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Ultrafast manipulation of the NiO antiferromagnetic order via sub-gap optical excitation

Wang, Xiaocui (author)
Uppsala universitet,FREIA
Engel, Robin Y. (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.;Univ Hamburg, Dept Phys, Luruper Chaussee 149, D-22761 Hamburg, Germany.
Vaskivskyi, Igor (author)
Jozef Stefan Inst, Dept Complex Matter, Jamova Cesta 39, Ljubljana 1000, Slovenia.
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Turenne, Diego (author)
Uppsala universitet,FREIA
Shokeen, Vishal (author)
Uppsala universitet,FREIA
Yaroslavtsev, Alexander (author)
Uppsala universitet,FREIA
Grånäs, Oscar, 1979- (author)
Uppsala universitet,Materialteori
Knut, Ronny (author)
Uppsala universitet,Institutionen för fysik och astronomi
Schunck, Jan O. (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.;Univ Hamburg, Dept Phys, Luruper Chaussee 149, D-22761 Hamburg, Germany.
Dziarzhytski, Siarhei (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.
Brenner, Guenter (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.
Wang, Ru-Pan (author)
Univ Hamburg, Dept Phys, Luruper Chaussee 149, D-22761 Hamburg, Germany.
Kuhlmann, Marion (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.
Kuschewski, Frederik (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.
Bronsch, Wibke (author)
Elettra Sincrotrone Trieste SCpA, I-34149 Basovizza, Italy.
Schuessler-Langeheine, Christian (author)
Helmholtz Zentrum Berlin Mat & Energie, Albert Einstein Str 15, D-12489 Berlin, Germany.
Styervoyedov, Andriy (author)
Max Planck Inst Mikrostrukturphys, Weinberg 2, D-06120 Halle, Germany.
Parkin, Stuart S. P. (author)
Max Planck Inst Mikrostrukturphys, Weinberg 2, D-06120 Halle, Germany.
Parmigiani, Fulvio (author)
Elettra Sincrotrone Trieste SCpA, I-34149 Basovizza, Italy.
Eriksson, Olle, 1960- (author)
Uppsala universitet,Institutionen för fysik och astronomi
Beye, Martin (author)
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany.;Univ Hamburg, Dept Phys, Luruper Chaussee 149, D-22761 Hamburg, Germany.
Dürr, Hermann (author)
Uppsala universitet,FREIA
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 (creator_code:org_t)
2022
2022
English.
In: Faraday discussions. - : Royal Society of Chemistry (RSC). - 1359-6640 .- 1364-5498. ; 237:0, s. 300-316
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L-2-edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 +/- 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

Subject headings

NATURVETENSKAP  -- Fysik -- Den kondenserade materiens fysik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Condensed Matter Physics (hsv//eng)

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