scholarly journals Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Elem Sci Anth ◽  
2017 ◽  
Vol 5 ◽  
Author(s):  
B. Zhang ◽  
R. C. Owen ◽  
J. A. Perlinger ◽  
D. Helmig ◽  
M. Val Martín ◽  
...  
Keyword(s):  
Long Range ◽  
North Atlantic ◽  
Long Range Transport ◽  
Free Troposphere ◽  
Upper Troposphere ◽  
Chemical Signatures ◽  
Range Transport ◽  
Transport Patterns ◽  
Background Air ◽  
Butane Isomers

Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport,on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions(NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O3 and nitrogen oxides. The d[O3]/d [CO] value was used to investigate O3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest d [O3]/d [CO], which was likely due to intense CO production and depressed O3 production in wildfire plumes. Slightly enhanced O3 and d [O3]/d [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.

scholarly journals Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada

2008 ◽  
Vol 8 (11) ◽  
pp. 2999-3014 ◽  
Author(s):  
A. van Donkelaar ◽  
R. V. Martin ◽  
W. R. Leaitch ◽  
A. M. Macdonald ◽  
T. W. Walker ◽  
...  
Keyword(s):  
British Columbia ◽  
North America ◽  
Long Range ◽  
East Asian ◽  
Chemical Transport ◽  
Long Range Transport ◽  
Free Troposphere ◽  
Range Transport ◽  
Transport Experiment ◽  
Sulfur Emissions

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500–900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72–85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m3 (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m3.

scholarly journals First simultaneous measurements of peroxyacetyl nitrate (PAN) and ozone at Nam Co in the central Tibetan Plateau: impacts from the PBL evolution and transport processes

2017 ◽  
Author(s):  
Xiaobin Xu ◽  
Hualong Zhang ◽  
Weili Lin ◽  
Ying Wang ◽  
Shihui Jia
Keyword(s):  
Long Range ◽  
Early Morning ◽  
Diurnal Variations ◽  
Long Range Transport ◽  
Nam Co ◽  
Monsoon Period ◽  
Air Masses ◽  
Upper Troposphere ◽  
Central Tibetan Plateau ◽  
Range Transport

Abstract. Both peroxyacetyl nitrate (PAN) and ozone (O3) are key photochemical products in the atmosphere. Most of the previous in-situ observations of both gases have been made in polluted regions and at low altitude sites. Here we present first simultaneous measurements of PAN and O3 at Nam Co (NMC, 90°57′ E, 30°46′ N, 4745 m  a.s.l.), a remote site in the central Tibetan Plateau (TP). The observations were made during summer periods in 2011 and 2012. The PAN concentrations averaged 0.36 ppb (range: 0.11–0.76 ppb) and 0.44 ppb (range: 0.21–0.99 ppb) during 16–25 August 2011 and 15 May to 13 July 2012, respectively. The O3 concentration varied from 27.9 ppb to 96.4 ppb, with an average of 60.0 ppb. Profound diurnal cycles of PAN and O3 were observed, with minimum values around 05:00 LT, steep rises in the early morning, and broader platforms of high values during 09:00–20:00 LT. We find that the evolution of planetary boundary layer (PBL) played a key role in shaping the diurnal patterns of both gases, particularly the rapid increases of PAN and O3 in the early morning. Air entrainment from the free troposphere into the PBL seemed to cause the early morning increase and be a key factor of sustaining the daytime high concentrations of both gases. The days with higher daytime PBL (about 3 km) showed stronger diurnal variations of both gases and were mainly distributed in the drier pre-monsoon period, while those with shallower daytime PBL (about 2 km) showed minor diurnal variations of both gases and were mainly distributed in the humid monsoon period. Episodes of higher PAN levels were observed occasionally at NMC. These PAN episodes were caused either by rapid downward transport of air masses from the middle/upper troposphere or by long-range transport of PAN plumes from North India. The PAN level in the downward transport cases ranged from 0.5 ppb to 0.7 ppb and may indicate the PAN abundance in the middle/upper troposphere. In the long-range transport case, the PAN level varied in the range of 0.6–1.0 ppb. This long-range transport process influenced most of the western and central TP region for about a week in early June 2012. Our results suggest that polluted air masses from South Asia can significantly enhance the PAN level over the TP. As PAN act as a reservoir of NOx, the impacts of pollution transport from South Asia on tropospheric photochemistry over the TP region deserve further studies.

scholarly journals Lagrangian formation pathways of moist anomalies in the trade-wind region during the dry season: two case studies from EUREC<sup>4</sup>A

2021 ◽  
Author(s):  
Leonie Villiger ◽  
Heini Wernli ◽  
Maxi Boettcher ◽  
Martin Hagen ◽  
Franziska Aemisegger
Keyword(s):  
Long Range ◽  
North Atlantic ◽  
Large Scale ◽  
Cold Front ◽  
Trade Wind ◽  
Long Range Transport ◽  
The North ◽  
Range Transport ◽  
The North Atlantic ◽  
The Tropics

Abstract. Shallow clouds in the trade-wind region over the North Atlantic contribute substantially to the global radiative budget. In the vicinity of the Caribbean island Barbados, they appear in different mesoscale organisation patterns with distinct net cloud radiative effects (CRE). Cloud formation processes in this region are typically controlled by the prevailing large-scale subsidence. However, occasionally weather systems from remote origin cause significant disturbances. This study investigates the complex cloud-circulation interactions during the field campaign EUREC4A (Elucidate the Couplings Between Clouds, Convection and Circulation) from 16 January to 20 February 2020, using a combination of Eulerian and Lagrangian diagnostics. Based on observations and ERA5 reanalyses, we identify the relevant processes and characterise the formation pathways of two moist anomalies above the Barbados Cloud Observatory (BCO), one in the lower (~1000–650 hPa) and one in the middle troposphere (~650–300 hPa). These moist anomalies are associated with strongly negative CRE values and with contrasting long-range transport processes from the extratropics and the tropics, respectively. The low-level moist anomaly is characterised by an unusually thick cloud layer, high precipitation totals and a strongly negative CRE. Its formation is connected to an “extratropical dry intrusion” (EDI) that interacts with a trailing cold front. A quasi-climatological (2010–2020) analysis reveals that EDIs lead to different conditions at the BCO depending on how they interact with the associated cold front. Based on this climatology, we discuss the relevance of the strong large-scale forcing by EDIs for the low-cloud patterns near the BCO and the related CRE. The second case study about the mid-tropospheric moist anomaly is associated with an extended and persistent mixed-phase shelf cloud and the lowest daily CRE value observed during the campaign. Its formation is linked to “tropical mid-level detrainment” (TMD), which refers to detrainment from tropical deep convection near the melting layer. The quasi-climatological analysis shows that TMDs consistently lead to mid-tropospheric moist anomalies over the BCO and that the detrainment height controls the magnitude of the anomaly. However, no systematic relationship was found between the amplitude of this mid-tropospheric moist anomaly and the CRE at the BCO. Overall, this study reveals the important impact of the long-range transport, driven by dynamical processes either in the extratropics or the tropics, on the variability of the vertical structure of moisture and clouds, and on the resulting CRE in the North Atlantic winter trades.

scholarly journals Pitfalls with the use of enhancement ratios or normalized excess mixing ratios measured in plumes to characterize pollution sources and aging

2013 ◽  
Vol 6 (8) ◽  
pp. 2155-2158 ◽  
Author(s):  
R. J. Yokelson ◽  
M. O. Andreae ◽  
S. K. Akagi
Keyword(s):  
Remote Sensing ◽  
Boundary Layer ◽  
Data Interpretation ◽  
Long Range Transport ◽  
Free Troposphere ◽  
Single Source ◽  
Atmospheric Research ◽  
Mixing Ratios ◽  
Range Transport ◽  
Background Air

Abstract. Normalized excess mixing ratios (NEMRs), also known as enhancement ratios, are a common way to characterize plumes of pollution in atmospheric research. As single-source pollutant plumes disperse in the atmosphere, they are diluted by mixing with the adjacent background air. Changes in the composition of this background air can cause large changes to the NEMR that is subsequently measured by remote-sensing, airborne, or ground-based instruments. This scenario is common when boundary layer plumes enter the free troposphere and could also impact long-range transport or plumes near the top of the troposphere. We provide a context for these issues and an example showing that neglect of this effect could lead to serious errors in data interpretation.

scholarly journals Analysis of aircraft and satellite measurements from the intercontinental chemical transport experiment (INTEX-B) to quantify long-range transport of East Asian Sulfur to Canada

2008 ◽  
Vol 8 (1) ◽  
pp. 4017-4057 ◽  
Author(s):  
A. van Donkelaar ◽  
R. V. Martin ◽  
W. R. Leaitch ◽  
A. M. Macdonald ◽  
T. W. Walker ◽  
...  
Keyword(s):  
British Columbia ◽  
North America ◽  
Long Range ◽  
East Asian ◽  
Chemical Transport ◽  
Long Range Transport ◽  
Free Troposphere ◽  
Range Transport ◽  
Transport Experiment ◽  
Sulfur Emissions

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant. Measured sulfate plumes in the free troposphere over British Columbia exceeded 1 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Trends in Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 63% of the measured sulfate at 600 hPa over British Columbia is due to East Asian sources. Simulation of INTEX-B and May 1985 aircraft measurements off the northwest coast of the United States reveals a 2.4–3.4 fold increase in the relative contribution of East Asian sulfate to the total burden. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.14–0.19 μg/m3 (~30%) and account for 40% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.27 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, suggesting current East Asian emissions degrade local air quality.

scholarly journals Measurement report: Long-range transport patterns into the tropical northwest Pacific during the CAMP<sup>2</sup>Ex aircraft campaign: chemical composition, size distributions, and the impact of convection

2021 ◽  
Vol 21 (5) ◽  
pp. 3777-3802
Author(s):  
Miguel Ricardo A. Hilario ◽  
Ewan Crosbie ◽  
Michael Shook ◽  
Jeffrey S. Reid ◽  
Maria Obiminda L. Cambaliza ◽  
...  
Keyword(s):  
Long Range ◽  
Southwest Monsoon ◽  
Long Range Transport ◽  
Northwest Pacific ◽  
Back Trajectories ◽  
Air Masses ◽  
China Sea ◽  
Range Transport ◽  
Transport Patterns ◽  
The Impact

Abstract. The tropical Northwest Pacific (TNWP) is a receptor for pollution sources throughout Asia and is highly susceptible to climate change, making it imperative to understand long-range transport in this complex aerosol-meteorological environment. Measurements from the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex; 24 August to 5 October 2019) and back trajectories from the National Oceanic and Atmospheric Administration Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) were used to examine transport into the TNWP from the Maritime Continent (MC), peninsular Southeast Asia (PSEA), East Asia (EA), and the West Pacific (WP). A mid-campaign monsoon shift on 20 September 2019 led to distinct transport patterns between the southwest monsoon (SWM; before 20 September) and monsoon transition (MT; after 20 September). During the SWM, long-range transport was a function of southwesterly winds and cyclones over the South China Sea. Low- (high-) altitude air generally came from MC (PSEA), implying distinct aerosol processing related to convection and perhaps wind shear. The MT saw transport from EA and WP, driven by Pacific northeasterly winds, continental anticyclones, and cyclones over the East China Sea. Composition of transported air differed by emission source and accumulated precipitation along trajectories (APT). MC air was characterized by biomass burning tracers while major components of EA air pointed to Asian outflow and secondary formation. Convective scavenging of PSEA air was evidenced by considerable vertical differences between aerosol species but not trace gases, as well as notably higher APT and smaller particles than other regions. Finally, we observed a possible wet scavenging mechanism acting on MC air aloft that was not strictly linked to precipitation. These results are important for understanding the transport and processing of air masses with further implications for modeling aerosol lifecycles and guiding international policymaking to public health and climate, particularly during the SWM and MT.

scholarly journals Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections

2013 ◽  
Vol 13 (15) ◽  
pp. 7511-7529 ◽  
Author(s):  
A. D. Clarke ◽  
S. Freitag ◽  
R. M. C. Simpson ◽  
J. G. Hudson ◽  
S. G. Howell ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Long Range ◽  
Dimethyl Sulfide ◽  
Large Fraction ◽  
Equatorial Pacific ◽  
Long Range Transport ◽  
Quasi Equilibrium ◽  
Free Troposphere ◽  
Inter Tropical Convergence Zone ◽  
Range Transport

Abstract. Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were strongly influenced by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while ~25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining ~10% were inferred to be sea salt aerosol. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were mostly volatile at 360 °C with a number mode peak of around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant (3000 km or more) deep convection. Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. ~10 000 km away) and occurred in layers indicative of combustion sources (biomass burning season) partially scavenged by precipitation. These had number modes near 60–80 nm dry diameter with a large fraction of CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) prior to entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and in the FT just above the inversion, confirming that subsidence and entrainment of FT aerosol strongly influenced MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km also imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day timescale. The observed FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. Nonetheless, in spite of its importance, this source of CCN number is not well represented in most current models and is generally not detectable by satellite because of the low aerosol scattering in such layers as a result of cloud scavenging. In addition, our measurements confirm nucleation in the MBL was not evident during PASE and argue against a localized linear relation in the MBL between dimethyl sulfide (DMS) and CCN suggested by the CLAW hypothesis. However, when the FT is not impacted by long-range transport, sulfate aerosol derived from DMS pumped aloft in the ITCZ (Inter-Tropical Convergence Zone) can provide a source of CCN to the boundary layer via FT teleconnections involving more complex non-linear processes.

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