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Surface Sensitive Investigations of the Interaction of Atmospheric Acidic Trace Gases with Ice Surfaces

Applicant Bartels-Rausch Thorsten
Number 149629
Funding scheme Project funding (Div. I-III)
Research institution Paul Scherrer Institut
Institution of higher education Paul Scherrer Institute - PSI
Main discipline Climatology. Atmospherical Chemistry, Aeronomy
Start/End 01.03.2014 - 30.11.2017
Approved amount 243'652.00
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All Disciplines (2)

Discipline
Climatology. Atmospherical Chemistry, Aeronomy
Other disciplines of Physics

Keywords (20)

quasi-liquid layer; premelting; liquid like layer; Synchrotron radiation; snow air partitioning; qll; laboratory study; dissociation of acids; adsorption; ice; snow; Arctic; Polar; Antarctica; Eis; Schnee; Adsorption; Spurengase; Säuren; Kistallstrucktur

Lay Summary (German)

Lead
Chemische Prozesse im Schnee der Polargebiete sind gut untersucht. Feldstudien haben die Freisetzung von Spurengase und Umweltgiften in die Atmosphäre als deren Konsequenz gezeigt. Die grundliegenden Mechanismen dieser Austauschprozesse sind ist hingegen weniger bekannt. Eine offene Frage ist, ob durch die Aufnahme von Spurengasen die Anordnung der Wassermoleküle an der Schneeoberfläche modifiziert wird. Eine solche Rückkopplung könnte die weitere Aufnahme von Spurengasen durch Schnee erhöhen.
Lay summary

Ein vertieftes Verständnis der Rolle des Schnees in der Umwelt ist das Ziel dieses Projektes. Insbesondere wollen wir die Wechselwirkung zwischen Spurengasen in der Atmosphäre und der Oberfläche der Schneekristalle auf der molekularen Ebene aufklären. Wesentlich zum Erreichen dieses Ziels beitragen wird die Verwendung einer neu entwickelten  spektroskopischen Methode an der Synchrotron Lichtquelle Schweiz SLS des Paul Scherrer Instituts. Diese Methode erlaubt direkte Rückschlüsse auf die Anordnung der Dieses Projekt untersucht die fundamentalen Grundlagen der Wechselwirkung von Eis mit Gasen. 

 

Dieses Wissen ist essentiell um Umweltbeobachtungen zu verstehen und um diese in globalen Modellen zu beschreiben. Ähnliche Fragestellungen mit Bezug zu Eis sind nicht nur in den Umweltwissenschaften aktuell, sondern auch in den Materialwissenschaften, Biologie, und Astrophysik.  an Schneekristalloberflächen. Wir zielen darauf ab Änderungen dieser Struktur bei Anwesenheit von Spurengasen zu beobachten, und  zu untersuchen wie diese die Aufnahme der Spurengase beeinflussen. 

 

 

Direct link to Lay Summary Last update: 03.10.2013

Responsible applicant and co-applicants

Employees

Name Institute

Publications

Publication
Disordered Adsorbed Water Layers on TiO 2 Nanoparticles under Subsaturated Humidity Conditions at 235 K
Orlando Fabrizio, Artiglia Luca, Yang Huanyu, Kong Xiangrui, Roy Kanak, Waldner Astrid, Chen Shuzhen, Bartels-Rausch Thorsten, Ammann Markus (2019), Disordered Adsorbed Water Layers on TiO 2 Nanoparticles under Subsaturated Humidity Conditions at 235 K, in The Journal of Physical Chemistry Letters, 10(23), 7433-7438.
Coexistence of Physisorbed and Solvated HCl at Warm Ice Surfaces
Kong Xiangrui, Waldner Astrid, Orlando Fabrizio, Artiglia Luca, Huthwelker Thomas, Ammann Markus, Bartels-Rausch Thorsten (2017), Coexistence of Physisorbed and Solvated HCl at Warm Ice Surfaces, in The Journal of Physical Chemistry Letters, 8(19), 4757-4762.
Experimental Evidence for the Formation of Solvation Shells by Soluble Species at a Nonuniform Air–Ice Interface
Bartels-Rausch Thorsten, Orlando Fabrizio, Kong Xiangrui, Artiglia Luca, Ammann Markus (2017), Experimental Evidence for the Formation of Solvation Shells by Soluble Species at a Nonuniform Air–Ice Interface, in {ACS} Earth and Space Chemistry, 1(9), 572-579.
The Environmental Photochemistry of Oxide Surfaces and the Nature of Frozen Salt Solutions: A New in Situ XPS Approach
Orlando Fabrizio, Waldner Astrid, Bartels-Rausch Thorsten, Birrer Mario, Kato Shunsuke, Lee Ming-Tao, Proff Christian, Huthwelker Thomas, Kleibert Armin, van Bokhoven Jeroen, Ammann Markus (2016), The Environmental Photochemistry of Oxide Surfaces and the Nature of Frozen Salt Solutions: A New in Situ XPS Approach, in Topics in Catalysis, 59(5-7), 591-604.

Collaboration

Group / person Country
Types of collaboration
Hendrik Bluhm/Lawrence Berkeley National Laboratory United States of America (North America)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
SAOG - Swiss Working Group for Surface and Interface Science Talk given at a conference Caught in the act: Interfacial acid base chemistry 31.01.2019 Fribourg, Switzerland Bartels-Rausch Thorsten;
International Global Atmospheric Chemistry Science Meeting Talk given at a conference Caught in the act: Interfacial acid base chemistry 25.09.2018 Takamatsu Kagawa, Japan Bartels-Rausch Thorsten;
Seminar at the Institute of Low Temperature Science Kokkaido University Individual talk Hot acids caught in the act: Interfacial acid base chemistry 21.09.2018 Hokkaido, Japan Bartels-Rausch Thorsten;
European Geoscience Union General Assembly Talk given at a conference Fundamentals of interfacial acid-base chemistry in ice 08.04.2018 Wien, Austria Bartels-Rausch Thorsten;
Swiss Geoscience Meeting Talk given at a conference Fundamentals of Multiphase Chemistry at the surface of environmental Snow 18.11.2017 Davos, Switzerland Waldner Astrid;
Faraday Discussion: Atmospheric Chemistry in the Anthropocene Poster Quasi-liquid ice in the Anthropocene 22.04.2017 York, Great Britain and Northern Ireland Bartels-Rausch Thorsten;
International Global Atmospheric Chemistry (IGAC) workshop: The Cryosphere and ATmospheric CHemistry (CATCH) Poster Hunting liquid micro-pockets and quasi-liquid layers in presence of salt or acidic trace gases with Near Ambient Pressure X-ray core-electron spectroscopy 20.04.2017 Guyancourt, France Bartels-Rausch Thorsten;
American Geophysical Union Fall Meeting Talk given at a conference Hunting liquid micro-pockets and quasi-liquid layers in snow and ice: Melting and Pre-melting of ice in presence of HCl, NaCl, or formic acid as seen by core electron spectroscopy and its implications for chemical reactivity. 12.12.2016 San Fransisco, United States of America Bartels-Rausch Thorsten;
APXPS 2016 - 3rd Annual Workshop on Ambient Pressure X-ray Photoelectron Spectroscopy Talk given at a conference HCl on the ice surface: insights from ambient pressure spectroscopies 12.12.2016 Oxford, Great Britain and Northern Ireland Waldner Astrid;
International Global Atmospheric Chemistry Science Meeting Poster Phase transition in salt solutions at the bulk and interface with core level spectroscopy 26.09.2016 Breckenridge, United States of America Bartels-Rausch Thorsten;
International Global Atmospheric Chemistry Science Meeting Poster Acidic trace gas interaction with ice: XPS and NEXAFS analysis with the new NAPP chamber for solid interfaces at SLS 26.09.2016 Breckenridge, United States of America Waldner Astrid; Bartels-Rausch Thorsten;
European Geosciences Union General Assembly Poster Hunting liquid micro-pockets in snow and ice: Phase transition in salt solutions at the bulk and interface with X-ray photoelectron spectroscopy. 17.04.2016 Wien, Austria Bartels-Rausch Thorsten;
Seminar at the University of Lille Individual talk Atmospheric and Cryospheric Chemistry :: Ice, liquids, and quasi liquids in the lab 21.03.2016 Lille, France Bartels-Rausch Thorsten;
2nd Ambient Pressure X-Ray Photoelectron Spectroscopy Workshop Talk given at a conference Acidic tarce gas interaction with ice: XPS analysis with the new NAPP chamber for solid interfaces at SLS 07.12.2015 Berkeley, United States of America Waldner Astrid;
Swiss Geoscience Meeting Poster The nature of frozen salt solutions: A new in-situ XPS approach 20.11.2015 Basel, Switzerland Bartels-Rausch Thorsten;
European Geoscience Union General Assembly Poster Adsorption and dissociation of acidic trace gases on ice surfaces - Caught in the act with core level spectroscopy 12.04.2015 Wien, Austria Waldner Astrid; Bartels-Rausch Thorsten;
Swiss Global Change Day Poster Interaction of acidic trace gases with ice 01.04.2015 Bern, Switzerland Waldner Astrid;
Fourth workshop of the Air Ice Chemical Interactions (AICI) task Poster Acidic trace gas adsorption on ice: XPS and NEXAFS analysis with the new napp solid chamber at SLS 13.10.2014 Cambridge, Great Britain and Northern Ireland Bartels-Rausch Thorsten; Waldner Astrid;
The European Network, Atmospheric composition change Summer School Poster Molecular picture of acids adsorbed at ice surfaces - surface sensitive near ambient pressure photoemission spectroscopy at SLS 22.06.2014 Urbino, Italy Waldner Astrid;


Self-organised

Title Date Place
Fourth workshop of the Air Ice Chemical Interactions (AICI) task 13.10.2014 Cambridge, Great Britain and Northern Ireland

Associated projects

Number Title Start Funding scheme
178962 Interfacial Chemistry of Ice: Photolysis and Acid-Base Equilibria in the QLL and Brine 01.08.2018 Project funding (Div. I-III)
121857 The uptake of peroxynitric acid on ice surfaces: The role of grain boundaries and of dissociation 01.06.2009 Project funding (Div. I-III)
169176 Multiphase kinetics and chemistry at aqueous solution and mineral oxide - air interfaces 01.01.2017 Project funding (Div. I-III)
140400 The uptake of peroxynitric acid on ice surfaces: The role of grain boundaries and of dissociation 01.06.2012 Project funding (Div. I-III)
155999 The impact of the physical micro-environment of impurities in snow on their re-distribution during metamorphism, chemical reactivity, and transfer to ice core archives. 01.05.2015 Project funding (Div. I-III)
139139 Near ambient pressure photoelectron spectroscopy for environmental and catalysis research 01.12.2011 R'EQUIP

Abstract

Chemistry and physical processes in Earth's ice and snow cover can change the composition of the atmosphere and the contaminant content of the snow. It has thus direct impacts on geochemical cycles and the climate system. Our ability to predict the fate of chemicals in snow or air masses in exchange with snow or ice on a regional scale or to model those in snow chemistry models is currently hampered by our limited understanding of the underlying processes on a molecular level. This project aims at investigating how atmospheric trace gases interact with ice surfaces upon adsorption. This interaction is the initial (final) step in exchange processes between surface snow or ice clouds with the surrounding air and also of fundamental importance to understand how dopants can modify the structure of the water molecule network that form the ice crystal. It has been proposed that dopants can lead to a disorder in the structure at the air-ice interface and that this disordered region represents a reservoir to which large amounts of trace gases can be dissolved and in which chemistry is rapidly occurring. The ability to disorder the ice surface would thus represent a significant feedback mechanism by which the uptake of trace gases is enhanced. We hypothesise a more complex picture of this interaction of trace gases with ice, where they form a hydration shell in their vicinity. At low concentration this may not necessarily lead to a widespread disorder of the whole ice surface. The impact of this locally constrained disorder on the ice crystal is essentially open. The unique approach of the proposed research to test this hypotheses is to combine two surface sensitive spectroscopic methods to directly probe the hydrogen-bonding network at the ice surface ( ~1 nm depth) and the concentration, depth profile (~1 to 10 nm), and dissociation degree of the dopant. This will allow relating the extent of surface disorder on the neat ice surface with the amount and mobility of acids taken up from the gas-phase on the same set-up and ice sample. Use of our new near-ambient pressure photoelectron spectroscopy end station (NAPP) will allow performing experiments on ice at temperature close to the melting point. The endstation is also designed for optimal use of sticky, highly acidic trace gases such as HCl that have a high environmental importance. The results will be supported by more classical experiments such as IR spectroscopy and kinetic experiments in coated wall flow tubes. Even with the focus on adsorption of acidic trace gases (HCl, HNO3, formic acid) to ice, results of this study will be of high relevance also for other chemical processes in ice and snow as we expect them to reveal fundamental aspects of the ice surface and how it interacts with dopants. This is of interest not only in environmental science but also in material science, cryobiology, and astrophysics.
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