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  • 1. Bull, James N.
    et al.
    Buntine, Jack T.
    Scholz, Michael S.
    Carrascosa, Eduardo
    Giacomozzi, Linda
    Stockholm University, Faculty of Science, Department of Physics.
    Stockett, Mark H.
    Stockholm University, Faculty of Science, Department of Physics.
    Bieske, Evan J.
    Photodetachment and photoreactions of substituted naphthalene anions in a tandem ion mobility spectrometer2019In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 217, p. 34-46Article in journal (Refereed)
    Abstract [en]

    Substituted naphthalene anions (deprotonated 2-naphthol and 6-hydroxy-2-naphthoic acid) are spectroscopically probed in a tandem drift tube ion mobility spectrometer (IMS). Target anions are selected according to their drift speed through nitrogen buffer gas in the first IMS stage before being exposed to a pulse of tunable light that induces either photodissociation or electron photodetachment, which is conveniently monitored by scavenging the detached electrons with trace SF6 in the buffer gas. The photodetachment action spectrum of the 2-naphtholate anion exhibits a band system spanning 380-460 nm with a prominent series of peaks spaced by 440 cm(-1), commencing at 458.5 nm, and a set of weaker peaks near the electron detachment threshold corresponding to transitions to dipole-bound states. The two deprotomers of 6-hydroxy-2-naphthoic acid are separated and spectroscopically probed independently. The molecular anion formed from deprotonation of the hydroxy group gives rise to a photodetachment action spectrum similar to that of the 2-naphtholate anion with an onset at 470 nm and a maximum at 420 nm. Near the threshold, the photoreaction with SF6 is observed with displacement of an OH group by an F atom. In contrast, the anion formed from deprotonation of the carboxylic acid group gives rise to a photodissociation action spectrum, recorded on the CO2 loss channel, lying at much shorter wavelengths with an onset at 360 nm and maximum photoresponse at 325 nm.

  • 2. Donahue, Neil M.
    et al.
    Ortega, Ismael K.
    Chuang, Wayne
    Riipinen, Ilona
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Riccobono, Francesco
    Schobesberger, Siegfried
    Dommen, Josef
    Baltensperger, Urs
    Kulmala, Markku
    Worsnop, Douglas R.
    Vehkamäki, Hanna
    How do organic vapors contribute to new-particle formation?2013In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 165, p. 91-104Article in journal (Refereed)
    Abstract [en]

    Highly oxidised organic vapors can effectively stabilize sulphuric acid in heteronuclear clusters and drive new-particle formation. We present quantum chemical calculations of cluster stability, showing that multifunctional species can stabilize sulphuric acid and also present additional polar functional groups for subsequent cluster growth. We also model the multi-generation oxidation of vapors associated with secondary organic aerosol formation using a two-dimensional volatility basis set. The steady-state saturation ratios and absolute concentrations of extremely low volatility products are sufficient to drive new-particle formation with sulphuric acid at atmospherically relevant rates.

  • 3.
    Galkin, Maxim V.
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Di Francesco, Davide
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Edlund, Ulrica
    Samec, Joseph S. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Sustainable sources need reliable standards2017In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 202, p. 281-301Article in journal (Refereed)
    Abstract [en]

    This review discusses the challenges within the research area of modern biomass fractionation and valorization. The current pulping industry focuses on pulp production and the resulting cellulose fiber. Hemicellulose and lignin are handled as low value streams for process heat and the regeneration of process chemicals. The paper and pulp industry have therefore developed analytical techniques to evaluate the cellulose fiber, while the other fractions are given a low priority. In a strive to also use the hemicellulose and lignin fractions of lignocellulosic biomass, moving towards a biorefining concept, there are severe shortcomings with the current pulping techniques and also in the analysis of the biomass. Lately, new fractionation techniques have emerged which valorize a larger extent of the lignocellulosic biomass. This progress has disclosed the shortcomings in the analysis of mainly the hemicellulose and lignin structure and properties. To move the research field forward, analytical tools for both the raw material, targeting all the wood components, and the generated fractions, as well as standardized methods for evaluating and reporting yields are desired. At the end of this review, a discourse on how such standardizations can be implemented is given.

  • 4.
    Gatchell, Michael
    et al.
    Stockholm University, Faculty of Science, Department of Physics. Universität Innsbruck, Austria.
    Martini, Paul
    Laimer, Felix
    Goulart, Marcelo
    Calvo, Florent
    Scheier, Paul
    Spectroscopy of corannulene cations in helium nanodroplets2019In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 217, p. 276-289Article in journal (Refereed)
    Abstract [en]

    Helium tagging in action spectroscopy is an efficient method for measuring the absorption spectra of complex molecular ions with minimal perturbations to the gas phase spectra. We have used superfluid helium nanodroplets doped with corannulene to prepare cations of these molecules complexed with different numbers of He atoms. In total we identify 13 different absorption bands from corannulene cations between 5500 angstrom and 6000 angstrom. The He atoms cause a small, chemically induced redshift of the band positions of the corannulene ion. By studying this effect as a function of the number of solvating atoms we are able to identify the formation of solvation structures that are not visible in the mass spectrum. The solvation features detected using action spectroscopy agree very well with the results of atomistic modeling based on path-integral molecular dynamics simulations. By additionally doping our He droplets with D-2, we produce protonated corannulene ions. The absorption spectrum of these ions differs significantly from the case of the radical cations as the numerous narrow bands are replaced by a broad absorption feature that spans nearly 2000 angstrom in width.

  • 5.
    Geppert, Wolf
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Hamberg, Mathias
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Österdahl, Fabian
    Stockholm University, Faculty of Science, Department of Physics.
    Hellberg, Fredrik
    Stockholm University, Faculty of Science, Department of Physics.
    Zhaunerchyk, Vitali
    Stockholm University, Faculty of Science, Department of Physics.
    Ehlerding, Anneli
    Stockholm University, Faculty of Science, Department of Physics.
    Millar, Tom
    Queen's University Belfast.
    Roberts, Helen
    Queen's University Belfast.
    Semaniak, Jacek
    Jan Kochanowski University, Kielce.
    af Ugglas, Magnus
    Stockholm University, Faculty of Science, Department of Physics.
    Källberg, Anders
    Stockholm University, Faculty of Science, Department of Physics.
    Simonsson, Ansgar
    Stockholm University, Faculty of Science, The Manne Siegbahn Laboratory .
    Kaminska, Magdalena
    Jan Kochanowski University.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Dissociative recombination of protonated methanol2006In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 133, p. 177-190Article in journal (Refereed)
    Abstract [en]

    The branching ratios of the different reaction pathways and the overall rate coefficients of the dissociative recombination reactions of CH3OH2+ and CD3OD2+ have been measured at the CRYRING storage ring located in Stockholm, Sweden. Analysis of the data yielded the result that formation of methanol or deuterated methanol accounted for only 3 and 6% of the total rate in CH3OH2+ and CD3OD2+, respectively. Dissociative recombination of both isotopomeres mainly involves fragmentation of the C–O bond, the major process being the three-body break-up forming CH3, OH and H (CD3, OD and D). The overall cross sections are best fitted by s = 1.2 ± 0.1 × 10-15 E-1.15±0.02 cm2 and s = 9.6 ± 0.9 × 10-16 E-1.20±0.02 cm2 for CH3OH2+ and CD3OD2+, respectively. From these values thermal reaction rate coefficients of k(T) = 8.9 ± 0.9 ×10-7 (T/300)-0.59±0.02 cm3 s-1 (CH3OH2+) and k(T) = 9.1 ± 0.9 × 10-7 (T/300)-0.63±0.02 cm3 s-1(CD3OD2+) can be calculated. A non-negligible formation of interstellar methanol by the previously proposed mechanism via radiative association of CH3+ and H2O and subsequent dissociative recombination of the resulting CH3OH2+ ion to yield methanol and hydrogen atoms is therefore very unlikely.

  • 6.
    Lyubartsev, Alexander
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Physical Chemistry.
    Mirzoev, Alexander
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Physical Chemistry.
    Chen, Li Jun
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Physical Chemistry.
    Laaksonen, Aatto
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Physical Chemistry.
    Systematic coarse-graining of molecular models by the Newton inversion method2010In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 144, p. 43-56Article in journal (Refereed)
    Abstract [en]

    Systematic construction of coarse-grained molecular models from detailed atomistic simulations, and even from ab initio simulations is discussed. Atomistic simulations are first performed to extract structural information about the system, which is then used to determine effective potentials for a coarse-grained model of the same system. The statistical-mechanical equations expressing the canonical properties in terms of potential parameters can be inverted and solved numerically according to the iterative Newton scheme. In our previous applications, known as the Inverse Monte Carlo, radial distribution functions were inverted to reconstruct pair potential, while in a more general approach the targets can be other canonical averages. We have considered several examples of coarse-graining; for the united atom water model we suggest an easy way to overcome the known problem of high pressure. Further, we have developed coarse-grained models for L- and D-prolines, dissolved here in an organic solvent (dimethylsulfoxide), keeping their enantiomeric properties from the corresponding all-atom proline model. Finally, we have revisited the previously developed coarse-grained lipid model based on an updated all-atomic force field. We use this model in large-scale meso-scale simulations demonstrating spontaneous formation of different structures, such as vesicles, micelles, and multi-lamellar structures, depending on thermodynamical conditions.

  • 7. Miller, Amy L.
    et al.
    Bowker, Michael
    García-Trenco, Andrés
    Socci, Joseph
    Richards, Nia
    Hutchings, Graham
    Collis, Nicola
    Early, James
    Freakely, Simon
    Burch, Robbie
    Howard, Mark
    Gross, Elad
    Kortaba, Andrzej
    Landau, Miron V.
    Anderson, James
    Weckhuysen, Bert
    Kondrat, Simon
    Naranov, Evgeny
    Douthwaite, John Mark
    Tiruvalam, Ram
    Iqbal, Sarwat
    Parker, Luke
    Shah, Parag
    Nowicka, Ewa
    Ueda, Wataru
    Piovano, Alessandro
    Landon, Philip
    Fischer, Nico
    Reece, Christian
    Gates, Bruce
    Lamb, Michael
    Jackman, Eoin
    Jakubek, Tomasz
    Corma, Avelino
    Claeys, Michael
    Svengren, Henrik
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Friend, Cynthia
    Lennon, David
    Makepeace, Joshua
    Hunter, Hazel
    Manyar, Haresh
    Application of novel catalysts: general discussion2016In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 188, p. 399-426Article in journal (Refereed)
  • 8. Pandis, Spyros N.
    et al.
    Donahue, Neil M.
    Murphy, Benjamin N.
    Riipinen, Ilona
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Fountoukis, Christos
    Karnezi, Eleni
    Patoulias, David
    Skyllakou, Ksakousti
    Introductory lecture: Atmospheric organic aerosols: insights from the combination of measurements and chemical transport models2013In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 165, p. 9-24Article in journal (Refereed)
    Abstract [en]

    The formation, atmospheric evolution, properties, and removal of organic particulate matter remain some of the least understood aspects of atmospheric chemistry despite the importance of organic aerosol (OA) for both human health and climate change. Here, we summarize our recent efforts to deal with the chemical complexity of the tens of thousands of organic compounds in the atmosphere using the volatility-oxygen content framework (often called the 2D-Volatility Basis Set, 2D-VBS). Our current ability to measure the ambient OA concentration as a function of its volatility and oxygen to carbon (O : C) ratio is evaluated. The combination of a thermodenuder, isothermal dilution and Aerosol Mass Spectrometry (AMS) together with a mathematical aerosol dynamics model is a promising approach. The development of computational modules based on the 2D-VBS that can be used in chemical transport models (CTMs) is described. Approaches of different complexity are tested against ambient observations, showing the challenge of simulating the complex chemical evolution of atmospheric OA. The results of the simplest approach describing the net change due to functionalization and fragmentation are quite encouraging, reproducing both the observed OA levels and O : C in a variety of conditions. The same CTM coupled with source-apportionment algorithms can be used to gain insights into the travel distances and age of atmospheric OA. We estimate that the average age of OA near the ground in continental locations is 1-2 days and most of it was emitted (either as precursor vapors or particles) hundreds of kilometers away. Condensation of organic vapors on fresh particles is critical for the growth of these new particles to larger sizes and eventually to cloud condensation nuclei (CCN) sizes. The semivolatile organics currently simulated by CTMs are too volatile to condense on these tiny particles with high curvature. We show that chemical aging reactions converting these semivolatile compounds to extremely low volatility compounds can explain the observed growth rates of new particles in rural environments.

  • 9. Parker, Stewart F.
    et al.
    Amieiro-Fonseca, Alvaro
    Gregory, Duncan
    Noreus, Dag
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Inorganic and Structural Chemistry.
    Yvon, Klaus
    Preface2011In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 151, p. 9-9Article in journal (Refereed)
  • 10. Percival, Carl J.
    et al.
    Welz, Oliver
    Eskola, Arkke J.
    Savee, John D.
    Osborn, David L.
    Topping, David O.
    Lowe, Douglas
    Utembe, Steven R.
    Bacak, Asan
    McFiggans, Gordon
    Cooke, Michael C.
    Xiao, Ping
    Archibald, Alexander T.
    Jenkin, Michael E.
    Derwent, Richard G.
    Riipinen, Ilona
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mok, Daniel W. K.
    Lee, Edmond P. F.
    Dyke, John M.
    Taatjes, Craig A.
    Shallcross, Dudley E.
    Regional and global impacts of Criegee intermediates on atmospheric sulphuric acid concentrations and first steps of aerosol formation2013In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 165, p. 45-73Article in journal (Refereed)
    Abstract [en]

    Carbonyl oxides (Criegee intermediates), formed in the ozonolysis of alkenes, are key species in tropospheric oxidation of organic molecules and their decomposition provides a non-photolytic source of OH in the atmosphere (Johnson and Marston, Chem. Soc. Rev., 2008, 37, 699, Harrison et al., Sci. Total Environ., 2006, 360, 5, Gab et al., Nature, 1985, 316, 535, ref. 1-3). Recently it was shown that small Criegee intermediates, C.I.'s, react far more rapidly with SO2 than typically represented in tropospheric models, (Welz, Science, 2012, 335, 204, ref. 4) which suggested that carbonyl oxides could have a substantial influence on the atmospheric oxidation of SO2. Oxidation of SO2 is the main atmospheric source of sulphuric acid (H2SO4), which is a critical contributor to aerosol formation, although questions remain about the fundamental nucleation mechanism (Sipila et al., Science, 2010, 327, 1243, Metzger et al., Proc. Natl. Acad. Sci. U. S. A., 2010 107, 6646, Kirkby et al., Nature, 2011, 476, 429, ref. 5-7). Non-absorbing atmospheric aerosols, by scattering incoming solar radiation and acting as cloud condensation nuclei, have a cooling effect on climate (Intergovernmental Panel on Climate Change (IPCC), Climate Change 2007: The Physical Science Basis, Cambridge University Press, 2007, ref. 8). Here we explore the effect of the Criegees on atmospheric chemistry, and demonstrate that ozonolysis of alkenes via the reaction of Criegee intermediates potentially has a large impact on atmospheric sulphuric acid concentrations and consequently the first steps in aerosol production. Reactions of Criegee intermediates with SO2 will compete with and in places dominate over the reaction of OH with SO2 (the only other known gas-phase source of H2SO4) in many areas of the Earth's surface. In the case that the products of Criegee intermediate reactions predominantly result in H2SO4 formation, modelled particle nucleation rates can be substantially increased by the improved experimentally obtained estimates of the rate coefficients of Criegee intermediate reactions. Using both regional and global scale modelling, we show that this enhancement is likely to be highly variable spatially with local hot-spots in e. g. urban outflows. This conclusion is however contingent on a number of remaining uncertainties in Criegee intermediate chemistry.

  • 11.
    Siegbahn, Per E. M.
    et al.
    Stockholm University, Faculty of Science, Department of Physics. Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Borowski, Tomasz
    Comparison of QM-only and QM/MM models for the mechanism of tyrosinase2011In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 148, p. 109-117Article in journal (Refereed)
    Abstract [en]

    Two previous studies on the mechanism of tyrosinase have given quite conflicting results. In a QM-only study using a rather small model, a mechanism was suggested in which the tyrosine proton is removed before catalysis. This was followed by catalytic cycles where a superoxo ligand attacks the phenolate ring. In another, more recent study, at the QM/MM level including the entire protein in the model, a quite different mechanism was instead advocated where a bridging O(2)H ligand was homolytically cleaved. That mechanism was rejected in the earlier QM-only study as having a prohibitively large barrier for O-O bond cleavage. In the present study, this discrepancy between the previous studies is investigated by new QM-only and QM/MM calculations.

  • 12.
    Stockett, Mark H.
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Björkhage, Mikael
    Stockholm University, Faculty of Science, Department of Physics.
    Cederquist, Henrik
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Zettergren, Henning
    Stockholm University, Faculty of Science, Department of Physics.
    Storage time dependent photodissociation action spectroscopy of polycyclic aromatic hydrocarbon cations in the cryogenic electrostatic storage ring DESIREE2019In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 217, p. 126-137Article in journal (Refereed)
    Abstract [en]

    The multi-photon photodissociation action spectrum of the coronene cation (C24H12+) has been measured in the cryogenic electrostatic storage ring DESIREE (Double ElectroStatic Ion Ring ExpEriment) as a function of storage time. These measurements reveal not only the intrinsic absorption profile of isolated coronene cations, but also the rate at which hot-band absorptions are quenched by radiative cooling. Just after injection, the action spectrum is severely reddened by hot-band absorptions. These hot bands fade with a time constant of 200 ms, which is consistent with radiative cooling via infrared emission from vibrational transitions. A comparison of the present results to those obtained in cryogenic ion trap experiments is discussed at length.

  • 13.
    Svengren, Henrik
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Torapava, N.
    Athanassiadis, Ioannis
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Ali, S. Imran
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Johnsson, Mats
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    A transition metal oxofluoride offering advantages in electrocatalysis and potential use in applications2016In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 188, p. 481-498Article in journal (Refereed)
    Abstract [en]

    The recently described solid solution ( Co,Ni,Mn)(3)Sb4O6F6 has proved stable and efficient as a catalyst for electrocatalytic water oxidation. The end component Co3Sb4O6F6 was found to be most efficient, maintaining a current density of j = 10 mA cm(-2) at an overpotential of 443 mV with good capability. At this current density, O-2 and H-2 were produced in the ratio 1 : 2 without loss of faradaic current against a Pt-cathode. A morphological change in the crystallite surface was observed after 0.5 h, however, even after 64.5 h, the overall shape and size of the small crystallites were unaffected and the electrolyte contained only 0.02 at% Co. It was also possible to conclude from in situ EXAFS measurements that the coordination around Co did not change. The oxofluorides express both hydrophilic and hydrophobic surface sites, incorporate a flexible metalloid element and offer the possibility of a mechanism that differs from other inorganic catalytic pathways previously described.

  • 14. Yang, Sihai
    et al.
    Callear, Samantha K.
    Ramirez-Cuesta, Anibal J.
    David, William I. F.
    Sun, Junliang
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Inorganic and Structural Chemistry.
    Blake, Alexander J.
    Champness, Neil R.
    Schroeder, Martin
    Pore with gate: modulating hydrogen storage in metal-organic framework materials via cation exchange2011In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 151, p. 19-36Article in journal (Refereed)
    Abstract [en]

    A range of anionic metal-organic framework (MOF) materials has been prepared by combination of In(III) with tetracarboxylate isophthalate-based ligands. These materials incorporate organic cations, either H(2)ppz(2+) (ppz = piperazine) or Me(2)NH(2)(+), that are hydrogen bonded to the pore wall. These cations act as a gate controlling entry of N(2) and H(2) gas into and out of the porous host. Thus, hysteretic adsorption/desorption for N(2) and H(2) is observed in these systems, reflecting the role of the bulky hydrogen bonded organic cations in controlling the kinetic trapping of substrates. Post-synthetic cation exchange with Li(+) leads to removal of the organic cation and the formation of the corresponding Li(+) salts. Replacement of the organic cation with smaller Li(+) leads to an increase in internal surface area and pore volume of the framework material, and in some cases to an increase in the isosteric heat of adsorption of H(2) at zero coverage, as predicted by theoretical modelling. The structures, characterisation and analysis of these charged porous materials as storage portals for H(2) are discussed. Inelastic neutron scattering experiments confirm interaction of H(2) with the carboxylate groups of the isophthalate ligands bound to In(III) centres.

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