We report on the magnetic and phononic excitation spectrum of Sr3Cr2O8 determined by THz and infrared (IR) spectroscopy, and electron spin resonance (ESR) measurements across the Jahn-Teller transition, which is detected by specific-heat measurements to occur at TJT = 285 K. We identify the singlet-triplet excitations in the dimerized ground state and estimate the exchange couplings in the system. ESR absorptions were observed up to T * = 120 K with a linewidth ∝ exp (−∆/kBT ) and ∆/kB = 388 K indicating a phonon-mediated spin relaxation via the excited orbital state of the Cr e doublet in the orbitally ordered state. Upon entering the low-symmetry Jahn-Teller distorted phase below TJT , we find an extended regime T * < T < TJT where the IR active phonons change only gradually with decreasing temperature. This regime is associated with strong fluctuations in the orbital and lattice degrees of freedom in agreement with the loss of the ESR signal above T * . Using the measured magnetic and phononic excitation spectrum we model the orbital contribution to the specific heat and find the persistence of strong fluctuations far below TJT .PACS numbers: 78.30.-j,71.70.-d,76.30.-v,78.20.-e Orbital degrees of freedom (DOF) and their coupling to other DOF play an important role in understanding the physics in many transition-metal compounds including colossal magnetoresistive manganites, vanadates, and iron-based superconductors.1-3 Orbital ordering (OO) mechanisms, 4 collective orbital excitations, 5 and frustration effects in the orbital sector have attracted considerable attention and formed the research field of orbital physics. Exotic ground states such as orbital and spinorbital liquids have been explored both experimentally and theoretically.6 Orbital fluctuations play an important role in the formation of these states and may even induce a dimerization of spins via magnetoelastic coupling.
7Here we investigate the OO transition in the spingapped dimerized system Sr 3 Cr 2 O 8 . This compound has come into focus due to the occurrence of a field-induced magnon condensation.8,9 The room temperature crystal structure of Sr 3 Cr 2 O 8 was determined to be hexagonal with space group R3m.10 Each Cr 5+ ion with spin S = 1/2 is surrounded by an oxygen tetrahedron and couples antiferromagnetically to adjacent Cr 5+ ions along c direction, forming a spin singlet ground state at low temperatures. The tetrahedral crystal field splits the 3d levels into lower-lying doubly-degenerated e and triplydegenerated t orbitals. Thus, the Cr 5+ ions are JahnTeller (JT) active and a JT transition to a monoclinic structure with three twinned domains and space group C 2/c has been reported by neutron experiments to occur at 275 K.11,12 Primarily associated with the antiferrodistortive displacement of the apical oxygen ions this transition is suggested to be accompanied by the splitting of the e doublet into a lower-lying d 3z 2 −r 2 and excited d x 2 −y 2 orbital, and an antiferro-orbital ordering of d 3z 2 −r 2 orbitals. In addition, thi...