Piezoelectric polar nanoregions and relaxation-coupled resonances in relaxor ferroelectrics

Abstract

\indent It is a generally accepted fact that the unique dielectric properties of relaxor ferroelectrics are related to the formation of polar nanoregion (PNRs). Less well recognized is the corollary that, because they are polar and therefore lack inversion symmetry, PNRs are also piezoelectric at the nanoscale and can therefore behave as nanoresonators. Using the particular relaxor ferroelectric K$_{\tt1-x}$Li$_{\tt x}$TaO$_{\tt 3}$ (KLT), we show that, when electrically excited into oscillation, these piezoelectric nanoresonators can drive macroscopic electro-mechanical resonances. Unexpectedly however, pairs of coupled resonances are observed, with one of the two exhibiting a characteristic Fano-like lineshape. The complex resonance spectra can be described equally well by two alternative but complementary models both involving two resonances coupled through a relaxation: a purely classical one based on two coupled damped harmonic oscillators and a semi-classical based on two discrete excitations coupled to each other through a continuum. Together, they provide complementary perspectives on the underlying physics of the system. Both reproduce the rapid evolution of the resonance spectrum across three wide temperature ranges, including a phase transition range. In the high temperature range, the coupling between modes is due to the collective $\pi$ relaxation of the lithium ions within PNRs and in the phase transition range to "heterophase relaxation" of the surrounding lattice between its high temperature cubic and low temperature tetragonal phases. The coupling is suppressed in the intermediate range of the collective $\pi/2$ relaxation of the lithium ions. Incidentally, the measured dielectric spectra are shown to bear a surprising but justifiable resemblance to the optical spectra of certain atomic vapors that exhibit electromagnetically induced transparency.