Ferroelectric lead-free K
x
Na1–x
NbO3 (KNN) perovskite,
whose piezoelectric
properties can be comparable to those of traditional Pb-based systems,
has aroused wide concern in recent years. However, the specific influences
of the stress field on KNN’s structure and piezoelectric properties
have not been well clarified and there are few descriptions about
the temperature–pressure phase diagram. Here, we analyzed the
phonon mode behavior and structural evolution of K0.5Na0.5NbO3-0.05LiNbO3 (KNN-LN) and MnO2-doped single crystals with pressure- and temperature-dependent
phase structure variations by theoretical calculation, polarized Raman
scattering, and infrared reflectance spectra. The different phase
structures can be predicted at high pressure using the CALYPSO method
with its same-name code. The rhombohedral → orthorhombic →
tetragonal → cubic phase transition process can be discovered
in detail by Raman spectra under different temperatures and pressures.
The phase coexistence on the thermal phase boundary was confirmed
by basic anastomosis. Meanwhile, it was found
that the substitution of Mn in the NbO6 octahedron aggravates
the deformation of high pressure on KNN-LN and the substitution of
Mn at the B-site intensifies the structural evolution more severely
than at the A-site. The present study aims at exploring octahedra
tilt, phonon vibrations, and the internal structure on the general
critical phase boundary in KNN-LN crystals. It provides effective
help for the study of lead-free perovskite phase transformation and
the improvement in piezoelectric properties under a high-pressure
field.