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arXiv:2210.05005 · Physical review. B./Physical review. B

Quadratic Zeeman spectral diffusion of thulium ion population in an yttrium gallium garnet crystal

Jacob H. Davidson, Antariksha Das, Nir Alfasi, R. L. Cone, Charles W. Thiel, Wolfgang Tittel

Published Mar 9, 2023• 4 citations
arXivHTMLPDF

Abstract

The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.

DOI
10.1103/physrevb.107.094105

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Quantum Communications and Quantum Imaging•Nov 6, 2018•0 citations
The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.
Abstract Rare-earth ion-doped crystals are of great interest for quantum memories, a central component in future quantum repeaters. To assess the promise of 1 % Tm3+-doped yttrium gallium garnet (Tm:YGG), we report measurements of optical coherence and energy-level lifetimes of its 3H 6 ↔ 3 H4 transition at a temperature of around 500 mK and various magnetic fields. Using spectral hole burning (SHB), we find hyperfine ground-level (Zeeman level) lifetimes of several minutes at magnetic fields of less than 1000 G. We also measure coherence time exceeding one millisecond using two-pulse photon echoes. Three-pulse photon echo and SHB measurements reveal that due to spectral diffusion, the effective coherence time reduces to a few µs over a timescale of around two hundred seconds. Finally, temporal and frequency-multiplexed storage of optical pulses using the atomic frequency comb protocol is demonstrated. Our results suggest Tm:YGG to be promising for multiplexed photonic quantum memory for quantum repeaters.
We report on light slowing down in a rare-earth-metal-ion-doped crystal by persistent spectral hole burning. The absence of motion of the active ions, the large inhomogeneous broadening, the small homogeneous width, and the long lifetime of the hyperfine shelving states make this material convenient for the burning of narrow persistent spectral holes. Since the hole can be burnt long before the arrival of the input signal, there is no need for a strong-coupling field, illuminating the sample simultaneously with the input signal, in contrast with procedures such as electromagnetically induced transparency or coherent population oscillations. Analyzing the slowing down process, we point out the role played by the off-resonant atom. Most of the incoming information is carried over to off-resonant atoms, while the pulse is confined within the sample. The observed speed-of-light reduction factor exceeds 105{10}^{5}105.
We present a detailed study of the lifetime of optical spectral holes due to population storage in Zeeman sublevels of Nd3+:Y2SiO5{\mathrm{Nd}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Nd3+:Y2​SiO5​. The lifetime is measured as a function of magnetic field strength and orientation, temperature, and Nd3+{\mathrm{Nd}}^{3+}Nd3+ doping concentration. At the lowest temperature of 3 K we find a general trend where the lifetime is short at low field strengths, then increases to a maximum lifetime at a few hundred mT, and then finally decays rapidly for high field strengths. This behavior can be modeled with a relaxation rate dominated by ${\mathrm{Nd}}^{3+}\ensuremath{-}{\mathrm{Nd}}^{3+}$ cross relaxation at low fields and spin lattice relaxation at high magnetic fields. The maximum lifetime depends strongly on both the field strength and orientation, due to the competition between these processes and their different angular dependencies. The cross relaxation limits the maximum lifetime for concentrations as low as 30 ppm of Nd3+{\mathrm{Nd}}^{3+}Nd3+ ions. By decreasing the concentration to less than 1 ppm we could completely eliminate the cross relaxation, reaching a lifetime of 3.8 s at 3 K. At higher temperatures the spectral hole lifetime is limited by the magnetic-field-independent Raman and Orbach processes. In addition we show that the cross relaxation rate can be strongly reduced by creating spectrally large holes of the order of the optical inhomogeneous broadening. Our results are important for the development and design of new rare-earth-ion doped crystals for quantum information processing and narrow-band spectral filtering for biological tissue imaging.
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 Y3Al5O12 (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.
With their optical wavelength in the near infrared (790--800 nm) and their unique spectroscopic properties at cryogenic temperatures, thulium-doped crystals are at the center of many architectures linked to classical signal processing and quantum information. In this work, we focus on Tm-doped YSO, a compound that was left aside in the mid-1990s due to its rather short optical coherence lifetime. By means of time-resolved hole-burning spectroscopy, we investigate the anisotropic enhanced nuclear Zeeman effect and demonstrate deep, sub-MHz, persistent spectral hole burning under specific magnetic field orientation, and magnitude. By estimating the experimental parameters corresponding to a real-scale ultrasound optical tomography setup using Tm:YSO as a spectral filter, we validate Tm:YSO as a promising compound for medical imaging in the human body.
We study Lambda-type electromagnetically induced transparency (EIT) in cryogenically-cooled, europium and praseodymium doped yttrium orthosilicate (Eu:YSO and Pr:YSO). We use spectral hole burning techniques to vary the optical inhomogeneous width of the sub-ensemble of atoms participating in the EIT. The effect of inhomogeneous broadening has been studied in the context of Doppler broadened gases, but less so in solids where motional effects are absent and the coherence is not limited by the transit of atoms through the optical field. Rare earth doped crystals, like many solid-state systems, exhibit spectral hole burning in which a narrowband laser field optically pumps atoms to states in the ground manifold that are dark with respect to the applied field, opening up a transparency window that persists after the pumping laser is shuttered. More complex sequences of fields at multiple frequencies can create arbitrary spectral profiles, within bounds set by the particular energy level structure of the atoms. For both Eu:YSO and Pr:YSO, there are three hyperfine ground states and three hyperfine excited states (at zero magnetic field) and all nine transitions are dipole-allowed with varying transition strengths. We use spectral hole-burning techniques to prepare a sub-ensemble of atoms in a particular frequency class and a particular ground spin state, while also pumping atoms out of another ground state to create a Lambda system. We observe the same functional dependence of the EIT width on the optical inhomogeneous width and independently calibrated control field Rabi frequency in both systems.