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We characterize the 795 nm $^3$H$_6$ to $^3$H$_4$ transition of Tm$^{3+}$ in a Ti$^{4+}$:LiNbO$_{3}$ waveguide at temperatures as low as 800 mK. Coherence and hyperfine population lifetimes -- up to 117 $mu$s and 2.5 hours, respectively -- exceed tho se at 3 K at least ten-fold, and are equivalent to those observed in a bulk Tm$^{3+}$:LiNbO$_{3}$ crystal under similar conditions. We also find a transition dipole moment that is equivalent to that of the bulk. Finally, we prepare a 0.5 GHz-bandwidth atomic frequency comb of finesse $>$2 on a vanishing background. These results demonstrate the suitability of rare-earth-doped waveguides created using industry-standard Ti-indiffusion in LiNbO$_3$ for on-chip quantum applications.
High-quality rare-earth-ion (REI) doped materials are a prerequisite for many applications such as quantum memories, ultra-high-resolution optical spectrum analyzers and information processing. Compared to bulk materials, REI doped powders offer low- cost fabrication and a greater range of accessible material systems. Here we show that crystal properties, such as nuclear spin lifetime, are strongly affected by mechanical treatment, and that spectral hole burning can serve as a sensitive method to characterize the quality of REI doped powders. We focus on the specific case of thulium doped Y$_2$Al$_5$O$_{12}$ (Tm:YAG). Different methods for obtaining the powders are compared and the influence of annealing on the spectroscopic quality of powders is investigated on a few examples. We conclude that annealing can reverse some detrimental effects of powder fabrication and, in certain cases, the properties of the bulk material can be reached. Our results may be applicable to other impurities and other crystals, including color centers in nano-structured diamond.
Nano-structuring impurity-doped crystals affects the phonon density of states and thereby modifies the atomic dynamics induced by interaction with phonons. We propose the use of nano-structured materials in the form of powders or phononic bandgap cry stals to enable or improve persistent spectral hole-burning and coherence for inhomogeneously broadened absorption lines in rare-earth-ion-doped crystals. This is crucial for applications such as ultra-precise radio-frequency spectrum analyzers and optical quantum memories. As an example, we discuss how phonon engineering can enable spectral hole burning in erbium-doped materials operating in the convenient telecommunication band, and present simulations for density of states of nano-sized powders and phononic crystals for the case of Y2SiO5, a widely-used material in current quantum memory research.
Decoherence of the 795 nm $^3$H$_6$ to $^3$H$_4$ transition in 1%Tm$^{3+}$:Y$_3$Ga$_5$O$_{12}$ (Tm:YGG) is studied at temperatures as low as 1.2 K. The temperature, magnetic field, frequency, and time-scale (spectral diffusion) dependence of the opti cal coherence lifetime is measured. Our results show that the coherence lifetime is impacted less by spectral diffusion than other known thulium-doped materials. Photon echo excitation and spectral hole burning methods reveal uniform decoherence properties and the possibility to produce full transparency for persistent spectral holes across the entire 56 GHz inhomogeneous bandwidth of the optical transition. Temperature-dependent decoherence is well described by elastic Raman scattering of phonons with an additional weaker component that may arise from a low density of glass-like dynamic disorder modes (two-level systems). Analysis of the observed behavior suggests that an optical coherence lifetime approaching one millisecond may be possible in this system at temperatures below 1 K for crystals grown with optimized properties. Overall, we find that Tm:YGG has superior decoherence properties compared to other Tm-doped crystals and is a promising candidate for applications that rely on long coherence lifetimes, such as optical quantum memories and photonic signal processing.
We investigate the relevant spectroscopic properties of the 795 nm $^3$H$_6$$leftrightarrow$$^3$H$_4$ transition in 1% Tm$^{3+}$:Y$_3$Ga$_5$O$_{12}$ at temperatures as low as 1.2 K for optical quantum memories based on persistent spectral tailoring o f narrow absorption features. Our measurements reveal that this transition has uniform coherence properties over a 56 GHz bandwidth, and a simple hyperfine structure split by $pm$44 MHz/T with lifetimes of up to hours. Furthermore, we find a $^3$F$_4$ population lifetime of 64 ms -- one of the longest lifetimes observed for an electronic level in a solid --, and an exceptionally long coherence lifetime of 490 $mu$s -- the longest ever observed for optical transitions of Tm$^{3+}$ ions in a crystal. Our results suggest that this material allows realizing broadband quantum memories that enable spectrally multiplexed quantum repeaters.
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