Direct observation of ultrafast hydrogen bond strengthening in liquid water

Jie Yang^{1

2

3}, Riccardo Dettori⁴, J Pedro F Nunes⁵, Nanna H List^{6

7

8}, Elisa Biasin^{6

7}, Martin Centurion⁵, Zhijiang Chen⁶, Amy A Cordones⁷, Daniel P Deponte⁶, Tony F Heinz^{7

9}, Michael E Kozina^{6

7}, Kathryn Ledbetter^{7

10}, Ming-Fu Lin⁶, Aaron M Lindenberg^{7

11

12}, Mianzhen Mo⁶, Anders Nilsson¹³, Xiaozhe Shen⁶, Thomas J A Wolf^{6

7}, Davide Donadio¹⁴, Kelly J Gaffney¹⁵, Todd J Martinez^{16

17

18}, Xijie Wang¹⁹

Affiliations

¹ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang1@tsinghua.edu.cn.
² Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang1@tsinghua.edu.cn.
³ Center of Basic Molecular Science, Department of Chemistry, Tsinghua University, Beijing, China. jieyang1@tsinghua.edu.cn.
⁴ Department of Chemistry, University of California-Davis, Davis, CA, USA.
⁵ Department of Physics, University of Nebraska-Lincoln, Lincoln, NE, USA.
⁶ SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁷ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁸ Department of Chemistry, Stanford University, Stanford, CA, USA.
⁹ Department of Applied Physics, Stanford University, Stanford, CA, USA.
¹⁰ Department of Physics, Stanford University, Stanford, CA, USA.
¹¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
¹² Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹³ Department of Physics, AlbaNova University Center, Stockholm University, Stockholm, Sweden.
¹⁴ Department of Chemistry, University of California-Davis, Davis, CA, USA. ddonadio@ucdavis.edu.
¹⁵ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. kgaffney@slac.stanford.edu.
¹⁶ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. todd.martinez@stanford.edu.
¹⁷ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. todd.martinez@stanford.edu.
¹⁸ Department of Chemistry, Stanford University, Stanford, CA, USA. todd.martinez@stanford.edu.
¹⁹ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. wangxj@slac.stanford.edu.

PMID: 34433948
DOI: 10.1038/s41586-021-03793-9

Free article

Direct observation of ultrafast hydrogen bond strengthening in liquid water

Jie Yang et al. Nature. 2021 Aug.

Free article

. 2021 Aug;596(7873):531-535.

doi: 10.1038/s41586-021-03793-9. Epub 2021 Aug 25.

Authors

Affiliations

¹ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang1@tsinghua.edu.cn.
² Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang1@tsinghua.edu.cn.
³ Center of Basic Molecular Science, Department of Chemistry, Tsinghua University, Beijing, China. jieyang1@tsinghua.edu.cn.
⁴ Department of Chemistry, University of California-Davis, Davis, CA, USA.
⁵ Department of Physics, University of Nebraska-Lincoln, Lincoln, NE, USA.
⁶ SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁷ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁸ Department of Chemistry, Stanford University, Stanford, CA, USA.
⁹ Department of Applied Physics, Stanford University, Stanford, CA, USA.
¹⁰ Department of Physics, Stanford University, Stanford, CA, USA.
¹¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
¹² Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹³ Department of Physics, AlbaNova University Center, Stockholm University, Stockholm, Sweden.
¹⁴ Department of Chemistry, University of California-Davis, Davis, CA, USA. ddonadio@ucdavis.edu.
¹⁵ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. kgaffney@slac.stanford.edu.
¹⁶ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. todd.martinez@stanford.edu.
¹⁷ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. todd.martinez@stanford.edu.
¹⁸ Department of Chemistry, Stanford University, Stanford, CA, USA. todd.martinez@stanford.edu.
¹⁹ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. wangxj@slac.stanford.edu.

PMID: 34433948
DOI: 10.1038/s41586-021-03793-9

Abstract

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network¹, including unusually efficient vibrational energy redistribution and relaxation². An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments^2-7. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

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References

1. Stillinger, F. H. Water revisited. Science 209, 451–457 (1980). - PubMed - DOI
1. Perakis, F. et al. Vibrational spectroscopy and dynamics of water. Chem. Rev. 116, 7590–7607 (2016). - PubMed - DOI
1. Lindner, J. et al. Vibrational relaxation of pure liquid water. Chem. Phys. Lett. 421, 329–333 (2006). - DOI
1. Ramasesha, K., De Marco, L., Mandal, A. & Tokmakoff, A. Water vibrations have strongly mixed intra- and intermolecular character. Nat. Chem. 5, 935–940 (2013). - PubMed - DOI
1. Bakker, H. J. et al. Transient absorption of vibrationally excited water. J. Chem. Phys. 116, 2592–2598 (2002). - DOI

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Direct observation of ultrafast hydrogen bond strengthening in liquid water

Affiliations

Direct observation of ultrafast hydrogen bond strengthening in liquid water

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Abstract

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