Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

Science ◽  
1998 ◽  
Vol 279 (5347) ◽  
pp. 49-53 ◽  
Author(s):  
P. O. Wennberg
Keyword(s):  
Upper Troposphere ◽  
Nitrogen Radicals ◽  
Hydrogen Radicals

scholarly journals NOypartitioning from measurements of nitrogen and hydrogen radicals in the upper troposphere

1999 ◽  
Vol 26 (1) ◽  
pp. 51-54 ◽  
Author(s):  
E. R. Keim ◽  
S. A. McKeen ◽  
R. S. Gao ◽  
S. G. Donnelly ◽  
R. C. Wamsley ◽  
...  
Keyword(s):  
Upper Troposphere ◽  
Hydrogen Radicals

scholarly journals Evaluation of simulated photochemical partitioning of oxidized nitrogen in the upper troposphere

2010 ◽  
Vol 10 (8) ◽  
pp. 20125-20165 ◽  
Author(s):  
B. H. Henderson ◽  
R. W. Pinder ◽  
J. Crooks ◽  
R. C. Cohen ◽  
W. T. Hutzell ◽  
...  
Keyword(s):  
Initial Conditions ◽  
Recent Observation ◽  
Chemical Mechanism ◽  
Upper Troposphere ◽  
Chemical Mechanisms ◽  
Convection Model ◽  
Photochemical Aging ◽  
Hydrogen Radicals ◽  
Evaluation Platform

Abstract. Regional and global chemical transport models underpredict NOx (NO+NO2) in the upper troposphere where it is a precursor to the greenhouse gas ozone. The NOx bias been shown in model evaluations using aircraft data (Singh et al., 2007) and total column NO2 (molecules cm−2) from satellite observations (Napelenok et al., 2008). The causes of NOx underpredictions have yet to be fully understood due to the interconnected nature of simulated emission, transport, and chemistry processes. Recent observation-based studies suggest that, in the upper troposphere, simulated chemistry overpredicts hydrogen radicals (OH• and HO2•) and would convert NOx to HNO3 too quickly (Olson et al., 2006; Bertram et al., 2007; Ren et al., 2008). Since typical chemistry evaluation techniques are not available for upper tropospheric conditions, this study develops an evaluation platform from in situ observations, stochastic convection, and deterministic chemistry. We derive a stochastic convection model and optimize it using two simulated datasets of time since convection, one based on meteorology and the other on chemistry. The chemistry surrogate for time since convection is calculated using seven different chemical mechanisms, all of which predict shorter time since convection than our meteorological analysis. We evaluate chemical simulations by inter-comparison and by pairing results with observations based on NOx:HNO3, a photochemical aging indicator. Inter-comparison reveals individual chemical mechanism biases and recommended updates. Evaluation against observations shows that all chemical mechanisms overpredict NOx removal relative to long-lived methanol and carbon monoxide. All chemical mechanisms underpredict observed NOx by at least 30%, and further evaluation is necessary to refine simulation sensitivities to initial conditions and chemical rate uncertainties.

scholarly journals Measurements of the sum of HO<sub>2</sub>NO<sub>2</sub> and CH<sub>3</sub>O<sub>2</sub>NO<sub>2</sub> in the remote troposphere

2003 ◽  
Vol 3 (6) ◽  
pp. 5689-5710 ◽  
Author(s):  
J. G. Murphy ◽  
J. A. Thornton ◽  
P. J. Wooldridge ◽  
D. A. Day ◽  
R. S. Rosen ◽  
...  
Keyword(s):  
Thermal Dissociation ◽  
Ozone Production ◽  
Upper Troposphere ◽  
Polar Latitude ◽  
Peroxynitric Acid ◽  
Spring Equinox ◽  
Permanent Loss ◽  
Research Aircraft ◽  
The Difference ◽  
Hydrogen Radicals

Abstract. The chemistry of peroxynitric acid (HO2NO2) and methyl peroxynitrate (CH3O2NO2) is predicted to be particularly important in the upper troposphere where temperatures are frequently low enough that these compounds do not rapidly decompose. At temperatures below 240 K, we calculate that about 20% of NOy in the mid and polar latitude upper troposphere is HO2NO2. Under these conditions, the reaction of OH with HO2NO2 is estimated to account for as much as one third of the permanent loss of hydrogen radicals. During the Tropospheric Ozone Production about the Spring Equinox (TOPSE) campaign, we used thermal dissociation laser-induced fluorescence (TD-LIF) to measure the sum of peroxynitrates (SPNs equivanlent HO2NO2 + CH3O2NO2 + PAN + PPN + ...), aboard the NCAR C-130 research aircraft. We infer the sum of HO2NO2 and CH3O2NO2 as the difference between SPN measurements and gas chromatographic measurements of the two major peroxy acyl nitrates, peroxy acetyl nitrate (PAN) and peroxy propionyl nitrate (PPN). Comparison with NOy and other nitrogen oxide measurements confirms the importance of HO2NO2 and CH3O2NO2 to the reactive nitrogen budget and shows that current thinking about the chemistry of these species is approximately correct. The temperature dependence of the inferred concentrations corroborates the contribution of overtone photolysis to the photochemistry of peroxynitric acid.

scholarly journals Measurements of the sum of HO<sub>2</sub>NO<sub>2</sub> and CH<sub>3</sub>O<sub>2</sub>NO<sub>2</sub> in the remote troposphere

2004 ◽  
Vol 4 (2) ◽  
pp. 377-384 ◽  
Author(s):  
J. G. Murphy ◽  
J. A. Thornton ◽  
P. J. Wooldridge ◽  
D. A. Day ◽  
R. S. Rosen ◽  
...  
Keyword(s):  
High Latitude ◽  
Thermal Dissociation ◽  
Ozone Production ◽  
Upper Troposphere ◽  
Peroxynitric Acid ◽  
Spring Equinox ◽  
Permanent Loss ◽  
Research Aircraft ◽  
The Difference ◽  
Hydrogen Radicals

Abstract. The chemistry of peroxynitric acid (HO2NO2) and methyl peroxynitrate (CH3O2NO2)is predicted to be particularly important in the upper troposphere where temperatures are frequently low enough that these compounds do not rapidly decompose. At temperatures below 240K, we calculate that about 20% of NOy in the mid- and high-latitude upper troposphere is HO2NO2. Under these conditions, the reaction of OH with HO2NO2 is estimated to account for as much as one third of the permanent loss of hydrogen radicals. During the Tropospheric Ozone Production about the Spring Equinox (TOPSE) campaign, we used thermal dissociation laser-induced fluorescence (TD-LIF) to measure the sum of peroxynitrates (PNs HO2NO2+CH3O2NO2+PAN+PPN+...) aboard the NCAR C-130 research aircraft. We infer the sum of HO2NO2 and CH3O2NO2 as the difference between PN measurements and gas chromatographic measurements of the two major peroxy acyl nitrates, peroxy acetyl nitrate (PAN) and peroxy propionyl nitrate (PPN). Comparison with NOy and other nitrogen oxide measurements confirms the importance of HO2NO2 and CH3O2NO2 to the reactive nitrogen budget and shows that current thinking about the chemistry of these species is approximately correct. During the spring high latitude conditions sampled during the TOPSE experiment, the model predictions of the contribution of (HO2NO2+CH3O2NO2) to NOy are highly temperature dependent: on average 30% of NOy at 230K, 15% of NOy at 240K, and 5% of NOy above 250K. The temperature dependence of the inferred concentrations corroborates the contribution of overtone photolysis to the photochemistry of peroxynitric acid. A model that includes IR photolysis (J=1x10-5s-1) agreed with the observed sum of HO2NO2+CH3O2NO2 to better than 35% below 240K where the concentration of these species is largest.

scholarly journals The photochemistry of acetone in the upper troposphere: A source of odd-hydrogen radicals

1997 ◽  
Vol 24 (24) ◽  
pp. 3177-3180 ◽  
Author(s):  
S. A. McKeen ◽  
T. Gierczak ◽  
J. B. Burkholder ◽  
P. O. Wennberg ◽  
T. F. Hanisco ◽  
...  
Keyword(s):  
Upper Troposphere ◽  
Hydrogen Radicals

scholarly journals Comparison of ISS–CATS and CALIPSO–CALIOP Characterization of High Clouds in the Tropics

2020 ◽  
Vol 12 (23) ◽  
pp. 3946
Author(s):  
Pasquale Sellitto ◽  
Silvia Bucci ◽  
Bernard Legras
Keyword(s):  
Optical Properties ◽  
Space Station ◽  
Satellite Observation ◽  
Observation Data ◽  
Upper Troposphere ◽  
Cloud Properties ◽  
Synchronous Orbit ◽  
The Tropics ◽  
High Clouds

Clouds in the tropics have an important role in the energy budget, atmospheric circulation, humidity, and composition of the tropical-to-global upper-troposphere–lower-stratosphere. Due to its non-sun-synchronous orbit, the Cloud–Aerosol Transport System (CATS) onboard the International Space Station (ISS) provided novel information on clouds from space in terms of overpass time in the period of 2015–2017. In this paper, we provide a seasonally resolved comparison of CATS characterization of high clouds (between 13 and 18 km altitude) in the tropics with well-established CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observation) data, both in terms of clouds’ occurrence and cloud optical properties (optical depth). Despite the fact that cloud statistics for CATS and CALIOP are generated using intrinsically different local overpass times, the characterization of high clouds occurrence and optical properties in the tropics with the two instruments is very similar. Observations from CATS underestimate clouds occurrence (up to 80%, at 18 km) and overestimate the occurrence of very thick clouds (up to 100% for optically very thick clouds, at 18 km) at higher altitudes. Thus, the description of stratospheric overshoots with CATS and CALIOP might be different. While this study hints at the consistency of CATS and CALIOP clouds characterizaton, the small differences highlighted in this work should be taken into account when using CATS for estimating cloud properties and their variability in the tropics.

Low-Temperature Post-Oxidation Annealing Using Atomic Hydrogen Radicals Generated by High-Temperature Catalyzer for Improvement in Reliability of Thermal Oxides on 4H-SiC

2006 ◽  
Vol 527-529 ◽  
pp. 999-1002
Author(s):  
Junji Senzaki ◽  
Atsushi Shimozato ◽  
Kenji Fukuda
Keyword(s):  
High Temperature ◽  
Low Temperature ◽  
Atomic Hydrogen ◽  
High Reliability ◽  
Hydrogen Atmosphere ◽  
Exposed Sample ◽  
New Apparatus ◽  
Hydrogen Radical ◽  
Hydrogen Radicals ◽  
Sic Wafer

Low-temperature post-oxidation annealing (POA) process of high-reliability thermal oxides grown on 4H-SiC using new apparatus that generates atomic hydrogen radicals by high-temperature catalyzer has been investigated. Atomic hydrogen radicals were generated by thermal decomposition of H2 gas at the catalyzer surface heated at high temperature of 1800°C, and then exposed to the sample at 500°C in reactor pressure of 20 Pa. The mode and maximum values of field-to-breakdown are 11.0 and 11.2 MV/cm, respectively, for the atomic hydrogen radical exposed sample. In addition, the charge-to-breakdown at 63% cumulative failure of the thermal oxides for atomic hydrogen radical exposed sample was 0.51 C/cm2, which was higher than that annealed at 800°C in hydrogen atmosphere (0.39 C/cm2). Consequently, the atomic hydrogen radical exposure at 500°C has remarkably improved the reliability of thermal oxides on 4H-SiC wafer, and is the same effect with high-temperature hydrogen POA at 800°C.

scholarly journals Atmospheric influences on infrared-laser signals used for occultation measurements between Low Earth Orbit satellites

2011 ◽  
Vol 4 (10) ◽  
pp. 2273-2292 ◽  
Author(s):  
S. Schweitzer ◽  
G. Kirchengast ◽  
V. Proschek
Keyword(s):  
Wind Speed ◽  
Solar Radiation ◽  
Thermal Radiation ◽  
Rayleigh Scattering ◽  
Infrared Laser ◽  
Low Earth Orbit ◽  
Earth Orbit ◽  
Wind Speed Profile ◽  
Upper Troposphere ◽  
Trace Species

Abstract. LEO-LEO infrared-laser occultation (LIO) is a new occultation technique between Low Earth Orbit (LEO) satellites, which applies signals in the short wave infrared spectral range (SWIR) within 2 μm to 2.5 μm. It is part of the LEO-LEO microwave and infrared-laser occultation (LMIO) method that enables to retrieve thermodynamic profiles (pressure, temperature, humidity) and altitude levels from microwave signals and profiles of greenhouse gases and further variables such as line-of-sight wind speed from simultaneously measured LIO signals. Due to the novelty of the LMIO method, detailed knowledge of atmospheric influences on LIO signals and of their suitability for accurate trace species retrieval did not yet exist. Here we discuss these influences, assessing effects from refraction, trace species absorption, aerosol extinction and Rayleigh scattering in detail, and addressing clouds, turbulence, wind, scattered solar radiation and terrestrial thermal radiation as well. We show that the influence of refractive defocusing, foreign species absorption, aerosols and turbulence is observable, but can be rendered small to negligible by use of the differential transmission principle with a close frequency spacing of LIO absorption and reference signals within 0.5%. The influences of Rayleigh scattering and terrestrial thermal radiation are found negligible. Cloud-scattered solar radiation can be observable under bright-day conditions, but this influence can be made negligible by a close time spacing (within 5 ms) of interleaved laser-pulse and background signals. Cloud extinction loss generally blocks SWIR signals, except very thin or sub-visible cirrus clouds, which can be addressed by retrieving a cloud layering profile and exploiting it in the trace species retrieval. Wind can have a small influence on the trace species absorption, which can be made negligible by using a simultaneously retrieved or a moderately accurate background wind speed profile. We conclude that the set of SWIR channels proposed for implementing the LMIO method (Kirchengast and Schweitzer, 2011) provides adequate sensitivity to accurately retrieve eight trace species of key importance to climate and atmospheric chemistry (H2O, CO2, 13CO2, C18OO, CH4, N2O, O3, CO) in the upper troposphere/lower stratosphere region outside clouds under all atmospheric conditions. Two further species (HDO, H218O) can be retrieved in the upper troposphere.

scholarly journals Implications of GNSS-Inferred Tropopause Altitude Associated with Terrestrial Gamma-Ray Flashes

2021 ◽  
Vol 13 (10) ◽  
pp. 1939
Author(s):  
Tao Xian ◽  
Gaopeng Lu ◽  
Hongbo Zhang ◽  
Yongping Wang ◽  
Shaolin Xiong ◽  
...  
Keyword(s):  
Gamma Ray ◽  
Thermal Structure ◽  
Deep Convection ◽  
Caribbean Sea ◽  
Negative Bias ◽  
Upper Troposphere ◽  
Cold Anomaly ◽  
The Caribbean ◽  
Geographic Distributions

The thermal structure of the environmental atmosphere associated with Terrestrial Gamma-ray Flashes (TGFs) is investigated with the combined observations from several detectors (FERMI, RHESSI, and Insight-HXMT) and GNSS-RO (SAC-C, COSMIC, GRACE, TerraSAR-X, and MetOp-A). The geographic distributions of TGF-related tropopause altitude and climatology are similar. The regional TGF-related tropopause altitude in Africa and the Caribbean Sea is 0.1–0.4 km lower than the climatology, whereas that in Asia is 0.1–0.2 km higher. Most of the TGF-related tropopause altitudes are slightly higher than the climatology, while some of them have a slightly negative bias. The subtropical TGF-producing thunderstorms are warmer in the troposphere and have a colder and higher tropopause over land than the ocean. There is no significant land–ocean difference in the thermal structure for the tropical TGF-producing thunderstorms. The TGF-producing thunderstorms have a cold anomaly in the middle and upper troposphere and have stronger anomalies than the deep convection found in previous studies.

AEROSOL PRODUCTION IN THE UPPER TROPOSPHERE

2001 ◽  
Vol 32 ◽  
pp. 1047-1048
Author(s):  
C.F. CLEMENT ◽  
I.J. FORD ◽  
C.H. TWOHY
Keyword(s):  
Upper Troposphere
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