Coherent light–matter interfaces are key elements for many quantum information processing architectures. Rare-earth ion (REI)-containing systems featuring narrow inter-configurational f–f transitions are suitable for creating such interfaces. Recently, narrow homogeneous linewidths (Γ h ) and long nuclear spin lifetimes ( T 1spin ) associated with two Eu 3+ complexes featuring the 5 D 0 → 7 F 0 f–f transition have been reported, elucidating that REI-molecule-based coherent light–matter interfaces can be obtained. In this study, we report a homogeneous linewidth of 2.8 MHz at 4.2 K, corresponding to an optical coherence lifetime ( T 2opt ) of 114 ns (0.11 μs), associated with the 5 D 0 → 7 F 0 transition of the prototypical charge neutral Eu 3+ complex─[Eu(trensal)]. Moreover, we have observed long nuclear spin lifetimes ( T 1spin ) up to 460 ± 80 s at 4.2 K for the complex and efficient optical pumping of hyperfine levels of the 5 D 0 ground state. The results presented in this study indicate that narrow homogeneous linewidths and long nuclear spin lifetimes could be a generic property of molecular Eu 3+ complexes featuring the 5 D 0 → 7 F 0 transition.
Coherent light–matter interfaces are key elements for many quantum information processing architectures. Rare-earth ion (REI)-containing systems featuring narrow inter-configurational f–f transitions are suitable for creating such interfaces. Recently, narrow homogeneous linewidths (Γ h ) and long nuclear spin lifetimes ( T 1spin ) associated with two Eu 3+ complexes featuring the 5 D 0 → 7 F 0 f–f transition have been reported, elucidating that REI-molecule-based coherent light–matter interfaces can be obtained. In this study, we report a homogeneous linewidth of 2.8 MHz at 4.2 K, corresponding to an optical coherence lifetime ( T 2opt ) of 114 ns (0.11 μs), associated with the 5 D 0 → 7 F 0 transition of the prototypical charge neutral Eu 3+ complex─[Eu(trensal)]. Moreover, we have observed long nuclear spin lifetimes ( T 1spin ) up to 460 ± 80 s at 4.2 K for the complex and efficient optical pumping of hyperfine levels of the 5 D 0 ground state. The results presented in this study indicate that narrow homogeneous linewidths and long nuclear spin lifetimes could be a generic property of molecular Eu 3+ complexes featuring the 5 D 0 → 7 F 0 transition.
Abstract The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)- based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of 2 ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0→7 F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 +/- 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 +/- 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 +/- 0.4 s have been obtained. The results presented in this study are a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.
Abstract Coordination complexes of rare‐earth ions (REI) show optical transitions with narrow linewidths enabling the creation of coherent light‐matter interfaces for quantum information processing (QIP) applications. Among the REI‐based complexes, Eu(III) complexes showing the 5D0→7F0 transition are of interest for QIP applications due to the narrow linewidths associated with the transition. Herein, we report on the synthesis, structure, and optical properties of a novel Eu(III) complex and its Gd(III) analogue composed of 2,9‐bis(pyrazol‐1‐yl)‐1,10‐phenanthroline (dpphen) and three nitrate (NO3) ligands. The Eu(III) complex—[Eu(dpphen)(NO3)3]—showed sensitized metal‐centred emission (5D0→7FJ; J=0,1,2,3, 4, 5, or 6) in the visible region, upon irradiation of the ligand‐centred band at 369 nm, with the 5D0→7F0 transition centred at 580.9 nm. Spectral hole‐burning (SHB) studies of the complex with stoichiometric Eu(III) concentration revealed a narrow homogeneous linewidth (Γh) of 1.55 MHz corresponding to a 0.205 μs long optical coherence lifetime (T2opt). Remarkably, long nuclear spin lifetimes (T1spin) of up to 41 s have been observed for the complex. The narrow optical linewidths and long T1spin lifetimes obtained for the Eu(III) complex showcase the utility of Eu(III) complexes as tuneable, following molecular engineering principles, coherent light‐matter interfaces for QIP applications.
The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ions (REIs) are suitable candidates for QIP protocols due to their extraordinary photo-physical and magnetic quantum properties such as long optical and spin coherence lifetimes (T2). However, molecules incorporating REIs, despite having advantageous properties such as atomically exact quantum tunability, inherent scalability, and large portability, have not yet been studied for QIP applications. As a first testimony of the usefulness of REI molecules for optical QIP applications, we demonstrate in this study that narrow spectral holes can be burned in the inhomogeneously broadened 5D0→7F0 optical transition of a binuclear Eu(III) complex, rendering a homogeneous linewidth (Γh) = 22 ± 1 MHz, which translates as T2=14.5± 0.7 ns at 1.4 K. Moreover, long-lived spectral holes are observed, demonstrating efficient polarization of Eu(III) ground state nuclear spins, a fundamental requirement for all-optical spin initialization and addressing. These results elucidate the usefulness of REI-based molecular complexes as versatile coherent light-spin interfaces for applications in quantum communications and processing.
Rare earth ions are actively investigated as optically addressable spin systems for quantum technologies thanks to their long optical and spin coherence lifetimes. 171Yb3+, which has 1/2 electron and nuclear spins, recently raised interest for its simple hyperfine structure that moreover can result in long coherence lifetimes at zero magnetic field, an unusual property for paramagnetic rare earth ions. Here, we report on the optical inhomogeneous and homogeneous linewidths in 171Yb3+:Y2SiO5 (site 2) for different doping concentrations. While inhomogeneous linewidth is not correlated to 171Yb3+ concentration, the homogeneous one strongly decreases between 10 and 2 ppm doping level, reaching 255 Hz at 3 K. This is attributed to a slowing down of 171Yb3+ ground state spin flip-flops.
Ultralong-lived Coherent States in Eu3+:Y2O3 Optical Ceramics for Quantum Memories
Rare earth ions (REI) in solid materials are among the leading systems for quantum technology applications. However, developing practical REI quantum devices with long-lived coherent states remains challenging due to great growth difficulties of high-quality REI materials and a lack of comprehensive understanding of REI's decoherence mechanisms. Here we realize a record optical coherence time of 421.5 ± 10.5 μs for the 7F0→5D0 transition and more than 30 hours lifetime for the 7F0 hyperfine spin states in Eu3+:Y2O3 optical ceramics. We report the elimination of two-level-system induced optical decoherence in short-range ordered crystals. Meanwhile, a new decoherence mechanism caused by new kinds of perturbing magnetic centers is identified below 1.5 K. We further demonstrate the coherent light storage over 5 μs by using the atomic frequency comb protocol. These results open up prospects for the realization of practical quantum memories and large scale quantum communications with REI optical ceramics.
Rare earth ions (REI) in solid materials are among the leading systems for quantum technology applications. However, developing practical REI quantum devices with long-lived coherent states remains challenging due to great difficulties in growing high-quality REI materials and incomplete understanding of their decoherence mechanisms. In this work, we report a long optical coherence time of 422 ± 11 μs for the 7F0 → 5D0 transition, as well as a lifetime exceeding 30 hours for the 7F0 hyperfine spin states in Eu3+:Y2O3 optical ceramics. We identify the absence of two-level-system induced optical decoherence in short-range-ordered crystals and a decoherence mechanism caused by perturbing magnetic centers that were not detected previously below 1.5 K. Furthermore, we demonstrate coherent light storage over 5 μs by using the atomic frequency comb protocol. These results provide a promising proof-of-principle demonstration of quantum memory using Eu3+:Y2O3 optical ceramic system, highlighting its significant potential for practical quantum applications. Rare earth ions (REI) in solids are promising for quantum technologies. Here, the authors demonstrate a record optical coherence lifetime and the absence of two-level-system induced decoherence in Eu3+:Y2O3 optical ceramics. These findings advance the optimization of REI-based quantum systems and enable tailored material designs.