Chiral Polar Eu2(SeO3)2(SO4)(H2O)2: A Pathway Toward Narrow Optical Linewidths and Microsecond Lifetimes for Quantum Memory Candidates
Stoichiometric materials of Eu(III) offer a promising platform for quantum memories attributable to their unique capability to display a distinctive, nondegenerate J = 0 transition, which enables precise mapping of optical quantum states into their hyperfine structure for reliable storage and retrieval on demand. However, placing Eu(III) into chiral polar structures, which are necessary for achieving narrow spectral linewidths and long optical lifetimes, is a daunting task. Here, we discover Eu2(SeO3)2(SO4)(H2O)2, a rare Eu(III) material that exhibits chiral polar symmetries encompassing both local and global structures. This unique structure is shaped by an appropriate combination of asymmetric ligands. The chirality fosters dipole-dipole interactions and J-mixing, as characterized by second-harmonic generation, photoluminescence, and magnetic susceptibility. The broken inversion symmetry is supported by the phase-matching behavior of second-harmonic generation. The J = 0 transition is observed at 578 nm with a narrow linewidth at 78 K and a microsecond-scale optical lifetime. The analysis of magnetic susceptibility data using Van Vleck theory results in an effective magnetic moment of 3.33 μB/Eu3+ and J-mixing. Heat capacity data reveal underlying phonon dynamics in the material. This study demonstrates a pathway toward realizing new stoichiometric Eu3+ compounds with potential for optically addressable quantum memory applications.