Vibrational resonant inelastic X-ray scattering in liquid acetic acid: a ruler for molecular chain lengths

Viktoriia Savchenko; Iulia Emilia Brumboiu; Victor Kimberg; Michael Odelius; Pavel Krasnov; Ji-Cai Liu; Jan-Erik Rubensson; Olle Björneholm; Conny Såthe; Johan Gråsjö; Minjie Dong; Annette Pietzsch; Alexander Föhlisch; Thorsten Schmitt; Daniel McNally; Xingye Lu; Sergey P Polyutov; Patrick Norman; Marcella Iannuzzi; Faris Gel'mukhanov; Victor Ekholm

doi:10.1038/s41598-021-83248-3

Vibrational resonant inelastic X-ray scattering in liquid acetic acid: a ruler for molecular chain lengths

Sci Rep. 2021 Feb 18;11(1):4098. doi: 10.1038/s41598-021-83248-3.

Authors

Viktoriia Savchenko^{1

2

3}, Iulia Emilia Brumboiu^{4

5}, Victor Kimberg^{6

7

8}, Michael Odelius⁹, Pavel Krasnov^{10

11}, Ji-Cai Liu¹², Jan-Erik Rubensson¹³, Olle Björneholm¹³, Conny Såthe¹⁴, Johan Gråsjö^{13

15}, Minjie Dong¹³, Annette Pietzsch¹⁶, Alexander Föhlisch^{16

17}, Thorsten Schmitt¹⁸, Daniel McNally¹⁸, Xingye Lu¹⁸, Sergey P Polyutov^{10

11}, Patrick Norman⁴, Marcella Iannuzzi¹⁹, Faris Gel'mukhanov^{4

10

11}, Victor Ekholm^{13

14}

Affiliations

¹ Department of Theoretical Chemistry and Biology, KTH Royal Institute of Technology, 10691, Stockholm, Sweden. [email protected].
² International Research Center of Spectroscopy and Quantum Chemistry-IRC SQC, Siberian Federal University, Krasnoyarsk, Russia, 660041. [email protected].
³ Kirensky Institute of Physics, Federal Research Center KSC SB RAS, Krasnoyarsk, Russia, 660036. [email protected].
⁴ Department of Theoretical Chemistry and Biology, KTH Royal Institute of Technology, 10691, Stockholm, Sweden.
⁵ Department of Chemistry, Korea Advanced Institute of Science and Technology, Daejeon, 34141, Korea.
⁶ Department of Theoretical Chemistry and Biology, KTH Royal Institute of Technology, 10691, Stockholm, Sweden. [email protected].
⁷ International Research Center of Spectroscopy and Quantum Chemistry-IRC SQC, Siberian Federal University, Krasnoyarsk, Russia, 660041. [email protected].
⁸ Kirensky Institute of Physics, Federal Research Center KSC SB RAS, Krasnoyarsk, Russia, 660036. [email protected].
⁹ Department of Physics, AlbaNova University Center, Stockholm University, 106 91, Stockholm, Sweden. [email protected].
¹⁰ International Research Center of Spectroscopy and Quantum Chemistry-IRC SQC, Siberian Federal University, Krasnoyarsk, Russia, 660041.
¹¹ Kirensky Institute of Physics, Federal Research Center KSC SB RAS, Krasnoyarsk, Russia, 660036.
¹² Department of Mathematics and Physics, North China Electric Power University, Beijing, 102206, China.
¹³ Department of Physics and Astronomy, Uppsala University, Box 516, 751 20, Uppsala, Sweden.
¹⁴ MAX IV Laboratory, Lund University, Box 118, 221 00, Lund, Sweden.
¹⁵ Department of Medicinal Chemistry, Uppsala University, Box 574, 75123, Uppsala, Sweden.
¹⁶ Institute for Methods and Instrumentation in Synchrotron Radiation Research FG-ISRR, Helmholtz-Zentrum Berlin für Materialien und Energie Albert-Einstein-Strasse 15, Berlin, 12489, Germany.
¹⁷ Institut für Physik und Astronomie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, 14476, Potsdam, Germany.
¹⁸ Swiss Light Source, Photon Science Division, Paul Scherrer Institut, 5232, Villigen PSI, Switzerland.
¹⁹ Physical Chemistry Institute, University of Zürich, 8057, Zurich, Switzerland.

Abstract

Quenching of vibrational excitations in resonant inelastic X-ray scattering (RIXS) spectra of liquid acetic acid is observed. At the oxygen core resonance associated with localized excitations at the O-H bond, the spectra lack the typical progression of vibrational excitations observed in RIXS spectra of comparable systems. We interpret this phenomenon as due to strong rehybridization of the unoccupied molecular orbitals as a result of hydrogen bonding, which however cannot be observed in x-ray absorption but only by means of RIXS. This allows us to address the molecular structure of the liquid, and to determine a lower limit for the average molecular chain length.

Publication types

Research Support, Non-U.S. Gov't