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Atmosphere
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Theoretical Chemistry of Atmospheric Processes
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Theoretical Chemistry of Atmospheric Processes

A special issue of Atmosphere (ISSN 2073-4433). This special issue belongs to the section "Air Quality".

Deadline for manuscript submissions: closed (16 July 2021) | Viewed by 20536

Special Issue Editor

Dr. Luís Pedro Viegas

E-Mail Website
Guest Editor
Coimbra Chemistry Center, University of Coimbra, 3004-531 Coimbra, Portugal
Interests: electronic structure calculations; multiconformer transition state theory; nonadiabatic transition state theory; atmospheric chemistry; quantum tunneling

Special Issue Information

Dear Colleagues,

Atmospheric chemistry occurs within a fabric of profoundly complicated atmospheric dynamics through kilometers of several atmospheric layers. Understanding the underlying theoretical details of the atmosphere's chemical processes is of fundamental importance, not only to assist the interpretation of observational/field and laboratory measurements, but also to contribute to the building blocks of theoretical models with good predictive capability. At present, one of the highest priority societal challenges concerns climate change, namely the impact of anthropogenic global warming and also of air pollution, for which successful responses and solutions will benefit greatly from the knowledge resulting from atmospheric chemistry research. Such information is considered to be of great value in guiding the necessary policies to mitigate the hazardous consequences of climate change. Within this context, the importance of theoretical and computational chemistry is unquestionable.

The present issue invites researchers to submit their novel and unpublished research addressing a broad range of topics, from fundamental method development to applied studies concerning kinetic modelling, reaction path finding, structure activity relationships, modelling of heterogeneous reactions, cluster formation from atmospheric vapours and photochemical aspects of air pollution.

Dr. Luís Pedro Viegas
Guest Editor

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • theoretical and computational chemistry
  • tropospheric chemistry
  • electronic structure calculations
  • modelling
  • gas phase kinetics

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Published Papers (7 papers)

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Editorial

Jump to: Research, Review

2 pages, 155 KiB  
Editorial
Theoretical Chemistry of Atmospheric Processes
by Luís Pedro Viegas
Atmosphere 2022, 13(2), 309; https://doi.org/10.3390/atmos13020309 - 12 Feb 2022
Viewed by 1249
Abstract
Atmospheric chemistry occurs within a fabric of profoundly complicated dynamics through several atmospheric layers [...] Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)

Research

Jump to: Editorial, Review

16 pages, 586 KiB  
Article
A Theoretical Study of the N2 + H2 Reactive Collisions for High Vibrational and Translational Energies
by Juan de Dios Garrido and Maikel Yusat Ballester
Atmosphere 2021, 12(10), 1349; https://doi.org/10.3390/atmos12101349 - 15 Oct 2021
Cited by 2 | Viewed by 1939
Abstract
High translational temperatures appear in the air inside the shock waves layers created by relatively large meteorites, reentry space vehicles, and hypersonic missiles. Under these conditions, reactions between molecular nitrogen and hydrogen are energetically permitted. In the present work, a quasiclassical trajectories study [...] Read more.
High translational temperatures appear in the air inside the shock waves layers created by relatively large meteorites, reentry space vehicles, and hypersonic missiles. Under these conditions, reactions between molecular nitrogen and hydrogen are energetically permitted. In the present work, a quasiclassical trajectories study of the N2(v′)+H2(v″) reaction for relative translational energies covering the range of translational energy 20.0≤Etr/kcalmol−1≤120.0 is presented. In the calculations, several values of vibrational quantum numbers v′=0,4,6,8,10,12 and v″=4,6,8,10,12 have been considered. To model the interatomic interactions, a six-dimension global potential energy surface for the ground electronic state of N2H2 was used. The specific initial state reaction cross-sections and rate coefficients are reported. The energy effects produced by the reaction that could influence the shock wave modeling are here considered. An analysis of the possible impact of these processes under the atmospheric composition is also presented. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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11 pages, 5627 KiB  
Article
Tri-Base Synergy in Sulfuric Acid-Base Clusters
by Hong-Bin Xie and Jonas Elm
Atmosphere 2021, 12(10), 1260; https://doi.org/10.3390/atmos12101260 - 27 Sep 2021
Cited by 13 | Viewed by 2886
Abstract
Synergistic effects between different bases can greatly enhance atmospheric sulfuric acid (SA)-base cluster formation. However, only the synergy between two base components has previously been investigated. Here, we extend this concept to three bases by studying large atmospherically relevant (SA)3(base)3 [...] Read more.
Synergistic effects between different bases can greatly enhance atmospheric sulfuric acid (SA)-base cluster formation. However, only the synergy between two base components has previously been investigated. Here, we extend this concept to three bases by studying large atmospherically relevant (SA)3(base)3 clusters, with the bases ammonia (A), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA) and ethylenediamine (EDA). Using density functional theory—ωB97X-D/6-31++G(d,p)—we calculate the cluster structures and vibrational frequencies. The thermochemical parameters are calculated at 29,815 K and 1 atm, using the quasi-harmonic approximation. The binding energies of the clusters are calculated using high level DLPNO-CCSD(T0)/aug-cc-pVTZ. We find that the cluster stability in general depends on the basicity of the constituent bases, with some noteworthy additional guidelines: DMA enhances the cluster stability, TMA decreases the cluster stability and there is high synergy between DMA and EDA. Based on our calculations, we find it highly likely that three, or potentially more, different bases, are involved in the growth pathways of sulfuric acid-base clusters. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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17 pages, 4205 KiB  
Article
Theoretical Studies on the Reaction Mechanism and Kinetics of Ethylbenzene-OH Adduct with O2 and NO2
by Tingting Lu, Mingqiang Huang, Xin Lin, Wei Zhang, Weixiong Zhao, Changjin Hu, Xuejun Gu and Weijun Zhang
Atmosphere 2021, 12(9), 1118; https://doi.org/10.3390/atmos12091118 - 31 Aug 2021
Cited by 5 | Viewed by 2494
Abstract
The OH-initiated reaction of ethylbenzene results in major OH addition, and the formed ethylbenzene-OH adducts subsequently react with O2 and NO2, which determine the components of the oxidation products. In this study, nine possible reaction paths of the most stable [...] Read more.
The OH-initiated reaction of ethylbenzene results in major OH addition, and the formed ethylbenzene-OH adducts subsequently react with O2 and NO2, which determine the components of the oxidation products. In this study, nine possible reaction paths of the most stable ethylbenzene-OH adduct, EB-Ortho (2-ethyl-hydroxycyclohexadienyl radical intermediate), with O2 and NO2 were studied using density functional theory and conventional transition state theory. The calculated results showed that ethyl-phenol formed via hydrogen abstraction was the major product of the EB-Ortho reaction with O2 under atmospheric conditions. Peroxy radicals generated from O2 added to EB-Ortho could subsequently react with NO and O2 to produce 5-ethyl-6-oxo-2,4-hexadienal, furan, and ethyl-glyoxal, respectively. However, nitro-ethylbenzene formed from NO2 addition to EB-Ortho was the predominant product of the EB-Ortho reaction with NO2 at room temperature. The total calculated rate constant of the EB-Ortho reaction with O2 and NO2 was 9.57 × 10−16 and 1.78 × 10−11 cm3 molecule−1 s−1, respectively, approximately equivalent to the experimental rate constants of toluene-OH adduct reactions with O2 and NO2. This study might provide a useful theoretical basis for interpreting the oxygen-containing and nitrogen-containing organics in anthropogenic secondary organic aerosol particles. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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18 pages, 2002 KiB  
Article
Kinetics of the Reactions of Ozone with Halogen Atoms in the Stratosphere
by S. Vijayakumar, Duminda S. Ranasinghe and David M. Wilmouth
Atmosphere 2021, 12(8), 1053; https://doi.org/10.3390/atmos12081053 - 17 Aug 2021
Cited by 2 | Viewed by 3271
Abstract
It is well established that reaction cycles involving inorganic halogens contribute to the depletion of ozone in the atmosphere. Here, the kinetics of O3 with halogen atoms (Cl, Br, and I) were investigated between 180 and 400 K, expanding the temperature range [...] Read more.
It is well established that reaction cycles involving inorganic halogens contribute to the depletion of ozone in the atmosphere. Here, the kinetics of O3 with halogen atoms (Cl, Br, and I) were investigated between 180 and 400 K, expanding the temperature range relative to prior studies. Canonical variational transition state theory including small curvature tunneling correction (CVT/SCT) were considered, following the construction of the potential energy surfaces. MRCI + Q/aug-ano-pVTZ//MP2/aug-cc-pV(T + d)Z and MRCI + Q/aug-ano-RCC-VTZP//MP2/aug-cc-pV(T + d)Z levels of theory were used to calculate the kinetic parameters. Calculated rate coefficients were used to fit the Arrhenius equations, which are obtained to be k1 = (3.48 ± 0.4) × 10−11 exp[(−301 ± 64)/T] cm3 molecule−1 s−1, k2 = (3.54 ± 0.2) × 10−11 exp[(−990 ± 35)/T] cm3 molecule−1 s−1 and k3 = (1.47 ± 0.1) × 10−11 exp[(−720 ± 42)/T] cm3 molecule−1 s−1 for the reactions of O3 with Cl, Br, and I atoms, respectively. The obtained rate coefficients for the reactions of O3 with halogen atoms using CVT/SCT are compared to the latest recommended rate coefficients by the NASA/JPL and IUPAC evaluations. The reactivity trends and pathways of these reactions are discussed. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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26 pages, 3020 KiB  
Article
O3 Concentration and Its Relation with BVOC Emissions in a Subtropical Plantation
by Jianhui Bai
Atmosphere 2021, 12(6), 711; https://doi.org/10.3390/atmos12060711 - 31 May 2021
Cited by 7 | Viewed by 3335
Abstract
An empirical model of O3 is developed using the measurements of emissions of biogenic volatile organic compounds (BVOCs), O3 concentration, global solar radiation, photosynthetically active radiation (PAR) and meteorological variables in a subtropical Pinus plantation, China, during 2013–2016. In view of [...] Read more.
An empirical model of O3 is developed using the measurements of emissions of biogenic volatile organic compounds (BVOCs), O3 concentration, global solar radiation, photosynthetically active radiation (PAR) and meteorological variables in a subtropical Pinus plantation, China, during 2013–2016. In view of the different structures of isoprene and monoterpenes, two empirical models of O3 concentration are developed, considering PAR absorption and scattering due to gases, liquids and particles (GLPs), as well as PAR attenuation caused by O3 and BVOCs. The estimated O3 is in agreement with the observations, and validation of the O3 empirical model is conducted. O3 concentrations are more sensitive to changes in PAR and water vapor than S/Q (horizontal diffuse to global solar radiation) and BVOC emissions. O3 is positive to changes in isoprene emission at low light and high GLPs, or negative at high light and low GLPs; O3 is negative to changes in monoterpene emissions. O3 are positive with the changes of PAR, water vapor and S/Q. It is suggested to control human-induced high BVOC emissions, regulate plant cutting, and reduce NOx and SO2 emissions more strictly than ever before. There are inverted U-shape interactions between O3 and its driving factors, and S/Q controls their turning points. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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Review

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10 pages, 277 KiB  
Review
Theoretical Chemistry and the Calculation of the Atmospheric State
by Adrian F. Tuck
Atmosphere 2021, 12(6), 727; https://doi.org/10.3390/atmos12060727 - 6 Jun 2021
Cited by 8 | Viewed by 3364
Abstract
Theoretical chemists have been actively engaged for some time in processes such as ozone photodissociation, overtone photodissociation in nitric acid, pernitric acid, sulphuric acid, clusters and in small organic acids. The last of these have shown very different behaviours in the gas phase, [...] Read more.
Theoretical chemists have been actively engaged for some time in processes such as ozone photodissociation, overtone photodissociation in nitric acid, pernitric acid, sulphuric acid, clusters and in small organic acids. The last of these have shown very different behaviours in the gas phase, liquid phase and importantly at the air–water interface in aqueous aerosols. The founder of molecular dynamics, B J Alder, pointed out long ago that hydrodynamic behaviour emerged when the symmetry of a random, thermalised population of hard spheres—billiard balls—was broken by a flux of energetic molecules. Despite this, efforts over two centuries to solve turbulence by finding top-down solutions to the Navier–Stokes equation have failed. It is time for theoretical chemistry to try a bottom-up solution. Gibbs free energy that drives the circulation arises from the entropy difference between the incoming low-entropy beam of visible and ultraviolet photons and the outgoing higher-entropy flux of infrared photons over the whole 4π solid angle. The role of the most energetic molecules with the highest velocities will affect the rovibrational line shapes of water, carbon dioxide and ozone in the far wings, where there is the largest effect on radiative transfer and hence on calculations of atmospheric temperature. The atmospheric state is determined by the interaction of radiation, chemistry and fluid dynamics on the microscopic scale, with propagation through the mesoscale to the macroscale. It will take theoretical chemistry to simulate that accurately. A challenging programme of research for theoretical chemistry is proposed, involving ab initio simulation by molecular dynamics of an air volume, starting in the upper stratosphere. The aim is to obtain scaling exponents for turbulence, providing a physical method for upscaling in numerical models. Turbulence affects chemistry, radiation and fluid dynamics at a fundamental, molecular level and is thus of basic concern to theoretical chemistry as it applies to the atmosphere, which consists of molecules in motion. Full article
(This article belongs to the Special Issue Theoretical Chemistry of Atmospheric Processes)
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