Photoinduced suppression of the ferroelectric instability in PbTe

The interactions between electrons and phonons drive a large array of
technologically relevant material properties including ferroelectricity,
thermoelectricity, and phase-change behaviour. In the case of many group IV-VI,
V, and related materials, these interactions are strong and the materials exist
near electronic and structural phase transitions. Their close proximity to
phase instability produces a fragile balance among the various properties. The
prototypical example is PbTe whose incipient ferroelectric behaviour has been
associated with large phonon anharmonicity and thermoelectricity. Experimental
measurements on PbTe reveal anomalous lattice dynamics, especially in the soft
transverse optical phonon branch. This has been interpreted in terms of both
giant anharmonicity and local symmetry breaking due to off-centering of the Pb
ions. The observed anomalies have prompted renewed theoretical and
computational interest, which has in turn revived focus on the extent that
electron-phonon interactions drive lattice instabilities in PbTe and related
materials. Here, we use Fourier-transform inelastic x-ray scattering (FT-IXS)
to show that photo-injection of free carriers stabilizes the paraelectric
state. With support from constrained density functional theory (CDFT)
calculations, we find that photoexcitation weakens the long-range forces along
the cubic direction tied to resonant bonding and incipient ferroelectricity.
This demonstrates the importance of electronic states near the band edges in
determining the equilibrium structure.