scholarly journals The decrease in mid-stratospheric tropical ozone since 1991

2015 ◽  
Vol 15 (8) ◽  
pp. 4215-4224 ◽  
Author(s):  
G. E. Nedoluha ◽  
D. E. Siskind ◽  
A. Lambert ◽  
C. Boone

Abstract. While global stratospheric O3 has begun to recover, there are localized regions where O3 has decreased since 1991. Specifically, we use measurements from the Halogen Occultation Experiment (HALOE) for the period 1991–2005 and the NASA Aura Microwave Limb Sounder (MLS) for the period 2004–2013 to demonstrate a significant decrease in O3 near ~ 10 hPa in the tropics. O3 in this region is very sensitive to variations in NOy, and the observed decrease can be understood as a spatially localized, yet long-term increase in NOy. In turn, using data from MLS and from the Atmospheric Chemistry Experiment (ACE), we show that the NOy variations are caused by decreases in N2O which are likely linked to long-term variations in dynamics. To illustrate how variations in dynamics can affect N2O and O3, we show that by decreasing the upwelling in the tropics, more of the N2O can photodissociate with a concomitant increase in NOy production (via N2O + O(1D) → 2NO) at 10 hPa. Ultimately, this can cause an O3 decrease of the observed magnitude.

2015 ◽  
Vol 15 (1) ◽  
pp. 453-480 ◽  
Author(s):  
G. E. Nedoluha ◽  
D. E. Siskind ◽  
A. Lambert ◽  
C. Boone

Abstract. While global stratospheric O3 has begun to recover, there are localized regions where O3 has decreased since 1991. Specifically, we use measurements from the Halogen Occultation Experiment (HALOE) for the period 1991–2005 and the NASA/Aura Microwave Limb Sounder (MLS) for the period 2004–2013 to demonstrate a significant decrease in O3 near ~10 hPa in the tropics. O3 in this region is very sensitive to variations in NOy, and the observed decrease can be understood as a spatially localized, yet long term increase in NOy. In turn, using data from MLS and from the Atmospheric Chemistry Experiment (ACE), we show that the NOy variations are caused by decreases in N2O which are likely linked to long term variations in dynamics. To illustrate how variations in dynamics can affect N2O and O3, we show that by decreasing the upwelling in the tropics, more of the N2O can photodissociate with a concomitant increase in NOy production (via N2O+O(1D → 2 NO) at 10 hPa. Ultimately, this can cause an O3 decrease of the observed magnitude.


2010 ◽  
Vol 10 (4) ◽  
pp. 8623-8655
Author(s):  
A. Jones ◽  
J. Urban ◽  
D. P. Murtagh ◽  
C. Sanchez ◽  
K. A. Walker ◽  
...  

Abstract. Previous analyses of satellite and ground-based measurements of hydrogen chloride (HCl) and chlorine monoxide (ClO) have suggested that total inorganic chlorine in the upper stratosphere is on the decline. We create HCl and ClO time series using satellite data sets with the intension of extending them to beyond November 2008 so that an update can be made on the long term evolution of these two species. We use the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data for the HCl analysis, and the Odin Sub-Millimetre Radiometer (SMR) and the Aura Microwave Limb Sounder (Aura-MLS) measurements for the study of ClO. Altitudes between 35 and 45 km and three latitude bands between 60° S–60° N for HCl, and 20° S–20° N for ClO are studied. HCl shows values to be reducing from peak 1997 values by −4.4% in the tropics and between −6.4% to −6.7% per decade in the mid-latitudes. Trend values are significantly different from a zero trend at the 2 sigma level. ClO is decreasing in the tropics by −7.1% ± 7.8%/decade based on measurements made from December 2001. As both of these species contribute most to the chlorine budget at these altitudes then HCl and ClO should decrease at similar rates. The results found here confirm how effective the 1987 Montreal protocol objectives and its amendments have been in reducing the total amount of inorganic chlorine.


2013 ◽  
Vol 13 (2) ◽  
pp. 4221-4287 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer-tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the VMR from tropical ground-based AGAGE sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 195 + (−) 75 (42) yr (CH4), 69 + (−) 65 (23) yr (CH3Cl) and 123 + (−) 53 (28) yr (N2O). The errors on these values are the weighted 1-σ non-systematic errors. The stratospheric lifetime of CH3Cl represents the first calculations of the stratospheric lifetime of CH3Cl using data from a space based instrument.


2013 ◽  
Vol 13 (14) ◽  
pp. 6921-6950 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer–tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the volume mixing ratio (VMR) from tropical ground based AGAGE (Advanced Global Atmospheric Gases Experiment) sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 69 + (−) 65 (23) yr (CH3Cl), 123 + (−) 53 (28) yr (N2O) and 195 + (−) 75 (42) yr (CH4). The errors on these values are the weighted 1σ non-systematic errors. Systematic errors were estimated by recalculating lifetimes using VMRs which had been modified to reflect differences between ACE-FTS retrieved VMRs and those from other instruments. The results of these calculations, including systematic errors, were as follows: 113 + (−) 32 (20) for CFC-12, 123 + (−) 83 (35) for N2O, 195 + (−) 139 (57) for CH4, 35 + (−) 14 (8) for CCl4 and 69 + (−) 2119 (34) yr for CH3Cl. For CH3Cl & CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.


2021 ◽  
Author(s):  
Nathaniel J. Livesey ◽  
William G. Read ◽  
Lucien Froidevaux ◽  
Alyn Lambert ◽  
Michelle L. Santee ◽  
...  

Abstract. The Microwave Limb Sounder (MLS), launched on NASA's Aura spacecraft in 2004, measures vertical profiles of the abundances of key atmospheric species from the upper troposphere to the mesosphere with daily near-global coverage. We review the first 15 years of the record of H2O and N2O measurements from the MLS 190-GHz subsystem (along with other 190-GHz information), with a focus on their long-term stability, largely based on comparisons with measurements from other sensors. These comparisons generally show signs of an increasing drift in the MLS version 4 (v4) H2O record starting around 2010. Specifically, comparisons with v4.1 measurements from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) indicate a ~2–3 %/decade drift over much of the stratosphere, increasing to as much as ~7 %/decade around 46 hPa. Larger drifts, of around 7–11 %/decade, are seen in comparisons to balloon-borne frost point hygrometer measurements in the lower stratosphere. In contrast, the MLS v4 N2O product is shown to be generally decreasing over the same period (when an increase in stratospheric N2O is expected, reflecting a secular growth in emissions), with a more pronounced drift in the lower stratosphere than that found for H2O. Detailed investigations of the behavior of the MLS 190-GHz subsystem reveal a drift in its sideband fraction (the relative sensitivity of the 190-GHz receiver to the two different parts of the microwave spectrum it observes). Our studies indicate that sideband fraction drift accounts for much of the observed changes in the MLS H2O product and some portion of the changes seen in N2O. The 190-GHz sideband fraction drift has been corrected in the new version 5 MLS algorithms, which have now been used to reprocess the entire MLS record. As a result of this correction, the MLS v5 H2O record shows no statistically significant drifts compared to ACE-FTS. However, statistically significant drifts remain between MLS v5 and frost point measurements, though they are reduced. Drifts in v5 N2O are about half the size of those in v4 but remain statistically significant. Scientists are advised to use MLS v5 data in all future studies. Quantification of inter-regional and seasonal-to-annual changes in MLS H2O and N2O will not be affected by the drift. However, caution is advised in studies using the MLS record to examine long-term (multi-year) variability and trends in either of these species, especially N2O; such studies should only be undertaken in consultation with the MLS team. Importantly, this drift does not affect any of the MLS observations made in other spectral regions such as O3, HCl, CO, ClO, or temperature.


2007 ◽  
Vol 7 (23) ◽  
pp. 6075-6084 ◽  
Author(s):  
M. Toohey ◽  
B. M. Quine ◽  
K. Strong ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
...  

Abstract. Low-resolution atmospheric thermal emission spectra collected by balloon-borne radiometers over the time span of 1990–2002 are used to retrieve vertical profiles of HNO3, CFC-11 and CFC-12 volume mixing ratios between approximately 10 and 35 km altitude. All of the data analyzed have been collected from launches from a Northern Hemisphere mid-latitude site, during late summer, when stratospheric dynamic variability is at a minimum. The retrieval technique incorporates detailed forward modeling of the instrument and the radiative properties of the atmosphere, and obtains a best fit between modeled and measured spectra through a combination of onion-peeling and optimization steps. The retrieved HNO3 profiles are consistent over the 12-year period, and are consistent with recent measurements by the Atmospheric Chemistry Experiment-Fourier transform spectrometer satellite instrument. We therefore find no evidence of long-term changes in the HNO3 summer mid-latitude profile, although the uncertainty of our measurements precludes a conclusive trend analysis.


Author(s):  
Anatoly V. Belov ◽  
Raisa T. Gushchina ◽  
Nataly Shlyk ◽  
Victor Yanke

The paper presents preliminary results of a comparison of long-term variations of the cosmic ray flux using data from the network of ground-based detectors with direct flux measurements on the PAMELA and AMS-02 magnetic spectrometers and a series of balloon stratospheric soundings. The analysis showed good agreement for the entire period of continuous ground-based monitoring of cosmic ray variations.


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