scholarly journals What do <sup>14</sup>CO measurements tell us about OH?

2007 ◽  
Vol 7 (4) ◽  
pp. 10405-10438 ◽  
Author(s):  
M. C. Krol ◽  
J. Fokke Meirink ◽  
P. Bergamaschi ◽  
J. E. Mak ◽  
D. Lowe ◽  
...  

Abstract. The possible use of 14CO measurements to constrain hydroxyl radical (OH) concentrations in the atmosphere is investigated.14CO is mainly produced in the upper atmosphere from cosmic radiation. During transport to measurement locations at the Earth's surface 14CO is oxidized by OH. In this paper, the sensitivity of 14CO mixing ratio measurements to the 3-D OH distribution is assessed with the TM5 model. Simulated 14CO mixing ratios compare reasonably well with atmospheric measurements taken at five locations worldwide. As a next step, the sensitivity of 14CO measurements to OH is calculated with the adjoint TM5 model. For our sensitivity calculations the adjoint methodology outlined in the paper offers computational advantages compared to forward model calculations. The results indicate that 14CO measurements, especially those taken in the tropics, are sensitive to OH in a spatially confined region. Moreover, the OH sensitivity at a certain location varies strongly over time due to meteorological variability. On average, 14CO measurements are about 5 times more sensitive to OH at high latitudes than to OH in the tropics. Moreover, the measurements are sensitive to OH in the main 14CO source region in the upper atmosphere. It will therefore be difficult to assign model-measurement discrepancies to either the 14CO source uncertainty or to the OH sink. Nevertheless, the large distance between the 14CO source region and the measurement locations should allow the retrieval of information on OH. Specifically, the sensitivity to OH in the lower atmosphere during a relatively short time span may offer the possibility to constrain local OH. These efforts will strongly depend on the number of measurements available and on our ability to accurately model the 14CO transport.

Author(s):  
Petra Koucká Knížová ◽  
Jan Laštovička ◽  
Daniel Kouba ◽  
Zbyšek Mošna ◽  
Katerina Podolská ◽  
...  

The ionosphere represents part of the upper atmosphere. Its variability is observed on a wide-scale temporal range from minutes, or even shorter, up to scales of the solar cycle and secular variations of solar energy input. Ionosphere behavior is predominantly determined by solar and geomagnetic forcing. However, the lower-lying atmospheric regions can contribute significantly to the resulting energy budget. The energy transfer between distant atmospheric parts happens due to atmospheric waves that propagate from their source region up to ionospheric heights. Experimental observations show the importance of the involvement of the lower atmosphere in ionospheric variability studies in order to accurately capture small-scale features of the upper atmosphere. In the Part I Coupling, we provide a brief overview of the influence of the lower atmosphere on the ionosphere and summarize the current knowledge. In the Part II Coupling Evidences Within Ionospheric Plasma—Experiments in Midlatitudes, we demonstrate experimental evidence from mid-latitudes, particularly those based on observations by instruments operated by the Institute of Atmospheric Physics, Czech Academy of Sciences. The focus will mainly be on coupling by atmospheric waves.


2012 ◽  
Vol 12 (4) ◽  
pp. 11035-11077 ◽  
Author(s):  
Z. Buys ◽  
N. Brough ◽  
G. Huey ◽  
D. Tanner ◽  
R. von Glasow ◽  
...  

Abstract. There is much debate over the source of bromine radicals in the atmosphere that drives polar boundary layer ozone depletion events (ODEs), but there is strong evidence to suggest a source associated with the sea ice zone. Here we report the first high temporal resolution measurements of Br2, BrCl and BrO in coastal Antarctica, made using a Chemical Ionisation Mass Spectrometer (CIMS). Mixing ratios ranged from instrumental detection limits to 13 pptv for BrO, 45 pptv for Br2, and 6 pptv for BrCl. We find evidence for blowing snow as a source of reactive bromine both directly during a storm and subsequently from recycling of bromide deposited on the continental snowpack. An unusual event of trans-continental air mass transport might have been responsible for severe surface ozone depletion observed at Halley. The halogen source region was the Bellingshausen Sea, to the west of the Antarctic Peninsula, the air mass having spent 3 1/2 days in complete darkness prior to arrival at Halley. We, further, identify an artefact in daytime BrCl measurements arising from conversion of HOBr, similar to that already identified for CIMS observations of Br2. Model calculations using the MISTRA 0-D model suggest a 50–60% conversion of HOBr to Br2, and 5–10% conversion to BrCl. Careful data filtering enabled us to use the halogen observations, in conjunction with the MISTRA model, to explore the temperature dependence of the Br2:BrCl ratio. We find evidence of a ratio shift towards Br2 at temperatures below ~−21 °C, suggesting a relationship with hydrohalite (NaCl.2H2O) precipitation. This suite of Antarctic data provides the first analogue to similar measurements made in the Arctic.


2018 ◽  
Vol 18 (3) ◽  
pp. 1977-1996 ◽  
Author(s):  
Catalina Tsai ◽  
Max Spolaor ◽  
Santo Fedele Colosimo ◽  
Olga Pikelnaya ◽  
Ross Cheung ◽  
...  

Abstract. Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH) in the lower atmosphere, in particular in winter when other OH sources are less efficient. The nighttime formation of HONO and its photolysis in the early morning have long been recognized as an important contributor to the OH budget in polluted environments. Over the past few decades it has become clear that the formation of HONO during the day is an even larger contributor to the OH budget and additionally provides a pathway to recycle NOx. Despite the recognition of this unidentified HONO daytime source, the precise chemical mechanism remains elusive. A number of mechanisms have been proposed, including gas-phase, aerosol, and ground surface processes, to explain the elevated levels of daytime HONO. To identify the likely HONO formation mechanisms in a wintertime polluted rural environment we present LP-DOAS observations of HONO, NO2, and O3 on three absorption paths that cover altitude intervals from 2 to 31, 45, and 68 m above ground level (a.g.l.) during the UBWOS 2012 experiment in the Uintah Basin, Utah, USA. Daytime HONO mixing ratios in the 2–31 m height interval were, on average, 78 ppt, which is lower than HONO levels measured in most polluted urban environments with similar NO2 mixing ratios of 1–2 ppb. HONO surface fluxes at 19 m a.g.l., calculated using the HONO gradients from the LP-DOAS and measured eddy diffusivity coefficient, show clear upward fluxes. The hourly average vertical HONO flux during sunny days followed solar irradiance, with a maximum of (4.9 ± 0.2)  ×  1010 molec. cm−2 s−1 at noontime. A photostationary state analysis of the HONO budget shows that the surface flux closes the HONO budget, accounting for 63 ± 32 % of the unidentified HONO daytime source throughout the day and 90 ± 30 % near noontime. This is also supported by 1-D chemistry and transport model calculations that include the measured surface flux, thus clearly identifying chemistry at the ground as the missing daytime HONO source in this environment. Comparison between HONO surface flux, solar radiation, NO2 and HNO3 mixing ratios, and results from 1-D model runs suggest that, under high NOx conditions, HONO formation mechanisms related to solar radiation and NO2 mixing ratios, such as photo-enhanced conversion of NO2 on the ground, are most likely the source of daytime HONO. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the main source of HONO.


1971 ◽  
Vol 40 ◽  
pp. 394-400
Author(s):  
Wayne E. McGovern

The satellite Titan is commonly quoted as possessing an atmosphere consisting of at least 2 × 104 cm atm of methane. Plausible additional atmospheric constituents like hydrogen and helium are assumed to have completely escaped from the satellite. However, the employment of recent techniques to the upper atmosphere of Titan permits an improved estimate of the upper limits of the hydrogen to methane and helium to methane mixing ratios existing in the lower atmosphere of Titan, namely 10−6±1 and 10−3.5±0.5.


2017 ◽  
Author(s):  
Catalina Tsai ◽  
Max Spolaor ◽  
Santo Fedele Colosimo ◽  
Olga Pikelnaya ◽  
Ross Cheung ◽  
...  

Abstract. Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH) in the lower atmosphere, in particular in winter when other OH sources are less efficient. The nighttime formation of HONO and its photolysis in the early morning have long been recognized as an important contributor to the OH budget in polluted environments. Over the past few decades it has become clear that the formation of HONO during the day is an even larger contributor to the OH budget, and additionally provides a pathway to recycle NOx. Despite the recognition of this unidentified HONO daytime source, the precise chemical mechanism remains elusive. A number of mechanisms have been proposed, including gas-phase, aerosol, and ground surface processes, to explain the elevated levels of daytime HONO. To identify the likely HONO formation mechanisms in a wintertime polluted rural environment we present LP-DOAS observations of HONO, NO2, and O3 on three absorption paths that cover altitude intervals from 2 m to 31 m, 45 m, and 68 m agl during the UBWOS 2012 experiment in the Uintah Basin, Utah, USA. Daytime HONO mixing ratios in the 2–31 m height interval were, on average, 78 ppt, which is lower than HONO levels measured in most polluted urban environments with similar NO2 mixing ratios of 1–2 ppb. HONO surface fluxes at 16 m agl, calculated using the HONO gradients from the LP-DOAS and measured eddy diffusivity coefficient, show clear upward fluxes. The hourly average vertical HONO flux during sunny days followed solar irradiance, with a maximum of (4.9 ± 0.2) x 1010 molec. cm−2 s−1 at noontime. A photo-stationary state analysis of the HONO budget shows that the surface flux closes the HONO budget, accounting for 63 ± 32 % of the unidentified HONO daytime source throughout the day and 90 ± 30 % near noontime. This is also supported by 1D chemistry and transport model calculations that include the measured surface flux, thus clearly identifying chemistry at the ground as the missing daytime HONO source in this environment. Comparison between HONO surface flux, solar radiation, NO2 and HNO3 mixing ratios and results from 1D model runs suggest that, under high NOx conditions, HONO formation mechanisms related to solar radiation and NO2 mixing ratios, such as photo-enhanced conversion of NO2 on the ground, are most likely the source of daytime HONO. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the main source of HONO.


2008 ◽  
Vol 8 (16) ◽  
pp. 5033-5044 ◽  
Author(s):  
M. C. Krol ◽  
J. F. Meirink ◽  
P. Bergamaschi ◽  
J. E. Mak ◽  
D. Lowe ◽  
...  

Abstract. The possible use of 14CO measurements to constrain hydroxyl radical (OH) concentrations in the atmosphere is investigated. 14CO is mainly produced in the upper atmosphere from cosmic radiation. Measurements of 14CO at the surface show lower concentrations compared to the upper atmospheric source region, which is the result of oxidation by OH. In this paper, the sensitivity of 14CO mixing ratio surface measurements to the 3-D OH distribution is assessed with the TM5 model. Simulated 14CO mixing ratios agree within a few molecules 14CO cm−3 (STP) with existing measurements at five locations worldwide. The simulated cosmogenic 14CO distribution appears mainly sensitive to the assumed upper atmospheric 14C source function, and to a lesser extend to model resolution. As a next step, the sensitivity of 14CO measurements to OH is calculated with the adjoint TM5 model. The results indicate that 14CO measurements taken in the tropics are sensitive to OH in a spatially confined region that varies strongly over time due to meteorological variability. Given measurements with an accuracy of 0.5 molecules 14CO cm−3 STP, a good characterization of the cosmogenic 14CO fraction, and assuming perfect transport modeling, a single 14CO measurement may constrain OH to 0.2–0.3×106 molecules OH cm−3 on time scales of 6 months and spatial scales of 70×70 degrees (latitude×longitude) between the surface and 500 hPa. The sensitivity of 14CO measurements to high latitude OH is about a factor of five higher. This is in contrast with methyl chloroform (MCF) measurements, which show the highest sensitivity to tropical OH, mainly due to the temperature dependent rate constant of the MCF–OH reaction. A logical next step will be the analysis of existing 14CO measurements in an inverse modeling framework. This paper presents the required mathematical framework for such an analysis.


The transmission of wireless signals to very great distances, and certain other phenomena associated with wireless telegraphy, have been ascribed by several writers to the presence of a conducting layer in the upper atmosphere. Such a layer, if it were conducting in the ordinary sense, would act as a screen in respect of electrical effects which had their origin external to the layer, and further, as has been shown, electrical disturbances set up in the space between the conducting layer and the earth’s surface would subside so slowly that the time required to establish an approximately steady state would be very great. It appears natural, therefore, to assume that, if there is reflexion from the upper atmosphere, there must also be radiation through it to allow a steady state to be attained in a comparatively short time, and the simplest hypothesis consistent with this is that the upper atmosphere differs from the lower atmosphere in respect of the constants involved in the propagation of electrical effects through the atmosphere, viz., the specific inductive capacity and the magnetic permeability. It is proposed to investigate on this hypothesis the condition that a steady state of electrical oscillation can be established in the lower atmosphere in a comparatively short time, and the distribution of electric and magnetic forces on the earth’s surface due to a simple oscillator near to the surface when this condition is satisfied.


2021 ◽  
Vol 13 (8) ◽  
pp. 1454
Author(s):  
Anatoliy A. Nusinov ◽  
Tamara V. Kazachevskaya ◽  
Valeriya V. Katyushina

Modeling the upper atmosphere and ionospheres on the basis of a mathematical description of physical processes requires knowledge of ultraviolet radiation fluxes from the Sun as an integral part of the model. Aeronomic models of variations in the radiation flux in the region of extreme (EUV) and far (FUV) radiation, based mainly on the data of the last TIMED mission measurements of the solar spectrum, are proposed. The EUVT model describes variations in the 5–105 nm spectral region, which are responsible for the ionization of the main components of the earth’s atmosphere. The FUVT model describes the flux changes in the 115–242 nm region, which determines heating of the upper atmosphere and the dissociation of molecular oxygen. Both models use the intensity of the hydrogen Lyman-alpha line as an input parameter, which can currently be considered as one of the main indices of solar activity and can be measured with relatively simpler photometers. A comparison of the results of model calculations with observations shows that the model error does not exceed 1–2% for the FUVT model, and 5.5% for EUVT, which is sufficient for calculating the parameters of the ionosphere and thermosphere.


Religions ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 545
Author(s):  
Gary Carville

The Second Vatican Council and, in particular, its Constitution on the Sacred Liturgy, changed much in the daily life of the Church. In Ireland, a country steeped in the Catholic tradition but largely peripheral to the theological debates that shaped Vatican II, the changes to liturgy and devotional practice were implemented dutifully over a relatively short time span and without significant upset. But did the hierarchical manner of their reception, like that of the Council itself, mean that Irish Catholics did not receive the changes in a way that deepened their spirituality? And was the popular religious memory of the people lost through a neglect of liturgical piety and its place in the interior life, alongside what the Council sought to achieve? In this essay, Dr Gary Carville will examine the background to the liturgical changes at Vatican II, the contribution to their formulation and implementation by leaders of the Church in Ireland, the experiences of Irish Catholic communities in the reception process, and the ongoing need for a liturgical formation that brings theology, memory, and practice into greater dialogue.


Author(s):  
Anders Raustorp ◽  
Andreas Fröberg

Background: The objectives of this study were to explore the effect of time, long-term tracking, and the proportion of objectively measured physical activity (PA) from early adolescence to the mid-thirties. Methods: PA was measured as mean steps per day (SPD) with pedometers during 2000 (T1), 2003 (T2), 2005 (T3), 2010 (T4), 2016 (T5) and 2020 (T6). Data from 64 participants (n = 32 males) were analysed from their early adolescence (T1) to their mid-thirties (T6). Results: SPD decreased in the total sample and among males and females (all, p < 0.001). Males took more mean SPD than females during T1 (p = 0.002), whereas females took more mean SPD during T2 (p = 0.009) and T6 (p = 0.008). Males’ mean SPD tracked between T1 and T2 (p = 0.021), T2 and T3 (p = 0.030), T3 and T4 (p = 0.015) and T4 and T5 (p = 0.003). Females’ mean SPD tracked between T3 and T4 (p = 0.024) and T5 and T6 (p < 0.001). In the total sample, more mean SPD were found on weekdays compared to weekend days at T3 (p = 0.017) and T5 (p < 0.001). Conclusions: SPD decreased between T1 and T6. Mean SPD tracked low-to-moderate in the short time span. From late adolescence to the mid-thirties, more mean SPD was observed during weekdays compared to weekend days.


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