scholarly journals A Machine Learning Examination of Hydroxyl Radical Differences Among Model Simulations for CCMI-1

2019 ◽  
Author(s):  
Julie M. Nicely ◽  
Bryan N. Duncan ◽  
Thomas F. Hanisco ◽  
Glenn M. Wolfe ◽  
Ross J. Salawitch ◽  
...  

Abstract. Hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting CH4 lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among ten models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D) due mostly to clouds, mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapor, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, CH4, the photolysis frequency of NO2 by visible light (JNO2), overhead O3 column, and temperature account for little-to-no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapor on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, O3 column, and temperature are also in reasonably good agreement between the two studies, though a discrepancy in the CH4 response highlights a need for further examination of the CH4 feedback on the abundance of OH.

2020 ◽  
Vol 20 (3) ◽  
pp. 1341-1361 ◽  
Author(s):  
Julie M. Nicely ◽  
Bryan N. Duncan ◽  
Thomas F. Hanisco ◽  
Glenn M. Wolfe ◽  
Ross J. Salawitch ◽  
...  

Abstract. The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.


2021 ◽  
Vol 22 (14) ◽  
pp. 7637
Author(s):  
Liliya T. Sahharova ◽  
Evgeniy G. Gordeev ◽  
Dmitry B. Eremin ◽  
Valentine P. Ananikov

The processes involving the capture of free radicals were explored by performing DFT molecular dynamics simulations and modeling of reaction energy profiles. We describe the idea of a radical recognition assay, where not only the presence of a radical but also the nature/reactivity of a radical may be assessed. The idea is to utilize a set of radical-sensitive molecules as tunable sensors, followed by insight into the studied radical species based on the observed reactivity/selectivity. We utilize this approach for selective recognition of common radicals—alkyl, phenyl, and iodine. By matching quantum chemical calculations with experimental data, we show that components of a system react differently with the studied radicals. Possible radical generation processes were studied involving model reactions under UV light and metal-catalyzed conditions.


Atmosphere ◽  
2021 ◽  
Vol 12 (3) ◽  
pp. 291
Author(s):  
Jinpeng Lu ◽  
Fei Xie ◽  
Hongying Tian ◽  
Jiali Luo

Stratospheric water vapor (SWV) changes play an important role in regulating global climate change, and its variations are controlled by tropopause temperature. This study estimates the impacts of tropopause layer ozone changes on tropopause temperature by radiative process and further influences on lower stratospheric water vapor (LSWV) using the Whole Atmosphere Community Climate Model (WACCM4). It is found that a 10% depletion in global (mid-low and polar latitudes) tropopause layer ozone causes a significant cooling of the tropical cold-point tropopause with a maximum cooling of 0.3 K, and a corresponding reduction in LSWV with a maximum value of 0.06 ppmv. The depletion of tropopause layer ozone at mid-low latitudes results in cooling of the tropical cold-point tropopause by radiative processes and a corresponding LSWV reduction. However, the effect of polar tropopause layer ozone depletion on tropical cold-point tropopause temperature and LSWV is opposite to and weaker than the effect of tropopause layer ozone depletion at mid-low latitudes. Finally, the joint effect of tropopause layer ozone depletion (at mid-low and polar latitudes) causes a negative cold-point tropopause temperature and a decreased tropical LSWV. Conversely, the impact of a 10% increase in global tropopause layer ozone on LSWV is exactly the opposite of the impact of ozone depletion. After 2000, tropopause layer ozone decreased at mid-low latitudes and increased at high latitudes. These tropopause layer ozone changes at different latitudes cause joint cooling in the tropical cold-point tropopause and a reduction in LSWV. Clarifying the impacts of tropopause layer ozone changes on LSWV clearly is important for understanding and predicting SWV changes in the context of future global ozone recovery.


2018 ◽  
Vol 31 (3) ◽  
pp. 929-943 ◽  
Author(s):  
Fei Xie ◽  
Xin Zhou ◽  
Jianping Li ◽  
Quanliang Chen ◽  
Jiankai Zhang ◽  
...  

Abstract Time-slice experiments with the Whole Atmosphere Community Climate Model, version 4 (WACCM4), and composite analysis with satellite observations are used to demonstrate that the Indo-Pacific warm pool (IPWP) can significantly affect lower-stratospheric water vapor. It is found that a warmer IPWP significantly dries the stratospheric water vapor by causing a broad cooling of the tropopause, and vice versa for a colder IPWP. Such imprints in tropopause temperature are driven by a combination of variations in the Brewer–Dobson circulation in the stratosphere and deep convection in the troposphere. Changes in deep convection associated with El Niño–Southern Oscillation (ENSO) reportedly have a small zonal mean effect on lower-stratospheric water vapor for strong zonally asymmetric effects on tropopause temperature. In contrast, IPWP events have zonally uniform imprints on tropopause temperature. This is because equatorial planetary waves forced by latent heat release from deep convection project strongly onto ENSO but weakly onto IPWP events.


2013 ◽  
Vol 13 (14) ◽  
pp. 6877-6886 ◽  
Author(s):  
D. Scheiben ◽  
A. Schanz ◽  
B. Tschanz ◽  
N. Kämpfer

Abstract. In this paper, we compare the diurnal variations in middle-atmospheric water vapor as measured by two ground-based microwave radiometers in the Alpine region near Bern, Switzerland. The observational data set is also compared to data from the chemistry–climate model WACCM. Due to the small diurnal variations of usually less than 1%, averages over extended time periods are required. Therefore, two time periods of five months each, December to April and June to October, were taken for the comparison. The diurnal variations from the observational data agree well with each other in amplitude and phase. The linear correlation coefficients range from 0.8 in the upper stratosphere to 0.5 in the upper mesosphere. The observed diurnal variability is significant at all pressure levels within the sensitivity of the instruments. Comparing our observations with WACCM, we find that the agreement of the phase of the diurnal cycle between observations and model is better from December to April than from June to October. The amplitudes of the diurnal variations for both time periods increase with altitude in WACCM, but remain approximately constant at 0.05 ppm in the observations. The WACCM data are used to separate the processes that lead to diurnal variations in middle-atmospheric water vapor above Bern. The dominating processes were found to be meridional advection below 0.1 hPa, vertical advection between 0.1 and 0.02 hPa and (photo-)chemistry above 0.02 hPa. The contribution of zonal advection is small. The highest diurnal variations in water vapor as seen in the WACCM data are found in the mesopause region during the time period from June to October with diurnal amplitudes of 0.2 ppm (approximately 5% in relative units).


2012 ◽  
Vol 25 (16) ◽  
pp. 5471-5493 ◽  
Author(s):  
Jacola A. Roman ◽  
Robert O. Knuteson ◽  
Steven A. Ackerman ◽  
David C. Tobin ◽  
Henry E. Revercomb

Abstract Precipitable water vapor (PWV) observations from the National Center of Atmospheric Research (NCAR) SuomiNet networks of ground-based global positioning system (GPS) receivers and the National Oceanic and Atmospheric Administration (NOAA) Profiler Network (NPN) are used in the regional assessment of global climate models. Study regions in the U.S. Great Plains and Midwest highlight the differences among global climate model output from the Fourth Assessment Report (AR4) Special Report on Emissions Scenarios (SRES) A2 scenario in their seasonal representation of column water vapor and the vertical distribution of moisture. In particular, the Community Climate System model, version 3 (CCSM3) is shown to exhibit a dry bias of over 30% in the summertime water vapor column, while the Goddard Institute for Space Studies Model E20 (GISS E20) agrees well with PWV observations. A detailed assessment of vertical profiles of temperature, relative humidity, and specific humidity confirm that only GISS E20 was able to represent the summertime specific humidity profile in the atmospheric boundary layer (<3%) and thus the correct total column water vapor. All models show good agreement in the winter season for the region. Regional trends using station-elevation-corrected GPS PWV data from two complimentary networks are found to be consistent with null trends predicted in the AR4 A2 scenario model output for the period 2000–09. The time to detect (TTD) a 0.05 mm yr−1 PWV trend, as predicted in the A2 scenario for the period 2000–2100, is shown to be 25–30 yr with 95% confidence in the Oklahoma–Kansas region.


2013 ◽  
Vol 13 (2) ◽  
pp. 3859-3880 ◽  
Author(s):  
D. Scheiben ◽  
A. Schanz ◽  
B. Tschanz ◽  
N. Kämpfer

Abstract. In this paper, we compare the diurnal variations in middle atmospheric water vapor as measured by two ground-based microwave radiometers in the Alpine region near Bern, Switzerland. The observational data set is also compared to data from the chemistry-climate model WACCM. Due to the small diurnal variations of usually less than 1%, averages over extended time periods are required. Therefore, two time periods of five months each, December to April and June to October, were taken for the comparison. The diurnal variations from the observational data agree well with each other in amplitude and phase. The linear correlation coefficients range from 0.8 in the upper stratosphere to 0.5 in the upper mesosphere. The observed diurnal variability is significant at all pressure levels within the sensitivity of the instruments. Comparing our observations with WACCM, we find that the agreement of the phase of the diurnal cycle between observations and model is better from December to April than from June to October. The amplitudes of the diurnal variations for both time periods increase with altitude in WACCM, but remain approximately constant at 0.05 parts per million in the observations. The WACCM data is used to separate the processes that lead to diurnal variations in middle atmospheric water vapor above Bern. The dominating processes were found to be meridional advection below 0.1 hPa, vertical advection between 0.1 and 0.02 hPa and (photo-)chemistry above 0.02 hPa. The contribution of zonal advection is small. The highest diurnal variations in water vapor are found in the mesopause region during the time period from June to October with diurnal amplitudes of 0.2 ppm (approximately 5% in relative units).


2020 ◽  
Vol 20 (21) ◽  
pp. 13011-13022
Author(s):  
Yuanhong Zhao ◽  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Xin Lin ◽  
Antoine Berchet ◽  
...  

Abstract. Decadal trends and interannual variations in the hydroxyl radical (OH), while poorly constrained at present, are critical for understanding the observed evolution of atmospheric methane (CH4). Through analyzing the OH fields simulated by the model ensemble of the Chemistry–Climate Model Initiative (CCMI), we find (1) the negative OH anomalies during the El Niño years mainly corresponding to the enhanced carbon monoxide (CO) emissions from biomass burning and (2) a positive OH trend during 1980–2010 dominated by the elevated primary production and the reduced loss of OH due to decreasing CO after 2000. Both two-box model inversions and variational 4D inversions suggest that ignoring the negative anomaly of OH during the El Niño years leads to a large overestimation of the increase in global CH4 emissions by up to 10 ± 3 Tg yr−1 to match the observed CH4 increase over these years. Not accounting for the increasing OH trends given by the CCMI models leads to an underestimation of the CH4 emission increase by 23 ± 9 Tg yr−1 from 1986 to 2010. The variational-inversion-estimated CH4 emissions show that the tropical regions contribute most to the uncertainties related to OH. This study highlights the significant impact of climate and chemical feedbacks related to OH on the top-down estimates of the global CH4 budget.


2013 ◽  
Vol 26 (1) ◽  
pp. 231-245 ◽  
Author(s):  
Michael Winton ◽  
Alistair Adcroft ◽  
Stephen M. Griffies ◽  
Robert W. Hallberg ◽  
Larry W. Horowitz ◽  
...  

Abstract The influence of alternative ocean and atmosphere subcomponents on climate model simulation of transient sensitivities is examined by comparing three GFDL climate models used for phase 5 of the Coupled Model Intercomparison Project (CMIP5). The base model ESM2M is closely related to GFDL’s CMIP3 climate model version 2.1 (CM2.1), and makes use of a depth coordinate ocean component. The second model, ESM2G, is identical to ESM2M but makes use of an isopycnal coordinate ocean model. The authors compare the impact of this “ocean swap” with an “atmosphere swap” that produces the GFDL Climate Model version 3 (CM3) by replacing the AM2 atmospheric component with AM3 while retaining a depth coordinate ocean model. The atmosphere swap is found to have much larger influence on sensitivities of global surface temperature and Northern Hemisphere sea ice cover. The atmosphere swap also introduces a multidecadal response time scale through its indirect influence on heat uptake. Despite significant differences in their interior ocean mean states, the ESM2M and ESM2G simulations of these metrics of climate change are very similar, except for an enhanced high-latitude salinity response accompanied by temporarily advancing sea ice in ESM2G. In the ESM2G historical simulation this behavior results in the establishment of a strong halocline in the subpolar North Atlantic during the early twentieth century and an associated cooling, which are counter to observations in that region. The Atlantic meridional overturning declines comparably in all three models.


2016 ◽  
Vol 33 (11) ◽  
pp. 2353-2372 ◽  
Author(s):  
Tammy M. Weckwerth ◽  
Kristy J. Weber ◽  
David D. Turner ◽  
Scott M. Spuler

AbstractA water vapor micropulse differential absorption lidar (DIAL) instrument was developed collaboratively by the National Center for Atmospheric Research (NCAR) and Montana State University (MSU). This innovative, eye-safe, low-power, diode-laser-based system has demonstrated the ability to obtain unattended continuous observations in both day and night. Data comparisons with well-established water vapor observing systems, including radiosondes, Atmospheric Emitted Radiance Interferometers (AERIs), microwave radiometer profilers (MWRPs), and ground-based global positioning system (GPS) receivers, show excellent agreement. The Pearson’s correlation coefficient for the DIAL and radiosondes is consistently greater than 0.6 from 300 m up to 4.5 km AGL at night and up to 3.5 km AGL during the day. The Pearson’s correlation coefficient for the DIAL and AERI is greater than 0.6 from 300 m up to 2.25 km at night and from 300 m up to 2.0 km during the day. Further comparison with the continuously operating GPS instrumentation illustrates consistent temporal trends when integrating the DIAL measurements up to 6 km AGL.


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