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Ultrafast laser excitation provides a means to transiently realize long-rangeordered electronic states of matter that are hidden in thermal equilibrium.Recently, this approach has unveiled a variety of thermally inaccessibleordered 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 remainelusive owing to the challenge of directly manipulating and detecting them withlight. Here we demonstrate a method to induce a dynamical transition from athermally allowed to a thermally forbidden spin-orbit entangled quadrupolarordered state in Ca$_2$RuO$_4$ by coherently exciting a phonon that is stronglycoupled to the order parameter. Combining probe photon energy-resolved coherentphonon spectroscopy measurements with model Hamiltonian calculations, we showthat the dynamical transition is manifested through anomalies in thetemperature, pump excitation fluence, and probe photon energy dependence of thestrongly coupled phonon. With this procedure, we introduce a general pathway touncover hidden multipolar ordered states and to control their re-orientation onultrashort timescales.

A coherent phonon-induced hidden quadrupolar ordered state in Ca$_2$RuO$_4$