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arXiv:1812.10369 · Physical review. B./Physical review. B

Deep and persistent spectral holes in thulium-doped yttrium orthosilicate for imaging applications

Caroline Venet, B. Car, Lucile Veissier, François Ramaz, Anne Louchet-Chauvet

Published Mar 1, 2019• 1 citation
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevb.99.115102

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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.
Thulium-doped crystals are considered for programmable filtering. Such a filter can be achieved by Spectral Hole Burning (SHB). One optically pumps the active ions into a long-lived shelving state, opening a narrow transparency window in the crystal absorption band. We investigate a new shelving scheme in Tm:YAG where the thulium ions are pumped into a ground state nuclear Zeeman sublevel, instead of their natural 10ms-lifetime metastable state. The shelving time is increased to several seconds, reducing the residual population in the transparency window by orders of magnitude. This should enhance the filter's dynamic range, which is essential in demanding filtering applications like ultrasound optical tomography.
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.
Decoherence of the 795 nm 3H6^{3}\mathrm{H}{}_{6}3H6​ to 3H4^{3}\mathrm{H}{}_{4}3H4​ transition in 11%{\mathrm{Tm}}^{3+}:{\mathrm{Y}}_{3}{\mathrm{Ga}}_{5}{\mathrm{O}}_{12}1 (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 optical 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 1 ms 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.
With the development of extremely precise spectral filters based on spectral hole burning and slow light effects, the idea of their implementation in an Ultrasound Optical Tomography (UOT) medical imaging technique arose. Simulations have shown that the resulting Contrast-to-Noise (CNR) ratio is fairly good at depths up to 5 cm but decreases dramatically when probing deeper in tissue. One of the possible enhancements of this technique is to include a phase conjugator after the filter to reverse and amplify ultrasound-tagged photons and send them back to the area of interest. This project tries to investigate the possibilities of using rare-earth-ion-doped crystals as potential phase-conjugating elements in the UOT and is specifically aimed at studying the properties of an optical phase conjugation process in these media. Experimental work was done on two crystals doped with Praseodymium and the phase-conjugated signal was studied as a function of different parameters with results discussed and presented in the respective section. In particular, efficient phase conjugation was observed in a 6-mm thick Pr:YSO crystal with reflectivity values reaching up to 124 \%. Further outlook and possible applications are given at the end of the thesis.
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.
Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.