Prize Talk: Earle K. Plyler Prize for Molecular Spectroscopy & Dynamics. Talk Title: X-ray laser probing of ultrafast surface catalysis and the anomalous properties of water

ORAL · Invited

Abstract

I will demonstrate how x-ray lasers, such as LCLS at the SLAC National Accelerator Laboratory and PAL in Korea, are used to address basic scientific questions in chemical Physics. The first example will illustrate that we can observe surface catalytic reactions in real time using optical pump- x-ray-probe techniques. It has allowed for the detection of transient reaction intermediates in CO desrorption and for probing configurations close to the transition state during CO oxidation both on Ruthenium.

The second example will illustrate how it is now possible to probe water in the deep supercooled regime, where ice crystallization occurs rapidly. Using x-ray laser scattering on ultrafast timescales important features in the behavior of supercooled water could be revealed related to the existence of a liquid-liquid transition around 200 K and 1-2 kbar, and that the thermodynamic response function shows maxima at 230 K and 1 bar. Both observations are only consistent with the existence of a liquid-liquid critical point in deep supercooled water. Such a critical point cause fluctuations extending all the way up to ambient conditions and thereby points to the origin of waters anomalous properties.

* This research has been supported by the the Swedish Research Council under Grant No 2013-8823, Knut and Alice Wallenberg Foundation under Grant No 2016.0042, the European Research Council (ERC) Advanced Grant under Project No. 667205 and the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program to the Ultrafast Catalysis FWP 100435 at SLAC National Accelerator Laboratory under Contract DE-AC02-76SF00515.

Publication: (1) Liquid-liquid Phase Separation in Supercooled Water from Ultrafast Heating of Low Density Amorphous Ice
K. Amann-Winkel, K. H. Kim, N. Giovambattista, M. L. Parada,, A. Späh, F. Perakis, H. Pathak, C Yang, D. Mariedahl, T. Eklund, T. J. Lane, S. You, S. Jeong, M. Weston, J. H. Lee, I. Eom, M. Kim, J. Park, S. H. Chun, P. H. Poole and A. Nilsson
Nature Comm. 14, 442 (2023).
(2) Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time Resolved X-ray Spectroscopy
S. Schreck, E. Diesen, M. Dell'Angela, C. Liu, M. Weston, F. Capotondi, H. Ogasawara, J. LaRue, R. Costantini, M. Beye, P. S. Miedema, J. H. Halldin, J. Gladh, B. Liu, H-Y. Wang, F. Perakis, F. Cavalca, S. Koroidov, P. Amann, E. Pedersoli, D. Naumenko, I. Nikolov, L. Raimondi, F. Abild-Pedersen, T. F. Heinz, J. Voss, A. C. Luntz, A. Nilsson
Phys. Rev. Lett. 129, 276001 (2022).
(3) Experimental Observation of the Liquid-Liquid Transition in Bulk Supercooled Water under Pressure
K. H. Kim, K. Amann-Winkel, N. Giovambattista, A. Späh, F. Perakis, H. Pathak, M. L. Parada, C Yang, D. Mariedahl, T. Eklund, T. J. Lane, S. You, S. Jeong, M. Weston, J. H. Lee, I. Eom, M. Kim, J. Park, S. H. Chun, P. H. Poole and A. Nilsson
Science 370, 978 (2020).
(4) Maxima in the Thermodynamic Response and Correlation Functions of Deeply Supercooled Water
K. H. Kim, A. Späh, H. Pathak, F. Perakis, D. Mariedahl, K. Amann-Winkel, J. A. Sellberg, J. H. Lee, S. Kim, J. Park, K. H. Nam, T. Katayama and A. Nilsson
Science 358, 1589 (2017).
(5) Probing the Transition State Region in Catalytic CO Oxidation on Ru
H. Öström, H. Öberg, H. Xin, J. LaRue, M. Beye, M. Dell'Angela, J. Gladh, M. L. Ng, J. A. Sellberg, S. Kaya, G. Mercurio, D. Nordlund, M. Hantschmann, F. Hieke, D. Kühn, W. F. Schlotter, G. L. Dakovski, J. J. Turner, M. P. Minitti, A. Mitra, S. P. Moeller, A. Föhlisch, M. Wolf, W. Wurth, M. Persson, J. K. Nørskov, F. Abild-Pedersen, H. Ogasawara, L. G. M Pettersson, A. Nilsson
Science 347, 978 (2015).
(6) Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature
J. A. Sellberg, C. Huang, T. A. McQueen, N. D. Loh, H. Laksmono, D. Schlesinger, R. G. Sierra, D. Nordlund, C. Y. Hampton, D. Starodub, D. P. DePonte, M. Beye, C. Chen, A. V. Martin, A. Barty, K. T. Wikfeldt, T. M. Weiss, C. Caronna, J. Feldkamp, L. B. Skinner, M. M. Seibert, M. Messerschmidt, G. J.Williams, S. Boutet, L. G. M. Pettersson, M. J. Bogan and A. Nilsson
Nature 510, 381 (2014).
(10) Real-Time Observation of Surface Bond Breaking with an X-ray Laser
M. Dell'Angela, T. Anniyev, M. Beye, R. Coffee, A. Föhlisch, J. Gladh, T. Katayama, S. Kaya, O. Krupin, A. Møgelhøj, D. Nordlund, J. K. Nørskov, H. Öberg, H. Ogasawara, H. Öström, L. G. M. Pettersson, W. F. Schlotter, J. A. Sellberg, F. Sorgenfrei, J. Turner, M. Wolf, W. Wurth, A. Nilsson
Science 339, 1302 (2013).

Presenters

  • Anders R Nilsson

    Stockholm University

Authors

  • Anders R Nilsson

    Stockholm University