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Statements

Subject Item
n2:RIV%2F61388963%3A_____%2F14%3A00432523%21RIV15-GA0-61388963
rdf:type
skos:Concept n13:Vysledek
dcterms:description
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 approximate to 40 angstrom. The electron subsequently shrinks due to solvation and thereby leaves the terahertz observation window very quickly, within approximate to 200 fs. 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 approximate to 40 angstrom. The electron subsequently shrinks due to solvation and thereby leaves the terahertz observation window very quickly, within approximate to 200 fs.
dcterms:title
Direct observation of the collapse of the delocalized excess electron in water Direct observation of the collapse of the delocalized excess electron in water
skos:prefLabel
Direct observation of the collapse of the delocalized excess electron in water Direct observation of the collapse of the delocalized excess electron in water
skos:notation
RIV/61388963:_____/14:00432523!RIV15-GA0-61388963
n4:aktivita
n5:P n5:I
n4:aktivity
I, P(GBP208/12/G016)
n4:cisloPeriodika
8
n4:dodaniDat
n15:2015
n4:domaciTvurceVysledku
n14:2793911 Uhlig, Frank
n4:druhVysledku
n6:J
n4:duvernostUdaju
n9:S
n4:entitaPredkladatele
n18:predkladatel
n4:idSjednocenehoVysledku
11648
n4:idVysledku
RIV/61388963:_____/14:00432523
n4:jazykVysledku
n17:eng
n4:klicovaSlova
hydrated electron; THz spectroscopy; ab initio molecular dynamics
n4:klicoveSlovo
n11:hydrated%20electron n11:ab%20initio%20molecular%20dynamics n11:THz%20spectroscopy
n4:kodStatuVydavatele
GB - Spojené království Velké Británie a Severního Irska
n4:kontrolniKodProRIV
[301A72A42C58]
n4:nazevZdroje
Nature Chemistry
n4:obor
n8:CF
n4:pocetDomacichTvurcuVysledku
2
n4:pocetTvurcuVysledku
5
n4:projekt
n16:GBP208%2F12%2FG016
n4:rokUplatneniVysledku
n15:2014
n4:svazekPeriodika
6
n4:tvurceVysledku
Savolainen, J. Hamm, P. Uhlig, Frank Jungwirth, Pavel Ahmed, S.
n4:wos
000341371100012
s:issn
1755-4330
s:numberOfPages
5
n7:doi
10.1038/NCHEM.1995