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Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet

Nature Photonics volume 9, pages 506–510 (2015)Cite this article

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Abstract

Manipulating the macroscopic phases of solids using ultrashort light pulses has resulted in spectacular phenomena, including metal–insulator transitions1,2,3, superconductivity4 and subpicosecond modification of magnetic order5. The development of this research area strongly depends on the understanding and optical control of fundamental interactions in condensed matter, in particular the exchange interaction. However, disentangling the timescales relevant for the contributions of the exchange interaction and spin dynamics to the exchange energy, Eex, is a challenge. Here, we introduce femtosecond stimulated Raman scattering to unravel the ultrafast photo-induced dynamics of magnetic excitations at the edge of the Brillouin zone. We find that femtosecond laser excitation of the antiferromagnet KNiF3 triggers a spectral shift of the two-magnon line, the energy of which is proportional to Eex. By unravelling the photo-induced modification of the two-magnon line frequency from a dominating nonlinear optical effect, we find that Eex is increased by the electromagnetic stimulus.

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Figure 1: Concept of the FSRS experiment on KNiF3.
Figure 2: SRS measurements on KNiF3.
Figure 3: Experimental peak shift of the 2M line from the RG and RL components of the stimulated Raman spectra.

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Acknowledgements

The authors thank R.V. Pisarev for providing the sample, P.H.M. van Loosdrecht and A. Caretta for performing spontaneous Raman measurements and Th. Rasing for continuous support. S. Mukamel is acknowledged for critical reading of the manuscript and useful insights. This research was partially supported by the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO), de Stichting voor Fundamenteel Onderzoek der Materie (FOM), the European Research Council (ERC) under the European Union's Seventh Framework Program (FP7/2007-2013) grant agreements no. 207916 (Femtoscopy) and no. 257280 (Femtomagnetism).

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Authors and Affiliations

  1. Dipartimento di Fisica, Universitá di Roma ‘La Sapienza’, Roma, I-00185, Italy

    G. Batignani, N. Di Palo, C. Ferrante, E. Pontecorvo & T. Scopigno

  2. Dipartimento di Scienze Fisiche e Chimiche, Universitá degli Studi dell'Aquila, L'Aquila, I-67100, Italy

    G. Batignani

  3. Radboud University Nijmegen, Institute for Molecules and Materials, Nijmegen, 6525, AJ, The Netherlands

    D. Bossini & A. Kimel

  4. Dipartimento di Fisica, IFN-CNR, Politecnico di Milano, Piazza L. da Vinci 32, Milano, 20133, Italy

    G. Cerullo

  5. Center for Life Nano Science @Sapienza, Istituto Italiano di Tecnologia, 295 Viale Regina Elena, Roma, I-00161, Italy

    T. Scopigno

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  1. G. Batignani
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Contributions

D.B., G.C., A.K. and T.S. conceived the project. D.B. and A.K. suggested the idea to probe the exchange energy via the 2M line. G.B., N.D.P., C.F., E.P. and T.S. designed the experiment and the method to interpret the FSRS data to obtain the 2ML dynamics. E.P., with assistance from G.B., D.B. and N.D.P., led the experimental activity. G.B., with help from N.D.P. and C.F., performed data analysis and numerical modelling. T.S. directed the research, and wrote the manuscript with G.B. and D.B. All authors discussed the results and implications and commented on the manuscript.

Corresponding author

Correspondence to T. Scopigno.

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The authors declare no competing financial interests.

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Batignani, G., Bossini, D., Di Palo, N. et al. Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet. Nature Photon 9, 506–510 (2015). https://doi.org/10.1038/nphoton.2015.121

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