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Cloud Condensation Nuclei Particle Counter (CCN) Instrument Handbook

The Cloud Condensation Nuclei Counter—CCN (Figure 1) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility instrument for measuring the concentration of aerosol particles that can act as cloud condensation nuclei [1, 2]. The CCN draws the sample aerosol through a column with thermodynamically unstable supersaturated water vapor that can condense onto aerosol particles. Particles that are activated, i.e., grown larger in this process, are counted (and sized) by an Optical Particle Counter (OPC). Thus, activated ambient aerosol particle number concentration as a function of supersaturation is measured. Models CCN-100 and CCN-200 differ only in the number of humidifier columns and related subsystems: CCN-100 has one column and CCN-200 has two columns along with dual flow systems and electronics.

54 ENVIRONMENTAL SCIENCES↗

Simulations of the collection of mesospheric dust particles with a rocket instrument

We investigate the collection of dust particles in the mesosphere with the MESS (MEteoric Smoke Sampler) instrument that is designed to fly on a sounding rocket. We assume that the ice particles that form in the polar mesosphere between 80 and 85 km altitude in summer contain meteoric smoke particles; and these should be collected with MESS. The instrument consists of a collection device with an opening and closure mechanism, as well as an attached conic funnel which increases the sampling area in comparison to the collection area. Dust particles are collected either directly after passing through the instrument or indirectly after colliding with and fragmenting on the funnel wall. We calculate the dust and fragment trajectories in the detector to determine the collection efficiency for different particle sizes, rocket velocities, and heights, and we find the final velocities and the temperatures of the particles. The considered design has a sampling area of 62.78 mm diameter and a collection area of 20 mm diameter. For the conditions at the rocket launch site in Andøya, Norway, we estimate the collection of meteoric smoke particles contained in the ice particles to be ~10 12 –10 14 amu mm –2 . The estimated temperatures suggest that the composition of these smoke particles is not affected by the collection. Our calculations also show that keeping the instrument open above 85 km altitude increases the amount of small smoke particles that are directly collected. The directly collected smoke particles are heated as they decelerate, which can affect their composition.

47 OTHER INSTRUMENTATION↗

Miniaturized Optical Particle Counter (MOPC) Instrument Handbook

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) aerosol counting, composition, extinction, and sizing system (ACCESS) includes a base module (9400), a filter sampler (9401), an advanced mixing condensation particle counter (MCPC, 9403), a miniaturized optical particle counter (mOPC, 9405), and a single-channel tricolor absorption photometer (STAP, 9406). This handbook focuses on the mOPC, which measures the aerosol particle size distribution between 0.19 and 3 μm.

54 ENVIRONMENTAL SCIENCES↗

Advanced Mixing Condensation Particle Counter (aMCPC) Instrument Handbook

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s aerosol counting, composition, extinction, and sizing system (ACCESS) includes a base module (9400), a filter sampler (9401), an advanced mixing condensation particle counter (aMCPC, 9403), a miniaturized optical practical counter (MOPC, 9405), and a single-channel tricolor absorption photometer (STAP, 9406). This handbook focuses on the aMCPC, which measures the ultra-fast total aerosol particle number concentration at 180 ms response rate with a detection diameter (D 50 = 7 nm).

54 ENVIRONMENTAL SCIENCES↗

Cloud Particle Imager (CPI) and 3-View Cloud Particle Imager (3V-CPI) Instrument Handbook

The cloud particle imager (CPI) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility instrument for measuring the concentration and size of cloud droplet and ice crystals. Hydrometeors entering the tube will be detected by a system of two continuous wave lasers that are perpendicular to each other, monitoring the sample volume. When a hydrometeor obscures both laser beams it is inside the sample volume and a third laser is triggered to illuminate the hydrometeor and a camera records a two-dimensional image. The CPI records images with a resolution of 2.3 μm. Since the camera has 1024 x 1024 pixels, the maximum detectable size is 2.3 mm x 2.3 mm.

54 ENVIRONMENTAL SCIENCES↗

ARM Data for Examining the Ice-Nucleating Particles from SGP Part II (ExINP-SGP II) Aerodynamic Particle Sizer, Condensation Particle Counter, and Meteorological Instrument Data Analysis

Knowledge of airborne particulate matter (PM), especially the particles that have supermicron diameters, is key for understanding ice-nucleating particles (INPs). Supported by the Atmospheric Radiation Measurement (ARM) user facility, we sampled PM and surface soil materials at the Southern Great Plains observatory (SGP; 36° 36′ 18″ N, 97° 29′ 6″ W) to systematically compare the INP abundance and ice nucleation efficiency of different SGP samples (i.e., airborne versus surface materials). The field campaign, named Examing INP from SGP II (ExINP-SGP II), was conducted from 20 January to 20 April, 2021. Our data analysis products include (1) physical surface sorption characterization data (i.e., BET, pore volume) of two sets of samples -- SGP Soil and USDA, (2) X-ray diffraction spectra for the same two samples, (3) immersion freezing assay-based ice nucleation active mass density data as a function of freezing temperature for both ambient and surface samples, and (4) time-series data of ambient meteorological conditions, concentration particle counter-derived aerosol particle concentration, and aerosol particle sizer measurement during ExINP-SGP II.

54 ENVIRONMENTAL SCIENCES↗

Aerosol emissions from water-lean solvents for post-combustion CO 2 capture

Advanced water-lean solvents (WLS) for post-combustion CO 2 capture have been gaining interest due to their ability to reduce the parasitic penalty from energy needed for solvent regeneration. Commercial implementation of these novel CO 2 capture technologies hinges on successful control of amine emissions. RTI conducted a parametric study of fundamental and operational variables influence on overall amine aerosol and vapor emissions from our water-lean solvent eCO 2 Sol™ using our 6-kW equivalent bench-scale gas absorption system. The parametric testing used a simulated flue gas with 15 % CO 2 , 2.3–4.2 % H 2 O, and 0–6 ppm sulfite (SO 3 ) to examine the impact of the presence of aerosols to the capture performance and amine emissions from the system. The SO 3 reacts with water in the flue gas to create H 2 SO 4 , which forms liquid aerosol droplets and provide nucleation sites for growth of aerosols. Scanning Mobility Particle Sizer and Aerodynamic Particle Sizer instruments monitored the aerosol particle size distribution. Parametric testing results suggested that the presence of the aerosols in the flue gas could increase the overall amine emissions by 10X compared to the baseline emissions from WLS’s vapor pressure. Principal component analysis (PCA) and projection to latent squares (PLS) developed models to predict the aerosol-based amine emissions from process data. The predictive PLS model had a correlation coefficient (Q 2 ) of 0.92 and could predict the aerosol-based emissions from the NAS process with ±15 % accuracy (average absolute deviation, AAD). The PLS regression model also identified key variables affecting aerosol-based emissions from WLS.

42 ENGINEERING↗

Experimental Report: Multi-Instrument Comparison of AAF Condensation Particle Counters

Condensation particle counters (CPCs), also known as condensation nucleus counters (CNCs) are sophisticated instruments designed to measure the concentration of aerosol particles in the atmosphere. These devices are pivotal in environmental monitoring, industrial applications, and scientific research, particularly in atmospheric studies. CPCs are vital for understanding the role of aerosols in climate systems. Aerosols influence cloud formation, radiative forcing, and atmospheric chemistry. By providing accurate measurements of particle concentrations and distributions, CPCs contribute to models that predict atmospheric impact and weather patterns (Mei et al. 2021). CPCs operate by enlarging submicron particles, including those as small as a few nanometers, to sizes detectable by optical methods. This report delves into the mechanisms, importance, and contributions of CPCs to atmospheric research at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF), highlighting their role in advancing air quality assessment, pollution control, and atmospheric studies.

54 ENVIRONMENTAL SCIENCES↗

TRAC Time Tags of individual particle samples collected for microscopy analysis at RMBL [AMF2] from June 2023 to August 2023

The dataset presents the time tags of individual particle samples collected on microscopy substrates during the Surface Atmosphere Integrated Field Laboratory (SAIL) campaign in Gothic, CO. A Time Resolved Aerosol Collector was deployed at the Rocky Mountain Biological Laboratory, 200 m north of AMF2 to collect ambient particles. The instrument inlet was placed 5 m above ground level. Particles are deposited on 400 mesh copper carbon-B film TEM grids (Ted Pella 01814-F). Samples are sealed and currently stored at Purdue University. A subset of the samples can be shared. Please contact dataset authors for more information. The dataset reports the sample start times in UTC and MST along with the sample ID, used to guide its location and retrieval from the storage plate. TRAC sampling started on June 17, 2023, and ended on July 31, 2023.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Single Particle Soot Photometer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Single Particle Soot Photometer (Droplet Measurements Technology) Data Notes: Contact us if you want additional data products from this instrument. Reported data is the black carbon (rBC) number and mass concentration with diagnostic flags. The SP2 measures incandescence from particles that is induced with a 1064 Nd-YAG laser. Particles that absorb the laser energy and then emit radiation is assumed to contain black carbon. The amount of intensity of radiation is related to the mass of absorbing material in the particle. Here, we calibrate the incandescence intensity to size selected Regal Black (Cabot) nebulized from solution. Data provided for the EPCAPE campaign used the combined broadband high-gain + low-gain channels (BHBL). Each channel has a lower threshold of detection equivalent to 2-s of the respective channel noise. Thresholding has been applied to select between the high-gain and low-gain channels. The detection limit is 80-540 nm (Deq) or 0.36- 55 fg. It is assumed that rBC is the only aerosol type that is in significant concentration in the sampled atmosphere that absorbs the laser energy. Particle data are integrated over 10 second windows to calculate a rBC number and mass concentration. QC/QA: • Diagnostic flags that impacted measured concentration: - Sample, Sheath, and Purge Flow Rates: Despite observing fluctuations in all flows, the rBC detection and mass quantification are generally observed to be stable, although large changes in sample flow rate did impact detection efficiency. A flag was implemented for sample flow deviations >12 cm3/min from the set point averaged over 30 seconds - Laser Power: Detection efficiency decreases with laser power and deviations in laser power also affect mass quantification. Flag for laser power is set for deviations in laser current from the set value >5 mA. - Primary Detector Threshold: Primary thresholding is the signal value which determines whether a “particle” is recorded. Thresholding errors occur when the threshold value is too HIGH and real particles are ignored. • Several periods without data: - 16-18 Nov: Ultra Zero Air generator failure, flows deviated significantly from set points. rBC # conc recovered but questionable. - 20-21 Nov: Offline for calibrations for several hours each day. - 25-27 Nov: Data is missing. - 30 Nov: Power outage 3 Dec: SP2 hard-drive full. - 3 Dec: Power Outage Header: - BHBL_NumbConc[#/cc]: Refers to the number concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in particles per cubic centimeter. - BHBL_BCMass_Conc[ug/m3]: Refers to the mass concentration of refractory black carbon (rBC) measured from combined broadband high-gain and low-gain channels, expressed in micrograms per cubic meter. - NoData_Flag[bool]: A boolean flag that indicates whether no data was recorded during a measurement. - NoBC_Flag[bool]: A boolean flag indicating whether no black carbon particles were recorded during the measurement. - Laser_Flag[bool]: A boolean flag indicating deviations in laser current during the measurement. - SampleFlow_Flag[bool]: A boolean flag indicating deviations from the set sample flow rate during the measurement. - PrimThresh_Flag[bool]: A boolean flag indicating deviations from the set primary threshold during the measurement, potentially ignoring real particles. - Manual_Flag[bool]: A boolean flag indicating manual intervention or adjustments during the measurement. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active or inactive during the measurement.

54 ENVIRONMENTAL SCIENCES↗

Experimental Report: Multi-Instrument Comparison of AAF Size Distribution Instruments

Aerosols are particles suspended in the atmosphere, ranging in size from nanometers to micrometers. Their size distribution affects key atmospheric processes, including nucleation, coagulation, scavenging, activation, and radiative properties (Seinfeld and Pandis 2016). Aerosol size distribution is a critical parameter in atmospheric science, influencing processes such as cloud formation and radiative forcing. Accurate representation of aerosol size distributions is essential for understanding their impact on climate, air quality, and human health. However, aerosol size and composition vary significantly across time and space due to meteorological conditions and natural or anthropogenic sources. (Wu and Boor 2021). Various instruments are used to measure aerosol size distributions, each with distinct principles, advantages, and limitations. This report begins with an in-depth overview of aerosol size-distribution comparison studies, focusing on the passive cavity aerosol spectrometer probe (PCASP), portable optical particle spectrometer (POPS), ultra-high-sensitivity aerosol spectrometer (UHSAS), aerodynamic particle sizer (APS), and scanning mobility particle sizer (SMPS). All of these instruments are used by the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF), which commissioned this comparison and report. The report evaluates the strengths and weaknesses of these instruments, highlights their applications, and discusses efforts to merge data from multiple instruments for comprehensive analysis.

54 ENVIRONMENTAL SCIENCES↗

Progress in end-to-end optimization of fundamental physics experimental apparata with differentiable programming

In this article we examine recent developments in the research area concerning the creation of end-to-end models for the complete optimization of measuring instruments. The models we consider rely on differentiable programming methods and on the specification of a software pipeline including all factors impacting performance — from the data-generating processes to their reconstruction and the inference on the parameters of interest — along with the careful specification of a utility function well aligned with the end goals of the experiment. Building on previous studies originated within the MODE Collaboration, we focus specifically on applications involving instruments for particle physics experimentation, as well as industrial and medical applications that share the detection of radiation as their data-generating mechanism. This report illustrates the most recent advancements in the area, and outlines, for each of the discussed applications as well as for automatic differentiation itself, ongoing and future work.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

EPCAPE-PT-LANL Measurements: Condensation Particle Counter

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Condensational particle counter 3070 (TSI) Calibration: No calibration during the campaign. Files: data_10sec_CPC.csv, data_10min_CPC.csv Header: - NumberConcentration[/cm3]: Number concentration of aerosol particles measured by the CPC, expressed in particles per cubic centimeter. - NumberConcentration[/cm3]_QC: Number concentration of aerosol particles after quality control adjustments or filtering, expressed in particles per cubic centimeter. - QualityControl_Flag[bool]: A boolean flag indicating whether the measurement is flagged for quality control checks, (0=pass) - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement

54 ENVIRONMENTAL SCIENCES↗

Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers

Knowledge of the chemical composition and mixing state of aerosols at a single-particle level is critical for gaining insights into atmospheric processes. One common tool to make these measurements is single-particle mass spectrometry. There remains a need to compare the performance of different single-particle mass spectrometers (SPMSs). An intercomparison of SPMSs was conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology (KIT) in November 2014, as part of the first phase of the Fifth International Workshop on Ice Nucleation (FIN-01). In this paper we compare size distributions and mass spectra of atmospherically relevant particle types measured by five SPMSs. These include different minerals, desert and soil dusts, soot, bioaerosol (Snomax; protein granule), secondary organic aerosol (SOA), and SOA-coated mineral particles. Most SPMSs reported similar vacuum aerodynamic diameter (d va ) within typical instrumental ranges from ~100–200 nm (lower limit) to ~2–3 µm (upper limit). In general, all SPMSs exhibited a wide dynamic range (up to ~10 3 ) and high signal-to-noise ratio (up to ~10 4 ) in mass spectra. Common spectral features with small diversities in mass spectra were found with high average Pearson's correlation coefficients, i.e., for average positive spectra r avg-pos =0.74 ± 0.12 and average negative spectra r avg-neg =0.67 ± 0.22. We found that instrument-specific detection efficiency (DE) was more dependent on particle size than particle type, and particle identification favored the use of bipolar, rather than monopolar, instruments. Particle classification from “blind experiments” showed that all instruments differentiated SOA, soot, and soil dust and detected subtle changes in the particle internal mixing but had difficulties differentiating among specific mineral types and dusts. This study helps to further understand the capabilities and limitations of the single-particle mass spectrometry technique in general and the specific performance of the instrument in characterizing atmospheric aerosol particles.

54 ENVIRONMENTAL SCIENCES↗