X-ray emission spectroscopy of bulk liquid water in no-man's land

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X-ray emission spectroscopy of bulk liquid water in no-man's land

Sellberg, Jonas A. (author): Stockholms universitet,Fysikum,SLAC National Accelerator Laboratory, USA

McQueen, Trevor A. (author)

Laksmono, Hartawan (author)

Schreck, Simon (author)

Beye, Martin (author)

DePonte, Daniel P. (author)

Kennedy, Brian (author): Lund University,Lunds universitet,MAX IV-laboratoriet,MAX IV Laboratory

Nordlund, Dennis (author)

Sierra, Raymond G. (author)

Schlesinger, Daniel (author): Stockholms universitet,Fysikum

Tokushima, Takashi (author)

Zhovtobriukh, Iurii (author): Stockholms universitet,Fysikum

Eckert, Sebastian (author)

Segtnan, Vegard H. (author)

Ogasawara, Hirohito (author)

Kubicek, Katharina (author)

Techert, Simone (author)

Bergmann, Uwe (author)

Dakovski, Georgi L. (author)

Schlotter, William F. (author)

Harada, Yoshihisa (author)

Bogan, Michael J. (author)

Wernet, Philippe (author)

Foehlisch, Alexander (author)

Pettersson, Lars G. M. (author): Stockholms universitet,Fysikum

Nilsson, Anders (author): Stockholms universitet,Fysikum,SLAC National Accelerator Laboratory, USA

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2015-01-28
2015
English.
In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 142:4

Related links:: https://bib-pubdb1.d...; show more...; http://dx.doi.org/10...; https://urn.kb.se/re...; https://doi.org/10.1...; https://lup.lub.lu.s...; show less...

Journal article (peer-reviewed)

Abstract Subject headings

The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (T-H) of similar to 232 K [J. A. Sellberg et al., Nature 510, 381-384 (2014)]. Here, we utilize a similar approach to study the structure of bulk liquid water below T-H using oxygen K-edge x-ray emission spectroscopy (XES). Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387-400 (2008)] at higher temperatures, we expected the ratio of the 1b(1)' and 1b(1) peaks associated with the lone-pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen (H-) bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone-pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more important.

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NATURAL SCIENCES: NATURAL SCIENCES; and Physical Science ...

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...

Articles in the publication: Journal of Chemi ...

By the university: Stockholm University; Lund University

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X-ray emission spectroscopy of bulk liquid water in no-man's land

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