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Atmospheric Surface Science

Investigating atmospheric interactions on the molecular level using nonlinear optical spectroscopy
ASS_EGU2018

⇒ Our Session in the EGU General Assembly: AS3.2 - Atmospheric Surface Science. Links: 2018 , 2019

 

Introduction

Atmospheric Surface Science is a new research line has been set out in IMKAAF after three successful grants:

  1. Start-Up-Budget (STUB 2012) in 2012 from the competence field Earth and Environment, KIT for “building a supercooled SHG system and performing a feasibility study on water/ice-nucleation-agent interface”.
  2. Research grant (DFG, AB 604/1-1) in 2014 from the German Research Foundation (DFG) to study “Elementary processes of heterogeneous ice nucleation observed by nonlinear optical spectroscopy”.
  3. Research grant (DFG, AB 604/1-2) in 2017 from DFG to proceed with advanced studies on “Elementary processes of heterogeneous ice nucleation observed by nonlinear optical spectroscopy: The role of hydroxyl groups on the surfaces of mineral aerosol particles”

The aim of this research is to investigate atmospheric interactions on the molecular level.

 

Scientific Background

Studying atmospheric aerosol-cloud-climate interactions (e.g. heterogeneous ice nucleation) is important for understanding our climate system. For example, despite all investigations on particle size and surface properties of IN agents upon nucleation efficiency, no clear statement is given about ice nucleation process. Technical and environmental issues require a good understanding of water freezing on the surfaces of ice-nucleating agents, particularly on the molecular level. On a molecular level, ice nucleation by a surface remains poorly understood. The microscopic mechanisms of heterogeneous ice nucleation and the characteristics that make some surfaces more effective for ice nucleation are still unclear. It is believed that good ice-nucleating surfaces are those which can reduce the free energy barrier for nucleation and/or template water in ice-like structure. However, some experiments showed that it is not always the case. Additionaly, aging of aerosoles particles in atmospher under different temperature, humidity, acidity and basicity changes their optical and chemical properties.

 

Objectives

The scientific goal in general is to provide a clear picture on aerosol-water and -ice interactions under atmospheric conditions. One of the interests is to draw a sharp line between water and ice molecular properties during heterogeneous ice nucleation processes. This requires information about the abundance and degree of order of water molecules at the water and ice surfaces at different supersaturation conditions. For instance, a complete picture about the world wide puzzling ice nucleation process requires an access to a wide range of molecular vibrations. Probing the individual vibrational bands of water and ice vibrations as well as the molecular vibrations of ice-nucleating agents is part of thie work.

 

Research and methodology

Bulk techniques, like FTIR, cannot recognize the contribution of the surface molecules due to their infinitesimal contribution to the overall detectable signal. However, second order nonlinear optical techniques can do. Second Harmonic Generation (SHG), as well as Sum Frequency Generation (SFG), is highly sensitive optical probe of surfaces and interfaces. A brand new Femtosecond laser system (Solstice, 800nm, 3.5mJ, 80fs) is available at the IMK-AAF and is utilized in this work. A supercooled SHG setup is build in total-internal-reflection (TIR) geometry to probe the abundance and degree of order of water molecules on the surface of ice-nucleating agents before, during and after the phase change. A precise temperature-controlled bidirectional optically-accessible cold stage is coupled to the system for this purpose. A complete picture about the world wide puzzling ice nucleation processes requires an access to a wide range of molecular vibrations. Probing the individual vibrational bands of water-like and ice-like vibrations as well as the molecular vibrations of ice-nucleating agents is a challenge. In a future step, the supercooled SHG setup will be upgraded to supercooled SFG to describe this system physically and chemically simultaneously.

Preliminary Results                  

 

 

For further information please contact Dr. Ahmed Abdelmonem

 

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Related publications:

  • Abdelmonem, A.; Backus, E. H. G.; Bonn, M. Ice Nucleation at the Water-Sapphire Interface: Transient Sum Frequency Response without Evidence for Transient Ice Phase. The Journal of Physical Chemistry C 2018, DOI: 10.1021/acs.jpcc.8b07480.
  • Abdelmonem, A.; Wang, Y.; Lützenkirchen, J.; Alves, M. E., Calcium uptake on kaolinite, gibbsite: effects of sulfate, pH, and salt concentration with additional insight from second harmonic generation on temperature dependencies with sapphire basal planes and the potential relevance to ice nucleation. 2018, InTech (submitted, accepted, 2018).
  • Lützenkirchen, J., Scharnweber, T., Ho, T.; Striolo, A., Sulpizi, M., and Abdelmonem, A.* A set-up for simultaneous measurement of second harmonic generation and streaming potential and some test applications. Journal of Colloid and Interface Science 2018, 529, 294-305. DOI: https://doi.org/10.1016/j.jcis.2018.06.017. (Free access until August 04, 2018 on ScienceDirect under: https://authors.elsevier.com/a/1XDtM4-sDJKjZ)
  • Abdelmonem, A.: Direct molecular-level characterization of different heterogeneous freezing modes on mica – Part 1, Atmos. Chem. Phys., 17, 10733-10741, doi: 10.5194/acp-17-10733-2017, 2017.
  • Abdelmonem, A., Backus, E. H. G., Hoffmann, N., Sánchez, M. A., Cyran, J. D., Kiselev, A., and Bonn, M.: Surface-charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001), Atmos. Chem. Phys., 17, 7827-7837, doi: 10.5194/acp-17-7827-2017, 2017.
  • Preocanin, T., Abdelmonem, A., Montavon, G., and Luetzenkirchen, J.: Charging Behavior of Clays and Clay Minerals in Aqueous Electrolyte Solutions — Experimental Methods for Measuring the Charge and Interpreting the Results, in: Clays, Clay Minerals and Ceramic Materials Based on Clay Minerals, edited by: Nascimento, G. M. D., InTech, 51-88, 2016.
  • Abdelmonem, A., Lützenkirchen, J., and Leisner, T.: Probing ice-nucleation processes on the molecular level using second harmonic generation spectroscopy, Atmos. Meas. Tech., 8, 3519-3526, doi: 10.5194/amt-8-3519-2015, 2015.