We present general guidelines for finding solid-state systems that could serve as coherent electronspin-photon interfaces even at relatively high temperatures, where phonons are abundant but cooling is easier, and show that transition-metal ions in various crystals could comply with these guidelines.As an illustrative example, we focus on divalent nickel ions in magnesium oxide.We perform electron-spinresonance spectroscopy and polarization-sensitive magneto-optical fluorescence spectroscopy of a dense ensemble of these ions and find that (i) the ground-state electron spin stays coherent at liquid-helium temperatures for several microseconds and (ii) there exist energetically well-isolated excited states that can couple to two ground-state spin sublevels via optical transitions of orthogonal polarizations.The latter implies that fast coherent optical control over the electron spin is possible.We then propose schemes for optical initialization and control of the ground-state electron spin using polarized optical pulses, as well as two schemes for implementing a noise-free broadband quantum optical memory at near-telecom wavelengths in this material system.
We present general guidelines for finding solid-state systems that could serve as coherent electronspin-photon interfaces even at relatively high temperatures, where phonons are abundant but cooling is easier, and show that transition-metal ions in various crystals could comply with these guidelines.As an illustrative example, we focus on divalent nickel ions in magnesium oxide.We perform electron-spinresonance spectroscopy and polarization-sensitive magneto-optical fluorescence spectroscopy of a dense ensemble of these ions and find that (i) the ground-state electron spin stays coherent at liquid-helium temperatures for several microseconds and (ii) there exist energetically well-isolated excited states that can couple to two ground-state spin sublevels via optical transitions of orthogonal polarizations.The latter implies that fast coherent optical control over the electron spin is possible.We then propose schemes for optical initialization and control of the ground-state electron spin using polarized optical pulses, as well as two schemes for implementing a noise-free broadband quantum optical memory at near-telecom wavelengths in this material system.
All-optical addressing and coherent control of single solid-state based quantum bits is a key tool for fast and precise control of ground-state spin qubits. So far, all-optical addressing of qubits was demonstrated only in a very few systems, such as color centers and quantum dots. Here, we perform high-resolution spectroscopic of native and implanted single rare earth ions in solid, namely, a cerium ion in yttrium aluminum garnet (YAG) crystal. We find narrow and spectrally stable optical transitions between the spin sublevels of the ground and excited optical states. Utilizing these transitions we demonstrate the generation of a coherent dark state in electron spin sublevels of a single Ce^{3+} ion in YAG by coherent population trapping.
Abstract Color centers in wide-bandgap semiconductors are attractive systems for quantum technologies since they can combine long-coherent electronic spin and bright optical properties. Several suitable centers have been identified, most famously the nitrogen-vacancy defect in diamond. However, integration in communication technology is hindered by the fact that their optical transitions lie outside telecom wavelength bands. Several transition-metal impurities in silicon carbide do emit at and near telecom wavelengths, but knowledge about their spin and optical properties is incomplete. We present all-optical identification and coherent control of molybdenum-impurity spins in silicon carbide with transitions at near-infrared wavelengths. Our results identify spin S = 1/2 for both the electronic ground and excited state, with highly anisotropic spin properties that we apply for implementing optical control of ground-state spin coherence. Our results show optical lifetimes of ~60 ns and inhomogeneous spin dephasing times of ~0.3 μs, establishing relevance for quantum spin-photon interfacing.
We report on optical detection of a single photostable Ce(3+) ion in an yttrium aluminium garnet (YAG) crystal and on its magneto-optical properties at room temperature. The spin quantum state of the emitting level of a single cerium ion in YAG can be initialized by a circularly polarized laser pulse. Coherent precession of the electron spin is read out by observing temporal behavior of circularly polarized fluorescence of the ion. This implies direct mapping of the spin quantum state of Ce(3+) ion onto the polarization state of the emitted photon and represents the quantum interface between a single spin and a single photon.
Spin-photon interfaces based on solid-state defects are key building blocks for scalable quantum networks and hybrid quantum platforms. Optimizing light-matter coupling in these systems requires precise knowledge of the optical transition dipole polarization, yet for many promising quantum emitters this quantity is hard to determine and therefore remains poorly characterized. Here, we develop a framework for reconstructing electric transition dipole polarization in spin-1/2 solid-state defects directly from ensemble spectroscopy. The approach combines the response of photoluminescence spectra to magnetic field, optical polarization, and strain. Applied to erbium ions in silicon, a particularly challenging system containing multiple crystallographic subsites, the framework identifies strain-induced shifts as the origin of asymmetric ensemble spectra and enables simultaneous determination of the optical dipole polarization and strain-orbital coupling tensor. The resulting model predicts how cavity-ion coupling depends on crystallographic orientation and magnetic-field direction, which we verify using single erbium ions coupled to a nanophotonic cavity. Together, these results establish a broadly applicable route for extracting microscopic properties of solid-state quantum emitters from ensemble spectroscopy and for engineering optimized spin-photon and spin-phonon interfaces.
Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. They are intensively studied as the most promising candidates for the realization of solid-state quantum bits. However, these systems coupled to a complex environment which can result in rapid loss of spin coherence or optical instability. Finding an alternative solid-state single system with remarkable optical and spin properties is the motivation of this dissertation. Rare earth ions doped in inorganic crystal hosts provide promises not only by the high quality factor 4f-4f optical transitions but also by the well preserved and long-lived spin states, with the applications from solid-state laser spectroscopy to quantum information processing. However, for almost three decades, not being able to identify single rare earth elements in solids is the obstacle to achieve their full potential functionality. We demonstrated the first direct optical detection of single rare earth ions (praseodymium) in solids in 2012. This research was covered in my Master Degree Thesis. This dissertation presents experimental progress in optically detecting other single rare earth species in crystals, understanding their fundamental spectroscopy properties and coherently controlling them, which is mainly focused on single trivalent cerium ions in different host materials. Following the optical detection of single cerium ions in yttrium aluminum garnet (YAG), the optical and spin properties of single Ce ions are investigated. Single Ce ions show good photostability under the pulsed laser excitation. Still, like in other solid emitters, photo-induced dynamics of single Ce ions is observed, however, in a counterintuitive way under the continuous laser irradiation. To understand this behavior, we proposed a charge dynamics model, and developed a novel method to suppress this undesired charge dynamics. With this approach, we obtain the photoluminescence excitation spectrum of single Ce ions in YAG under a CW laser excitation. Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. We show the spin state has a coherence time of 290 ns, which is dominated by the surrounding aluminum nuclear spin bath and impurities induced electron spin bath. The coherence time can be extended to 2 ms through dynamical decoupling method, which approaches closely to the upper limit 4.5 ms due to spin-lattice relaxation. This result indicates single Ce electron spin can be a good solid-state qubit. With the combination of optical and spin manipulations of single Ce ions, a quantum interface between a single spin and a single photon is observed by monitoring the temporal behavior of circularly polarized emission photons from the ion. We obtain the Larmor precession of the excited spin state, indicating the direct mapping of the excited spin states of single Ce ions onto the polarization states of the fluorescence photons. Furthermore, with both optical and spin access, we all-optically demonstrate coherent population trapping of a single Ce spin qubit. To scale up the system for further applications, we present the nano-scale engineering of rare earth species in YAG crystal, with the acquirement of the production yield of Ce and Pr implantation (53 and 91% respectively). The optical and spin properties of single implanted Ce ions show fairly good performance, which paves the way towards coherent coupling of single rare earth qubits in a small volume. Besides the study of single Ce ions, the spectroscopy properties of single praseodymium ions in YAG crystal are investigated. We obtain the photoluminescence excitation spectrum and the hyperfine splitting of a single praseodymium ion. All-optical control of a single praseodymium ion is achieved. In this dissertation, we solve the key problem of optically detecting, spectrally studying and coherently manipulating single rare earth ions in solids. The developed methods including optical detection, initialization, readout, coherent control and nanoscale production of single rare earth elements in crystals offer novel and powerful tools for understanding and exploring the fundamental spectroscopy properties of single rare earth elements in solids. It paves a way towards constructing scalable quantum network based on single rare earth solid-state qubits.
Rare-earth related electron spins in crystalline hosts are unique material systems, as they can potentially provide a direct interface between telecom band photons and long-lived spin quantum bits. Specifically, their optically accessible electron spins in solids interacting with nuclear spins in their environment are valuable quantum memory resources. Detection of nearby individual nuclear spins, so far exclusively shown for few dilute nuclear spin bath host systems such as the nitrogen-vacancy center in diamond or the silicon vacancy in silicon carbide, remained an open challenge for rare earths in their host materials, which typically exhibit dense nuclear spin baths. Here, we present the electron spin spectroscopy of single Ce^{3+} ions in a yttrium orthosilicate host, featuring a coherence time of T_{2}=124 μs. This coherent interaction time is sufficiently long to isolate proximal ^{89}Y nuclear spins from the nuclear spin bath of ^{89}Y. Furthermore, it allows for the detection of a single nearby ^{29}Si nuclear spin, native to the host material with ∼5% abundance. This study opens the door to quantum memory applications in rare-earth ion related systems based on coupled environmental nuclear spins, potentially useful for quantum error correction schemes.