Design rules, accurate enthalpy prediction, and synthesis of stoichiometric Eu3+ quantum memory candidates

17 October 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Stoichiometric Eu3+ compounds have recently shown promise for building dense, optically addressable quantum memory as the cations’ long nuclear spin coherence times and shielded 4f electron optical transitions provide reliable memory platforms. Implementing such a system, though, requires ultra-narrow inhomogeneous linewidth compounds. Finding this rare linewidth behavior within a wide range of potential chemical spaces remains difficult, and while exploratory synthesis is often guided by density functional theory (DFT) calculations, lanthanides’ 4f electrons pose unique challenges for stability predictions. Here, we report DFT procedures that reliably reproduce known phase diagrams and that correctly predict two experimentally realized quantum memory candidates. We are the first to synthesize the double perovskite halide Cs2NaEuF6. It is an air-stable compound with a calculated band gap of 6.9 eV that surrounds Eu3+ with mononuclidic elements, which are desirable for avoiding inhomogeneous linewidth broadening. We also analyze computational database entries to identify phosphates and iodates as the next generation of chemical spaces for stoichiometric quantum memory system studies. This work identifies new candidate platforms for exploring chemical effects on quantum memory candidates’ inhomogeneous linewidth while also providing a framework for screening Eu3+ compound stability with DFT.

Keywords

lanthanides
DFT
materials design
materials synthesis
qubit
quantum memory

Supplementary materials

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Supporting Information
Description
The document contains additional information about the DFT tests, procedures, and results. It also contains additional experimental data from the new material synthesis attempts.
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New Phase Relaxed CIFs
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The zip file contains CIFs with the DFT-relaxed structures for the proposed compounds.
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