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Negatively charged group-IV defects in diamond show great potential as quantum network nodes due to their efficient spin-photon interface. However, reaching sufficiently long coherence times remains a challenge. In this work, we demonstrate coherent control of germanium vacancy center (GeV) at millikelvin temperatures and extend its coherence time by several orders of magnitude to more than 20 ms. We model the magnetic and amplitude noise as an Ornstein-Uhlenbeck process, reproducing the experimental results well. The utilized method paves the way to optimized coherence times of group-IV defects in various experimental conditions and their successful applications in quantum technologies

Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this study, we report the coherent optical property of a single negatively-charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform-limit estimated from the lifetime measurement. We observe four orders of magnitude different linewidths of the two zero-phonon-lines, and find that that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Due to the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond., Comment: 13 pages,4 figures

While nitrogen-vacancy (NV-) centers have been extensively investigated in the context of spin-based quantum technologies, the spin-state readout is conventionally performed optically, which may limit miniaturization and scalability. Here, we report photoelectric readout of ground-state cross-relaxation features, which serves as a method for measuring electron spin resonance spectra of nanoscale electronic environments and also for microwave-free sensing. As a proof of concept, by systematically tuning NV centers into resonance with the target electronic system, we extracted the spectra for the P1 electronic spin bath in diamond. Such detection may enable probing optically inactive defects and the dynamics of local spin environment. We also demonstrate a magnetometer based on photoelectric detection of the ground-state level anticrossings (GSLAC), which exhibits a favorable detection efficiency as well as magnetic sensitivity. This approach may offer potential solutions for determining spin densities and characterizing local environment.

Striving for nanometer-sized solid-state single-photon sources, we investigate atom-like quantum emitters based on single germanium vacancy (GeV) centers isolated in crystalline nanodiamonds (NDs). Cryogenic characterization indicated symmetry-protected and bright (> 10^6 counts/s with off-resonance excitation) zero-phonon optical transitions with up to 6-fold enhancement in energy splitting of their ground states as compared to that found for GeV centers in bulk diamonds (i.e., up to 870 GHz in highly strained NDs vs 150 GHz in bulk). Utilizing lithographic alignment techniques, we demonstrate an integrated nanophotonic platform for deterministic interfacing plasmonic waveguides with isolated GeV centers in NDs that enables 10-fold enhancement of single-photon decay rates along with the emission direction control by judiciously designing and positioning a Bragg reflector. This approach allows one to realize the unidirectional emission from single-photon dipolar sources introducing a novel method that is alternative to the propagation-direction-dependent techniques based on chiral interactions or topological protection. The developed plasmon-based nanophotonic platform opens thereby new perspectives for quantum nanophotonics in general and for realizing entanglement between single photons and spin qubits, in particular.

In this work, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6 ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This work paves the way towards realization of building blocks of quantum hardware with an efficient spin-photon interface based on the SiV color center coupled to a long lasting nuclear memory., Comment: 6 pages, 4 figures

Tin-vacancy (SnV) color centers were created in diamond by ion implantation and subsequent high temperature annealing up to 2100 {\deg}C at 7.7 GPa. The first-principles calculation suggests that the large atom of tin can be incorporated into the diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The SnV center shows a sharp zero phonon line at 619 nm at room temperature. This line splits into four peaks at cryogenic temperatures with a larger ground state splitting of ~850 GHz than those of color centers based on other IV group elements, silicon-vacancy (SiV) and germanium vacancy (GeV) centers. The excited state lifetime was estimated to be ~5 ns by Hanbury Brown-Twiss interferometry measurements on single SnV quantum emitters. The order of the experimentally obtained optical transition energies comparing with the SiV and GeV centers is good agreement with the theoretical calculations., Comment: 10 pages, 4 figures and Supplementary 3 pages, 2 figures

The investigation of single atoms in solids, with both optical and nuclear spin access is of particularly interest with applications ranging from nanoscale sensing to quantum computation. Here, we study the optical and spin properties of single praseodymium ions in an yttrium aluminum garnet (YAG) crystal at cryogenic temperature. The single nuclear spin of single praseodymium ions is detected through a background-free optical upconverting readout technique. Single ions show stable photoluminescence (PLE) with spectrally resolved hyperfine splitting of the praseodymium ground state. Based on this measurement, optical Rabi and optically detected magnetic resonance (ODMR) measurements are performed to study the spin coherence properties. Our results reveal that the spin coherence time of single praseodymium nuclear spins is limited by the strong spin-phonon coupling at experimental temperature., Comment: 5 pages, 4 figures

A solid-state system combining a stable spin degree of freedom with an efficient optical interface is highly desirable as an element for integrated quantum optical and quantum information systems. We demonstrate a bright color center in diamond with excellent optical properties and controllable electronic spin states. Specifically, we carry out detailed optical spectroscopy of a Germanium Vacancy (GeV) color center demonstrating optical spectral stability. Using an external magnetic field to lift the electronic spin degeneracy, we explore the spin degree of freedom as a controllable qubit. Spin polarization is achieved using optical pumping, and a spin relaxation time in excess of 20 $\mu$s is demonstrated. Optically detected magnetic resonance (ODMR) is observed in the presence of a resonant microwave field. ODMR is used as a probe to measure the Autler-Townes effect in a microwave-optical double resonance experiment. Superposition spin states were prepared using coherent population trapping, and a pure dephasing time of about 19 ns was observed. Prospects for realizing coherent quantum registers based on optically controlled GeV centers are discussed., Comment: 6 pages, 4 figures

We demonstrate a quantum nanophotonics platform based on germanium-vacancy (GeV) color centers in fiber-coupled diamond nanophotonic waveguides. We show that GeV optical transitions have a high quantum efficiency and are nearly lifetime-broadened in such nanophotonic structures. These properties yield an efficient interface between waveguide photons and a single GeV without the use of a cavity or slow-light waveguide. As a result, a single GeV center reduces waveguide transmission by $18 \pm 1\%$ on resonance in a single pass. We use a nanophotonic interferometer to perform homodyne detection of GeV resonance fluorescence. By probing the photon statistics of the output field, we demonstrate that the GeV-waveguide system is nonlinear at the single-photon level., Comment: 5 pages and 5 figures. Supplemental Material, 4 pages and 1 figure, available as an ancillary file

Hybrid photoelectric detection of NV magnetic resonances (PDMR) is anticipated to lead to scalable quantum chip technology. To achieve this goal, it is crucial to prove that PDMR readout is compatible with the coherent spin control. Here we present PDMR MW pulse protocols that filter background currents related to ionization of NS0 defects and achieve a high contrast and S/N ratio. We demonstrate Rabi and Ramsey protocols on shallow nitrogen-implanted electronic grade diamond and the coherent readout of ~ 5 NV spins, as a first step towards the fabrication of scalable photoelectric quantum devices.

Rare-earth ions doped into desired locations of optical crystals might enable a range of novel integrated photonic devices for quantum applications. With this aim, we have investigated the production yield of cerium and praseodymium by means of ion implantation. As a measure, the collected fluorescence intensity from both, implanted samples and single centers was used. With a tailored annealing procedure for cerium, a yield up to 53% was estimated. Praseodymium yield amounts up to 91%.

Doping of substrates at desired locations is a key technology for spin-based quantum memory devices. Focused ion beam implantation is well-suited for this task due to its high spacial resolution. In this work, we investigate ion-beam implanted erbium ensembles in Yttrium Orthosilicate crystals by means of confocal photoluminescence spectroscopy. The sample temperature and the post-implantation annealing step strongly reverberate in the properties of the implanted ions. We find that hot implantation leads to a higher activation rate of the ions. At high enough fluences, the relation between the fluence and final concentration of ions becomes non-linear. Two models are developed explaining the observed behaviour.

All-optical addressing and control of single solid-state based qubits allows for scalable architectures of quantum devices such as quantum networks and quantum simulators. So far, all-optical addressing of qubits was demonstrated only for color centers in diamond and quantum dots. Here, we demonstrate generation of coherent dark state of a single rare earth ion in a solid, namely a cerium ion in yttrium aluminum garnet (YAG). The dark state was formed under the condition of coherent population trapping. Furthermore, high-resolution spectroscopic studies of native and implanted single Ce ions have been performed. They revealed narrow and spectrally stable optical transitions between the spin sublevels of the ground and excited optical states, indicating the feasibility of interfacing single photons with a single electron spin of a cerium ion., Comment: 5 pages, 4 figures

Rare-earth-doped crystals are excellent hardware for quantum storage of optical information. Additional functionality of these materials is added by their waveguiding properties allowing for on-chip photonic networks. However, detection and coherent properties of rare-earth single-spin qubits have not been demonstrated so far. Here, we present experimental results on high-fidelity optical initialization, effcient coherent manipulation, and optical readout of a single electron spin of Ce$^{3+}$ ion in a YAG crystal. Under dynamic decoupling, spin coherence lifetime reaches $T_2$=2 ms and is almost limited by the measured spin-lattice relaxation time $T_1$=3.8 ms. Strong hyperfine coupling to aluminium nuclear spins suggests that cerium electron spins can be exploited as an interface between photons and long-lived nuclear spin memory. Combined with high brightness of Ce$^{3+}$ emission and a possibility of creating photonic circuits out of the host material, this makes cerium spins an interesting option for integrated quantum photonics., Comment: 10 pages, 4 figures

Electron and nuclear spins associated with point defects in insulators are promising systems for solid state quantum technology. While the electron spin usually is used for readout and addressing, nuclear spins are exquisite quantum bits and memory systems. With these systems single-shot readout of nearby nuclear spins as well as entanglement aided by the electron spin has been shown. While the electron spin in this example is essential for readout it usually limits nuclear spin coherence. This has set of the quest for defects with spin-free ground states. Here, we isolate a hitherto unidentified defect in diamond and use it at room temperature to demonstrate optical spin polarization and readout with exceptionally high contrast (up to 45%), coherent manipulation of an individual excited triplet state spin, and coherent nuclear spin manipulation using the triplet electron spin as a meta-stable ancilla. By this we demonstrate nuclear magnetic resonance and Rabi oscillations of the uncoupled nuclear spin in the spin-free electronic ground state. Our study demonstrates that nuclei coupled to single metastable electron spins are useful quantum systems with long memory times despite electronic relaxation processes., Comment: 4 pages, 5 figures

We report on optical detection of a single photostable Ce3+ ion in an yttrium aluminium garnet (YAG) crystal and on its magneto-optical properties at room temperature. The quantum state of an electron spin of the emitting level of cerium ion in YAG can be initialized by circularly polarized laser pulse. Furthermore, its quantum state can be read out by observing temporal behaviour of circularly polarized fluorescence of the ion. This implies direct mapping of the spin quantum state of Ce3+ ion onto the polarization state of the emitted photon and represents one-way quantum interface between a single spin and a single photon.

In this paper, we study the photoinduced switching of the nitrogen-vacancy (NV) center between two different charge states - negative (NV-) and neutral (NV0) at liquid helium temperature. The conversion of NV- to NV0 on a single defect is experimentally proven and its rate scales quadratically with power under resonant excitation. In addition, we found that resonant excitation of the neutral NV changes the charge state, recovering its negative configuration. This type of conversion significantly improves spectral stability of NV- defect and allows high fidelity initialization of the spin qubit. A possible mechanism for ionization and recovery of the NV- defect is discussed. This study provides better understanding of the charge dynamics of the NV center, which is relevant for quantum information processing based on NV defect in diamond., Comment: 5 pages, 4 figures

The realization of photonic crystals (PC) in diamond is of major importance for the entire field of spintronics based on fluorescent centers in diamond. The processing steps for the case of diamond differ from those commonly used, due to the extreme chemical and mechanical properties of this material. The present work summarizes the state of the art in the realization of PC's in diamond. It is based on the creation of a free standing diamond membrane into which the desired nano-sized patterns are milled by the use of Focused-Ion-Beam (FIB). The optimal fabrication-oriented structure parameters are predicted by simulations. The milling strategies, the method of formation the diamond membrane, recipes for dielectric material-manipulation in FIB and optical characterization constraints are discussed in conjunction with their implication on PC cavity design. The thus produced structures are characterized via confocal photoluminescence., Comment: 25 pages, 9 figures

Optical detection of single defect centers in the solid state is a key element of novel quantum technologies. This includes the generation of single photons and quantum information processing. Unfortunately the brightness of such atomic emitters is limited. Therefore we experimentally demonstrate a novel and simple approach that uses off-the-shelf optical elements. The key component is a solid immersion lens made of diamond, the host material for single color centers. We improve the excitation and detection of single emitters by one order of magnitude, as predicted by theory., Comment: 10 pages, 3 figures

In this paper, we study the optical properties of single defects emitting in the near infrared in nanodiamonds at liquid helium temperature. The nanodiamonds are synthesized using a microwave chemical vapor deposition method followed by nickel implantation and annealing. We show that single defects exhibit several striking features at cryogenic temperature: the photoluminescence is strongly concentrated into a sharp zero-phonon line in the near infrared, the radiative lifetime is in the nanosecond range and the emission is perfectly linearly polarized. The spectral stability of the defects is then investigated. An optical resonance linewidth of 4 GHz is measured using resonant excitation on the zero-phonon line. Although Fourier-transform limited emission is not achieved, our results show that it might be possible to use consecutive photons emitted in the near infrared by single defects in diamond nanocrystals to perform two photon interference experiments, which are at the heart of linear quantum computing protocols., Comment: 12pages, 5 figures

In this report, the polarization properties of the photoluminescence emitted by single nitrogen-vacancy (NV) color centers in diamond are investigated using resonant excitation at cryogenic temperature. We first underline that the two excited-state orbital branches are associated with two orthogonal transition dipoles. Using selective excitation of one dipole, we then show that the photoluminescence is partially unpolarized owing to fast relaxation between the two orbitals induced by the thermal bath. This result might be important in the context of the realization of indistinguishable single photons using NV defect in diamond., Comment: 4 pages, 4 figures

We report a study of the 3E excited-state structure of single nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model of the excited-state structure is developed and shows excellent agreement with experimental observations. Besides, we show that the two orbital branches associated with the 3E excited-state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of diamond-based quantum information processing., Comment: 4 pages, 4 figures

The dynamics of single electron and nuclear spins in a diamond lattice with different 13C nuclear spin concentration is investigated. It is shown that coherent control of up to three individual nuclei in a dense nuclear spin cluster is feasible. The free induction decays of nuclear spin Bell states and single nuclear coherences among 13C nuclear spins are compared and analyzed. Reduction of a free induction decay time T2* and a coherence time T2 upon increase of nuclear spin concentration has been found. For diamond material with depleted concentration of nuclear spin, T2* as long as 30 microseconds and T2 of up to 1.8 ms for the electron spin has been observed. The 13C concentration dependence of T2* is explained by Fermi contact and dipolar interactions with nuclei in the lattice. It has been found that T2 decreases approximately as 1/n, where n is 13C concentration, as expected for an electron spin interacting with a nuclear spin bath., Comment: 4 pages, 4 figures, 1 movie (avi), 1 supplementary material (pdf)