Trends in Bandgap of Epitaxial $\textit{A}$$_2$$\textit{B}$$_2$O$_7$ ($\textit{A}$ = Sn, Pb; $\textit{B}$ = Nb, Ta) Films Fabricated by Pulsed Laser Deposition

TL;DR

This study investigates the optical bandgap trends in epitaxial A2B2O7 pyrochlore films, revealing how composition influences electronic properties and confirming theoretical predictions about hybridized states.

Contribution

It establishes growth conditions for specific pyrochlore films and provides experimental data on their optical bandgaps, supporting theoretical models of hybridization effects.

Findings

Bandgap energies increase from Sn to Pb and from Nb to Ta.

Pb2B2O7 has a less dispersive valence band than Sn2B2O7.

Experimental results align with theoretical predictions of hybridized states.

Abstract

Pyrochlore oxides $A_2B_2$O$_7$ have been a fruitful playground for condensed matter physics because of the unique geometry in the crystal structure. Especially focusing on the $A$-site tetrahedral sub-lattice, in particular, pyrochlore oxides $A_2B_2$O$_7$ ($A$ = Sn, Pb and $B$ = Nb, Ta), recent theoretical studies predict the emergence of the "quasi-flat band" structure as a result of the strong hybridization between filled $A$-n$s$ and O-2$p$ orbitals. In this work, we have established the growth conditions of Sn$_2$Nb$_2$O$_7$, Sn$_2$Ta$_2$O$_7$, Pb$_2$Nb$_2$O$_7$, and Pb$_2$Ta$_2$O$_7$ films by pulsed laser deposition on Y-stabilized ZrO$_2$ (111) substrates to elucidate their optical properties. Absorption-edge energies, both for direct and indirect bandgaps, increase in the order of Sn$_2$Nb$_2$O$_7$, Sn$_2$Ta$_2$O$_7$, Pb$_2$Nb$_2$O$_7$, and Pb$_2$Ta$_2$O$_7$. This tendency can be well explained by considering the energy level of the constituent elements. A comparison of the difference between direct and indirect bandgaps reveals that Pb$_2B_2$O$_7$ tends to have a less dispersive valence band than Sn$_2B_2$O$_7$. Our findings are consistent with the theoretical predictions and are suggestive of the common existence of the hybridized states in this class of compounds.