Spin-state studies with XES and RIXS: From static to ultrafast

György Vankó, Amélie Bordage, Pieter Glatzel, Erik Gallo, Mauro Rovezzi, Wojciech Gawelda, Andreas Galler, Christian Bressler, Gilles Doumy, Anne Marie March, Elliot P. Kanter, Linda Young, Stephen H. Southworth, Sophie E. Canton, Jens Uhlig, Grigory Smolentsev, Villy Sundström, Kristoffer Haldrup, Tim Brandt van Driel, Martin Meedom NielsenKasper S. Kjaer, Henrik T. Lemke

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Abstract

We report on extending hard X-ray emission spectroscopy (XES) along with resonant inelastic X-ray scattering (RIXS) to study ultrafast phenomena in a pump-probe scheme at MHz repetition rates. The investigated systems include low-spin (LS) FeII complex compounds, where optical pulses induce a spin-state transition to their (sub)nanosecond-lived high-spin (HS) state. Time-resolved XES clearly reflects the spin-state variations with very high signal-to-noise ratio, in agreement with HS–LS difference spectra measured at thermal spin crossover, and reference HS–LS systems in static experiments, next to multiplet calculations. The 1s2p RIXS, measured at the Fe 1s pre-edge region, shows variations after laser excitation, which are consistent with the formation of the HS state. Our results demonstrate that X-ray spectroscopy experiments with overall rather weak signals, such as RIXS, can now be reliably exploited to study chemical and physical transformations on ultrafast time scales.

Original languageEnglish
JournalJournal of Electron Spectroscopy and Related Phenomena
Volume188
Pages (from-to)166-171
ISSN0368-2048
DOIs
Publication statusPublished - 2013

Keywords

  • Molecular switching
  • Time-resolved spectroscopy
  • X-ray spectroscopy
  • Spin transition
  • Photoinduced transition
  • Ultrafast phenomena
  • Pump-probe experiments

Cite this

Vankó, G., Bordage, A., Glatzel, P., Gallo, E., Rovezzi, M., Gawelda, W., ... Lemke, H. T. (2013). Spin-state studies with XES and RIXS: From static to ultrafast. Journal of Electron Spectroscopy and Related Phenomena, 188, 166-171. https://doi.org/10.1016/j.elspec.2012.09.012
Vankó, György ; Bordage, Amélie ; Glatzel, Pieter ; Gallo, Erik ; Rovezzi, Mauro ; Gawelda, Wojciech ; Galler, Andreas ; Bressler, Christian ; Doumy, Gilles ; March, Anne Marie ; Kanter, Elliot P. ; Young, Linda ; Southworth, Stephen H. ; Canton, Sophie E. ; Uhlig, Jens ; Smolentsev, Grigory ; Sundström, Villy ; Haldrup, Kristoffer ; Brandt van Driel, Tim ; Nielsen, Martin Meedom ; Kjaer, Kasper S. ; Lemke, Henrik T. / Spin-state studies with XES and RIXS: From static to ultrafast. In: Journal of Electron Spectroscopy and Related Phenomena. 2013 ; Vol. 188. pp. 166-171.
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title = "Spin-state studies with XES and RIXS: From static to ultrafast",
abstract = "We report on extending hard X-ray emission spectroscopy (XES) along with resonant inelastic X-ray scattering (RIXS) to study ultrafast phenomena in a pump-probe scheme at MHz repetition rates. The investigated systems include low-spin (LS) FeII complex compounds, where optical pulses induce a spin-state transition to their (sub)nanosecond-lived high-spin (HS) state. Time-resolved XES clearly reflects the spin-state variations with very high signal-to-noise ratio, in agreement with HS–LS difference spectra measured at thermal spin crossover, and reference HS–LS systems in static experiments, next to multiplet calculations. The 1s2p RIXS, measured at the Fe 1s pre-edge region, shows variations after laser excitation, which are consistent with the formation of the HS state. Our results demonstrate that X-ray spectroscopy experiments with overall rather weak signals, such as RIXS, can now be reliably exploited to study chemical and physical transformations on ultrafast time scales.",
keywords = "Molecular switching, Time-resolved spectroscopy, X-ray spectroscopy, Spin transition, Photoinduced transition, Ultrafast phenomena, Pump-probe experiments",
author = "Gy{\"o}rgy Vank{\'o} and Am{\'e}lie Bordage and Pieter Glatzel and Erik Gallo and Mauro Rovezzi and Wojciech Gawelda and Andreas Galler and Christian Bressler and Gilles Doumy and March, {Anne Marie} and Kanter, {Elliot P.} and Linda Young and Southworth, {Stephen H.} and Canton, {Sophie E.} and Jens Uhlig and Grigory Smolentsev and Villy Sundstr{\"o}m and Kristoffer Haldrup and {Brandt van Driel}, Tim and Nielsen, {Martin Meedom} and Kjaer, {Kasper S.} and Lemke, {Henrik T.}",
year = "2013",
doi = "10.1016/j.elspec.2012.09.012",
language = "English",
volume = "188",
pages = "166--171",
journal = "Journal of Electron Spectroscopy and Related Phenomena",
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Vankó, G, Bordage, A, Glatzel, P, Gallo, E, Rovezzi, M, Gawelda, W, Galler, A, Bressler, C, Doumy, G, March, AM, Kanter, EP, Young, L, Southworth, SH, Canton, SE, Uhlig, J, Smolentsev, G, Sundström, V, Haldrup, K, Brandt van Driel, T, Nielsen, MM, Kjaer, KS & Lemke, HT 2013, 'Spin-state studies with XES and RIXS: From static to ultrafast', Journal of Electron Spectroscopy and Related Phenomena, vol. 188, pp. 166-171. https://doi.org/10.1016/j.elspec.2012.09.012

Spin-state studies with XES and RIXS: From static to ultrafast. / Vankó, György ; Bordage, Amélie ; Glatzel, Pieter ; Gallo, Erik ; Rovezzi, Mauro ; Gawelda, Wojciech ; Galler, Andreas ; Bressler, Christian ; Doumy, Gilles ; March, Anne Marie ; Kanter, Elliot P. ; Young, Linda; Southworth, Stephen H.; Canton, Sophie E.; Uhlig, Jens; Smolentsev, Grigory; Sundström, Villy; Haldrup, Kristoffer; Brandt van Driel, Tim; Nielsen, Martin Meedom; Kjaer, Kasper S.; Lemke, Henrik T.

In: Journal of Electron Spectroscopy and Related Phenomena, Vol. 188, 2013, p. 166-171.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Spin-state studies with XES and RIXS: From static to ultrafast

AU - Vankó, György

AU - Bordage, Amélie

AU - Glatzel, Pieter

AU - Gallo, Erik

AU - Rovezzi, Mauro

AU - Gawelda, Wojciech

AU - Galler, Andreas

AU - Bressler, Christian

AU - Doumy, Gilles

AU - March, Anne Marie

AU - Kanter, Elliot P.

AU - Young, Linda

AU - Southworth, Stephen H.

AU - Canton, Sophie E.

AU - Uhlig, Jens

AU - Smolentsev, Grigory

AU - Sundström, Villy

AU - Haldrup, Kristoffer

AU - Brandt van Driel, Tim

AU - Nielsen, Martin Meedom

AU - Kjaer, Kasper S.

AU - Lemke, Henrik T.

PY - 2013

Y1 - 2013

N2 - We report on extending hard X-ray emission spectroscopy (XES) along with resonant inelastic X-ray scattering (RIXS) to study ultrafast phenomena in a pump-probe scheme at MHz repetition rates. The investigated systems include low-spin (LS) FeII complex compounds, where optical pulses induce a spin-state transition to their (sub)nanosecond-lived high-spin (HS) state. Time-resolved XES clearly reflects the spin-state variations with very high signal-to-noise ratio, in agreement with HS–LS difference spectra measured at thermal spin crossover, and reference HS–LS systems in static experiments, next to multiplet calculations. The 1s2p RIXS, measured at the Fe 1s pre-edge region, shows variations after laser excitation, which are consistent with the formation of the HS state. Our results demonstrate that X-ray spectroscopy experiments with overall rather weak signals, such as RIXS, can now be reliably exploited to study chemical and physical transformations on ultrafast time scales.

AB - We report on extending hard X-ray emission spectroscopy (XES) along with resonant inelastic X-ray scattering (RIXS) to study ultrafast phenomena in a pump-probe scheme at MHz repetition rates. The investigated systems include low-spin (LS) FeII complex compounds, where optical pulses induce a spin-state transition to their (sub)nanosecond-lived high-spin (HS) state. Time-resolved XES clearly reflects the spin-state variations with very high signal-to-noise ratio, in agreement with HS–LS difference spectra measured at thermal spin crossover, and reference HS–LS systems in static experiments, next to multiplet calculations. The 1s2p RIXS, measured at the Fe 1s pre-edge region, shows variations after laser excitation, which are consistent with the formation of the HS state. Our results demonstrate that X-ray spectroscopy experiments with overall rather weak signals, such as RIXS, can now be reliably exploited to study chemical and physical transformations on ultrafast time scales.

KW - Molecular switching

KW - Time-resolved spectroscopy

KW - X-ray spectroscopy

KW - Spin transition

KW - Photoinduced transition

KW - Ultrafast phenomena

KW - Pump-probe experiments

U2 - 10.1016/j.elspec.2012.09.012

DO - 10.1016/j.elspec.2012.09.012

M3 - Journal article

VL - 188

SP - 166

EP - 171

JO - Journal of Electron Spectroscopy and Related Phenomena

JF - Journal of Electron Spectroscopy and Related Phenomena

SN - 0368-2048

ER -