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All sources NASA NTRS DOE OSTI

DOE OSTI2023

Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments

Abstract As one of the least understood aerosol processes, nucleation can be a dominant source of atmospheric aerosols. Sulfuric acid (SA)-amine binary nucleation with dimethylamine (DMA) has been recognized as a governing mechanism in the polluted continental boundary layer. Here we demonstrate the importance of trimethylamine (TMA) for nucleation in the complex atmosphere and propose a molecular-level SA-DMA-TMA ternary nucleation mechanism as an improvement upon the conventional binary mechanism. Using the proposed mechanism, we could connect the gaseous amines to the SA-amine cluster signals measured in the atmosphere of urban Beijing. Results show that TMA can accelerate the SA-DMA-based new particle formation in Beijing by 50–100%. Considering the global abundance of TMA and DMA, our findings imply comparable importance of TMA and DMA to nucleation in the polluted continental boundary layer, with probably higher contributions from TMA in polluted rural environments and future urban environments with controlled DMA emissions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

Nanometer-scale mapping of irreversible electrochemical nucleation processes on solid Li-ion electrolytes

Electrochemical processes associated with changes in structure, connectivity or composition typically proceed via new phase nucleation with subsequent growth of nuclei. Understanding and controlling reactions requires the elucidation and control of nucleation mechanisms. However, factors controlling nucleation kinetics, including the interplay between local mechanical conditions, microstructure and local ionic profile remain inaccessible. Furthermore, the tendency of current probing techniques to interfere with the original microstructure prevents a systematic evaluation of the correlation between the microstructure and local electrochemical reactivity. In this work, the spatial variability of irreversible nucleation processes of Li on a Li-ion conductive glass-ceramics surface is studied with ,30 nm resolution. An increased nucleation rate at the boundaries between the crystalline AlPO4 phase and amorphous matrix is observed and attributed to Li segregation. This study opens a pathway for probing mechanisms at the level of single structural defects and elucidation of electrochemical activities in nanoscale volumes.

Kumar, Amit↗

DOE OSTI2016

Preferential nucleation during polymorphic transformations

Polymorphism is the ability of a solid material to exist in more than one phase or crystal structure. Polymorphism may occur in metals, alloys, ceramics, minerals, polymers, and pharmaceutical substances. Unresolved are the conditions for preferential nucleation during polymorphic transformations in which structural relationships or special crystallographic orientation relationships (OR’s) form between the nucleus and surrounding matrix grains. We measured in-situ and simultaneously the nucleation rates of grains that have zero, one, two, three and four special OR’s with the surrounding parent grains. These experiments show a trend in which the activation energy for nucleation becomes smaller – and therefore nucleation more probable - with increasing number of special OR’s. As a result, these insights contribute to steering the processing of polymorphic materials with tailored properties, since preferential nucleation affects which crystal structure forms, the average grain size and texture of the material, and thereby - to a large extent - the final properties of the material.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Following heterogeneous nucleation of CO 2 on H 2 O ice nanoparticles with microsecond resolution

Heterogeneous nucleation of CO 2 onto H 2 O ice particles may play an important role in proposed innovative CO 2 capture technologies, as well as in the formation of Martian clouds. In this work we follow the nucleation/condensation of CO 2 /H 2 O gas mixtures with microsecond resolution in supersonic Laval nozzles using pressure trace measurement (PTM) and small angle X-ray scattering (SAXS). The latent heat release detected by the PTM reveals that the first phase transition in the expanding CO 2 /H 2 O mixture is the formation of H 2 O ice particles by the homogeneous nucleation/condensation and freezing of H 2 O. This is followed by the heterogeneous nucleation and growth of CO 2 on the H 2 O ice particles. The onset conditions for heterogeneous nucleation, i.e. the partial pressure of CO 2 and temperature from PTM and the radius of gyration of the H 2 O ice particles from SAXS, were determined in the temperature range 124 to 146 K and for particles with radii of gyration in the range of 2.1 to 4.3 nm. The onset conditions suggest that the heterogeneous nucleation of CO 2 may start from the supercooled liquid phase under our conditions. Downstream of the onset point, the partial pressure of CO 2 and temperature rapidly approach the vapor–solid equilibrium line of CO 2 , showing that even if CO 2 condensation is initiated by heterogeneous nucleation of the liquid phase, it proceeds via growth of the solid.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Molecular Simulations of Heterogeneous Ice Nucleation. II. Peeling back the Layers

Coarse grained molecular dynamics simulations are presented in which the sensitivity of the ice nucleation rate to the hydrophilicity of a graphene nanoflake is investigated. We find that an optimal interaction strength for promoting ice nucleation exists, which coincides with that found previously for a face centered cubic (111) surface. We further investigate the role that the layering of interfacial water plays in heterogeneous ice nucleation and demonstrate that the extent of layering is not a good indicator of ice nucleating ability for all surfaces. Our results suggest that to be an efficient ice nucleating agent, a surface should not bind water too strongly if it is able to accommodate high coverages of water.

Cox, Stephen J.↗

DOE OSTI2018

Ice nucleation rates near ~225 K

We have measured the ice nucleation rates, J ice , in supercooled nano-droplets with radii ranging from 6.6 nm to 10 nm and droplet temperatures, T d , ranging from 225 K to 204 K. The initial temperature of the 10 nm water droplets is ~250 K, i.e., well above the homogeneous nucleation temperature for micron sized water droplets, T H ~235 K. The nucleation rates increase systematically from ~10 21 cm –3 s –1 to ~10 22 cm –3 s –1 in this temperature range, overlap with the nucleation rates and suggest that experiments with larger droplets would extrapolate smoothly the rates. Here, the sharp corner in the rate data as temperature drops is, however, difficult to match with available theory even if we correct classical nucleation theory and the physical properties of water for the high internal pressure of the nanodroplets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Effect of wetting on nucleation and growth of D 2 in confinement

We have performed a computational study to determine how the wetting of liquid deuterium to the walls of the material influences nucleation. We present the development of a pair-wise interatomic potential that includes zero-point motion of molecular deuterium. Deuterium is used in this study because of its importance to inertial confinement fusion and the potential to generate a superfluid state if the solidification can be suppressed. Our simulations show that wetting dominates undercooling compared to the pore geometries. We observe a transition from heterogeneous nucleation at the confining wall to homogeneous nucleation at the bulk of the liquid (and intermediate cases) as the interaction with the confining wall changes from perfect wetting to non-wetting. When nucleation is heterogeneous, the temperature needed for solidification changes by 4 K with decreasing deuterium-wall interaction, but it remains independent (and equal to the one from bulk samples) when homogeneous nucleation dominates. We find that growth and quality of the resulting microstructure also depends on the magnitude of liquid deuterium–wall interaction strength.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Enhanced polymorph metastability drives glycine nucleation in aqueous salt solutions

Crystal nucleation from aqueous solutions influences countless geological, biochemical, astrophysical, environmental, and materials science–related phenomena, including ice formation, the manufacturing of active pharmaceutical ingredients, development of diseases such as Alzheimer’s and the origin of life itself. Understanding and controlling nucleation is essential for designing materials with specific properties, developing strategies to inhibit or promote crystallization in various contexts and preventing pathological aggregation in neurodegenerative diseases. Similar to the protein structure prediction problem—where a single amino acid sequence can in theory adopt one most stable conformation but in practice may sample multiple competing conformations—crystal nucleation faces a parallel challenge: the same chemical species can form diverse polymorphs under different environmental conditions (e.g., temperature, pressure, solvent). Each polymorph presents its own set of physical and chemical properties, highlighting the importance of understanding and controlling polymorph selection in fields ranging from pharmaceuticals to materials design. Despite advances in experimental and computational methods for studying phase transitions and polymorph stability, nucleation remains challenging due to its nanoscale nature. Furthermore, in practical settings, salts and impurities can further influence crystal nucleation in diverse contexts, from scaling in pipelines and desalination plants to the durability of concrete and the efficiency of battery materials. This can lead to the formation of polymorphs that may differ from the most stable phase in pure solutions. Or, even though the final structure might appear same irrespective of whether the environment contained impurities or not, the mechanism through which it was formed might be completely different and not intuitive.

Wang, Ruiyu [University of Maryland, College Park,↗

DOE OSTI2022

Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides

To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS 2 ), here we report studies of the reactions of molybdenum hexafluoride (MoF 6 ) and hydrogen sulfide (H 2 S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 °C revealed temperature-dependent nucleation behavior of the MoF 6 precursor, which is attributed to variations in surface hydroxyl concentration with temperature. In situ Fourier transform infrared spectroscopy coupled with ex situ x-ray photoelectron spectroscopy (XPS) indicated the presence of molybdenum oxide and molybdenum oxyfluoride species during nucleation. Density functional theory calculations additionally support the formation of these species as well as predicted metal oxide to fluoride conversion. Residual gas analysis revealed reaction by-products, and the combined experimental and computational results provided insights into proposed nucleation surface reactions. With additional ALD cycles, Fourier transform infrared spectroscopy indicated steady film growth after ~13 cycles at 200 °C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS 2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 °C and below, while layered films with vertical platelets were observed at 250 °C. Finally, these results provide an improved understanding of MoS 2 nucleation, which can guide surface preparation for the deposition of few-layer films and advance MoS 2 toward integration into device manufacturing.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Reversible disorder-order transitions in atomic crystal nucleation

Nucleation in atomic crystallization remains poorly understood, despite advances in classical nucleation theory. The nucleation process has been described to involve a nonclassical mechanism that includes a spontaneous transition from disordered to crystalline states, but a detailed understanding of dynamics requires further investigation. In situ electron microscopy of heterogeneous nucleation of individual gold nanocrystals with millisecond temporal resolution shows that the early stage of atomic crystallization proceeds through dynamic structural fluctuations between disordered and crystalline states, rather than through a single irreversible transition. Our experimental and theoretical analyses support the idea that structural fluctuations originate from size-dependent thermodynamic stability of the two states in atomic clusters. These findings, based on dynamics in a real atomic system, reshape and improve our understanding of nucleation mechanisms in atomic crystallization.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Zinc-Nucleated D 2 and H 2 Crystal Formation from Their Liquids

Calorimetric measurements at University of Rochester Laboratory for Laser Energetics of D 2 crystallization from the melt indicate that zinc can act as a heterogeneous nucleation seed with suppressed supercooling. We further studied in this paper this effect for a variety of zinc substrates using the optical-access cryogenic sample cell at Lawrence Livermore National Laboratory. Small supercoolings are observed, some as low as 5 mK, but results depend on the zinc history and sample preparation. In general, thin samples prepared by physical vapor deposition were not effective in nucleating crystal formation. Larger (several-millimeter) granules showed greater supercooling suppression, depending on surface modification and granule size. Surfaces of these granules are morphologically varied and not uniform. Scanning electron microscope images were not able to correlate any particular surface feature with enhanced nucleation. Finally, application of classical nucleation theory to the observed variation of supercooling level with granule size is consistent with nucleation features with sizes <100 nm and with wetting angles of a few degrees.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Dual microscopy to explore enhanced atmospheric ice nucleation on multi-component aerosols

Using an optical microscopy setup adapted to in-situ studies of ice formation at ambient pressure, we examined a specific multicomponent mineral, microcline, with the ultimate aim of gaining a more realistic understanding of ice nucleation in Earth’s atmosphere. We focused on a perthitic feldspar, microcline, to test the hypothesis that co-existence in some feldspars of K-rich and Na-rich phases are contributing to enhanced ice nucleation. On a sample deliberately chosen to contain lamella, a typical perthitic microstructure, and flat surface regions next to each other, we performed a series of ice formation experiments. We found microcline to promote ice formation, causing a large number of ice nucleation events at around - 27°C. The number of ice nuclei decreased from experimental run to experimental run, indicating surface aging upon repeated exposure to humidity. An analysis of 10 experimental runs of identical conditions did not reveal an obvious enhancement of ice formation at the lamellar microstructure. Instead, we find efficient nucleation at various surface sites that produce orientationally aligned ice crystallites with asymmetric shape. Based on this observation we propose that surface steps running along select directions produce microfacets of an orientation that is favorable to enhanced ice nucleation, similar to previously reported for K-rich feldspars.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

AGN Activity in Nucleated Galaxies as Measured by Chandra

Motivated by theoretical expectations that nuclear star clusters (NSCs) in galactic centers may provide a favorable environment for supermassive black holes to form and/or efficiently grow, we set out to measure the fraction of nearby nucleated galaxies that also host an active galactic nucleus. We targeted a distance-limited sample of 98 objects with the Chandra X-ray Telescope, down to a uniform X-ray luminosity threshold of ∼10{sup 38} erg s{sup −1}. The sample is composed of 47 late-types and 51 early-types, enabling us to further investigate the active fraction as a function of galactic morphology. After correcting for contamination to the nuclear X-ray signal from bright X-ray binaries, we measure an active fraction f=11.2%{sub −4.9}{sup +7.4} (1σ C.L.) across the whole sample, in agreement with previous estimates based on a heterogeneous combination of optical, X-ray, and radio diagnostics, by Seth et al. After accounting for the different stellar mass distributions in our samples, we find no statistically significant difference in the active fraction of early- versus late-type nucleated galaxies, with f=10.6%{sub −4.9}{sup +11.9} and 10.8%{sub −6.3}{sup +11.3}, respectively. For the early-type nucleated galaxies, we are able to carry out a controlled comparison with a parent sample of non-nucleated galaxies covering the same stellar mass range, again finding no statistically significant difference in the active fraction. Taken at face value, our findings suggest that the presence of an NSC does not facilitate or enhance accretion-powered emission from a nuclear supermassive black hole. This is true even for late-type nucleated galaxies, home to bluer NSCs and arguably larger gas reservoirs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2015

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

Here, new measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH 4 HSO 4 , raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Understanding cirrus ice crystal number variability for different heterogeneous ice nucleation spectra

Abstract. Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, N i , is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of N i to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand N i variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, and simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of N i sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. N i sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Aircraft-derived particle fluxes distinguish entrainment zone and decoupled layer nucleation in marine boundary layers

The vertical distribution of freshly nucleated aerosol particles in the marine boundary layer remains poorly constrained, limiting our ability to represent new particle formation in climate models. Here we characterize 3–10 nm particle events, termed small particle events (SPEs), by deriving their vertical turbulent fluxes from aircraft measurements during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. To overcome stationarity limitations of traditional eddy covariance methods, we applied continuous wavelet transform analysis to data collected during June–July 2017 and January–February 2018 flights over the Azores. Our flux-based analysis revealed two distinct SPE scenarios with different vertical structures and spatial extents. The first featured nucleation in the entrainment zone, where free tropospheric air entrains into the boundary layer. The second showed nucleation in the decoupled layer, a stratified region between the well-mixed surface layer and cloud-topped upper boundary layer. In both cases, convergence of air masses from different layers diluted preexisting aerosol surface area to very low levels, creating conditions favorable for nucleation and generating strong downward particle fluxes. SPEs occurred in 15 % of flights, challenging prevailing theoretical expectations that new particle formation should rarely occur in marine boundary layers due to high condensation and coagulation sink capacity of sea spray aerosols. Aircraft-derived particle fluxes provide first observational constraints on the vertical location and source strength of likely nucleation regions in the remote marine boundary layer, improving aerosol source representations in climate models and reducing uncertainties in aerosol-cloud interactions.

Rasheeda Satheesh, Ajmal [North Carolina State Uni↗

DOE OSTI2016

The SPectrometer for Ice Nuclei (SPIN): An instrument to investigate ice nucleation

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Altogether, we report that the SPIN is able to reproduce previous INP counter measurements.

47 OTHER INSTRUMENTATION↗

DOE OSTI2019

Size-resolved ice nucleating particle (INP) concentrations from the MOSAiC campaign

Sample collection: Ground-based immersion mode ice nucleation measurements were conducted on samples collected at the U.S. DOE ARM AMF2 onboard the R/V Polarstern P-deck during MOSAiC from 23 Oct 2019 to 01 Oct 2020. Samples were collected using a Davis Rotating-drum Unit for Monitoring (DRUM; DRUMAir, LLC) cascading impactor in 4 stages (i.e., size bins). Instrument information on the model used, the DA400, can be found at the DRUMAir website (http://www.drumair.com/). Stages A, B, C, and D had particle size cuts at 2.96, 1.21, 0.34, and 0.15 µm in particle diameter, respectively. Strips of sample substrate (PFA, perfluoroalkoxy; McMaster) were adhered to each disc in each stage and coated with petrolatum to enable particles to stick on impact. The discs move slowly over time, such that aerosol loading is streaked onto the PFA. Every 24 hours, a blank is created on the PFA to separate daily samples. During MOSAiC, the pump typically pulled 20 – 35 lpm (average of 32 lpm) at the inlet with all the discs in place in each stage. Daily samples were collected for each of the four stages, equaling 28,800 – 50,400 total L of air (average of 46,080 L total L of air) per sample. Discs rotated for approximately 24 days before the sampling per strip was complete and changed to a new disc. Discs were stored frozen after collection. Sample preparation for analysis: Following collection and transport from MOSAiC to the Kreidenweis/DeMott laboratory, care of PI Creamean, in Fort Collins, CO, strips were removed from the discs and cut up to separate daily samples. Each daily portion of the strip was stored in separate sterile 15-mL centrifuge tubes and stored in a standard commercial freezer until analysis (approximately 4 – 12 months after collection). Sample analysis: Drop freezing assays (DFAs) were conducted on one daily sample set every 3 – 4 days of the study for all four stages using the Colorado State University (CSU) cold plate (CP). Sample set days were chosen to cover the entire year of MOSAiC and avoiding days where the AOS purge system was activated. Immediately after removal from the freezer, 2 mL of 0.1-µm filtered deionized water was added with a single-use sterile syringe directly to the tubes, then mixed using a vortex mixer for at least 30 minutes at 500 rpm to resuspend particles from the PFA into the deionized water. Following sample preparation, another single-use syringe was used to create 100 aliquots on a 3-inch diameter copper plate, then covered with a transparent plastic dome. The drops were approximately the same volume (2.5 µL each), though careful inspection. The plate was cooled at approximately 3 – 10 K min-1 from room temperature until all drops froze on the plate. Temperature was measured by an Omega thermocouple probes and meter. Drop freezing was visually detected but recorded through monitoring software to provide the time frozen, channel of the meter used, temperature, and cooling rate for each drop. Not all 100 drops were always detected; the total number of rows in each data file equals the number of drops recorded, which typically was > 80 %. Each sample was tested three times (i.e., a new set of 100 drops was created for each test). Data provided are files containing these parameters. From the freezing temperatures recorded, the fraction frozen was and INP concentrations were calculated per L of air using the equation from Vali (1971): [INPs] = −(ln(f)/Valiquot)*(Vsuspension/Vair) where f is the proportion of droplets not frozen, Valiquot is the volume of each aliquot (i.e., 2.5e-6 L), Vsuspension is the volume of the suspension (i.e., 0.002 L), and Vair is the volume of air per sample (i.e., 36000 L). Data usage guidance: There are three files included with this dataset: (1) dumcp_inp_concentrations.csv which includes cumulative INP concentrations binned every 0.5 °C from 0 to –30 °C for all samples and size ranges (i.e., DRUM stages) processed via DFA using the CSU CP; (2) dumcp_inp_standard_deviation.csv which includes the standard deviations for all samples and temperatures in dumcp_inp_concentrations.csv; and (3) dumcp_blank_concentrations_standard_deviation.csv which includes the INP concentrations and standard deviations for the deionized water and PFA blanks binned every 0.5 °C from 0 to –30 °C. The first column in each file represents the freezing temperature in °C binned every 0.5 °C from 0 to –30 °C (first cell in this column = header = “temp”). The second column in each file represents the standard deviation of each temperature bin in °C (first cell in this column = header = “temperr”). For file (1) dumcp_inp_concentrations.csv, the remaining columns indicate the INP concentrations per L of air for each temperature bin. For each sample column, the header in the first row indicates the stage (i.e., size bin as “A_”, “B_”, “C_”, or “D_”) and date (“_yyyymmdd) of collection. For file (2) dumcp_inp_standard_deviation.csv, the remaining columns indicate the INP concentration standard deviation per L of air for each temperature bin. For each sample column, the header in the first row indicates the stage (i.e., size bin as “A_”, “B_”, “C_”, or “D_”) and date (“_yyyymmdd) of collection. For file (3) dumcp_blank_concentrations_standard_deviation.csv, the remaining columns indicate the INP concentrations and standard deviations for the deionized water blank (“di_0.1” and “di_0.1sd” for the concentrations and standard deviations, respectively) and PFA blank (“pfa” and “pfasd” for the concentrations and standard deviations, respectively). Please see Creamean et al. (2019a; 2018a; 2018b; 2019b) for additional details on DRUM sample collection and offline processing. For questions or help with data interpretation, contact Dr. Jessie Creamean (jessie.creamean@colostate.edu). References: Creamean, J. M., Mignani, C., Bukowiecki, N., and Conen, F.: Using spectra characteristics to identify ice nucleating particle populations during winter storms in the Alps, Atmos. Chem. Phys., 19, 8123–8140, 2019a. Creamean, J. M., Kirpes, R. M., Pratt, K. A., Spada, N. S., Maahn, M., de Boer, G., Schnell, R. C., and China, S.: Marine and terrestrial influences on ice nucleating particles during continuous springtime measurements in an Arctic oilfield location, Atmospheric Chemistry and Physics, 18, 18023-18042, 10.5194/acp-18-18023-2018, 2018a. Creamean, J. M., Primm, K. M., Tolbert, M. A., Hall, E. G., Wendell, J., Jordan, A., Sheridan, P. J., Smith, J., and Schnell, R. C.: HOVERCAT: A novel aerial system for evaluation of aerosol-cloud interactions, Atmospheric Measurement Techniques, 11, 3969-3985, 10.5194/amt-11-3969-2018, 2018b. Creamean, J. M., Cross, J. N., Pickart, R., McRaven, L., Lin, P., Pacini, A., Hanlon, R., Schmale, D. G., Ceniceros, J., Aydell, T., Colombi, N., Bolger, E., and DeMott, P. J.: Ice nucleating particles carried from below a phytoplankton bloom to the Arctic atmosphere, Geophys. Res. Lett., 46, 8572-8581, https://doi.org/10.1029/2019GL083039, 2019b. Vali, G.: Quantitative Evaluation of Experimental Results an the Heterogeneous Freezing Nucleation of Supercooled Liquids, Journal of the Atmospheric Sciences, 28, 402-409, 10.1175/1520-0469(1971)028<0402:qeoera>2.0.co;2, 1971.

4-stage DRUM aerosol collector (DA400),Ice nuclei,↗