Abstract
The structure and lattice dynamics of the hybrid improper ferroelectric compound Ca3-xSrxTi2O7 (for x=0,0.6, and 0.9) have been studied with a combination of diffraction, inelastic scattering experiments, Raman spectroscopy, and calorimetry measurements, as well as first-principles simulations. Using inelastic neutron scattering, we have measured the phonon density of states (DOS) for x=0.9, which revealed a strong broadening but little change in phonon energies on heating from 10 K to 728 K across the ferroelectric phase transition temperature, TFE. Using inelastic X-ray scattering, the momentum-resolved phonon dispersions were measured from 80 K to 950 K on a single crystal (for x=0.6), and also revealed a strong phonon broadening but a small energy shift for acoustic modes on heating across TFE. Our Raman measurements (for x=0.6) showed robust rotational and oxygen breathing modes but soft tilt modes, consistent with previous measurements on similar compounds. Our density functional calculations achieve good agreement with both the phonon DOS and dispersions measured. We did not observe any unusual quadratic dispersion for c-polarized transverse acoustic modes, at odds with a recently predicted quasi-2D character, for either undoped (x=0) or doped (x=0.6) compounds.
Original language | English |
---|---|
Article number | 214304 |
Journal | Physical Review B |
Volume | 100 |
Issue number | 21 |
DOIs | |
State | Published - Dec 6 2019 |
Funding
Neutron and x-ray scattering measurements, Raman spectroscopy, thermal characterization, and modeling (D.B., J.L.N., X.H., T.L.A., O.D.) were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, through the Office of Science Early Career Research Program under Award No. DE-SC0016166. The work at Rutgers University was supported by the DOE under Grant No. DE-FG02-07ER46382. This research used resources of the Advanced Photon Source, a US Department of Energy Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The use of Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US DOE. Theoretical calculations were performed using resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.