0000000001331369
AUTHOR
Peter Hoppe
Measurement of sulfur isotope ratios in micrometer-sized samples by NanoSIMS
Abstract Sulfur isotope ratios of atmospheric aerosol particles can provide detailed information with regard to the origin and the transport of sulfur in the environment. The new Cameca NanoSIMS 50 ion microprobe technique permits analysis of individual aerosol particles with volumes down to 0.5 μm 3 and a precision for δ 34 S of 3–10‰ (2 σ ). This technique will set new standards in the analysis of isotope ratios in atmospheric aerosol. For the first time it is possible to directly compare chemical and isotopic composition of individual aerosol particles, identify internal and external mixtures and investigate reactions of anthropogenic gases with natural aerosol such as sea salt and miner…
DIRECT EVIDENCE FOR CONDENSATION IN THE EARLY SOLAR SYSTEM AND IMPLICATIONS FOR NEBULAR COOLING RATES
We have identified in an acid resistant residue of the carbonaceous chondrite Murchison a large number (458) of highly refractory metal nuggets (RMNs) that once were most likely hosted by Ca,Al-rich inclusions (CAIs). While osmium isotopic ratios of two randomly selected particles rule out a presolar origin, the bulk chemistry of 88 particles with sizes in the submicron range determined by energy dispersive X-ray (EDX) spectroscopy shows striking agreement with predictions of single-phase equilibrium condensation calculations. Both chemical composition and morphology strongly favor a condensation origin. Particularly important is the presence of structurally incompatible elements in particl…
Sulfur isotope ratio measurements of individual sulfate particles by NanoSIMS
Abstract The sulfur isotopic compositions of barite (BaSO4), anhydrite (CaSO4), gypsum (CaSO4·2H2O), mascagnite ((NH4)2SO4), thenardite (Na2SO4), boetite (K2SO4), epsomite (MgSO4·7H2O), magnesium sulfate (MgSO4·xH2O) and cysteine (an amino acid) were determined with a Cameca NanoSIMS 50 ion microprobe employing a Cs+ primary ion beam and measuring negative secondary ions. This ion microprobe permits the analysis of sulfur isotope ratios in sulfates on 0.001–0.5 ng of sample material, enabling the analysis of individual S-bearing particles with diameters as small as 500 nm. The grain-to-grain reproducibility of measurements is typically 5‰ (1σ) for micron-sized grains,
Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N
We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical c…
Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO2
Global sulfate production plays a key role in aerosol radiative forcing; more than half of this production occurs in clouds. We found that sulfur dioxide oxidation catalyzed by natural transition metal ions is the dominant in-cloud oxidation pathway. The pathway was observed to occur primarily on coarse mineral dust, so the sulfate produced will have a short lifetime and little direct or indirect climatic effect. Taking this into account will lead to large changes in estimates of the magnitude and spatial distribution of aerosol forcing. Therefore, this oxidation pathway-which is currently included in only one of the 12 major global climate models-will have a significant impact on assessmen…
Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68° N
Abstract. In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68° N,…
Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68° N
In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68…