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Probing Quantum Speed Limits with Ultracold Gases

Here, quantum speed limits (QSLs) rule the minimum time for a quantum state to evolve into a distinguishable state in an arbitrary physical process. These fundamental results constrain a notion of distance traveled by the quantum state, known as the Bures angle, in terms of the speed of evolution set by nonadiabatic energy fluctuations. I theoretically propose how to measure QSLs in an ultracold quantum gas confined in a time-dependent harmonic trap. In this highly-dimensional system of continuous variables, quantum tomography is prohibited. Yet, QSLs can be probed whenever the dynamics is self-similar by measuring as a function of time the cloud size of the ultracold gas. This makes it possible to determine the Bures angle and energy fluctuations, as I discuss for various ultracold atomic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Climatology of Linear Mesoscale Convective System Morphology in the United States based on Random Forests Method

This study uses machine learning methods, specifically the random forest (RF), on a radar-based mesoscale convective system (MCS) tracking dataset to classify the five types of linear MCS morphology in the contiguous United States during the period 2004-2016. The algorithm is trained using radar- and satellite-derived spatial and morphological parameters, and reanalysis environmental information from 5-26yr manually identified nonlinear and five linear MCS modes. The algorithm is then used to automate the classification of linear MCSs over 8 years with high accuracy, providing a systematic, long-term climatology of linear MCSs. Results reveal that nearly 40% of MCSs are classified as linear MCSs, in which half of the linear events belong to the type of system having a leading convective line. The occurrence of linear MCSs shows large annual and seasonal variations. On average, 113 linear MCSs occur annually during the warm season (through March to October), with most of these events clustered from May through August in the central eastern Great Plains. MCS characteristics, including duration, propagation speed, orientation, and system cloud size, have large variability among the different linear modes. The systems having a trailing convective line and the systems having a back-building area of convection typically move more slowly and have higher precipitation rate, and thus have higher potential in producing extreme rainfall and flash flooding. Analysis of the environmental conditions associated with linear MCSs show that the storm-relative flow is of most importance in determining the organization mode of linear MCSs.

Cui, Wenjun↗

Computational Risk Analysis of Propane Releases in Maintenance Facilities

Liquefied petroleum gas (LPG) is a viable, cleaner alternative to traditional diesel fuel used in busses and other heavy-duty vehicles and could play a role in helping the US meet its lower emission goals. While the LPG industry has focused efforts on developing vehicles and fueling infrastructure, we must also establish safe parameters for maintenance facilities which are servicing LPG fueled vehicles. Current safety standards aid in the design of maintenance facilities, but additional quantitative analysis is needed to prove safeguards are adequate and suggest improvements where needed. In this report we aim to quantify the amount of flammable mass associated with propane releases from vehicle mounted fuel vessels within enclosed garages. Furthermore, we seek to qualify harm mitigation with variable ventilations and facility layout. To accomplish this we leverage validated computational resources at Sandia National Laboratories to simulate various release scenarios representative of real world vehicles and maintenance facilities. Flow solvers are used to predict the dynamics of fuel systems as well as the evolution of propane during release events. From our simulated results we observe that both inflow and outflow ventilation locations play a critical role in reducing flammable cloud size and potential overpressure values during a possible combustion event.

03 NATURAL GAS↗

Investigating Characteristic Droplet Size Distributions in Large Eddy Simulations of Stratocumulus Clouds

Cloud processes relevant to radiative and precipitation properties depend on the shape of the cloud droplet size distribution. Recent holographic observations revealed that cloud droplet populations do not have the same size distribution shapes throughout but form regions of characteristic distributions with similar microphysical properties. We investigate the existence and properties of these characteristic distributions within Large‐Eddy Simulations of stratocumulus clouds using Lagrangian and bin microphysics schemes. Distribution types are identified, revealing localized characteristic distributions that vary on the scale of the largest convective cell for simulations with bin microphysics. The results from the Lagrangian microphysics scheme hint at similar behavior. Compared to observations, the simulated clouds are much more uniform. Analysis of the LES results suggests a connection to the local entrainment rate, so the poorly resolved entrainment interface in LES may be a cause of the uniformity. The uniformity of the large‐scale forcing could also be a factor.

cloud droplet size distributions↗

Quantifying structural errors in cloud condensation nuclei activity from reduced representation of aerosol size distributions

Aerosol effects on clouds and radiation are the dominant contribution to uncertainty in radiative forcing relative to the pre-industrial atmosphere. While previous studies have assessed the impact of parametric uncertainty on modeled forcing, structural errors from the numerical representation of particle distributions have not been well quantified. Here we present a framework for quantifying error in aerosol size distributions and cloud condensation nuclei activity, which we apply to the widely used 4-mode version of the Modal Aerosol Module (MAM4). Box model predictions from the MAM4 are evaluated against the Particle Monte Carlo Model for Simulating Aerosol Interactions and Chemistry (PartMC-MOSAIC), a benchmark model that tracks the evolution of individual particles. We show that size distributions simulated by MAM4 diverge from those simulated by PartMC-MOSAIC after only a few hours of aging by condensation and coagulation in polluted conditions, which leads to large errors in modeled cloud condensation nuclei concentrations. We find that differences between MAM4 and PartMC-MOSAIC are largest under polluted conditions, where the size distribution evolves rapidly though aging by condensation of semi-volatile substances and coagulation among particles. These findings suggest that structural error in modeled aerosol properties contributes to the large inter-model variability in aerosol radiative forcing.

Fierce, Laura M.↗

Automated Identification of Characteristic Droplet Size Distributions in Stratocumulus Clouds Utilizing a Data Clustering Algorithm

Abstract Droplet-level interactions in clouds are often parameterized by a modified gamma fitted to a “global” droplet size distribution. Do “local” droplet size distributions of relevance to microphysical processes look like these average distributions? This paper describes an algorithm to search and classify characteristic size distributions within a cloud. The approach combines hypothesis testing, specifically, the Kolmogorov–Smirnov (KS) test, and a widely used class of machine learning algorithms for identifying clusters of samples with similar properties: density-based spatial clustering of applications with noise (DBSCAN) is used as the specific example for illustration. The two-sample KS test does not presume any specific distribution, is parameter free, and avoids biases from binning. Importantly, the number of clusters is not an input parameter of the DBSCAN-type algorithms but is independently determined in an unsupervised fashion. As implemented, it works on an abstract space from the KS test results, and hence spatial correlation is not required for a cluster. The method is explored using data obtained from the Holographic Detector for Clouds (HOLODEC) deployed during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The algorithm identifies evidence of the existence of clusters of nearly identical local size distributions. It is found that cloud segments have as few as one and as many as seven characteristic size distributions. To validate the algorithm’s robustness, it is tested on a synthetic dataset and successfully identifies the predefined distributions at plausible noise levels. The algorithm is general and is expected to be useful in other applications, such as remote sensing of cloud and rain properties. Significance Statement A typical cloud can have billions of drops spread over tens or hundreds of kilometers in space. Keeping track of the sizes, positions, and interactions of all of these droplets is impractical, and, as such, information about the relative abundance of large and small drops is typically quantified with a “size distribution.” Droplets in a cloud interact locally, however, so this work is motivated by the question of whether the cloud droplet size distribution is different in different parts of a cloud. A new method, based on hypothesis testing and machine learning, determines how many different size distributions are contained in a given cloud. This is important because the size distribution describes processes such as cloud droplet growth and light transmission through clouds.

54 ENVIRONMENTAL SCIENCES↗

Using aircraft measurements to characterize subgrid-scale variability of aerosol properties near the Atmospheric Radiation Measurement Southern Great Plains site

Abstract. Complex distributions of aerosol properties evolve in space and time as a function of emissions, new particle formation, coagulation, condensational growth, chemical transformation, phase changes, turbulent mixing and transport, removal processes, and ambient meteorological conditions. The ability of chemical transport models to represent the multi-scale processes affecting the life cycle of aerosols depends on their spatial resolution since aerosol properties are assumed to be constant within a grid cell. Subgrid-scale-dependent processes that affect aerosol populations could have a significant impact on the formation of particles, their growth to cloud condensation nuclei (CCN) sizes, aerosol–cloud interactions, dry deposition and rainout and hence their burdens, lifetimes, and radiative forcing. To address this issue, we characterize subgrid-scale variability in terms of measured aerosol number, size, composition, hygroscopicity, and CCN concentrations made by repeated aircraft flight paths over the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystem (HI-SCALE) campaign. Subgrid variability is quantified in terms of both normalized frequency distributions and percentage difference percentiles using grid spacings of 3, 9, 27, and 81 km that represent those typically used by cloud-system-resolving models as well as the current and next-generation climate models. Even though the SGP site is a rural location, surprisingly large horizontal gradients in aerosol properties were frequently observed. For example, 90 % of the 3, 9, and 27 km cell mean organic matter concentrations differed from the 81 km cell around the SGP site by as much as ∼ 46 %, large spatial variability in aerosol number concentrations and size distributions were found during new particle formation events, and consequently 90 % of the 3, 9, and 27 km cell mean CCN number concentrations differed from the 81 km cell mean by as much as ∼ 38 %. The spatial variability varied seasonally for some aerosol properties, with some having larger spatial variability during the spring and others having larger variability during the late summer. While measurements at a single surface site cannot reflect the surrounding variability of aerosol properties at a given time, aircraft measurements that are averaged within an 81 km cell were found to be similar to many, but not all, aerosol properties measured at the ground SGP site. This analysis suggests that it is reasonable to directly compare most ground SGP site aerosol measurements with coarse global climate model predictions. In addition, the variability quantified by the aircraft can be used as an uncertainty range when comparing the surface point measurements with model predictions that use coarse grid spacings.

54 ENVIRONMENTAL SCIENCES↗

Entrainment and aerosol effects on marine boundary-layer clouds: An investigation using ACE-ENA data from HOLODEC, G1, Pico and ACTOS (Final Report on Project Activities)

Marine boundary-layer clouds cover large regions of the globe and are known to strongly influence radiative balances. The microphysical properties and persistence of these clouds are tightly coupled with cloud-top entrainment and aerosol properties within both the boundary layer and the overlying free troposphere. This work addressed the microphysical response to entrainment and aerosol properties in marine stratocumulus clouds, using data from the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) project. Specifically, emphasis was placed on 1. extensive in situ measurements taken with the Atmospheric Radiation Measurement (ARM) G1 aircraft using the Holographic Detector for Clouds (Holodec) instrument; 2. airborne measurements obtained with the helicopter-borne Airborne Cloud Turbulence Observation System (ACTOS) operated by the Leibniz Institute for Tropospheric Research (TROPOS) during the first phase of ACE-ENA; and 3. above-boundary-layer, mountain-top measurements taken at the Pico Mountain Observatory (OMP) by the research group of the co-investigator and scientists from TROPOS during the first phase of ACE-ENA. The work is aligned with the topic “Warm Boundary-Layer Atmospheric Processes.” Key results include the following. Data from the Holographic Detector for Clouds (Holodec) were reprocessed, refined, and validated through a careful instrument intercomparison, resulting in a high-quality dataset available on the ARM archive for ACE-ENA. High-resolution ACTOS measurements of thermodynamics, microphysical, and turbulence properties were analyzed to explore the behavior of the entrainment velocity at cloud top. Analysis of the vertical variability of cloud droplet size distribution shape suggests that mixing is more inhomogeneous near cloud top, and more homogeneous deeper into the cloud. Analysis of aerosol measurements from OMP explored the mixing state and cloud condensation nucleus properties, as well as the implications for radiative forcing. Finally, a machine learning algorithm was developed for identifying characteristic cloud droplet size distributions, and was employed to explore microphysical regimes in stratocumulus clouds observed during ACE-ENA. The characteristic size distributions are narrow, and only when spatially averaged do they produce the broad “gamma” distributions typically assumed in models. This implies that precipitation development should account for variability and correlations in the distribution shape as well as the number concentration of cloud droplets.

54 ENVIRONMENTAL SCIENCES↗

Three-Channel Sunphotometer Cloud Mode Value-Added Product Report

A primary source of uncertainty in Earth system model (ESM) predictions is the representation of cloud processes and associated cloud feedback. Several fundamental cloud properties critical to the understanding of aerosol-cloud interactions are poorly constrained by observations, with key deficiencies in our observations of cloud and precipitation droplet sizes and cloud optical depth. Observations of these cloud properties are often challenging to estimate from remote-sensing platforms and costly to obtain from in situ aircraft. Nevertheless, observations of boundary-layer clouds, and improved knowledge of stratocumulus cloud (Sc) processes, are especially important to ESM advancement. This is because these clouds have extensive coverage and exert controls on boundary-layer dynamics and the global radiative energy balance.

54 ENVIRONMENTAL SCIENCES↗

Parallax-corrected VISST-derived pixel-level products from satellite GOES-16

The NASA Langley group led by William Smith produced GOES-16 satellite cloud retrievals over an approximate 10 by 10 degree region over the CACTI field campaign location. These retrievals are described here: https://www.arm.gov/capabilities/vaps/visst and are available for download here . They use algorithms historically called VISST that are now referred to as SatCORPS. More information can be found in Trepte et al. (2019), Minnis et al. (2021), and Yost et al. (2021). If using this dataset, please cite these references, the CACTI VISST dataset DOI found at the download link above, and this dataset’s DOI. The CACTI VISST pixel-level retrievals are on a 2 km spatial grid and available every 15 minutes (every 10 minutes late in the campaign), producing 21,765 files for the entire field campaign between October 2018 and April 2019. They are not corrected for parallax error, which is an offset in the actual geographical location of a cloud above the surface due to the satellite viewing the cloud partly from the side off nadir. This dataset applies a correction for parallax using the location relative to the satellite and the retrieved cloud top height above the surface, which allows the dataset to be geo-located with surface-based observations. The parallax correction for each location depends on the longitude, latitude and cloud top height above ground level (AGL) for that longitude and latitude in the original VISST files. The cloud top height AGL requires first computing the surface elevation at each VISST grid point. Data from the Advanced Spaceborne Thermal Emission and Reflection (ASTER) Global Digital Elevation Map Version 3 at 30-m resolution is projected onto the VISST grid using conservative coarsening (conserving surface elevation) in the xESMF Python package. The surface elevation is then subtracted from the VISST-retrieved cloud top height above mean sea level. These cloud top heights AGL are then combined with longitude and latitude to estimate the latitude and longitude corrections. Due to variability in cloud top height, the parallax shifts produce an irregular grid of values since higher cloud tops are shifted further than lower cloud tops. A ball tree-based neighbor search with Haversine distance is performed using the Python-based scikit-learn library to find the nearest VISST grid point to each parallax correction-shifted point. The data value of the shifted point is then assigned to that VISST grid point. In this manner, the irregular geographical shifts to correct for parallax are projected back to the rectilinear VISST grid. Because relatively higher clouds should obscure lower clouds, the variable values for the highest cloud top are preferentially chosen if two or more values are assigned to a grid point. The parallax correction should be viewed as an improved but still imperfect estimation of the cloud top locations, largely because the cloud top height is an imperfect retrieval. Please see the attached README document for further information. Users are encouraged to contact the authors with any additional questions.

54 ENVIRONMENTAL SCIENCES↗

Cloud microphysical response to entrainment and mixing is locally inhomogeneous and globally homogeneous: Evidence from the lab

Entrainment of dry air into clouds strongly influences cloud optical and precipitation properties and the response of clouds to aerosol perturbations. The response of cloud droplet size distributions to entrainment–mixing is examined in the Pi convection-cloud chamber that creates a turbulent, steady-state cloud. The experiments are conducted by injecting dry air with temperature (T e ) and flow rate (Q e ) through a flange in the top boundary, into the otherwise well-mixed cloud, to mimic the entrainment–mixing process. Due to the large-scale circulation, the downwind region is directly affected by entrained dry air, whereas the upwind region is representative of the background conditions. Droplet concentration (Cn) and liquid water content (L) decrease in the downwind region, but the difference in the mean diameter of droplets (D m ) is small. The shape of cloud droplet size distributions relative to the injection point is unchanged, to within statistical uncertainty, resulting in a signature of inhomogeneous mixing, as expected for droplet evaporation times small compared to mixing time scales. As T e and Q e of entrained air increase, however, Cn, L, and D m of the whole cloud system decrease, resulting in a signature of homogeneous mixing. The apparent contradiction is understood as the cloud microphysical responses to entrainment and mixing differing on local and global scales: locally inhomogeneous and globally homogeneous. This implies that global versus local sampling of clouds can lead to seemingly contradictory results for mixing, which informs the long-standing debate about the microphysical response to entrainment and the parameterization of this process for coarse-resolution models.

54 ENVIRONMENTAL SCIENCES↗

Climatology of the Vertical Profiles of Polarimetric Radar Variables and Retrieved Microphysical Parameters in Continental/Tropical MCSs and Landfalling Hurricanes

Most existing cloud models tend to overestimate the size of cloud ice particles and underestimate their concentration. This emphasizes the need to provide a reliable observational reference to optimize cloud model performance, particularly in areas of high concentration of ice at high altitudes. The dual-polarization radars give the community a unique opportunity to quantify cloud ice with a good accuracy using polarimetric radar retrievals. Here, in this study, we utilize the network of operational WSR-88D radars to build a climatology of the vertical profiles of radar variables, such as radar reflectivity Z, differential reflectivity Z DR , and specific differential phase K DP as well as the radar-retrieved vertical profiles of ice water content (IWC) above the melting layer and liquid water content below it, mean volume diameter D m , and total number concentration N t of ice and liquid particles. Such climatology was created for continental/marine mesoscale convective systems (MCSs) and tropical cyclones including hurricanes. The dataset includes 13 continental MCSs, 10 marine MCSs, and 11 tropical cyclones. Separate statistics of the “background” vertical profiles and the ones associated with high IWC aloft have been obtained in the course of this study. It is shown that continental MCSs exhibit larger size of ice in lower concentration aloft compared to the marine MCSs and especially tropical cyclones/hurricanes. A combination of high KDP and low Z aloft signifies lower D m , higher N t , and often substantial IWC.

54 ENVIRONMENTAL SCIENCES↗

Are turbulence effects on droplet collision–coalescence a key to understanding observed rain formation in clouds?

Rain formation is a critical factor governing the lifecycle and radiative forcing of clouds and therefore it is a key element of weather and climate. Cloud microphysics–turbulence interactions occur across a wide range of scales and are challenging to represent in atmospheric models with limited resolution. Based on past experiments and idealized numerical simulations, it has been postulated that cloud turbulence accelerates rain formation by enhancing drop collision–coalescence. We provide substantial evidence for significant impacts of turbulence on the evolution of cloud droplet size distributions and rain formation by comparing high-resolution observations of cumulus congestus clouds with state-of-the-art large-eddy simulations coupled with a Lagrangian particle-based microphysics scheme. Turbulent coalescence must be included in the model to accurately represent the observed drop size distributions, especially for drizzle drop sizes at lower heights in the cloud. Turbulence causes earlier rain formation and greater rain accumulation compared to simulations with gravitational coalescence only. The observed rain size distribution tail just above cloud base follows a power law scaling that deviates from theoretical scalings considering either a purely gravitation collision kernel or a turbulent kernel neglecting droplet inertial effects, providing additional evidence for turbulent coalescence in clouds. In contrast, large aerosols acting as cloud condensation nuclei (“giant CCN”) do not significantly impact rain formation owing to their long timescale to reach equilibrium wet size relative to the lifetime of rising cumulus thermals. Overall, turbulent drop coalescence exerts a dominant influence on rain initiation in warm cumulus clouds, with limited impacts of giant CCN.

54 ENVIRONMENTAL SCIENCES↗

Are Marine Low Cloud Droplet Concentrations Buffered by Entrained Aitken‐Mode Aerosol (Final Technical Report)

During the summertime, the high-latitude oceans come to life with green phytoplankton, which gain their energy from sunlight and are food for sea creatures small and large. When the phytoplankton are eaten or die, sulfur-rich gases are released under the ocean surface and mix into the air. Observations suggest that, over the Southern Ocean, frequent storms lift this air high into the atmosphere while raining out particulates like salt. As a result, the sulfur-rich air then spawns high concentrations of small ‘Aitken-mode’ aerosol particles. We hypothesize that these particles work their way down into the marine boundary layer, where they can replenish the supply of cloud-condensation nuclei scavenged by frequent precipitation. Further, this process maintains high concentrations of liquid cloud droplets in austral summer, promoting more sunlight to be reflected to space. We call this ‘Aitken buffering’. The primary objective of this project has been to document and test what role Aitken-mode aerosols play in clouds over the Southern Ocean and elsewhere. This effort has included three main components: 1) developing a computer model that realistically simulates the aerosol processes and the small-scale turbulent air motions that move aerosols around and create the clouds, 2) using that model to interpret and extend these observations for process understanding, by allowing different factors that contribute to the aerosol budget, such as surface wind speed, precipitation, surface gas exchange, etc. to be separated, and 3) studying Aitken-mode aerosol and its variability with a focus over the Southern Ocean and Antarctica, using data from Atmospheric Radiation Measurement (ARM) sites and other available observations. Initial computer studies in more idealized conditions found that elevated concentrations of Aitken-mode aerosols above the clouds could help prevent the breakup of those clouds by acting as cloud-condensation nuclei after they were entrained into the cloudy boundary layer. Simulations of a day during the ACE-ENA field campaign showed that Aitken-mode aerosols could also prevent cloud breakup under more realistic conditions. A new method that extracts information about Aitken-mode aerosols from measurements of aerosols onto which cloud droplets can form finds that Aitken-mode aerosols do vary seasonally over the Southern Ocean, with a peak in summertime, as described above. Other work during this project has focused on understanding how patterns of water vapor, clouds and precipitation are coupled within low-lying clouds over the oceans, and also on how cloud droplets cluster within clouds and how the distribution of cloud droplet sizes change as dry air is mixed into clouds, with the latter studies also using observations from ACE-ENA.

54 ENVIRONMENTAL SCIENCES↗

The Shortwave Spectral Radiometer for Atmospheric Science: Capabilities and Applications from the ARM User Facility

Industry advances have greatly reduced the cost and size of ground-based shortwave (SW) sensors for the ultraviolet, visible, and near-infrared spectral ranges that make up the solar spectrum, while simultaneously increasing their ruggedness, reliability, and calibration accuracy needed for outdoor operation. These sensors and collocated meteorological equipment are an important part of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility, which has supported parallel integrated measurements of atmospheric and surface properties for more than two decades at fixed and mobile sites around the world. The versatile capability of these ground-based measurements includes 1) rich spectral information required for retrieving cloud and aerosol microphysical properties, such as cloud phase, cloud particle size, and aerosol size distributions, and 2) high temporal resolution needed for capturing fast evolution of cloud microphysical properties in response to rapid changes in meteorological conditions. Here we describe examples of how ARM's spectral radiation measurements are being used to improve understanding of the complex processes governing microphysical, optical, and radiative properties of clouds and aerosol.

54 ENVIRONMENTAL SCIENCES↗