Abstract In the development of high-performance optical quantum memories, Er 3+ :CaWO 4 has emerged as a compelling rare-earth ion-doped solid-state platform owing to its long optical coherence times and compatibility with the 1550nm telecommunications band. In this work, we systematically investigate how optical polarisation and temperature influence the absorption strength, central wavelength, and linewidth of the Z 1 → Y 1 and Z 1 → Y 2 transitions, with light incident along the crystal a and c axes. We identify the Z 1 → Y 1 transition at 1532.6 nm with the incident laser propagating along the c -axis at cryogenic temperatures (∼3 K) as particularly advantageous for memory operation. Under these conditions, the transition exhibits a stable central wavelength, narrower linewidth, polarisation-independent absorption, and an enhanced absorption cross-section, while residing within the telecommunication C-band. These combined attributes position the Z 1 → Y 1 line as a robust and suitable point for Er 3+ :CaWO 4 based quantum memories.
Abstract In the development of high-performance optical quantum memories, Er 3+ :CaWO 4 has emerged as a compelling rare-earth ion-doped solid-state platform owing to its long optical coherence times and compatibility with the 1550nm telecommunications band. In this work, we systematically investigate how optical polarisation and temperature influence the absorption strength, central wavelength, and linewidth of the Z 1 → Y 1 and Z 1 → Y 2 transitions, with light incident along the crystal a and c axes. We identify the Z 1 → Y 1 transition at 1532.6 nm with the incident laser propagating along the c -axis at cryogenic temperatures (∼3 K) as particularly advantageous for memory operation. Under these conditions, the transition exhibits a stable central wavelength, narrower linewidth, polarisation-independent absorption, and an enhanced absorption cross-section, while residing within the telecommunication C-band. These combined attributes position the Z 1 → Y 1 line as a robust and suitable point for Er 3+ :CaWO 4 based quantum memories.
Polarisation and Temperature Dependence of Er3+:CaWO4 -- Towards a Solid-State Rare-Earth Ion-Doped Quantum Memory
In the endeavour of developing quantum memories, Er3+:CaWO4 has emerged as a promising rare-earth ion-doped (REID) crystal platform due to its long optical coherence times and compatibility with the 1550 nm telecommunications band. This work investigates the effects of polarisation and temperature on the absorption strength, central wavelength, and linewidth of the Z1→Y1 and Z1→Y2 optical transitions, with light incident along the crystal a and c axes. It is found that the Z1→Y1 transition at 1532.6 nm with the incident laser along the c-axis at cryogenic temperatures ($\sim$3 K) is particularly favourable. The transition exhibits a stable central wavelength, narrower linewidth, polarisation independence, larger absorption cross-section, and lies within the C-band -- attributes that make it highly suitable for quantum memory applications.
Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.
Isotopically enriched epitaxial CaWO4 thin films for Er3+ spin-photon quantum interfaces
Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability1−3. Among them, Er3+ doped CaWO4 is promising because it possesses narrow optical linewidth transitions and a long spin coherence time4−6. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% 183W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er3+ doped CaWO4 thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO4 thin films using an isotopically purified 186WO3 source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. 183W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO4 thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.
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.
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.
Rare Earth (RE) ion doped nanomaterials are promising candidates for a range of quantum technology applications. Among RE ions, the so-called Kramers' ions possess spin transitions in the GHz range at low magnetic fields, which allows for high-bandwidth multimode quantum storage, fast qubit operations as well as interfacing with superconducting circuits. They also present relevant optical transitions in the infrared. In particular, Er3+ has an optical transition in the telecom band, while Nd3+ presents a high-emission-rate transition close to 890 nm. In this paper, we measure spectroscopic properties that are of relevance to using these materials in quantum technology applications. We find the inhomogeneous linewidth to be 10.7 GHz for Er3+ and 8.2 GHz for Nd3+, and the excited state lifetime T1 to be 13.68 ms for Er3+ and $540\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ for Nd3+. We study the dependence of homogeneous linewidth on temperature for both samples, with the narrowest linewidth being 379 kHz (T2=839 ns) for Er3+ measured at 3 K, and 62 kHz (${T}_{2}=5.14\phantom{\rule{4pt}{0ex}}\textmu{}\mathrm{s}$) for Nd3+ measured at 1.6 K. Further, we investigate time-dependent homogeneous linewidth broadening due to spectral diffusion and the dependence of the homogeneous linewidth on magnetic field to get additional clarity of mechanisms that can influence the coherence time. In light of our results, we discuss two applications: single qubit-state readout and a Fourier-limited single photon source.