Revisiting matrix-based inversion of scanning mobility particle sizer (SMPS) and humidified tandem differential mobility analyzer (HTDMA) data

Tikhonov regularization is a tool for reducing noise amplification during data inversion. This work introduces RegularizationTools.jl, a general-purpose software package for applying Tikhonov regularization to data. The package implements well-established numerical algorithms and is suitable for systems of up to ~1000 equations. Included is an abstraction to systematically categorize specific inversion configurations and their associated hyperparameters. A generic interface translates arbitrary linear forward models defined by a computer function into the corresponding design matrix. This obviates the need to explicitly write out and discretize the Fredholm integral equation, thus facilitating fast prototyping of new regularization schemes associated with measurement techniques. Example applications include the inversion involving data from scanning mobility particle sizers (SMPSs) and humidified tandem differential mobility analyzers (HTDMAs). Inversion of SMPS size distributions reported in this work builds upon the freely available software DifferentialMobilityAnalyzers.jl. The speed of inversion is improved by a factor of ~200, now requiring between 2 and 5 ms per SMPS scan when using 120 size bins. Previously reported occasional failure to converge to a valid solution is reduced by switching from the L-curve method to generalized cross-validation as the metric to search for the optimal regularization parameter. Higher-order inversions resulting in smooth, denoised reconstructions of size distributions are now included in DifferentialMobilityAnalyzers.jl. This work also demonstrates that an SMPS-style matrixbased inversion can be applied to find the growth factor frequency distribution from raw HTDMA data while also accounting for multiply charged particles. The outcome of the aerosol-related inversion methods is showcased by inverting multi-week SMPS and HTDMA datasets from ground-based observations, including SMPS data obtained at Bodega Marine Laboratory during the CalWater 2/ACAPEX campaign and co-located SMPS and HTDMA data collected at the US Department of Energy observatory located at the Southern Great Plains site in Oklahoma, USA. Results show that the proposed approaches are suitable for unsupervised, nonparametric inversion of large-scale datasets as well as inversion in real time during data acquisition on low-cost reducedinstruction- set architectures used in single-board computers. The included software implementation of Tikhonov regularization is freely available, general, and domain-independent and thus can be applied to many other inverse problems arising in atmospheric measurement techniques and beyond.

Transport and transformation of atmospheric aerosol across Central Europe with emphasis on anthropogenic sources

<p>The trend in PM<sub>10</sub> concentrations in Europe has stagnated over the last two decades, showing only limited annual changes even though there are continued reductions in PM emissions. Possible reasons could be linked to both the aging processes of the particles in the atmosphere and their long-range transport. Therefore, better understanding the multiple origins of the atmospheric aerosol, their sources apportionment at different places are necessary for the development of efficient mitigation strategies. The ultimate objective of the project TRACE is to assess the transport and transformation of atmospheric aerosol across Central Europe with emphasis on anthropogenic sources (including coal and wood combustion) using synergic measurement methods (offline and online) and state-of-the art modelling tools including receptor-oriented models and Chemical transport models. Measurements were performed during winter and summer periods in 2021 simultaneously at three sampling places (Melpitz, DE, Kosetice, CZ, and Frydland, CZ) using state-of-the-art online and offline comprehensive chemical characterization of the atmospheric aerosol. Preliminary results from Scanning Mobility Particle Sizer (SMPS) showed peaks as high as 50 µg/m³ mass concentration during a dust event. Moreover, results from Aerosol Mass Spectrometer (AMS) and receptor modeling (RF) via Positive Matrix Factorization (PMF) from the winter campaign will be presented. </p>

Characterizing the performance of a POPS miniaturized optical particle counter when operated on a quadcopter drone

We first validate the performance of the Portable Optical Particle Spectrometer (POPS), a small light-weight and high sensitivity optical particle counter, against a reference scanning mobility particle sizer (SMPS) for a month-long deployment in an environment dominated by biomass burning aerosols. Subsequently, we examine any biases introduced by operating the POPS on a quadcopter drone, a DJI Matrice 200 V2. We report the root mean square difference (RMSD) and mean absolute difference (MAD) in particle number concentrations (PNCs) when mounted on the UAV and operating on the ground and when hovering at 10 m. When wind speeds are low (less than 2.6 m s−1), we find only modest differences in the RMSDs and MADs of 5 % and 3 % when operating at 10 m altitude. When wind speeds are between 2.6 and 7.7 m s−1 the RMSDs and MADs increase to 26.2 % and 19.1 %, respectively, when operating at 10 m altitude. No statistical difference in PNCs was detected when operating on the UAV in either ascent or descent. We also find size distributions of aerosols in the accumulation mode (defined by diameter, d, where 0.1 ≤ d ≤ 1 µm) are relatively consistent between measurements at the surface and measurements at 10 m altitude, while differences in the coarse mode (here defined by d > 1 µm) are universally larger. Our results suggest that the impact of the UAV rotors on the POPS PNCs are small at low wind speeds, but when operating under a higher wind speed of up to 7.6 m s−1, larger discrepancies occur. In addition, it appears that the POPS measures sub-micron aerosol particles more accurately than super-micron aerosol particles when airborne on the UAV. These measurements lay the foundations for determining the magnitude of potential errors that might be introduced into measured aerosol particle size distributions and concentrations owing to the turbulence created by the rotors on the UAV.

Ice nucleation activities of soot particles internally mixed with sulphuric acid at cirrus cloud conditions

Soot particles are important candidates for ice nucleating particles (INPs) in cirrus cloud formation which is known to exert a warming effect on climate. Bare soot particles, generally hydrophobic and fractal, mainly exist near emission sources. Coated or internally mixed soot particles are more abundant in the atmosphere and have a higher probability to impact cloud formation and climate. However, the ice nucleation ability of coated soot particles is not as well understood as that of freshly produced soot particles. In this study, two samples, a propane (C3H8) flame soot and a commercial carbon black were coated with varying wt % of sulphuric acid (H2SO4). The ratio of coating material mass to the mass of bare soot particle was controlled and progressively increased from less than 5 wt % to over 100 wt %. Both bare and coated soot particle ice nucleation activities were investigated with a continuous flow diffusion chamber operated at mixed-phase and cirrus cloud conditions. The mobility size and mass distribution of size selected soot particles with/without H2SO4 coating were measured by a scanning mobility particle sizer (SMPS) and a centrifugal particle mass analyser (CPMA) running in parallel. The mixing state and morphology of soot particles were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). In addition, the evidence for the presence of H2SO4 on coated soot particle surface is shown by Energy Dispersive X-ray spectroscopy (EDX). Our study demonstrates that H2SO4 coatings suppress the ice nucleation activity of soot particles to varying degrees depending on the coating thickness, but in a non-linear fashion. Thin coatings causing pore filling in the soot-aggregate inhibits pore condensation and freezing (PCF). Thick coatings promote particle ice activation via droplet homogeneous freezing. Overall, our findings reveal that H2SO4 coatings will suppress soot particle ice nucleation abilities in the cirrus cloud regime, having implications for the fate of soot particles with respect to cloud formation in the upper troposphere.

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles is subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ∼10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth and its dependence on both size and RH.

Application of Acoustic Agglomeration Technology to Improve the Removal of Submicron Particles from Vehicle Exhaust

The natural processes of interactions between aerosol particles in the ambient air through which they agglomerate is a vast area of chamber research and are inherent to many industries and are often inter-connected with transport engineering. Further improvement of symmetric methods for aerosol particle number and mass concentration reduction made it possible to create various synergic techniques. The study used a 1.9 TDI diesel internal combustion engine, which was supplied with diesel (D100) and second-generation biofuels (NExBTL100) with the EGR exhaust system on and off. Measurements were performed using a Bruel and Kjær “Type 9727” system for measurement of vibrations, a scanning mobility particle sizer (SMPS) and an original agglomeration chamber. The three modes of particle size distributions were observed in the size range from 10 to 470 nm for both D100 and NExBTL100 fuels with and without the use of the EGR system. The application of 21.3 kHz frequency sound with SPL 144.1 dB changed the NExBTL100 generated aerosol particle number concentration but did not sufficiently affect the concentration of D100 emitted particles. The greatest agglomeration effect (21.7 ± 10.0%) was observed in the range of extremely small NExBTL100 derived particles (10–70 nm) when used in combination with an EGR system.

Assessing the sources of particles at an urban background site using both regulatory instruments and low-cost sensors – a comparative study

Measurement and source apportionment of atmospheric pollutants are crucial for the assessment of air quality and the implementation of policies for their improvement. In most cases, such measurements use expensive regulatory-grade instruments, which makes it difficult to achieve wide spatial coverage. Low-cost sensors may provide a more affordable alternative, but their capability and reliability in separating distinct sources of particles have not been tested extensively yet. The present study examines the ability of a low-cost optical particle counter (OPC) to identify the sources of particles and conditions that affect particle concentrations at an urban background site in Birmingham, UK. To help evaluate the results, the same analysis is performed on data from a regulatory-grade instrument (SMPS, scanning mobility particle sizer) and compared to the outcomes from the OPC analysis. The analysis of the low-cost sensor data manages to separate periods and atmospheric conditions according to the level of pollution at the site. It also successfully identifies a number of sources for the observed particles, which were also identified using the regulatory-grade instruments. The low-cost sensor, due to the particle size range measured (0.35 to 40 µm), performed rather well in differentiating sources of particles with sizes greater than 1 µm, though its ability to distinguish their diurnal variation, as well as to separate sources of smaller particles, at the site was limited. The current level of source identification demonstrated makes the technique useful for background site studies, where larger particles with smaller temporal variations are of significant importance. This study highlights the current capability of low-cost sensors in source identification and differentiation using clustering approaches. Future directions towards particulate matter source apportionment using low-cost OPCs are highlighted.

The important roles of surface tension and growth rate in the contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration: evidence from field measurements in southern China

The contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration (NCCN) varies largely under different environments and depends on several key factors such as formation rate (J), growth rate (GR), distribution of preexisting particles, and properties of new particles during NPF events. This study investigates the contribution of NPF to the NCCN and its controlling factors based on measurements conducted at the Heshan supersite, in the Pearl River Delta (PRD) region of China during fall 2019. The size-resolved cloud condensation nuclei activity and size-resolved particle hygroscopicity were measured by a cloud condensation nuclei counter (CCNc) and a hygroscopic tandem differential mobility analyzer (HTDMA), respectively, along with a scanning mobility particle sizer (SMPS) and a diethylene glycol scanning mobility particle sizer (DEG-SMPS) for particle number size distribution (PNSD). A typical NPF event on 29 October was chosen to investigate the contribution of the NPF to NCCN under several supersaturation (SS) ratios. Two particle properties (hygroscopicity and surface tension) affect CCN activation with the latter being more important in terms of the CCN concentration (NCCN). A lower value of surface tension (i.e., 0.06 N m−1) than the pure-water assumption (0.073 N m−1) could increase the NCCN at SS = 1.0 % by about 20 % during the nonevent period and by about 40 % during the event. In addition, an earlier peak time corresponding to a lower critical diameter (D50) was also observed. The results show that high formation rate, growth rate, and low background particle concentration lead to high number concentrations of newly formed particles. The high growth rate was found to have the most significant impact on the NCCN, which can be attributed to the fact that a higher growth rate can grow particles to the CCN size in a shorter time before they are scavenged by preexisting particles. Two other NPF events (an event on 18 October in this campaign and an event on 12 December 2014 in Panyu) were chosen to perform sensitivity tests under different scenarios (growth rate, formation rate, and background particle concentration). The calculated NCCN at SS = 1.0 % on 12 December 2014 was significantly lower than that from the other two events. The event on 12 December was re-simulated using the growth rate taken from the event on 18 October which resulted in similar CCN concentrations between the two events (12 December and 18 October), implying that the growth rate is the major impact factor for CCN activation. Our results highlight the importance of growth rate and surface tension when evaluating the contribution of NPF to the NCCN.

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles are subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time-consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ~10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth, and its dependence on both size and RH.