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Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment

We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. I...

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Autores principales: Pontius, N., Beye, M., Trabant, C., Mitzner, R., Sorgenfrei, F., Kachel, T., Wöstmann, M., Roling, S., Zacharias, H., Ivanov, R., Treusch, R., Buchholz, M., Metcalf, P., Schüßler-Langeheine, C., Föhlisch, A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Crystallographic Association 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6158032/
https://www.ncbi.nlm.nih.gov/pubmed/30310825
http://dx.doi.org/10.1063/1.5042847
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author Pontius, N.
Beye, M.
Trabant, C.
Mitzner, R.
Sorgenfrei, F.
Kachel, T.
Wöstmann, M.
Roling, S.
Zacharias, H.
Ivanov, R.
Treusch, R.
Buchholz, M.
Metcalf, P.
Schüßler-Langeheine, C.
Föhlisch, A.
author_facet Pontius, N.
Beye, M.
Trabant, C.
Mitzner, R.
Sorgenfrei, F.
Kachel, T.
Wöstmann, M.
Roling, S.
Zacharias, H.
Ivanov, R.
Treusch, R.
Buchholz, M.
Metcalf, P.
Schüßler-Langeheine, C.
Föhlisch, A.
author_sort Pontius, N.
collection PubMed
description We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 ± 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices.
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spelling pubmed-61580322018-10-11 Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment Pontius, N. Beye, M. Trabant, C. Mitzner, R. Sorgenfrei, F. Kachel, T. Wöstmann, M. Roling, S. Zacharias, H. Ivanov, R. Treusch, R. Buchholz, M. Metcalf, P. Schüßler-Langeheine, C. Föhlisch, A. Struct Dyn Articles We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 ± 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices. American Crystallographic Association 2018-09-26 /pmc/articles/PMC6158032/ /pubmed/30310825 http://dx.doi.org/10.1063/1.5042847 Text en © 2018 Author(s). 2329-7778/2018/5(5)/054501/8 All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Articles
Pontius, N.
Beye, M.
Trabant, C.
Mitzner, R.
Sorgenfrei, F.
Kachel, T.
Wöstmann, M.
Roling, S.
Zacharias, H.
Ivanov, R.
Treusch, R.
Buchholz, M.
Metcalf, P.
Schüßler-Langeheine, C.
Föhlisch, A.
Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title_full Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title_fullStr Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title_full_unstemmed Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title_short Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment
title_sort probing the non-equilibrium transient state in magnetite by a jitter-free two-color x-ray pump and x-ray probe experiment
topic Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6158032/
https://www.ncbi.nlm.nih.gov/pubmed/30310825
http://dx.doi.org/10.1063/1.5042847
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