Photo-Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room-Temperature Diamond.

The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi-color confocal microscopy and density functional theory are used to examine photo-induced SiV recombination - from neutral, to single-, to double-negatively charged - over a broad spectral window in chemical-vapor-deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV- transition, a linear growth of the photo-recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV- , on the other hand, yields only fractional recombination into SiV2- , a finding that is interpreted in terms of a photo-activated electron tunneling process from proximal nitrogen atoms.

Phonon-induced population dynamics and intersystem crossing in nitrogen-vacancy centers.

We report direct measurement of population dynamics in the excited state manifold of a nitrogen-vacancy (NV) center in diamond. We quantify the phonon-induced mixing rate and demonstrate that it can be completely suppressed at low temperatures. Further, we measure the intersystem crossing (ISC) rate for different excited states and develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure. We discuss the model's implications for enhancing the NV center's performance as a room-temperature sensor.

Precision measurement of electronic ion-ion interactions between neighboring Eu3+ optical centers.

We report measurements of discrete excitation-induced frequency shifts on the 7F0→5D0 transition of the Eu+ center in La:Lu:EuCl3·6D2O resulting from the optical excitation of neighboring Eu3+ ions. Shifts of up to 46.081±0.005 MHz were observed. The magnitude of the interaction between neighboring ions was found to be significantly larger than expected from the electric dipole-dipole mechanism often observed in rare earth systems. We show that a large network of interacting and individually addressable centers can be created by lightly doping crystals otherwise stoichiometric in the optically active rare earth ion, and that this network could be used to implement a quantum processor with more than ten qubits.

Optimum photoluminescence excitation and recharging cycle of single nitrogen-vacancy centers in ultrapure diamond.

Important features in the spectral and temporal photoluminescence excitation of single nitrogen-vacancy (NV) centers in diamond are reported at conditions relevant for quantum applications. Bidirectional switching occurs between the neutral (NV(0)) and negatively charged (NV(-)) states. Luminescence of NV(-) is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of NV(0). The dark state of NV(-) is identified as NV(0). A narrow resonance is observed in the excitation spectra at 521 nm, which mediates efficient conversion to NV(0).

Low temperature studies of the excited-state structure of negatively charged nitrogen-vacancy color centers in diamond.

We report a study of the 3E excited-state structure of single negatively charged nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model is developed and shows excellent agreement with experimental observations. In addition, 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.

Photon echoes produced by switching electric fields.

We demonstrate photon echoes in Eu3+:Y2SiO5 by controlling the inhomogeneous broadening of the Eu3+ 7F0<-->5D0 optical transition. This transition has a linear Stark shift, and we induce inhomogeneous broadening by applying an external electric field gradient. After optical excitation, reversing the polarity of the field rephases the ensemble, resulting in a photon echo. This is the first demonstration of such a photon echo, and its application as a quantum memory is discussed.

Stopped light with storage times greater than one second using electromagnetically induced transparency in a solid.

We report on the demonstration of light storage for times greater than a second in praseodymium doped Y2SiO5 using electromagnetically induced transparency. The long storage times were enabled by the long coherence times possible for the hyperfine transitions in this material. The use of a solid-state system also enabled operation with the probe and coupling beam counter-propagating, allowing easy separation of the two beams. The efficiency of the storage was low because of the low optical thickness of the sample; as is discussed, this deficiency should be easy to rectify.

Demonstration of conditional quantum phase shift between ions in a solid.

Because of their long coherence times, dopant ions have been considered promising candidates for scalable solid state quantum computing. Here we demonstrate a conditional phase shift between two qubits based on an optical transition of europium ions. The demonstration uses ensembles that have been selected from a randomly doped sample using spectral hole burning techniques. The electron dipole-dipole interaction between the ions that usually causes instantaneous spectral diffusion is used to generate the conditional phase shift.

Raman heterodyne detection of electron paramagnetic resonance.

We report the detection of an electron paramagnetic resonance signal using Raman heterodyne spectroscopy, a rf -optical double-resonance technique. The signals are associated with the nitrogen-vacancy center in diamond, which has a spin-triplet ground state. A three-line spectrum associated with the nitrogen hyperfine structure is observed for various magnetic field strengths and crystal orientations.

Raman heterodyne detected electron-nuclear-double-resonance measurements of the nitrogen-vacancy center in diamond.

We report two new applications of the Raman heterodyne detection technique. Raman heterodyne detected electron-nuclear double resonance and a double rf resonance technique are used to obtain the hyperfine structure of the nitrogen-vacancy center in diamond.