Erbium-doped solids are potential candidates for the realization of a quantum memory for photons at telecommunication wavelengths. The implementation of quantum memory proposals in rare-earth-ion-doped solids require spectral tailoring of the inhomogeneous absorption profile by efficient population transfer between ground-state levels (spin polarization) using optical pumping. In this paper we investigate the limiting factors of efficient optical pumping between ground-state Zeeman levels in an erbium-doped ${\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$ crystal. We introduce two methods to overcome these limiting factors: stimulated emission using a second laser and spin mixing using radio frequency excitation. Both methods significantly improve the degree of spin polarization. Population transfer between two Zeeman levels with less than 10% of the total population in the initial ground state is achieved, corresponding to a spin polarization greater than 90%. In addition, we demonstrate spectral tailoring by isolating a narrow absorption peak within a large transparency window.
Erbium-doped solids are potential candidates for the realization of a quantum memory for photons at telecommunication wavelengths. The implementation of quantum memory proposals in rare-earth-ion-doped solids require spectral tailoring of the inhomogeneous absorption profile by efficient population transfer between ground-state levels (spin polarization) using optical pumping. In this paper we investigate the limiting factors of efficient optical pumping between ground-state Zeeman levels in an erbium-doped Y2SiO5 crystal. We introduce two methods to overcome these limiting factors: stimulated emission using a second laser and spin mixing using radio frequency excitation. Both methods significantly improve the degree of spin polarization. Population transfer between two Zeeman levels with less than 10% of the total population in the initial ground state is achieved, corresponding to a spin polarization greater than 90%. In addition, we demonstrate spectral tailoring by isolating a narrow absorption peak within a large transparency window.
Efficient optical pumping is an important tool for state initialization in quantum technologies, such as optical quantum memories. In crystals doped with Kramers rare-earth ions, such as erbium and neodymium, efficient optical pumping is challenging due to the relatively short population lifetimes of the electronic Zeeman levels, of the order of 100 ms at around 4 K. In this article we show that optical pumping of the hyperfine levels in isotopically enriched 145 Nd :Y 2 SiO 5 crystals is more efficient, owing to the longer population relaxation times of hyperfine levels. By optically cycling the population many times through the excited state a nuclear spin flip can be forced in the ground state hyperfine manifold, in which case the population is trapped for several seconds before relaxing back to the pumped hyperfine level. To demonstrate the effectiveness of this approach in applications we perform an atomic frequency comb memory experiment with 33% storage efficiency in 145 Nd :Y 2 SiO 5 , which is on a par with results obtained in non-Kramers ions, e.g. europium and praseodymium, where optical pumping is generally efficient due to the quenched electronic spin. Efficient optical pumping in neodymium-doped crystals is also of interest for spectral filtering in biomedical imaging, as neodymium has an absorption wavelength compatible with tissue imaging. In addition to these applications, our study is of interest for understanding spin dynamics in Kramers ions with nuclear spin.
Long-lived population storage in optically pumped levels of rare-earth ions doped into solids, referred to as persistent spectral hole burning, is of significant fundamental and technological interest. However, the demonstration of deep and persistent holes in rare-earth ion doped amorphous hosts, e.g., glasses, has remained an open challenge for many decades---a fact that motivates our work towards a better understanding of the interaction between impurities and vibrational modes in glasses. Here we report the observation and detailed characterization of such holes in an erbium-doped silica glass fiber cooled to below 1 K. We demonstrate population storage in electronic Zeeman sublevels of the erbium ground state with lifetimes up to 30 seconds and 80% spin polarization. In addition to its fundamental aspect, our investigation reveals a potential technological application of rare-earth ion doped amorphous materials, including at telecommunication wavelength.
Long-lived sub-levels of the electronic ground-state manifold of rare-earth ions in crystals can be used as atomic population reservoirs for photon echo-based quantum memories. We measure the dynamics of the Zeeman sub-levels of erbium ions that are doped into a lithium niobate waveguide, finding population lifetimes at cryogenic temperatures down to 0.7 K as long as seconds. Then, using these levels, we prepare and characterize atomic frequency combs (AFCs), which can serve as a memory for quantum light at 1532 nm wavelength. The results allow predicting a 0.1% memory efficiency, limited mainly by unwanted background absorption that we believe to be caused by excitation-induced erbium spin flips and frequency shifting due to two-level systems or non-equilibrium phonons. Hence, while it should be possible to create an AFC-based quantum memory in E r 3 + : T i 4 + : L i N b O 3 , improved crystal growth together with optimized AFC preparation will be required to make it suitable for applications in quantum communication.
Rare-earth ion-doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centers can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this paper, we study hyperfine and magnetic properties of a Y2SiO5 crystal doped with 171Yb3+ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin S=21 and nuclear spin I=21, which results in the simplest possible hyperfine level structure. In this work, we determine the hyperfine tensors for the ground and excited states on the optical $^{2}\mathrm{F}_{7/2}(0)\ensuremath{\longleftrightarrow}^{2}\mathrm{F}_{5/2}(0)$ transition by combining spectral hole burning and optically detected magnetic resonance techniques. The resulting spin Hamiltonians correctly predict the magnetic-field dependence of all observed optical-hyperfine transitions, from zero applied field up to fields where the Zeeman interaction is dominating the hyperfine interaction. Using the optical absorption spectrum, we can also determine the order of the hyperfine levels in both states. These results pave the way for realizing solid-state optical and microwave quantum memories based on a 171Yb3+:Y2SiO5 crystal.
Rare-earth doped crystals are promising systems for quantum information processing. In particular, paramagnetic rare earths could be used to build coherent interfaces with optical and microwave photons. In addition, isotopes with nonzero nuclear spins could provide long-lived states for quantum state storage and processing. Yb3+ is particularly interesting in this respect since it is the only paramagnetic rare earth with a spin-21 isotope, which corresponds to the simplest possible level structure. In this paper, we report on the optical and magnetic properties of Yb3+ in the two sites of Y2SiO5, a commonly used crystal for quantum applications. We measured optical inhomogeneous linewidths, peak absorption coefficients, oscillator strengths, and excited-state lifetimes. The Zeeman tensors were also determined in the ground and excited states, as well as the ground-state hyperfine tensor for the 171Yb3+ (I=21) isotope. These results suggest that Yb3+:Y2SiO5 is a promising material for applications like solid-state optical and microwave quantum memories.
The main aim of the present thesis is to demonstrate the efficient quantum memories for light employing coherent processes in rare-earth-ion-doped crystals. Rare-earth (RE) ions between lanthanum, with atomic number 57, and lutetium, with atomic number 71, have a partly filled 4f shell, which is spatially inside the full shells 5s, 5p, and 6s. Therefore, 4f-4f transitions are shielded from environmental noise. Less noise means longer lifetime and coherence times and, when the crystals are cooled down to about 4 K, these can be about 8 orders of magnitude longer than what is typical for electronic transitions in solids. In quantum information processing, we are looking for physical systems which are isolated from the environment and consequently have good coherence properties. The long coherence time of both optical and spin transitions, is the main attraction of rare-earth ions for quantum information processing. In the present thesis, we map a quantum state of light employing a 4f-4f transition of praseodymium doped in yttrium silicate. We mainly employed the ensemble approach and the atomic frequency comb (AFC) protocol for quantum memory demonstrations. Among several parameters that define quantum memory performance, we mostly focused on quantum memory efficiency. The overall memory efficiency is simply defined as the energy of the pulse recalled from the memory divided by the energy of the pulse sent in for storage in the memory. To maximize quantum memory efficiency, most protocols require high optical depth. This is a limitation for materials with rather good coherence properties but low optical depth. In the research described in the present thesis, we combined the use of a low finesse cavity and the ensemble approach and designed an impedance-match cavity to obtain the advantages of both approaches and thereby to implement an efficient quantum interface in a weakly absorbing solid-state medium. Based on the cavity configuration, we obtained 56% storage and retrieval efficiency, which is the highest storage and retrieval efficiency based on the AFC protocol reported in the research so far. In the present thesis, we demonstrated a narrow-band (about 2 MHz) spectral filter with a >30 dB intensity absorption/transmission ratio, which is based on the large (6 orders of magnitude) ratio between the inhomogeneous and homogeneous broadening of Pr3+ : Y2SiO5. Slow-light effects due to the strong dispersion created by the spectral filter improved the suppression of the filter by also utilizing the time domain. As an application, we detected weak diffuse light shifted by ultrasound from the carrier about 2 MHz, after a 9 cm thick biological tissue. The coupling between light and matter is directly related to the relative direction of the light polarization and transition dipole moment of atoms. I developed a simulation program that was able to investigate the polarization direction and ellipticity of polarization of optical radiation propagating through the crystal. This might open up new opportunities for the investigation of interesting physics regarding propagation effects and for the improvement of spectral engineering of RE ions in the future. In order to deal with the sharp homogeneous transitions of the RE ions, the frequency of our dye laser was stabilized against a highly stabilized Fabry-Perot cavity using the Pound-Drever-Hall locking scheme.