaxation measurements. Strong resistive response occurs when crystals are exposed to different environments. It was shown that SC response to the environment is extremely different at the surface as compared to the bulk due to the disorder surface chemistry. The nonlinear transport properties studied using ultrafast Kelvin probe force microscopy (G-KPFM) to unravel spatio-temporal charge dynamics at SC/electrode interface. The relaxation processes observed in pulse relaxation and G-KPFM measurements along with gas sensitivity of crystals suggest the presence of a triple-phase boundary between environment, electrode, and crystal. Results indicate that the environment is a nontrivial component in the operation of OMHP devices which is reminiscent of fuel cell systems. Furthermore, the triple-phase boundary can play a significant role in the transport properties of OMHPs due to the possibility of the redox processes coupled to the concentration of bulk ionic species. Finally, although instrumental for understanding the device characteristics of perovskites, our studies suggest a new opportunity of coupling the redox chemistry of the Br 2 –Br – pair that defines the bulk ionic conductivity of MAPbBr 3 with the redox chemistry of gaseous (or liquid) environment via a suitable electrocatalytic system to enable new class of energy storage devices and gas sensors.

36 MATERIALS SCIENCE↗