Stratospheric air intrusions promote global-scale new particle formation.

New particle formation in the free troposphere is a major source of cloud condensation nuclei globally. The prevailing view is that in the free troposphere, new particles are formed predominantly in convective cloud outflows. We present another mechanism using global observations.

Metals from spacecraft reentry in stratospheric aerosol particles.

Large increases in the number of low earth orbit satellites are projected in the coming decades [L. Schulz, K.-H.

HCOOH in the remote atmosphere: Constraints from Atmospheric Tomography (ATom) airborne observations.

Formic acid (HCOOH) is an important component of atmospheric acidity but its budget is poorly understood, with prior observations implying substantial missing sources. Here we combine pole-to-pole airborne observations from the Atmospheric Tomography Mission (ATom) with chemical transport model (GEOS-Chem CTM) and back trajectory analyses to provide the first global in-situ characterization of HCOOH in the remote atmosphere. ATom reveals sub-100 ppt HCOOH concentrations over most of the remote oceans, punctuated by large enhancements associated with continental outflow.

Sea spray aerosol concentration modulated by sea surface temperature.

Natural aerosols in pristine regions form the baseline used to evaluate the impact of anthropogenic aerosols on climate. Sea spray aerosol (SSA) is a major component of natural aerosols. Despite its importance, the abundance of SSA is poorly constrained.

A biogenic secondary organic aerosol source of cirrus ice nucleating particles.

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments.

Global Measurements of Brown Carbon and Estimated Direct Radiative Effects.

Brown carbon (BrC) is an organic aerosol material that preferentially absorbs light of shorter wavelengths. Global-scale radiative impacts of BrC have been difficult to assess due to the lack of BrC observational data. To address this, aerosol filters were continuously collected with near pole-to-pole latitudinal coverage over the Pacific and Atlantic basins in three seasons as part of the Atmospheric Tomography Mission.

A large source of cloud condensation nuclei from new particle formation in the tropics.

Cloud condensation nuclei (CCN) can affect cloud properties and therefore Earth's radiative balance. New particle formation (NPF) from condensable vapours in the free troposphere has been suggested to contribute to CCN, especially in remote, pristine atmospheric regions, but direct evidence is sparse, and the magnitude of this contribution is uncertain. Here we use in situ aircraft measurements of vertical profiles of aerosol size distributions to present a global-scale survey of NPF occurrence.

Efficient In-Cloud Removal of Aerosols by Deep Convection.

Convective systems dominate the vertical transport of aerosols and trace gases. The most recent in situ aerosol measurements presented here show that the concentrations of primary aerosols including sea salt and black carbon drop by factors of 10 to 10,000 from the surface to the upper troposphere. In this study we show that the default convective transport scheme in the National Science Foundation/Department of Energy Community Earth System Model results in a high bias of 10-1,000 times the measured aerosol mass for black carbon and sea salt in the middle and upper troposphere.

Ambient observations of sub-1.0 hygroscopic growth factor and (RH) values: Case studies from surface and airborne measurements.

This study reports on the first set of ambient observations of sub-1.0 hygroscopicity values (i.e.

Surface dimming by the 2013 Rim Fire simulated by a sectional aerosol model.

The Rim Fire of 2013, the third largest area burned by fire recorded in California history, is simulated by a climate model coupled with a size-resolved aerosol model. Modeled aerosol mass, number, and particle size distribution are within variability of data obtained from multiple-airborne in situ measurements. Simulations suggest that Rim Fire smoke may block 4-6% of sunlight energy reaching the surface, with a dimming efficiency around 120-150 W m per unit aerosol optical depth in the midvisible at 13:00-15:00 local time.

Airborne measurements of organosulfates over the continental U.S.

Unlabelled: Organosulfates are important secondary organic aerosol (SOA) components and good tracers for aerosol heterogeneous reactions. However, the knowledge of their spatial distribution, formation conditions, and environmental impact is limited. In this study, we report two organosulfates, an isoprene-derived isoprene epoxydiols (IEPOX) (2,3-epoxy-2-methyl-1,4-butanediol) sulfate and a glycolic acid (GA) sulfate, measured using the NOAA Particle Analysis Laser Mass Spectrometer (PALMS) on board the NASA DC8 aircraft over the continental U.

Single-Particle Time-of-Flight Mass Spectrometry Utilizing a Femtosecond Desorption and Ionization Laser.

Single-particle time-of-flight mass spectrometry has now been used since the 1990s to determine particle-to-particle variability and internal mixing state. Instruments commonly use 193 nm excimer or 266 nm frequency-quadrupled Nd:YAG lasers to ablate and ionize particles in a single step. We describe the use of a femtosecond laser system (800 nm wavelength, 100 fs pulse duration) in combination with an existing single-particle time-of-flight mass spectrometer.

Clarifying the dominant sources and mechanisms of cirrus cloud formation.

Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated.

Bond energies and structures of ammonia-sulfuric acid positive cluster ions.

New particle formation in the atmosphere is initiated by nucleation of gas-phase species. The small molecular clusters that act as seeds for new particles are stabilized by the incorporation of an ion. Ion-induced nucleation of molecular cluster ions containing sulfuric acid generates new particles in the background troposphere.