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DOE OSTI2025

Mechanistic Insight into Tunable Spin Relaxation in Two-Dimensional Type-II Ligand-Perovskite Heterostructures

Two-dimensional (2D) metal-halide perovskites with spin-dependent optical properties hold great promise for spintronic and quantum applications. However, their spin lifetimes, especially for n = 1 2D perovskites, are typically limited to subpicosecond time scales due to rapid spin relaxation driven by strong spin−orbit coupling (SOC), electron−hole exchange interactions, and phonon-mediated scattering. Here, we demonstrate that type-II ligand-perovskite heterostructures overcome these constraints by reducing electron−hole wave function overlap and exciton binding energy. Compared to the type-I 2D perovskite (PEA) 2 PbI 4 with a spin lifetime of 0.29 ps at room temperature, our engineered type-II systems achieve substantially extended spin lifetimes, ∼6.37 ps for (4Tm) 2 PbI 4 and ∼18.47 ps for (4TCNm) 2 PbI 4 . In both materials, spatial charge separation across the perovskite−ligand interface mitigates the Bir−Aronov− Pikus (BAP) mechanism. Temperature- and fluence-dependent measurements reveal Elliott−Yafet (EY)-dominated spin relaxation in (4Tm) 2 PbI 4 , consistent with the observation of coherent phonon oscillation, whereas (4TCNm) 2 PbI 4 exhibits D’yakonov−Perel (DP)-dominated spin relaxation, with weaker phonon coupling further suppressing the EY relaxation, enabling spin lifetimes up to ∼126.81 ps at 5 K. Our findings establish a structural design framework for tailoring spin dynamics in 2D perovskites, offering a promising strategy to engineering spin and optoelectronic properties via rational ligand engineering.

Excitons↗

DOE OSTI2026

J -Resolved Molecular Fingerprinting by Parahydrogen Hyperpolarized Low-Field NMR

A J-resolved spectroscopy that depends on homonuclear scalar coupling in the strong-coupling regime and heteronuclear coupling in the weak regime expands complex peak patterns to a second axis. Hyperpolarization by Signal Amplification by Reversible Exchange (SABRE) enables the spectroscopy at a low magnetic field of 0.82 mT. Overlapping peaks of molecules such as 3-fluoropyridine and 3,5-difluoropyridine are resolved. Density matrix simulations of the 1 H and 19 F spins indicate a strong dependence on the signs and values of the J-coupling constants, including the homonuclear couplings that are not directly observable. The best matching peak positions and intensities predict coupling constants, including couplings between chemically equivalent nuclear spins, ranging in magnitude from 0.4 to 9.0 Hz for the two molecules. Simulations of other spin systems show unique patterns for molecules containing 1 H and 19 F or 13 C. The dependence of the J-resolved peak patterns on all coupling constants in a spin system presents a new modality for portable and inexpensive identification of molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Organic Cation Influence on Organic–Inorganic Thermal Equilibration within 2D Metal Halide Perovskites

Two-dimensional inorganic–organic lead halide perovskites exhibit tunable optoelectronic properties that are dictated by alternating layers of metal halide octahedra and organic cations. In such hybrid materials, vibrational coupling and thermalization between the low mass, insulating, organic cation spacers, and high mass inorganic octahedra remains poorly understood. Here, in this study, using femtosecond infrared-pump electronic-probe (IPEP) spectroscopy, we investigate the role of organic cation identity regarding the kinetics of vibrational energy exchange and sublattice mechanical coupling. Linear aliphatic cation-containing 2D perovskites with 4, 6, or 8 carbons (butylammonium = BA, hexylammonium = HA, and octylammonium = OA) were produced as thin films and mid-infrared pump pulses and then selectively excited organic cation stretch vibrations. Thermal energy introduction was evaluated via visible-wavelength optical probing that conveys inorganic octahedra response, owing to changes in electronic absorption. Multiple distinct spectral shifts appear upon excitation of the organic cations. Following an initial optical Stark shift caused by pump–probe temporal overlap, a redshift occurs within the first 10 ps that we attribute to compression of the octahedra by the expanded organic layers. Subsequently, a blueshift of the bandgap occurs commensurate with equilibration of both sublattices at an elevated temperature with a time constant of 21.8 to 31.6 ps depending on the spacer identity, with thermal energy transfer slowing by nearly 50% for the longest linker. By examining the effect that altered cation identity has on vibrational energy exchange, this work begins to offer routes to tune nonequilibrium response as well as provides insight into the fundamental impacts of organic spacers on thermal energy exchange in perovskite materials.

Peifer, Shoshanna E. [Northwestern Univ., Evanston↗

DOE OSTI2020

Storage Conditions of Human Kidney Tissue Sections Affect Spatial Lipidomics Analysis Reproducibility

Lipids often are labile, unstable, and tend to degrade overtime, so it is of the upmost importance to study these molecules in their most native state. In this study, we sought to understand the optimal storage conditions for spatial lipidomic analysis of human kidney tissue sections. Specifically, we evaluated human kidney tissue sections on several different days throughout the span of a week using our established protocol for elucidating lipids using high mass resolution matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI). We studied kidney tissue sections stored under five different conditions: open stored at –80 °C, vacuumed sealed and stored at –80 °C, with matrix preapplied before storage at –80 °C, under a nitrogen atmosphere and stored at –80 °C, and at room temperature in a desiccator. Results were compared to data obtained from kidney tissue sections that were prepared and analyzed immediately after cryosectioning. Data was processed using METASPACE. After a week of storage, the sections stored at room temperature showed the largest amount of lipid degradation, while sections stored under nitrogen and at –80 °C retained the greatest number of overlapping annotations in relation to freshly cut tissue. Overall, we found that molecular degradation of the tissue sections was unavoidable over time, regardless of storage conditions, but storing tissue sections in an inert gas at low temperatures can curtail molecular degradation within tissue sections.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

Using Ambient Noise Seismic Interferometry and Local and Teleseismic Earthquakes to Determine Crustal Thickness and Moho Structure of the Northwestern Gulf of Mexico Margin

Abstract The northwestern part of the Gulf of Mexico has undergone two episodes of continental rifting and collision and produced structural artifacts that are now buried under many kilometers of sediments, complicating investigations of the region. The deep sedimentary package precludes outcrops and points to a need for the application of seismic techniques, but low rates of seismicity in the region and sparse seismic monitoring limit the utility of traditional seismic methods. We therefore use diverse data to perform two‐dimensional seismic tomography across the dry land portion of the margin. Data are gleaned from teleseismic and regional earthquakes, postcritical SsPmp arrivals, and direct P wave energy identified with seismic interferometry that were recorded by a broadband, three‐component array and partially overlapping short‐period, vertical‐component array. The Pn and postcritical SsPmp phase help constrain the Moho discontinuity, which a previous receiver function study suggested was absent beneath the seaward portion of this transect. A high‐velocity body is observed in the crust at the same location as the Houston Magnetic Anomaly, possibly marking rocks from the Alleghenian continental assembly. The crust thins from NW to SE, indicating that extension occurred mostly to the south of the Ouachita orogeny. Our model indicates that the margin's sediment package reaches a maximum thickness of ~15 km at the coast and becomes unresolvably thin near the Llano Uplift.

58 GEOSCIENCES↗

DOE OSTI2021

First Simultaneous Observation of STEVE and SAR Arc Combining Data From Citizen Scientists, 630.0 nm All‐Sky Images, and Satellites

Abstract On September 28, 2017 citizen scientist observations at Alberta, Canada (51°N, 113° W) detected aurora and a thin east‐west purplish arc, known as strong thermal emission velocity enhancement (STEVE) that lasted less than 20 min. All‐sky imagers at subauroral latitudes measured stable auroral red (SAR) arcs during the entire night. The imager at Bridger, MT (45.3°N, 108.9°W) also measured a STEVE. The overlapping geometry allowed to determine that the height of STEVE was 225–275 km. STEVE is brighter in the 630.0 nm images in the West and almost merges with the SAR arc in the East. A DMSP satellite pass in the southern hemisphere was at the conjugate location of the Bridger imager during the STEVE observation. When mapped into the northern hemisphere intense subauroral ion drift and subauroral polarization streams were detected associated with the two optical signatures measured in 630.0 nm.

Martinis, C.↗

DOE OSTI2021

Observations and Simulations of Dropout Events and Flux Decays in October 2013: Comparing MEO Equatorial With LEO Polar Orbit

We compare ESA PROBA-V observations of electron flux at LEO with those from the NASA Van Allen Probes mostly at MEO for October 2013. Dropouts are visible at all energy during four storms from both satellites. Equatorially trapped electron fluxes are higher than at LEO by 10 2 (<1 MeV) to 10 5 (>2.5 MeV). We observe a quite isotropic structure of the outer belt during quiet times, contrary to the inner belt, and pitch angle dependence of high energy injection. We find a very good overlap of the outer belt at MEO and LEO at ~0.5 MeV. We use test-particle simulations of the energetic electrons trapped in the terrestrial magnetic field to study the outer radiation belt electron flux changes during geomagnetic storms. We show that the Dst (Disturbance storm time) effect during the main phase of a geomagnetic storm results in a betatron mechanism causing outward radial drift and a deceleration of the electrons. This outward drift motion is energy independent, pitch angle-dependent, and represents a significant distance (~1 L-shell at L = 5 for moderate storms). At fixed L-shell, this causes a decay of the LEO precipitating flux (adiabatic outward motion), followed by a return to the normal state (adiabatic inward motion) during main and recovery phases. Dst effect, associated with magnetopause shadowing and radial diffusion can explain the main characteristics of outer radiation belt electron dropouts in October 2013. We also use Fokker-Planck simulations with event-driven diffusion coefficients at high temporal resolution, to distinguish instantaneous loss from the gradual scattering that depopulates the slot region and the outer belt after storms. Simulations reproduce the slot formation and the gradual loss in the outer belt. The typical energy dependence of these losses leads to the absence of scattering for relativistic and ultra-relativistic electrons in the outer belt, oppositely to dropouts.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Anthropogenic Impacts on Atmospheric Carbonyl Sulfide Since the 19th Century Inferred From Polar Firn Air and Ice Core Measurements

Carbonyl sulfide (COS) was measured in firn air collected during seven different field campaigns carried out at four different sites in Greenland and Antarctica between 2001 and 2015. A Bayesian probabilistic statistical model is used to conduct multisite inversions and to reconstruct separate atmospheric histories for Greenland and Antarctica. The firn air inversions cover most of the 20th century over Greenland and extend back to the 19th century over Antarctica. The derived atmospheric histories are consistent with independent surface air time series data from the corresponding sites and the Antarctic ice core COS records during periods of overlap. Atmospheric COS levels began to increase over preindustrial levels starting in the 19th century, and the increase continued for much of the 20th century. Atmospheric COS peaked at higher than present-day levels around 1975 CE over Greenland and around 1987 CE over Antarctica. An atmosphere/surface ocean box model is used to investigate the possible causes of observed variability. The results suggest that changes in the magnitude and location of anthropogenic sources have had a strong influence on the observed atmospheric COS variability.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Soil Respiration Response to Rainfall Modulated by Plant Phenology in a Montane Meadow, East River, Colorado, USA

Soil respiration is a primary component of the terrestrial carbon cycle. However, predicting the response of soil respiration to climate change remains a challenge due to the complex interactions between environmental drivers, especially plant phenology, temperature, and soil moisture. In this study, we use a 1-D diffusion-reaction model to calculate depth-resolved CO 2 production rates from soil CO 2 concentrations and surface efflux observations in a subalpine meadow in the East River watershed, CO. Modeled rates are compared to in situ soil temperature and moisture conditions and MODIS satellite enhanced vegetation index (EVI) representing plant phenology across three hydrologically distinct growing seasons from 2016-2018. While soil respiration correlated with temperature on diel timescales (p<0.05), seasonal variability was dominated by soil moisture and plant phenology (p<0.05). We observed significant respiration increases in response to precipitation events; however, magnitude and duration were significantly higher in 2017 than 2016 despite similar wetting characteristics. Based on MODIS EVI, we suggest the respiration response to rainfall is controlled by plant phenology, which in turn reflects the capacity of plants to respond to precipitation via increased photosynthesis and autotrophic respiration, behavior that is not captured in typical soil respiration pulse models. Projected changes in montane climate such as earlier snowmelt and prolonged fore-summer drought may decrease soil respiration fluxes by decreasing the overlap between peak productivity and the summer monsoon. Lastly, we observed significant late-season CO 2 fluxes from the deep sub-soil (>165 cm) that support growing evidence for the importance of sub-soil processes in driving integrated respiration fluxes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Assessing Uncertainties and Approximations in Solar Heating of the Climate System

In calculating solar radiation, climate models make many simplifications, in part to reduce computational cost and enable climate modeling, and in part from lack of understanding of critical atmospheric information. Whether known errors or unknown errors, the community's concern is how these could impact the modeled climate. The simplifications are well known and most have published studies evaluating them, but with individual studies it is difficult to compare. Here, we collect a wide range of such simplifications in either radiative transfer modeling or atmospheric conditions and assess potential errors within a consistent framework on climate-relevant scales. We build benchmarking capability around a solar heating code (Solar-J) that doubles as a photolysis code for chemistry and can be readily adapted to consider other errors and uncertainties. The broad classes here include: use of broad wavelength bands to integrate over spectral features; scattering approximations that alter phase function and optical depths for clouds and gases; uncertainty in ice-cloud optics; treatment of fractional cloud cover including overlap; and variability of ocean surface albedo. We geographically map the errors in W m -2 using a full climate re-creation for January 2015 from a weather forecasting model. For many approximations assessed here, mean errors are ~2 W m -2 with greater latitudinal biases and are likely to affect a model’s ability to match the current climate state. Combining this work with previous studies, we make priority recommendations for fixing these simplifications based on both the magnitude of error and the ease or computational cost of the fix.

58 GEOSCIENCES↗

DOE OSTI2022

Effect of the Grell-Freitas Deep Convection Scheme in Quasi-Uniform and Variable-Resolution Aquaplanet CAM Simulations

The Grell-Freitas deep convection scheme (GF) has been implemented in the Community Atmosphere Model (CAM) with the nonhydrostatic Model for Prediction Across Scales (MPAS) dynamical core. Aquaplanet simulations have been performed with a global quasi-uniform resolution mesh with ~120 km grid spacing and a variable resolution mesh employing a circular refined region with ~30 km grid spacing centering at the equator and ~120 km elsewhere. GF produces overall patterns of the general circulations comparable to those of other aquaplanet experiments, including those produced using the default Zhang-McFarlane convection scheme (ZM) in CAM Version 5.4. GF alleviates the overestimated occurrence of weak intensity precipitation characteristic of ZM due to GF’s different closure methods and deep-convection trigger conditions. Compared to ZM, the GF characteristics of the equatorial Kelvin waves are closer to observations. GF also better simulates precipitation at variable resolution, with no unrealistic wave distortion by the refinement. Overall, GF shows less sensitivity of convective precipitation and heating/moistening tendencies to changes in horizontal resolution compared to ZM. However, vertically-overlapped total cloud fraction simulated with GF in the tropics is more sensitive to the resolution than ZM due to the larger resolution-sensitivity of high-level cloud fraction in the tropics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Data Assimilative Optimization of WSA Source Surface and Interface Radii using Particle Filtering

TheWang-Sheeley-Arge (WSA) model estimates solar wind speed and interplanetary magnetic field polarity in the inner heliosphere using global photospheric magnetic field maps. WSA employs the Potential Field Source Surface (PFSS) and Schatten Current Sheet (SCS) models to determine the Sun's global coronal magnetic field. The PFSS and SCS models are connected through two radial parameters, the source surface and interface radii, which specify the overlap region between the inner SCS and outer PFSS models. Though both radii values are adjustable, they have typically been fixed to 2.5 solar radii. Our work highlights how solar wind predictions improve when the radii are allowed to vary over time. Data assimilation using particle filtering (sequential Monte Carlo) is used to infer optimal values over a fixed time window. Solar wind model predictions and satellite observations are compared with a newly developed quality-of-agreement prediction metric. The agreement metric between the model and observations is assumed to correspond to the probability of the two key WSA model parameters, the source surface and interface radii, where the highest metric value implies the optimal radii.We find that the optimal particle filter values of solar radii can perform twice as well as standard values for an exploratory period during Carrington Rotation 1901, with these values also reducing nonphysical kinking effects seen in solar magnetic field lines. Data assimilation choices of input realization and time frame have implications for variation in the solar wind over time. We present this work's theoretical context and practical applications for prediction accuracy.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Parsing Weather Variability and Wildfire Effects on the Post-Fire Changes in Daily Stream Flows: A Quantile-Based Statistical Approach and Its Application

Determining wildland fire impacts on streamflow can be problematic as the hydrology in burned watersheds is influenced by post-fire weather conditions. Here, this study presents a quantile-based analytical framework for assessing fire impacts on low and peak daily flow magnitudes, while accounting for post-fire weather influences. This framework entails (a) the bootstrap method to compute the relative change in the post-fire annual flow and weather statistics, (b) double mass analysis to detect if post-fire baseflow and quick-flow yield ratios are significantly altered, and (c) a quantile regression method to parse fire effects on flow at a specific quantile. We illustrate the applicability of this analytical framework using 44 western US streams with at least 5% of their watershed area burned. Results indicate that large, high-severity burns in upland watersheds can raise the streamflow magnitude at the 0. 05 th and 0. 95 th quantiles for at least the five post-fire years. Quantile regression results show that the median fire-related increase in flow for the five post-fire years can be up to 5,000% (Standard Error; S.E. < 2%) at the 0. 05 th E quantile and 161% (S.E. < 10%) at the 0. 95 th quantile. The fire-related increase in flow was often pronounced at the 0. 05 th quantile for streams in the Pacific Northwest and California regions. The difference in fire effects on flow (at both quantiles) across streams was related to post-fire weather, pyrology, physiography, and land cover. The proposed analytical framework can be useful for detecting and quantifying fire effects on the low and peak stream flows in burned watersheds without overlapping disturbances.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The Principal Hugoniot of Iron-Bearing Olivine to 1465 GPa

Shock compression experiments on natural compositions are imperative to accurately model planetary accretion and the interior dynamics of planets. Combining shock compression experiments from the Sandia Z Machine and the OMEGA EP laser facility with density functional theory-based molecular dynamics calculations, we report the first pressure-density-temperature (P-ρ-T) relationship of natural iron (Fe)-bearing olivine ((Mg 0.91 Fe 0.09 ) 2 SiO 4 ) on the principal Hugoniot between 166 and 1,465 GPa. Additionally, we report the first reflectivities of natural olivine liquid in this pressure range. Compared to the magnesium-endmember forsterite (Mg 2 SiO 4 ), the presence of Fe in typical mantle abundance (~9 wt% FeO) alters the U S -u P relation of olivine. Furthermore, the shock temperature and reflectivity of olivine are indistinguishable from forsterite where experimental conditions overlap. Both forsterite and olivine increase in reflectivity (and hence optical conductivity) with increasing temperature, with a maximum reflectivity of ~31% at shock velocities greater than 22 km/s (~800 GPa).

58 GEOSCIENCES↗

DOE OSTI2021

Probing the Magnetosheath Boundaries Using Interstellar Boundary Explorer (IBEX) Orbital Encounters

Inside the magnetosheath, the IBEX-Hi energetic neutral atom (ENA) imager measures a distinct background count rate that is more than 10 times the typical heliospheric ENA emissions observed when IBEX is outside the magnetosheath. The source of this enhancement is magnetosheath ions of solar wind (SW) origin that deflect around the Earth's magnetopause (MP), scatter and neutralize from the anti-sunward part of the IBEX-Hi sunshade, and continue into the instrument as neutral atoms, behaving indistinguishably from ENAs emitted from distant plasma sources. While this background pollutes observations of outer heliospheric ENAs, it provides a clear signature of IBEX crossings over the magnetospheric boundaries. In this study, we investigate IBEX encounters with the magnetosheath boundaries using ~8 yr of orbital data, and we determine the MP and bow shock (BS) locations derived from this background signal. We find 280 BS crossings from X GSE ~ 11 R e to X GSE ~ –36 R e and 241 MP crossings from X GSE ~ 6 R e to X GSE ~ –48 R e . We compare IBEX BS and MP crossing locations to those from IMP-8, Geotail, Cluster, Magion-4, ISEE, and Magnetospheric Multiscale Mission, and we find that IBEX crossing locations overlap with the BS and MP locations inferred from these other data sets. In this paper, we demonstrate how IBEX can be used to identify magnetosheath crossings, and extend boundary observations well past the terminator, thus further constraining future models of magnetosheath boundaries. Furthermore, we use the IBEX data set to show observational evidence of near-Earth magnetotail squeezing during periods of strong interplanetary magnetic field B y .

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Monitoring Fracture Saturation With Internal Seismic Sources and Twin Neural Networks

Seismic coda-wave analysis is a well-developed method for detecting subtle physical changes in complex media by measuring arrival times in the late-arriving energy from multiply scattered or reflected waves. However, a challenge arises when multiply scattered waves are not sufficiently separated in time from the direct arrivals to provide a clear coda wave train. Additional complications for monitoring changes in fracture systems arise when the signals originate from unsynchronized internal sources, such as natural or induced seismicity, from acoustic emission, or from transportable intra-fracture sources (chattering dust), that generate uncontrolled signals that vary in arrival time, amplitude and frequency content. Here, we use a twin neural network (TNN also known as a Siamese neural network) for dimensionality reduction to analyze signals from chattering dust to classify the fluid saturation state of a synthetic fracture system. The TNN with shared weights generates a low-dimensional representation of the data input by minimizing contrastive loss, serving as the input to a multiclass classifier that accurately classifies whether multiple fractures in a fracture system are fully saturated or partially saturated, or whether a change in saturation has occurred in different fractures in the system. Furthermore, these results show that information buried in unresolved codas from uncontrolled sources can be extracted using machine learning to monitor the evolution of fracture systems caused by physical and chemical processes even when the scattered and direct wave fields overlap.

58 GEOSCIENCES↗

DOE OSTI2021

Dairy Methane Emissions in California's San Joaquin Valley Inferred With Ground‐Based Remote Sensing Observations in the Summer and Winter

Abstract The dairy industry in the San Joaquin Valley (SJV) is one of California’s largest methane (CH 4 ) sources. Reducing dairy emissions is a priority for the state’s climate change plans. Observations of current dairy CH 4 emissions are key to monitoring actions taken toward this goal. To help support this, we present new ground‐based measurements of atmospheric column‐averaged CH 4 mixing ratio (XCH 4 ) gradients across a group of 600 dairies in the central SJV using EM27/SUN solar spectrometers. We used measurements from the 2019 summer and 2020 winter seasons for a top‐down emission inversion based on the WRF‐STILT model. Our top‐down estimates of the region’s dairy emissions range from 90% to 183% of the current CALGEM inventory’s emissions of 277 Gg/yr. In contrast to the strong temperature dependence found by earlier dairy CH 4 emission studies, we also find that our top‐down emissions during the winter measurement days are comparable to the summer measurement days, possibly due to seasonal changes in dairy management practices and meteorological conditions. Furthermore, we find significant interday variability in our measurements and find that our emission estimates overlap with earlier top‐down studies and bottom‐up inventories in this region. Our study demonstrates how analysis of ground‐based remotely sensed CH 4 gradient observations can help improve our understanding of CH 4 sources at scales relevant to mitigation policy. It also reflects the need for long‐term monitoring of CH 4 emissions in the region and at individual facilities to better understand their emissions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Trends in Downwelling Longwave Radiance Over the Southern Great Plains

Downwelling longwave radiation is an important part of the surface energy budget. Spectral trends in the downwelling longwave radiance (DLR) provide insight into the radiative drivers of climate change. In this research, we process and analyze a 23-year DLR record measured by the Atmospheric Emitted Radiance Interferometer (AERI) at the U.S. Department of Energy Atmospheric Radiation Program Southern Great Plains (SGP) site. Two AERIs were deployed at SGP with an overlapping observation period of about 10 years, which allows us to examine the consistency and accuracy of the measurements and to account for discrepancies between them due to errors associated with the instruments themselves. We then analyzed the all-sky radiance trends in DLR, which are associated with the surface warming trend at SGP during this same period and also the complex changes in meteorological conditions. For instance, the observed radiance in the CO2 absorption band follows closely the near-surface air temperature variations. The significant positive radiance trends in weak absorption channels, such as in the wings of the CO 2 band and in the weak absorption channels in the H 2 O vibration-rotational band, show earlier detectability of climate change. The magnitude of the radiance trend uncertainty in the DLR record mainly results from internal climate variability rather than from measurement error, which highlights the importance of continuing the DLR spectral measurements to unambiguously detect and attribute climate change.

54 ENVIRONMENTAL SCIENCES↗