Single site optical spectroscopy of coupled Er 3+ ion pairs in silicon
Guangchong Hu, Rose L. Ahlefeldt, Gabriele G. de Boo, Alexey Lyasota, Brett C. Johnson, Jeffrey Colin McCallum, Matthew J. Sellars, Chunming Yin, Sven M. J. Rogge
Abstract Individual optical emitters coupled via coherent interactions are attractive qubits for quantum communications applications. Here, we present the first study of single pairs of interacting rare earth ions and determine the interactions between ions in the pair with high resolution. We identify two examples of Er 3+ pair sites in Er implanted Si and characterise the interactions using optical Zeeman spectroscopy. We identify one pair as two Er 3+ ions in sites of at least C 2 symmetry coupled via a large, 200 GHz, Ising-like spin interaction in both optical ground and excited states. The high measurement resolution allows non-Ising contributions to the interaction of < 1 % to be observed, attributed to site distortion. By bringing two optical transitions into resonance with a magnetic field, we observe a 0.8 GHz optical interaction of unusual magnetic-dipole/electric-dipole character with strong polarization selection rules. We discuss the use of this type of strongly coupled, field-tunable rare earth pair system for quantum processing.
Abstract Individual optical emitters coupled via coherent interactions are attractive qubits for quantum communications applications. Here, we present the first study of single pairs of interacting rare earth ions and determine the interactions between ions in the pair with high resolution. We identify two examples of Er 3+ pair sites in Er implanted Si and characterise the interactions using optical Zeeman spectroscopy. We identify one pair as two Er 3+ ions in sites of at least C 2 symmetry coupled via a large, 200 GHz, Ising-like spin interaction in both optical ground and excited states. The high measurement resolution allows non-Ising contributions to the interaction of < 1 % to be observed, attributed to site distortion. By bringing two optical transitions into resonance with a magnetic field, we observe a 0.8 GHz optical interaction of unusual magnetic-dipole/electric-dipole character with strong polarization selection rules. We discuss the use of this type of strongly coupled, field-tunable rare earth pair system for quantum processing.
In this paper, we use electrically detected optical excitation spectroscopy of individual erbium ions in silicon to determine their optical and paramagnetic properties simultaneously. We demonstrate that this high spectral resolution technique can be exploited to observe interactions typically unresolvable in silicon using conventional spectroscopy techniques due to inhomogeneous broadening. In particular, we resolve the Zeeman splitting of the 4I15/2 ground and 4I13/2 excited state separately, and in strong magnetic fields, we observe the anticrossings between Zeeman components of different crystal-field levels. We discuss the use of this electronic detection technique to aid in the identification of the symmetry and structure of erbium sites in silicon.
This thesis investigates the potential of Er:YSO and Er:Si for quantum communication and computation applications. Erbium uniquely possess optical transitions in the 1.5 um region, making it suitable for both fibre telecommunication and silicon photonics. The properties of the I15/2↔I13/2 optical transition in Er:YSO have already been extensively studied. Over two decades ago, improvements in Er3+ dephasing time at 1.5 um were achieved by applying a 5T field along the D1 axis. More recently, a record 4.4 ms coherence time on the same optical transition was achieved using a 7T field. These investigations, among others, illustrate that large Er electron spins become thermally polarised with sufficient magnetic field. However, no long lived and coherent spin transitions associated with the Er ions had previously been identified, and such transitions are necessary for on-demand quantum state storage. To address this requirement, the optical and hyperfine transition properties of 167-Er:YSO were investigated in large magnetic fields. In a field of 7T, spectral hole lifetimes of 1 minute and hyperfine population lifetimes of 12 minutes were observed. These measurements illustrate the effect of spin-lattice relaxation in this system, and how it can be mitigated. Efficient spin-polarisation of the entire 167-Er hyperfine ensemble is also demonstrated. This is the first such demonstration in rare earth systems, and a key requirement for broadband optical storage. Moreover, a 1.3 second coherence time was recorded for an 167-Er:YSO hyperfine transition at 7T and 1.4 K. This is an improvement of several orders-of-magnitude over previous coherence measurements on spin-transitions in Er doped solids. This is also sufficient for maximal entanglement rates in quantum repeater networks that span distances of 1000 km or greater. With an optical transition at 1.5 um, Er is also an ideal candidate to connect silicon based quantum computers to the future quantum Internet. In particular, single Er:Si ions could be used to develop an optical-spin bus between P:Si qubits and fibre based quantum networks. Presented here is the first spectroscopic investigation of single Er:Si ions. This required a novel opto-electronic approach to single ion detection, where the Er ions are implanted into a nanometre scale fin-shaped Field Effect Transistor. With this approach it was possible to develop high resolution optical spectra, where both the electronic and hyperfine levels of individual Er ions were resolved. Long optical and spin coherence times are also important requirements for an optical-spin bus. To address the first requirement, an investigation of the optical lineshape was undertaken. Here it was determined that sources of Stark noise external to the transistor channel contribute a significant amount to optical homogeneous linewidth. However, the dominant noise contribution was determined to be short-range (from within the 30 nm wide channel) and the total homogeneous linewidth was measured to be 50 MHz. The site structure of an individual Er:Si ion was then analysed, using magnetic field rotation patterns and optical transitions between multiple crystal field levels. This site was determined to have approximately axial (C3) symmetry. The purpose of this study was to determine a magnetic field regime in which the Er electrons spin can be polarised, which is necessary for realising of long hyperfine lifetimes and coherence times.
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.
Er-doped Si is a promising candidate for quantum information applications due to its telecom wavelength optical transition and its compatibility with Si nanofabrication technologies. Recent spectroscopic studies based on photoluminescence excitation have shown multiple well-defined lattice sites that Er occupies in Si. Here we report a measurement of the Zeeman and hyperfine tensors of a single Er3+167 ion in Si. All the obtained tensors are highly anisotropic with the largest value principal axes aligning in nearly the same direction, and the trace of the lowest crystal field level g-tensor is 17.78±0.40. The results indicate that this specific Er site is likely to be a distorted cubic site that exhibits monoclinic (C1) symmetry. Finally, zero first-order-Zeeman fields are identified for this site and could be used to reduce decoherence of hyperfine spin states in future experiments.
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.
Er-doped Si is a promising candidate for quantum information applications due to its telecom wavelength optical transition and its compatibility with Si nanofabrication technologies. Recent spectroscopic studies based on photoluminescence excitation have shown multiple well-defined lattice sites that Er occupies in Si. Here we report a measurement of the Zeeman and hyperfine tensors of a single 167Er3+ ion in Si. All the obtained tensors are highly anisotropic with the largest value principal axes aligning in nearly the same direction, and the trace of the lowest crystal field level g-tensor is $17.78\ifmmode\pm\else\textpm\fi{}0.40$. The results indicate that this specific Er site is likely to be a distorted cubic site that exhibits monoclinic (C1) symmetry. Finally, zero first-order-Zeeman fields are identified for this site and could be used to reduce decoherence of hyperfine spin states in future experiments.