Strong coupling of lattice and orbital excitations in quantum magnet Ca${}_{10}$Cr${}_7$O${}_{28}$: Anomalous temperature dependence of Raman phonons

Abstract

We report low-temperature Raman signatures of the Heisenberg quantum magnet Ca${}_{10}$Cr${}_7$O${}_{28}$, showing clear anomalies in phonon mode frequencies and linewidths below $\sim$100 K. This crossover temperature lies in between the Jahn-Teller (JT) temperature scale ($>$ room temperature) and the temperature scale associated with the spin exchange interactions ($<$ 12 K). Our experimental observation is well captured by a novel secondary JT transition associated with a cooperative reorientation of the orbitals giving rise to anomalies in the temperature dependence of Raman frequencies and linewidths. Such orbital reorganisation, in turn, affects the spin-spin exchange interactions that decide the fate of the magnet at lower temperatures and hence provide important clues to understand the energetics of the possible lower temperature quantum paramagnetic phase.

5 pages, 3 figures

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