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Abstract We investigate the mechanisms responsible for single-lobed versus double-lobed angular distributions of emitted γ-rays in laser-irradiated plasmas, focusing on how direct laser acceleration (DLA) shapes the emission profile. Using test-particle calculations, we show that the efficiency of DLA plays a central role. In the inefficient DLA regime, electrons rapidly gain and lose energy within a single laser cycle, resulting in a double-lobed emission profile heavily influenced by laser fields. In contrast, in the efficient DLA regime, electrons steadily accumulate energy over multiple laser cycles, achieving much higher energies and emitting orders of magnitude more energy. This emission is intensely collimated and results in single-lobed profiles dominated by quasi-static azimuthal magnetic fields in the plasma. Particle-in-cell simulations demonstrate that lower-density targets create favorable conditions for some electrons to enter the efficient DLA regime. These electrons can dominate the emission, transforming the overall profile from double-lobed to single-lobed, even though inefficient DLA electrons remain present. These findings provide valuable insights for optimizing laser-driven γ-ray sources for applications requiring high-intensity, well-collimated beams.more » « less
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Iodine oxoacids are recognised for their significant contribution to the formation of new particles in marine and polar atmospheres. Nevertheless, to incorporate the iodine oxoacid nucleation mechanism into global simulations, it is essential to comprehend how this mechanism varies under various atmospheric conditions. In this study, we combined measurements from the CLOUD (Cosmic Leaving OUtdoor Droplets) chamber at CERN and simulations with a kinetic model to investigate the impact of temperature, ionisation, and humidity on iodine oxoacid nucleation. Our findings reveal that ion-induced particle formation rates remain largely unaffected by changes in temperature. However, neutral particle formation rates experience a significant increase when the temperature drops from +10 oC to −10 oC. Running the kinetic model with varying ionisation rates demonstrates that the particle formation rate only increases with a higher ionisation rate when the iodic acid concentration exceeds 1.5 × 107 cm^sup>−3, a concentration rarely reached in pristine marine atmospheres. Consequently, our simulations suggest that, despite higher ionisation rates, the charged cluster nucleation pathway of iodic acid is unlikely to be enhanced in the upper troposphere by higher ionisation rates. Instead, the neutral nucleation channel is likely to be the dominant channel in that region. Notably, the iodine oxoacid nucleation mechanism remains unaffected by changes in relative humidity from 2% to 80%. However, under unrealistically dry conditions (below 0.008% RH at +10 oC), iodine oxides (I2O4 and I2O5) significantly enhance formation rates. Therefore, we conclude that iodine oxoacid nucleation is the dominant nucleation mechanism for iodine nucleation in the marine and polar boundary layer atmosphere.more » « less
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The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H2SO4), stabilized by ammonia (NH3). However, in marine and polar regions, NH3is generally low, and H2SO4is frequently found together with iodine oxoacids [HIOx, i.e., iodic acid (HIO3) and iodous acid (HIO2)]. In experiments performed with the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated the interplay of H2SO4and HIOxduring atmospheric particle nucleation. We found that HIOxgreatly enhances H2SO4(-NH3) nucleation through two different interactions. First, HIO3strongly binds with H2SO4in charged clusters so they drive particle nucleation synergistically. Second, HIO2substitutes for NH3, forming strongly bound H2SO4-HIO2acid-base pairs in molecular clusters. Global observations imply that HIOxis enhancing H2SO4(-NH3) nucleation rates 10- to 10,000-fold in marine and polar regions.more » « less
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Abstract. Aerosol particles have an important role in Earth'sradiation balance and climate, both directly and indirectly throughaerosol–cloud interactions. Most aerosol particles in the atmosphere areweakly charged, affecting both their collision rates with ions and neutralmolecules, as well as the rates by which they are scavenged by other aerosolparticles and cloud droplets. The rate coefficients between ions and aerosolparticles are important since they determine the growth rates and lifetimesof ions and charged aerosol particles, and so they may influence cloudmicrophysics, dynamics, and aerosol processing. However, despite theirimportance, very few experimental measurements exist of charged aerosolcollision rates under atmospheric conditions, where galactic cosmic rays inthe lower troposphere give rise to ion pair concentrations of around 1000 cm−3. Here we present measurements in the CERN CLOUD chamber of therate coefficients between ions and small (<10 nm) aerosol particlescontaining up to 9 elementary charges, e. We find the rate coefficient of asingly charged ion with an oppositely charged particle increases from 2.0(0.4–4.4) × 10−6 cm3 s−1 to 30.6 (24.9–45.1) × 10−6 cm3 s−1 for particles with charges of 1 to9 e, respectively, where the parentheses indicate the ±1σuncertainty interval. Our measurements are compatible with theoreticalpredictions and show excellent agreement with the model ofGatti and Kortshagen (2008).more » « less
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Abstract. Currently, the complete chemical characterization of nanoparticles(< 100 nm) represents an analytical challenge, since these particlesare abundant in number but have negligible mass. Several methods forparticle-phase characterization have been recently developed to betterdetect and infer more accurately the sources and fates of sub-100 nmparticles, but a detailed comparison of different approaches is missing.Here we report on the chemical composition of secondary organic aerosol(SOA) nanoparticles from experimental studies of α-pinene ozonolysisat −50, −30, and −10 ∘C and intercompare the results measured by differenttechniques. The experiments were performed at the Cosmics Leaving OUtdoorDroplets (CLOUD) chamber at the European Organization for Nuclear Research(CERN). The chemical composition was measured simultaneously by fourdifferent techniques: (1) thermal desorption–differential mobility analyzer(TD–DMA) coupled to a NO3- chemical ionization–atmospheric-pressure-interface–time-of-flight (CI–APi–TOF) massspectrometer, (2) filter inlet for gases and aerosols (FIGAERO) coupled to anI− high-resolution time-of-flight chemical ionization mass spectrometer(HRToF-CIMS), (3) extractive electrospray Na+ ionizationtime-of-flight mass spectrometer (EESI-TOF), and (4) offline analysis offilters (FILTER) using ultra-high-performance liquid chromatography (UHPLC)and heated electrospray ionization (HESI) coupled to an Orbitraphigh-resolution mass spectrometer (HRMS). Intercomparison was performed bycontrasting the observed chemical composition as a function of oxidationstate and carbon number, by estimating the volatility and comparing thefraction of volatility classes, and by comparing the thermal desorptionbehavior (for the thermal desorption techniques: TD–DMA and FIGAERO) andperforming positive matrix factorization (PMF) analysis for the thermograms.We found that the methods generally agree on the most important compoundsthat are found in the nanoparticles. However, they do see different parts ofthe organic spectrum. We suggest potential explanations for thesedifferences: thermal decomposition, aging, sampling artifacts, etc. Weapplied PMF analysis and found insights of thermal decomposition in theTD–DMA and the FIGAERO.more » « less
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Abstract Iodine is a reactive trace element in atmospheric chemistry that destroys ozone and nucleates particles. Iodine emissions have tripled since 1950 and are projected to keep increasing with rising O 3 surface concentrations. Although iodic acid (HIO 3 ) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved. Here, in CLOUD atmospheric simulation chamber experiments that generate iodine radicals at atmospherically relevant rates, we show that iodooxy hypoiodite, IOIO, is efficiently converted into HIO 3 via reactions (R1) IOIO + O 3 → IOIO 4 and (R2) IOIO 4 + H 2 O → HIO 3 + HOI + (1) O 2 . The laboratory-derived reaction rate coefficients are corroborated by theory and shown to explain field observations of daytime HIO 3 in the remote lower free troposphere. The mechanism provides a missing link between iodine sources and particle formation. Because particulate iodate is readily reduced, recycling iodine back into the gas phase, our results suggest a catalytic role of iodine in aerosol formation.more » « less
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