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Direct observation of the collapse of the delocalized excess electron in water

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Direct observation of the collapse of the delocalized excess electron in water. / Savolainen, Janne; Uhlig, Frank; Ahmed, Saima; Hamm, Peter; Jungwirth, Pavel.

In: Nature Chemistry, Vol. 6, No. 8, 2014, p. 697-701.

Research output: Contribution to journalArticleScientificpeer-review

Harvard

Savolainen, J, Uhlig, F, Ahmed, S, Hamm, P & Jungwirth, P 2014, 'Direct observation of the collapse of the delocalized excess electron in water', Nature Chemistry, vol. 6, no. 8, pp. 697-701. https://doi.org/10.1038/nchem.1995

APA

Savolainen, J., Uhlig, F., Ahmed, S., Hamm, P., & Jungwirth, P. (2014). Direct observation of the collapse of the delocalized excess electron in water. Nature Chemistry, 6(8), 697-701. https://doi.org/10.1038/nchem.1995

Vancouver

Savolainen J, Uhlig F, Ahmed S, Hamm P, Jungwirth P. Direct observation of the collapse of the delocalized excess electron in water. Nature Chemistry. 2014;6(8):697-701. https://doi.org/10.1038/nchem.1995

Author

Savolainen, Janne ; Uhlig, Frank ; Ahmed, Saima ; Hamm, Peter ; Jungwirth, Pavel. / Direct observation of the collapse of the delocalized excess electron in water. In: Nature Chemistry. 2014 ; Vol. 6, No. 8. pp. 697-701.

Bibtex - Download

@article{d417633818ab48eabfe90430cc4d6268,
title = "Direct observation of the collapse of the delocalized excess electron in water",
abstract = "It is generally assumed that the hydrated electron occupies a quasi-spherical cavity surrounded by only a few water molecules in its equilibrated state. However, in the very moment of its generation, before water has had time to respond to the extra charge, it is expected to be significantly larger in size. According to a particle-in-a-box picture, the frequency of its absorption spectrum is a sensitive measure of the initial size of the electronic wavefunction. Here, using transient terahertz spectroscopy, we show that the excess electron initially absorbs in the far-infrared at a frequency for which accompanying ab initio molecular dynamics simulations estimate an initial delocalization length of ≈40 {\AA}. The electron subsequently shrinks due to solvation and thereby leaves the terahertz observation window very quickly, within ≈200 fs.",
author = "Janne Savolainen and Frank Uhlig and Saima Ahmed and Peter Hamm and Pavel Jungwirth",
year = "2014",
doi = "10.1038/nchem.1995",
language = "English",
volume = "6",
pages = "697--701",
journal = "Nature Chemistry",
issn = "1755-4330",
publisher = "Nature Publishing Group",
number = "8",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Direct observation of the collapse of the delocalized excess electron in water

AU - Savolainen, Janne

AU - Uhlig, Frank

AU - Ahmed, Saima

AU - Hamm, Peter

AU - Jungwirth, Pavel

PY - 2014

Y1 - 2014

N2 - It is generally assumed that the hydrated electron occupies a quasi-spherical cavity surrounded by only a few water molecules in its equilibrated state. However, in the very moment of its generation, before water has had time to respond to the extra charge, it is expected to be significantly larger in size. According to a particle-in-a-box picture, the frequency of its absorption spectrum is a sensitive measure of the initial size of the electronic wavefunction. Here, using transient terahertz spectroscopy, we show that the excess electron initially absorbs in the far-infrared at a frequency for which accompanying ab initio molecular dynamics simulations estimate an initial delocalization length of ≈40 Å. The electron subsequently shrinks due to solvation and thereby leaves the terahertz observation window very quickly, within ≈200 fs.

AB - It is generally assumed that the hydrated electron occupies a quasi-spherical cavity surrounded by only a few water molecules in its equilibrated state. However, in the very moment of its generation, before water has had time to respond to the extra charge, it is expected to be significantly larger in size. According to a particle-in-a-box picture, the frequency of its absorption spectrum is a sensitive measure of the initial size of the electronic wavefunction. Here, using transient terahertz spectroscopy, we show that the excess electron initially absorbs in the far-infrared at a frequency for which accompanying ab initio molecular dynamics simulations estimate an initial delocalization length of ≈40 Å. The electron subsequently shrinks due to solvation and thereby leaves the terahertz observation window very quickly, within ≈200 fs.

UR - http://www.scopus.com/inward/record.url?scp=84904805160&partnerID=8YFLogxK

U2 - 10.1038/nchem.1995

DO - 10.1038/nchem.1995

M3 - Article

VL - 6

SP - 697

EP - 701

JO - Nature Chemistry

JF - Nature Chemistry

SN - 1755-4330

IS - 8

ER -