Time-resolved photoelectron spectroscopy of solvated systems

 
    Dr. Matthew Brown

ETH Zürich
LPC / D-CHAB
HCI G217
CH-8093 Zürich

www.surfacescience.eth.ch
+41 44 632 3048
 
Project start   10.12.2011 
Project end   30.11.2014
     
Goal for 2014   The photoionization dynamics of liquid water will be measured with attosecond temporal resolution using the RABBIT technique. These measurements will be repeated using the attosecond streak camera and will be extended to measure the photoionization dynamics of solvated systems.
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Goals   The main goal of this project is the development of time-resolved photoelectron spectroscopy of solvated systems. Our initial target will be water itself with the goal of resolving the photoionization dynamics on an attosecond time scale and comparing the dynamics with gas-phase water. These studies will be extended to various solvated systems such as molecules, transition metal complexes and nanoparticles. In combination with a recently completed time-preserving monochromator for high-harmonic radiation, we will be able to investigate the mechanisms of electronic excitation and electronic dynamics in solvated systems, which have eluded previous investigations because of their extreme time scale. This insight may contribute to the design of more efficient catalysts or the understanding of biological processes.
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Contact  
Inga Jordan
LPC / D-CHAB HCI E214
+41 44 633 49 78
Laboratory for physical chemistry, ETH-Hönggerberg,
Wolfgang-Pauli-Str. 10,
8093 Zurich
 
Matthew Brown
ICB HCI G101
+41 44 632 30 48
Institute of Chemical and Bioengineering,

ETH-Hönggerberg,
Wolfgang-Pauli-Str. 10,
8093 Zurich

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Jeroen van Bokhoven
ICB
HCI E 127
+41 44 632 55 42
Institute of Chemical and Bioengineering,
ETH-Hönggerberg,
Wolfgang-Pauli-Str. 10,
8093 Zurich
 
 
Abstract    We have developed a new experimental setup combining a liquid microjet in high vacuum with an extreme-ultraviolet (XUV) laser source for time-resolved photoelectron studies of solvated systems. The XUV radiation is produced through high-harmonic generation and yields pulses with femtosecond to attosecond durations. The liquid microjet technique allows to bridge the pressure gap between ultrahigh-vacuum surface science and ambient pressure chemistry and thereby expands the scope of photoelectron spectroscopic investigations to the liquid phase.
We will study electronic dynamics in metal complexes, nanoparticles and biologically relevant molecules. In the first phase of the project, we will couple the new spectrometer to an innovative, actively stabilized interferometer to perform infrared / XUV pump-probe experiments with attosecond resolution. In the second phase, we will investigate the femtosecond dynamics following excitation of a solvated sample by an ultraviolet pump pulse.
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Publications   Brown, M.A., Duyckaerts, N., Redondo, A.B., Jordan, I., Nolting, F., Kleibert, A., Ammann, M., Wörner, H.J., van Bokhoven, J.A., and Abbas, Z. (2013a) Effect of Surface Charge Density on the Affinity of Oxide Nanoparticles for the Vapor-Water Interface. Langmuir 29, 5023-5029 (10.1021/la4005054) Brown-2013b (1.06 MB)

Brown, M.A., Jordan, I., Redondo, A.B., Kleibert, A., Woerner, H.J., and van Bokhoven, J.A. (2013b) In situ photoelectron spectroscopy at the liquid/nanoparticle interface. Surf Sci 610, 1-6 (10.1016/j.susc.2013.01.012) Brown-2013c (823 KB)

Brown, M.A., Redondo, A.B., Jordan, I., Duyckaerts, N., Lee, M.T., Ammann, M., Nolting, F., Kleibert, A., Huthwelker, T., Machler, J.P., Birrer, M., Honegger, J., Wetter, R., Wörner, H.J., and van Bokhoven, J.A. (2013c) A new endstation at the Swiss Light Source for ultraviolet photoelectron spectroscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy measurements of liquid solutions. Rev Sci Instrum 84,  073904 (10.1063/1.4812786) Brown-2013a (2.14 MB).

Jordan, I., Redondo, A.B., Brown, M.A., Fodor, D., Staniuk, M., Kleibert, A., Worner, H.J., Giorgi, J.B., and van Bokhoven, J.A. (2014) Non-uniform spatial distribution of tin oxide (SnO2) nanoparticles at the air-water interface. Chem Commun 50, 4242-4244 (10.1039/c4cc00720d) Jordan-2014 (1.25 MB).

Beloqui Redondo, A., Jordan, I., Ziazadeh, I., Kleibert, Giorgi, J.B., Wörner, H.J., May, S., Abbas, Z., and Brown, M.A. (2015) Nanoparticle-Induced Charge Redistribution of the Air–Water Interface. J Phys Chem C 119,  2661-2668 (10.1021/jp511915b) Beloqui-2015 (2.45 MB).


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