Ammonium nitrate particles formed in upper troposphere from ground ammonia sources during Asian monsoons

Höpfner, Michael; Ungermann, Jörn; Borrmann, Stephan; Wagner, Robert; Spang, Reinhold; Riese, Martin; Stiller, G. P.; Appel, Oliver; Batenburg, A. M.; Bucci, Silvia; Cairo, F.; Dragoneas, Antonis; Friedl-Vallon, Felix; Hünig, Andreas; Johansson, Sören; Krasauskas, Lukas; Legras, Bernard; Leisner, Thomas; Mahnke, Christoph; Möhler, Ottmar; Molleker, Sergej; Müller, Rolf; Neubert, Tom; Orphal, J.; Preusse, Peter; Rex, Markus; Saathoff, H.; Stroh, F.; Weigel, Ralf; Wohltmann, Ingo

doi:10.1038/s41561-019-0385-8

Cited by 114 publications

(207 citation statements)

References 86 publications

(40 reference statements)

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“…In a new finding, the model indicates the presence of gas‐phase ammonia, preferentially on the northern flank of the ASM anticyclone. This provides evidence to support spectral measurements made from the MIPAS satellite and aircraft limb IR measurements during the StratoClim campaign (Höpfner et al, , ). Backscatter estimates diagnosed from the model simulation are low compared with those obtained from CALIPSO observations.…”

Section: Discussionsupporting

confidence: 84%

“…Sulfate thus may not be the main contributor to the deficit in backscatter. Recent balloon‐based in situ observations of ATAL composition (Vernier et al, ) and data from the StratoClim airborne campaign (Höpfner et al, ) also suggest that sulfate may not be as important a component of the ATAL as previously assumed. The most likely explanation for this deficiency is that convective transport in the model, especially in the ATAL region, is too weak.…”

Section: Discussionmentioning

confidence: 96%

“…This coincides with a minimum in nitrate (and ratio NO 3 /(NO 3 + HNO 3 ); not shown) and may be due to elevated temperatures, associated with a dip in the isentropic surfaces. Höpfner et al () retrieved values of up to 150 ppt of gas‐phase ammonia locally from MIPAS spectra in the upper troposphere during the ASM, and found values of up to 1 ppb in single aircraft observations obtained during StratoClim. They attributed the elevated ammonium‐nitrate and gas‐phase ammonia to convection of ammonia from surface sources.…”

Section: Simulated Composition Of Atalmentioning

confidence: 99%

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Estimates of Regional Source Contributions to the Asian Tropopause Aerosol Layer Using a Chemical Transport Model

et al. 2020

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The Asian Tropopause Aerosol Layer (ATAL) represents an accumulation of aerosol in the upper troposphere and lower stratosphere associated with the Asian Summer Monsoon. Here we simulate the ATAL for summer 2013 with the GEOS‐Chem chemical transport model and explore the likely composition of ATAL aerosols and the relative contributions of regional anthropogenic sources versus those from farther afield. The model indicates significant contributions from organic aerosol, nitrate, sulfate, and ammonium aerosol, with regional anthropogenic precursor sources dominant. The model underestimates aerosol backscatter in the ATAL during summer 2013, compared with Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite instrument. Tests of a more physically based treatment of wet scavenging of SO2 in convective updrafts raise sulfate, eliminating the low bias with respect to CALIPSO backscatter in the ATAL, but lead to an unacceptable high bias of sulfate compared with in situ observations from aircraft over the United States. Source apportionment of the model results indicate the dominance of regional anthropogenic emissions from China and the Indian subcontinent to aerosol concentrations in the ATAL; ~60% of sulfate in the ATAL region in August 2013 is attributable to anthropogenic sources of SO2 from China (~30%) and from the Indian subcontinent (~30%), twice as much as in previously published estimates. Nitrate aerosol is found to be a dominant component of aerosol composition on the southern flank of the Asian Summer Monsoon anticyclone. Lightning sources of NOx are found to make a significant (10–15%) contribution to nitrate in the ATAL for the case studied.

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Section: Discussionsupporting

confidence: 84%

Section: Discussionmentioning

confidence: 96%

Section: Simulated Composition Of Atalmentioning

confidence: 99%

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Estimates of Regional Source Contributions to the Asian Tropopause Aerosol Layer Using a Chemical Transport Model

et al. 2020

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“…In our different approach, a very compact constant pressure inlet (CPI) setup, without additional pumping and a bypass flow was developed and flight proven for single particle and flash-vaporization type instruments, at altitudes from ground level up to 20 km altitude (e.g. Köllner et al, 2017;Schulz et al, 2018;Höpfner et al, 2019;Dragoneas et al, 2020;Schneider et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Application of an O-ring pinch device as a constant pressure inlet (CPI) for airborne sampling

Molleker¹,

Helleis²,

Klimach³

et al. 2020

Preprint

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We present a novel and compact design of a constant pressure inlet (CPI) developed for use in airborne aerosol mass 10 spectrometry. In particular the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, where efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hPa. The CPI device can also be used in gas phase sampling instruments in a large range of altitude and inlet pressure. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈0.1 l/min) upstream of an aerodynamic lens constant, deviating at most 15 by only ±2 % from a pre-set value. In our setup a pressure sensor downstream of the O-ring controls the pinch mechanism via a feedback loop and setpoint conditions are reached within seconds. The device was implemented in a few instruments, which were successfully operated on different research aircraft covering a wide range of ambient pressures, from sea level up to about 55 hPa. Details of operation and quality of aerosol particle transmission are evaluated by laboratory experiments and in-flight data with a single particle mass spectrometer.

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“…With Goddard Earth Observing System chemical transport model (GEOS-Chem) simulations, Gu et al (2016) implied that nitrate aerosol is the most dominant aerosol species in the ATAL. Höpfner et al (2019) recently suggested that ammonium nitrate particles could be transported into upper troposphere from ground ammonia sources by convection during Asian monsoons. Using the ECHAM/ MESSy Atmospheric Chemistry (EMAC) model, Ma et al (2019) indicated that the ATAL over the TP, to a large extent, is caused by mineral dust emitted from the northern TP and slope areas, lofted to an altitude of at least 10 km, and accumulating within the ASM.…”

Section: Introductionmentioning

confidence: 99%

In situ measurements and backward-trajectory analysis of high-concentration, fine-mode aerosols in the UTLS over the Tibetan Plateau

Liu

Bai

et al. 2019

Environ. Res. Lett.

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An aerosol layer in the upper troposphere and lower stratosphere over the Asian summer monsoon (ASM) regions, namely, the Asian tropopause aerosol layer (ATAL), has been observed based on satellite remote sensing and in situ measurements; however, its source is still under debate. In August 2018, an experimental campaign over the Tibetan Plateau at Golmud (GLM, 36.48°N, 94.93°E) was performed, during which a balloon-borne Portable Optical Particle Counter was used to measure the aerosol particle profile. Backward-trajectory simulations were conducted with the Massive-Parallel Trajectory Calculations model to investigate the possible sources and transport pathways of the observed particles. The in situ measurements showed a robust ATAL around the tropopause, 16 km above sea level, with a maximum aerosol number density of 35 cm −3 and a maximum aerosol mass concentration of 0.15 μg m −3 for particles with diameters between 0.14 and 3 μm. The aerosol particles in the ATAL are mostly smaller than 0.25 μm in diameter, accounting for 98% of all aerosol particles detected. The backward-trajectory analysis revealed that the air parcels arrived at the altitude of the ATAL through two separate pathways: (1) the uplift below the 360 K isentropic surface, where air parcels were first elevated to the upper troposphere and then joined the ASM anticyclonic circulation; and (2) the quasi-horizontal transport along the anticyclonic circulation, located approximately between the 360 and 420 K isentropic surfaces. The complex transport pathways may aggravate the challenge of analyzing the composition of the ATAL, and further observation campaigns are required to extend our knowledge.

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Ammonium nitrate particles formed in upper troposphere from ground ammonia sources during Asian monsoons

Cited by 114 publications

References 86 publications

Estimates of Regional Source Contributions to the Asian Tropopause Aerosol Layer Using a Chemical Transport Model

Estimates of Regional Source Contributions to the Asian Tropopause Aerosol Layer Using a Chemical Transport Model

Application of an O-ring pinch device as a constant pressure inlet (CPI) for airborne sampling

In situ measurements and backward-trajectory analysis of high-concentration, fine-mode aerosols in the UTLS over the Tibetan Plateau

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