Abstract : The research objective of this Directors Research Initiative was to work on developing solid-state quantum memory using cryogenically cooled rare-earth-ion-doped crystal, Nd3 :GaN. The samples were grown using the US Army Research Laboratorys molecular beam epitaxy (MBE) capabilities. The approach is based on the coherent transient interaction between light and the ions in a semiconductor. We investigated the energy level structure of the neodymium (Nd) ions embedded into the semiconductor crystal lattice, gallium nitride (GaN), and developed a quantum description of the 2- and 3-pulse photon echo effect. Epitaxial GaN:Nd was grown by plasma-assisted molecular beam epitaxy in a modular Gen II reactor using liquid gallium, solid Nd, and a nitrogen plasma. The photoluminescence (PL) spectrum from the lowest 4F3/2 multiplet to all 4I9/2 multiplets was measured by a free-space variable amplifier silicon diode. A demonstration of the coherence properties requires a high-quality sample with a narrow homogeneous broadening. For this reason, the PL linewidth was characterized for various growth conditions. The experiments were carried out to observe coherent effects, and various experimental setups are described. In parallel with experiments on the coherence properties of Nd3 :GaN, we also investigated the effect of a varying electric field on the Nd PL spectrum to provide a tunable memory. To vary the applied field, we designed and grew a series of Nd-doped GaN p-i-n structures, strain-balanced superlattice structures, and periodic unbalanced structures.
Abstract : The research objective of this Directors Research Initiative was to work on developing solid-state quantum memory using cryogenically cooled rare-earth-ion-doped crystal, Nd3 :GaN. The samples were grown using the US Army Research Laboratorys molecular beam epitaxy (MBE) capabilities. The approach is based on the coherent transient interaction between light and the ions in a semiconductor. We investigated the energy level structure of the neodymium (Nd) ions embedded into the semiconductor crystal lattice, gallium nitride (GaN), and developed a quantum description of the 2- and 3-pulse photon echo effect. Epitaxial GaN:Nd was grown by plasma-assisted molecular beam epitaxy in a modular Gen II reactor using liquid gallium, solid Nd, and a nitrogen plasma. The photoluminescence (PL) spectrum from the lowest 4F3/2 multiplet to all 4I9/2 multiplets was measured by a free-space variable amplifier silicon diode. A demonstration of the coherence properties requires a high-quality sample with a narrow homogeneous broadening. For this reason, the PL linewidth was characterized for various growth conditions. The experiments were carried out to observe coherent effects, and various experimental setups are described. In parallel with experiments on the coherence properties of Nd3 :GaN, we also investigated the effect of a varying electric field on the Nd PL spectrum to provide a tunable memory. To vary the applied field, we designed and grew a series of Nd-doped GaN p-i-n structures, strain-balanced superlattice structures, and periodic unbalanced structures.
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.
Quantum light-matter interfaces that reversibly map the quantum state of photons onto the quantum states of atoms, are essential components in the quantum engineering toolbox with applications in quantum communication, computing, and quantum-enabled sensing. In this talk I present our progress towards developing on-chip quantum light-matter interfaces based on nanophotonic resonators fabricated in rare-earth-doped crystals known to exhibit the longest optical and spin coherence times in the solid state. We recently demonstrated coherent control of neodymium (Nd3+) ions coupled to yttrium orthosilicate Y2SiO5 (YSO) photonic crystal nano-beam resonator. The coupling of the Nd3+ 883 nm 4I9/2-4F3/2 transition to the nano-resonator results in a 40 fold enhancement of the transition rate (Purcell effect), and increased optical absorption (~80%) - adequate for realizing efficient optical quantum memories via cavity impedance matching. Optical coherence times T2 up to 100 μs with low spectral diffusion were measured for ions embedded in photonic crystals, which are comparable to those observed in unprocessed bulk samples. This indicates that the remarkable coherence properties of REIs are preserved during nanofabrication process. Multi-temporal mode photon storage using stimulated photon echo and atomic frequency comb (AFC) protocols were implemented in these nano-resonators. Our current technology can be readily transferred to Erbium (Er) doped YSO devices, therefore opening the possibility of efficient on-chip optical quantum memory at 1.5 μm telecom wavelength. Integration with superconducting qubits can lead to devices for reversible quantum conversion of optical photons to microwave photons.
Development of a Scalable Quantum Memory Platform -- Materials Science of Erbium-Doped TiO2 Thin Films on Silicon
Rare-earth ions (REI) have emerged as an attractive candidate for solid-state qubits, particularly as a quantum memory. Their 4f-4f transitions are shielded by filled 5s and 5p orbitals, offering a degree of protection from external electric fields. Embedded within a thin film oxide host, REIs could enable a qubit platform with significant memory capabilities. Furthermore, a silicon-compatible thin film form factor would enable the use of standard semiconductor fabrication processes to achieve chip-based integrability and scalability for functional quantum networks. Towards this goal, we have carried out optical and microstructural studies of erbium-doped polycrystalline and epitaxial TiO2 thin films on Si (100), r-sapphire, and SrTiO3 (100). We observe that the inhomogeneous optical linewidth of the Er photoluminescence is comparable or better for polycrystalline Er:TiO2(grown on Si) in comparison to single crystal epitaxial films on sapphire or SrTiO3, implying a relative insensitivity to extended defects. We investigated the effect of the film/substrate and film/air interface and found that the inhomogeneous linewidth and spectral diffusion can be significantly improved via bottom buffer and top capping layers of undoped TiO2. Using such approaches, we obtain inhomogeneous linewidths of 5.2 GHz and spectral diffusion of 180 MHz in Er:TiO2 /Si(100) films and have demonstrated the engineerability of quantum-relevant properties in these thin films.
This thesis describes experiments aimed at developing a key component in applications such as quantum networks and long-distance quantum communication systems: quantum memories. Quantum memories for light using photon-echo and coherent rephrasing techniques have been developed. The work is carried out on rare-earth-ion-doped inorganic crystals. Several properties are associated with these crystals such as long coherence times and long-lived ground state sublevels that are particularly interesting in connection applications in the area of quantum information science. It is demonstrated the preparation of optical inhomogeneous absorption profiles such that the light only interacts with a specific transition at a selected frequency. Narrow absorbing structures with widths of <100 kHz have been prepared with no absorption in the surrounding spectral interval. Most of the experiments were carried out using Pr3+:Y2SiO5. However, in our search for suitable a Λ-system in the material under consideration, we also performed spectral hole-burning spectroscopy in Nd:Y2SiVO4. As part of the search for host materials for Pr, Pr:La2(WO4)3 crystal was characterized using a variety of methods, such as, hole burning and photon-echoes. Electromagnetically induced transparency was also observed in this crystal. The most important criteria for evaluating quantum memory performance and the most important physical requirements are discussed. After investigating the standard photon echo techniques and controlled reversible inhomogeneous broadening (CRIB) for quantum state storage, we considered an efficient multimode quantum memory protocol; the atomic frequency comb (AFC) protocol. Combs with peaks of widths 100-300 kHz and an optical depth of~ 10 were created by optical pumping inside an emptied region of the inhomogeneous profile of Pr3+:Y2SiO5, allowing us to improve the efficiency of light storage. Light storage combining a photon-echo technique based on an AFC and spin-wave storage have been demonstrated, and an experimental AFC scheme for the storage of weak coherent light pulses in Pr3+:Y2SiO5 is presented. Finally, we have investigated superradiance and slow light effects. Both these effects occur in the high optical depth regime and can influence the memory performance. Under certain conditions superradiance results in the immediate re-emission of the stored light in a single burst of coherent radiation, and inside spectrally structured materials, slow light effects may result when storage is performed.
Coherent quantum devices play a central role in quantum science and engineering. Rare-earth ions such as erbium in solids feature numerous 4f- intra-shell transitions that are effectively shielded from their crystalline surroundings by closed outer shells, allowing for long spin coherence times and narrow optical transitions. Recent ensemble experiments have established the rare-earth doped crystals as the leading materials for optical quantum memories. However, the development of large-scale quantum devices based on rare-earth doped materials has remained a challenge. Here we describe a scalable quantum photonic platform based on epitaxially grown oxide thin films doped with trivalent ions on silicon substrates. The platform builds upon the recent developments of high quality epitaxial rare-earth doped oxides on silicon, and highlights the integration of quantum coherent materials with existing silicon technologies for ultimate device scalability. The proposed device platform builds upon our capability to epitaxially grow high quality, near-lattice-matched Y2O3 thin films on silicon. The epitaxial thin film is of high structural quality and offers several distinct advantages: (1) significantly less optical loss and better quantum emitter coherence; (2) atomic precision placement of rare-earth emitters (via delta doping) with respect to the photonic mode for controllable ion-photon coupling; (3) scalable top-down device fabrication using standard lithography and etching techniques; (4) heterogeneous integration with silicon takes full advantage of existing silicon photonics technologies for routing, tuning, and modulation of the quantum emission from rare-earth ions.
This thesis describes a number of coherent processes, such as quantum information processing, superradiance and electromagnetically induced transparency, which have been experimentally implemented using rare-earth-ion-doped crystals. The rare-earths are a class of elements that have in common, an atomic structure that allows for very long lifetimes as well as coherence times, both on optical transitions and on spin transitions. These ions can be naturally trapped inside host crystals, and with the phonon vibrations removed by cooling down to cryogenic temperatures (< 4 K), they can be used for a number of different quantum information processes. Most experiments were carried out using PrYSO, but also other crystal types were investigated, such as Nd:YVO4, and La2(WO4)3. The characterization of the ions were done with a variety of methods, including among others, photon echo techniques and electromagnetically induced transparency. Quantum computing is a rapidly growing field and there are still many potential candidates for its implementation. In our work we have utilized the spin states of the Pr rare-earth ion as a qubit, and demonstrated arbitrary single qubit gates, which are important pieces towards a quantum computing realization in these systems. Most of the experimental work done for the thesis was carried out using an ensemble approach, that has the advantage of giving a strong readout signal, but for future scaling to multiple qubits, single instances are more promising, which is discussed. Quantum memories are crucial components in applications such as quantum networks and long distance quantum communication. In this thesis, work has been done to investigate how quantum memories can be implemented in rare-earth crystals. In particular, there are two protocols, CRIB and AFC, which were suggested with rare-earth crystals directly in mind, and both of these require high optical depth, for maximum recall efficiency. In this thesis, implications of being in the high optical depth regime, with phenomena such as superradiance, a collective effect that could cause the stored light to be immediately reemitted, and slow light effects that come from performing the storage inside spectrally structured materials, were investigated. In order to carry out the phase-sensitive experiments, a laser system with a very narrow linewidth of ~1 kHz at 606 nm was constructed, by locking the laser to a semi-persistent spectral hole. In addition, many experiments required advanced pulse shapes, such as complex sechyp pulses or pulses obtained from optimal control theory. In order to be able to accurately create such shapes, an elaborate system using an arbitrary waveform generator and two well calibrated AOMs, controlled from a computer, was also built.