NMR detection of dynamical processes in antiferroelectric nanoclusters during the order-disorder transition in NH4H2AsO4

TL;DR

This paper uses advanced NMR techniques to investigate the dynamics of antiferroelectric nanoclusters in NH4H2AsO4 during the order-disorder transition, revealing phase coexistence and cluster behavior near the transition temperature.

Contribution

It introduces a novel application of 15N NMR and 2D chemical exchange spectroscopy to study nanocluster dynamics in antiferroelectric materials.

Findings

Nanoclusters are dynamic with ~50 nm size.

Phase coexistence occurs within 2-3 K of T_N.

Cluster occupancy increases rapidly below T_N.

Abstract

We study the dynamics of inorganic antiferroelectric nanoclusters formed during an order-disorder transition and demonstrate the coexistence of the two phases in a region of 2-3 K around the transition temperature TN~215 K. Single crystals of NH4H2AsO4, a model hydrogen-bonded compound, show an antiferroelectric-paraelectric transition studied by means of highly sensitive magic angle spinning 15N NMR at 21.1 T. The phase co-existence is demonstrated by a double-peak structure of the chemical shift. Two-dimensional chemical exchange spectroscopy and spin-lattice relaxation time (T1) measurements show that the clusters are dynamic with sizes ~50 nm and lifetimes approaching seconds as T->TN. Their occupancy increases rapidly to fill the crystal volume below $T_N$. This study provides evidence for the commonality of the phase transitions in systems with electric properties and provides an improved spectroscopic method for such studies.