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Ultrafast frustration-breaking and magnetophononic driving of singlet excitations in a quantum magnet

Flavio Giorgianni1, Björn Wehinger1,2,3, Stephan Allenspach1,2, Nicola Colonna1,4*, Carlo Vicario1, Pascal Puphal1,5, Ekaterina Pomjakushina1, Bruce Normand1,6,7, Christian Rüegg1,2,7,8

1 Paul Scherrer Institute, CH-5232 Villigen-PSI, Switzerland.

2 Department of Quantum Matter Physics, University of Geneva, CH-1211 Geneva 4, Switzerland.

3 Department of Molecular Sciences and Nanosystems, Ca’ Foscari University of Venice, 30172 Venezia Mestre, Italy.

4 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

5 Max Planck Institute for Solid State Research, Heisenbergstrasse1, 70569 Stuttgart, Germany.

6 Lehrstuhl für Theoretische Physik I, Technische Universität Dortmund, Otto-Hahn-Strasse 4, 44221 Dortmund, Germany

7 Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

8 Institute of Quantum Electronics, ETH Zürich, CH-8093 Hönggerberg, Switzerland.

* Corresponding authors emails: nicola.colonna@psi.ch
DOI10.24435/materialscloud:tm-4t [version v2]

Publication date: Oct 17, 2023

How to cite this record

Flavio Giorgianni, Björn Wehinger, Stephan Allenspach, Nicola Colonna, Carlo Vicario, Pascal Puphal, Ekaterina Pomjakushina, Bruce Normand, Christian Rüegg, Ultrafast frustration-breaking and magnetophononic driving of singlet excitations in a quantum magnet, Materials Cloud Archive 2023.156 (2023), https://doi.org/10.24435/materialscloud:tm-4t


Ideal magnetic frustration forms the basis for the emergence of exotic quantum spin states that are entirely nonmagnetic. Such singlet spin states are the defining feature of the Shastry-Sutherland model, and of its faithful materials realization in the quantum antiferromagnet SrCu₂(BO₃)₂. To address these states on ultrafast timescales, despite their lack of any microscopic order parameter, we introduce a nonlinear magnetophononic mechanism to alter the quantum spin dynamics by driving multiple optical phonon modes coherently and simultaneously. We apply intense terahertz pulses to create a nonequilibrium modulation of the magnetic interactions that breaks the ideal frustration of SrCu₂(BO₃)₂, such that previously forbidden physics can be driven in a coherent manner. Specifically, this driving populates a purely magnetic excitation, the singlet branch of the two-triplon bound state, by resonance with the difference frequency of two pumped phonons. Our results demonstrate how light-driven phonons can be used for the ultrafast and selective manipulation of interactions in condensed matter, even at frequencies far from those of the pump spectrum, offering valuable additional capabilities for the dynamical control of quantum many-body phenomena.

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Magnetophononic Strongly correlated electrons Tera-hertz pump and probe Quantum magnetic materials H2020 MARVEL/P4 SNSF

Version history:

2023.156 (version v2) [This version] Oct 17, 2023 DOI10.24435/materialscloud:tm-4t
2021.175 (version v1) Oct 28, 2021 DOI10.24435/materialscloud:cp-6s