A5019033081- Atmospheric chemistry and aerosols
- Atmospheric Ozone and Climate
- Advanced Chemical Physics Studies
- Air Quality and Health Impacts
- Atmospheric aerosols and clouds
- Spectroscopy and Laser Applications
- Atmospheric and Environmental Gas Dynamics
- Crystallization and Solubility Studies
- Air Quality Monitoring and Forecasting
- X-ray Diffraction in Crystallography
- Photochromic and Fluorescence Chemistry
- Chemical Thermodynamics and Molecular Structure
- nanoparticles nucleation surface interactions
- Analytical Chemistry and Chromatography
- Spectroscopy and Quantum Chemical Studies
- Machine Learning in Materials Science
- Chemical and Physical Properties in Aqueous Solutions
- Photochemistry and Electron Transfer Studies
- Catalytic Processes in Materials Science
- Porphyrin and Phthalocyanine Chemistry
- Phase Equilibria and Thermodynamics
- Industrial Gas Emission Control
- Synthesis and Properties of Aromatic Compounds
- Vehicle emissions and performance
- Catalysis and Oxidation Reactions
Aarhus University
2017-2025
Helsinki Institute of Physics
2015-2017
University of Helsinki
2015-2017
University of Copenhagen
2011-2016
Center for Solar Energy Research and Studies
2016
Ørsted (Denmark)
2011-2015
DK4
2014
Abstract Over Boreal regions, monoterpenes emitted from the forest are main precursors for secondary organic aerosol (SOA) formation and primary driver of growth new particles to climatically important cloud condensation nuclei (CCN). Autoxidation leads rapid Highly Oxygenated Molecules (HOM). We have developed first model with near-explicit representation atmospheric particle (NPF) HOM formation. The can reproduce observed NPF, gas-phase composition SOA over forest. During spring, increases...
This work assesses different computational strategies for predicting structures and Gibb's free energies of reaction atmospheric prenucleation clusters. The performance 22 Density Functional Theory functionals in equilibrium molecules water clusters relevance is evaluated against experimental data using a test set eight clusters: SO2, H2SO4, CO2·H2O, CS2·H2O, OCS·H2O, SO2·H2O, SO3·H2O, H2SO4·H2O. Furthermore, the are tested compared their ability to predict energy formation five benchmark...
This work assesses the binding energies of atmospherically relevant clusters containing H2SO4, H2O, NH3 and (CH3)2NH using density functional theory. The performance seven DFT functionals (B3LYP, CAM-B3LYP, M06-2X, PW91, LC-PW91, PBE0 ωB97X-D) is evaluated against high level explicitly correlated coupled cluster methods a test set 107 clusters. Our studies show that all tested correlate well with results, but highly varying mean absolute errors. PBE0, PW91 M06-2X are found to perform...
Abstract. Over oceans and in coastal regions, methane sulfonic acid (MSA) is present substantial concentrations aerosols the gas phase. We an investigation into effect of MSA on sulfuric acid- dimethyl amine (DMA)-based cluster formation rates. From systematic conformational scans well-tested ab initio methods, we optimise structures all MSAx (H2SO4)yDMAz clusters where x + y ≤ 3 z 2. The resulting thermodynamic data are used Atmospheric Cluster Dynamics Code, evaluated by...
Monoethanolamine (MEA), a potential atmospheric pollutant from the capture unit of leading CO2 technology, could be removed by participating H2SO4-based new particle formation (NPF) as simple amines. Here we evaluated enhancing MEA on NPF examining molecular clusters and H2SO4 using combined quantum chemistry calculations kinetics modeling. The results indicate that at parts per trillion (ppt) level can enhance NPF. is less than dimethylamine (DMA), one strongest agents, much greater...
Knowledge about Setschenow salting constants, KS, the exponential dependence of Henry's Law coefficients on salt concentration, is particular importance to predict secondary organic aerosol (SOA) formation from soluble species in atmospheric waters with high concentrations, such as aerosols. We have measured KS glyoxal and methylglyoxal for atmospherically relevant salts (NH4)2SO4, NH4NO3, NaNO3, NaCl find that consistently "salts-in" (KS −0.16, −0.06, −0.065, −0.1 molality–1, respectively)...
We present the first binding energy benchmark set at CBS limit of strongly hydrogen bonded atmospheric molecular clusters.
We have collected, recomputed, and compiled a database consisting of 633 unique atmospherically relevant molecular clusters containing sulfuric acid, bases, oxidized organic compounds, water. The is composed strongly hydrogen-bonded spans neutral, negatively charged, positively charged atmospheric relevance. All the cluster structures vibrational frequencies been re-evaluated at ωB97X-D/6-31++G(d,p) level theory, single point energies refined using high-level DLPNO-CCSD(T)/aug-cc-pVTZ...
We investigate the utilization of domain local pair natural orbital coupled cluster (DLPNO-CCSD(T)) method for calculating binding energies atmospherical molecular clusters. Applied to small complexes relevance we find that DLPNO significantly reduces scatter in energy, which is commonly present DFT calculations. For medium sized clusters consisting sulfuric acid and bases yields a systematic underestimation energy compared canonical results. The errors appear be more random, while nature...
Abstract One key challenge in the field of exploitation solar energy is to store and make it available on demand. possibility use photochromic molecules that undergo light‐induced isomerization metastable isomers. Here we present efforts develop thermal storage systems based dihydroazulene (DHA)/vinylheptafulvene (VHF) photo/thermoswitch. New DHA derivatives with one electron‐withdrawing cyano group at position 1 or two phenyl substituents five‐membered ring were prepared by using different...
Recent experimental evidence suggests that diamines can enhance atmospheric new particle formation more efficiently compared to monoamines such as dimethylamine. Here we investigate the molecular interactions between sulfuric acid (sa) and diamine putrescine (put) using computational methods. The structure of up four molecules were obtained at ωB97X-D/6-31++G(d,p) level theory. We utilized a domain local pair natural orbital coupled cluster method (DLPNO-CCSD(T)/aug-cc-pVTZ) obtain highly...
We investigate the molecular interaction between methyl-substituted N,N,N',N'-ethylenediamines, propane-1,3-diamine, butane-1,4-diamine, and sulfuric acid using computational methods. Molecular structure of diamines their dimer clusters with is studied three density functional theory methods (PW91, M06-2X, ωB97X-D) 6-31++G(d,p) basis set. A high level explicitly correlated CCSD(T)-F12a/VDZ-F12 method used to obtain accurate binding energies. The reaction Gibbs free energies are evaluated...
Amines are recognized as significant enhancing species on methanesulfonic acid (MSA)-driven new particle formation (NPF). Monoethanolamine (MEA) has been detected in the atmosphere, and its concentration could be significantly increased once MEA-based postcombustion CO2 capture technology is widely implemented. Here, we evaluated potential of MEA MSA-driven NPF by examining MEA–MSA clusters using a combination quantum chemical calculations kinetics modeling. The results indicate that −OH...
Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to that of extensively studied sulfuric (SA)-driven process. Generally, enhancing potentials in SA-driven NPF follow basicity, while this not case for MSA-driven NPF, where structural effects dominate, making more prominent methylamine (MA) dimethylamine (DMA). Therefore, probing factors determining on key fully understanding contribution MSA...
This work assesses the performance of DLPNO-CCSD(T0), DLPNO-MP2, and density functional theory methods in calculating binding energies a representative test set 45 atmospheric acid–acid, acid–base, acid–water dimer clusters. The approximate is compared to high level explicitly correlated CCSD(F12*)(T)/complete basis (CBS) reference calculations. Out tested functionals, ωB97X-D3(BJ) shows best with mean deviation 0.09 kcal/mol maximum 0.83 kcal/mol. RI-CC2/aug-cc-pV(T+d)Z severely...
Abstract. Dimethyl sulfide (DMS) is the dominant biogenic sulfur compound in ambient marine atmosphere. Low-volatility acids from DMS oxidation promote formation and growth of aerosols ultimately alter cloud properties Earth's climate. We studied OH-initiated Aarhus University Research on Aerosol (AURA) smog chamber boundary layer (MBL) with aerosol dynamics gas- particle-phase chemistry kinetic multilayer model ADCHAM. Our work involved development a revised comprehensive multiphase...
Abstract. Atmospheric organic acids (OAs) are expected to enhance methanesulfonic acid (MSA)-driven new particle formation (NPF). However, the exact role of OAs in MSA-driven NPF remains unclear. Here, we employed a two-step strategy probe MSA–methylamine (MA) NPF. Initially, evaluated enhancing potential 12 commonly detected ternary MA–MSA–OA cluster by considering free energies (MSA)1(MA)1(OA)1 clusters and atmospheric concentrations OAs. It was found that formic (ForA) has highest...
Iodic acid (IA) has recently been recognized as a key driver for new particle formation (NPF) in marine atmospheres. However, the knowledge of which atmospheric vapors can enhance IA-induced NPF remains limited. The unique halogen bond (XB)-forming capacity IA makes it difficult to evaluate enhancing potential (EP) target compounds on based widely studied sulfuric systems. Herein, we employed three-step procedure EP nucleation precursors NPF. First, evaluated 63 by simulating free energies...
Abstract As one of the least understood aerosol processes, nucleation can be a dominant source atmospheric aerosols. Sulfuric acid (SA)-amine binary with dimethylamine (DMA) has been recognized as governing mechanism in polluted continental boundary layer. Here we demonstrate importance trimethylamine (TMA) for complex atmosphere and propose molecular-level SA-DMA-TMA ternary an improvement upon conventional mechanism. Using proposed mechanism, could connect gaseous amines to SA-amine...
The formation of molecular clusters and secondary aerosols in the atmosphere has a significant impact on climate. Studies typically focus new particle (NPF) sulfuric acid (SA) with single base molecule (e.g., dimethylamine or ammonia). In this work, we examine combinations synergy several bases. Specifically, used computational quantum chemistry to perform configurational sampling (CS) (SA)0-4(base)0-4 five different types bases: ammonia (AM), methylamine (MA), (DMA), trimethylamine (TMA),...
Pyruvic acid is an omnipresent compound in nature and found both the gas phase particle of atmosphere as well aqueous solution hydrosphere. Despite much literature on photochemical degradation stability pyruvic different chemical environments, study simultaneous interactions between gas-phase or similar carboxylic acids with water ions not well-understood. Here, we present a microhydrated molecular clusters containing structurally analogous lactic acid, propionic 2,2-dihydroxypropanoic by...