We explore optical coherence and spin dynamics of an isotopically purified 166 Er: 7 LiYF 4 crystal below 1 K and at weak magnetic fields < 0.3T. Crystals were grown in our lab and demonstrate narrow inhomogeneous optical broadening down to 16 MHz. Solid-state atomic ensembles with such narrow linewidths are very attractive for implementing of off-resonant Raman quantum memory and for the interfacing of superconducting quantum circuits and telecom C-band optical photons. Both applications require a low magnetic field of ∼10 mT. However, at conventional experimental temperatures T > 1.5 K, optical coherence of Er:LYF crystal attains time scale only at strong magnetic fields above 1.5 T. In the present work, we demonstrate that the deep freezing of Er:LYF crystal below 1 K results in the increase of optical coherence time to at weak fields.
We explore optical coherence and spin dynamics of an isotopically purified 166 Er: 7 LiYF 4 crystal below 1 K and at weak magnetic fields < 0.3T. Crystals were grown in our lab and demonstrate narrow inhomogeneous optical broadening down to 16 MHz. Solid-state atomic ensembles with such narrow linewidths are very attractive for implementing of off-resonant Raman quantum memory and for the interfacing of superconducting quantum circuits and telecom C-band optical photons. Both applications require a low magnetic field of ∼10 mT. However, at conventional experimental temperatures T > 1.5 K, optical coherence of Er:LYF crystal attains time scale only at strong magnetic fields above 1.5 T. In the present work, we demonstrate that the deep freezing of Er:LYF crystal below 1 K results in the increase of optical coherence time to at weak fields.
Enhancement of optical coherence in 167Er:Y2SiO5 crystal at sub-Kelvin temperatures
Er3+:Y2SiO5 crystal is a promising candidate with a great variety of its potential applications in quantum information processing and quantum communications ranging from optical/microwave quantum memories to circuit QED and microwave-to-optics frequency converters. Some of the above listed applications require ultra-low temperature environment, i.e., temperatures T≲0.1K. Most of the experiments with erbium doped crystals have been so far carried out at temperatures above 1.5~K. Therefore, only little information is known about Er3+:Y2SiO5 coherence properties at millikelvins. Here, we investigate optical decoherence of 167Er:Y2SiO5 crystal by performing 2- and 3-pulse echo experiments at millikelvin temperature range and at weak and moderate magnetic fields. We show that the deep freezing of the crystal results in an increase of optical coherence time by one order of magnitude compared to temperature of 1.5 Kelvin and magnetic field of $\sim$0.2~T, taken as a reference point. We further describe the detailed investigation of the decoherence mechanisms in this regime.
The longitudinal and transverse relaxation times for a transition between hyperfine sublevels of the lower electronic states of the 4 I 15/2 and 4 I 9/2 multiplets of 167 Er 3+ ions in 7 LiYF 4 crystals have been determined for the first time using two-pulse and stimulated photon echo measurements in zero magnetic field at a temperature of 4 K. The decay of the photon echo signal has been shown to be modulated, which is tentatively attributed to the superhyperfine interaction of the 167 Er 3+ ions with their 19 F − nearest neighbours. The contributions of various types of interaction to the ultranarrow linewidth (~24 MHz) of the transition in question are discussed. Our results demonstrate that this optical transition of the 167 Er 3+ ion in 7 LiYF 4 crystals is potentially attractive for use in Raman quantum memory schemes.
Rare-earth ions in solid-state hosts exhibit low homogeneous broadening and long spin coherence at cryogenic temperatures thus making them a promising candidate for optical quantum memories [1], optical-microwave transducers [2] and single dopant-based devices such as single photon emitters operating at the telecommunication wavelengths [3]. Here, we present an overview of the spin and optical properties of Er ensembles in Si accessed via resonant photoluminescence excitation (PLE) spectroscopy [4]. Samples were positioned directly on top of tailor-fabricated superconducting single photon detectors, placed in a dilution refrigerator unit and resonantly excited using fiber optics. Our method provided high collection efficiency and allowed spectral measurements of low Er density samples. The observed Er PLE spectra were strongly affected by the presence of co-dopants such as O, B or P reflecting their influence on the formation of optically active Er sites and corresponding Er optical transition energies. Higher O densities resulted in especially rich PLE spectra suggesting that a variety of Er-O complexes formed due to O doping. Lowering the O concentration, we achieved PLE spectra dominated by a single Er site in P doped samples. Interestingly, the Er spin relaxation and optical coherence properties were barely affected by the employed co-dopants and mainly depended on the Er concentration. By lowering the Er concentration from relatively high (1018cm-3) to low densities (1016cm-3), we were able to increase Er spin lifetimes from ~0.1 s to ~30 s. Long spin relaxation times allowed us to identify PLE spectra of new Er sites in Si. In both concentration regimes, we observed sub-MHz transient spectral holes suggesting long optical coherence times. Furthermore, we observed sub-MHz spin transitions in both natural and isotopically purified Si and achieved spin coherence times above 1 ms in isotopically purified Si. Narrow optical linewidths and long transverse and longitudinal spin relaxation times show that Er in Si is an excellent candidate for future quantum information and communication applications.
We obtain a low optical inhomogeneous linewidth of 25 MHz in the stoichiometric rare-earth crystal EuCl_{3}·6H_{2}O by isotopically purifying the crystal in ^{35}Cl. With this linewidth, an important limit for stoichiometric rare-earth crystals is surpassed: the hyperfine structure of ^{153}Eu is spectrally resolved, allowing the whole population of ^{153}Eu^{3+} ions to be prepared in the same hyperfine state using hole-burning techniques. This material also has a very high optical density, and can have long coherence times when deuterated. This combination of properties offers new prospects for quantum information applications. We consider two of these: quantum memories and quantum many-body studies. We detail the improvements in the performance of current memory protocols possible in these high optical depth crystals, and describe how certain memory protocols, such as off-resonant Raman memories, can be implemented for the first time in a solid-state system. We explain how the strong excitation-induced interactions observed in this material resemble those seen in Rydberg systems, and describe how these interactions can lead to quantum many-body states that could be observed using standard optical spectroscopy techniques.
When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.
Using a low-strain, isotopically pure crystal of YLiF4, we have measured extremely narrow inhomogeneous linewidths (as low as 40 MHz) for the optical transitions of Er3+ impurities. Inhomogeneous broadening due to strains and other defects is so low that a new mechanism limits the inhomogeneous linewidth: local magnetic fields due to fluorine nuclear spins. These ultranarrow lines enabled us to make the first direct measurement of the isotope shifts of f-f transitions in a solid, and we find for the isotopes 164Er, 166Er, 168Er, and 170Er a shift of 76\ifmmode\pm\else\textpm\fi{}2 MHz unit mass on the 4I15/2(1)4F9/2(1) transition. We show that this is consistent with a mechanism of coupling to zero-point vibrations.