Successive ferroelectric orders and magnetoelectric coupling without long-range magnetic order in highly frustrated pyrochlore compounds: Sm$_2$Ti$_{2-x}$V$_x$O$_7$

Sm$_2$Ti$_2$O$_7$, a member of rare-earth titanate pyrochlores, exhibits dipolar-octupolar antiferromagnetism below $T_N$ = 0.35 K. We observed two ferroelectric transitions at 182 ($T_{FE1}$) and 52 K ($T_{FE2}$), significantly higher than $T_N$ for Sm$_2$Ti$_{2-x}$V$_x$O$_7$ ($x$ = 0, 0.1). Although the ferroelectric transition temperatures remain unchanged, the polarization value decreases considerably with V doping. A structural transition to a polar $R3m$ rhombohedral phase from the cubic $Fd\bar{3}m$ structure occurs at $T_{FE1}$, involving a distortion in the pyochlore lattice. Remarkably, significant linear magnetoelectric coupling is observed in both compounds, with further enhancement of magnetoelectric coupling due to magnetic V doping. The existence of magnetoelectric coupling without long-range magnetic order in a frustrated pyrochlore system could enable the tailoring of magnetoelectric coupling properties, which can be further fine-tuned through V doping. The emergence of ferroelectricity in a frustrated magnetic system introduces an intriguing aspect to these compounds and paves the way for developing ferroelectric order driven by the alleviation of magnetic frustration in pyrochlore systems.