A coherent phonon-induced hidden quadrupolar ordered state in Ca2RuO4

Honglie Ning, Omar Mehio, Xinwei Li, Michael Buchhold, Mathias Driesse, Hengdi Zhao, Gang Cao and David Hsieh ()
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Honglie Ning: California Institute of Technology
Omar Mehio: California Institute of Technology
Xinwei Li: California Institute of Technology
Michael Buchhold: Universität zu Köln
Mathias Driesse: California Institute of Technology
Hengdi Zhao: University of Colorado
Gang Cao: University of Colorado
David Hsieh: California Institute of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-7

Abstract: Abstract Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic hidden states exhibiting higher multipolar ordering remain elusive owing to the challenge of directly manipulating and detecting them with light. Here we demonstrate a method to induce a dynamical transition from a thermally allowed to a thermally forbidden spin-orbit entangled quadrupolar ordered state in Ca2RuO4 by coherently exciting a phonon that is strongly coupled to the order parameter. Combining probe photon energy-resolved coherent phonon spectroscopy measurements with model Hamiltonian calculations, we show that the dynamical transition is manifested through anomalies in the temperature, pump excitation fluence, and probe photon energy dependence of the strongly coupled phonon. With this procedure, we introduce a general pathway to uncover hidden multipolar ordered states and to control their re-orientation on ultrashort timescales.

Date: 2023
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DOI: 10.1038/s41467-023-44021-4

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