Ultra-narrow optical linewidths in rare-earth molecular crystals

Diana Serrano (), Senthil Kumar Kuppusamy (), Benoît Heinrich, Olaf Fuhr, David Hunger, Mario Ruben () and Philippe Goldner ()
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Diana Serrano: Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie Paris
Senthil Kumar Kuppusamy: Institute for Quantum Materials and Technologies (IQMT), Karlsruhe Institute of Technology (KIT)
Benoît Heinrich: Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), CNRS-Université de Strasbourg
Olaf Fuhr: Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT)
David Hunger: Institute for Quantum Materials and Technologies (IQMT), Karlsruhe Institute of Technology (KIT)
Mario Ruben: Institute for Quantum Materials and Technologies (IQMT), Karlsruhe Institute of Technology (KIT)
Philippe Goldner: Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie Paris

Nature, 2022, vol. 603, issue 7900, 241-246

Abstract: Abstract Rare-earth ions (REIs) are promising solid-state systems for building light–matter interfaces at the quantum level1,2. This relies on their potential to show narrow optical and spin homogeneous linewidths, or, equivalently, long-lived quantum states. This enables the use of REIs for photonic quantum technologies such as memories for light, optical–microwave transduction and computing3–5. However, so far, few crystalline materials have shown an environment quiet enough to fully exploit REI properties. This hinders further progress, in particular towards REI-containing integrated nanophotonics devices6,7. Molecular systems can provide such capability but generally lack spin states. If, however, molecular systems do have spin states, they show broad optical lines that severely limit optical-to-spin coherent interfacing8–10. Here we report on europium molecular crystals that exhibit linewidths in the tens of kilohertz range, orders of magnitude narrower than those of other molecular systems. We harness this property to demonstrate efficient optical spin initialization, coherent storage of light using an atomic frequency comb, and optical control of ion–ion interactions towards implementation of quantum gates. These results illustrate the utility of rare-earth molecular crystals as a new platform for photonic quantum technologies that combines highly coherent emitters with the unmatched versatility in composition, structure and integration capability of molecular materials.

Date: 2022
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DOI: 10.1038/s41586-021-04316-2

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