Nanoscale Engineering of Closely-Spaced Electronic Spins in Diamond.

Numerous theoretical protocols have been developed for quantum information processing with dipole-coupled solid-state spins. Nitrogen vacancy (NV) centers in diamond have many of the desired properties, but a central challenge has been the positioning of NV centers at the nanometer scale that would allow for efficient and consistent dipolar couplings. Here we demonstrate a method for chip-scale fabrication of arrays of single NV centers with record spatial localization of about 10 nm in all three dimensions and controllable inter-NV spacing as small as 40 nm, which approaches the length scale of strong dipolar coupling. Our approach uses masked implantation of nitrogen through nanoapertures in a thin gold film, patterned via electron-beam lithography and dry etching. We verified the position and spin properties of the resulting NVs through wide-field super-resolution optically detected magnetic resonance imaging.

Modulation of nitrogen vacancy charge state and fluorescence in nanodiamonds using electrochemical potential.

The negatively charged nitrogen vacancy (NV(-)) center in diamond has attracted strong interest for a wide range of sensing and quantum information processing applications. To this end, recent work has focused on controlling the NV charge state, whose stability strongly depends on its electrostatic environment. Here, we demonstrate that the charge state and fluorescence dynamics of single NV centers in nanodiamonds with different surface terminations can be controlled by an externally applied potential difference in an electrochemical cell. The voltage dependence of the NV charge state can be used to stabilize the NV(-) state for spin-based sensing protocols and provides a method of charge state-dependent fluorescence sensing of electrochemical potentials. We detect clear NV fluorescence modulation for voltage changes down to 100 mV, with a single NV and down to 20 mV with multiple NV centers in a wide-field imaging mode. These results suggest that NV centers in nanodiamonds could enable parallel optical detection of biologically relevant electrochemical potentials.

Generation of ensembles of individually resolvable nitrogen vacancies using nanometer-scale apertures in ultrahigh-aspect ratio planar implantation masks.

A central challenge in developing magnetically coupled quantum registers in diamond is the fabrication of nitrogen vacancy (NV) centers with localization below ∼20 nm to enable fast dipolar interaction compared to the NV decoherence rate. Here, we demonstrate the targeted, high throughput formation of NV centers using masks with a thickness of 270 nm and feature sizes down to ∼1 nm. Super-resolution imaging resolves NVs with a full-width maximum distribution of 26 ± 7 nm and a distribution of NV-NV separations of 16 ± 5 nm.

Coherent spin control of a nanocavity-enhanced qubit in diamond.

A central aim of quantum information processing is the efficient entanglement of multiple stationary quantum memories via photons. Among solid-state systems, the nitrogen-vacancy centre in diamond has emerged as an excellent optically addressable memory with second-scale electron spin coherence times. Recently, quantum entanglement and teleportation have been shown between two nitrogen-vacancy memories, but scaling to larger networks requires more efficient spin-photon interfaces such as optical resonators. Here we report such nitrogen-vacancy-nanocavity systems in the strong Purcell regime with optical quality factors approaching 10,000 and electron spin coherence times exceeding 200 µs using a silicon hard-mask fabrication process. This spin-photon interface is integrated with on-chip microwave striplines for coherent spin control, providing an efficient quantum memory for quantum networks.

Surface Structure of Aerobically Oxidized Diamond Nanocrystals.

We investigate the aerobic oxidation of high-pressure, high-temperature nanodiamonds (5-50 nm dimensions) using a combination of carbon and oxygen K-edge X-ray absorption, wavelength-dependent X-ray photoelectron, and vibrational spectroscopies. Oxidation at 575 °C for 2 h eliminates graphitic carbon contamination (>98%) and produces nanocrystals with hydroxyl functionalized surfaces as well as a minor component (<5%) of carboxylic anhydrides. The low graphitic carbon content and the high crystallinity of HPHT are evident from Raman spectra acquired using visible wavelength excitation (λexcit = 633 nm) as well as carbon K-edge X-ray absorption spectra where the signature of a core-hole exciton is observed. Both spectroscopic features are similar to those of chemical vapor deposited (CVD) diamond but differ significantly from the spectra of detonation nanodiamond. The importance of these findings to the functionalization of nanodiamond surfaces for biological labeling applications is discussed.

Scalable fabrication of high purity diamond nanocrystals with long-spin-coherence nitrogen vacancy centers.

The combination of long spin coherence time and nanoscale size has made nitrogen vacancy (NV) centers in nanodiamonds the subject of much interest for quantum information and sensing applications. However, currently available high-pressure high-temperature (HPHT) nanodiamonds have a high concentration of paramagnetic impurities that limit their spin coherence time to the order of microseconds, less than 1% of that observed in bulk diamond. In this work, we use a porous metal mask and a reactive ion etching process to fabricate nanocrystals from high-purity chemical vapor deposition (CVD) diamond. We show that NV centers in these CVD nanodiamonds exhibit record-long spin coherence times in excess of 200 µs, enabling magnetic field sensitivities of 290 nT Hz(-1/2) with the spatial resolution characteristic of a 50 nm diameter probe.

Wide-field multispectral super-resolution imaging using spin-dependent fluorescence in nanodiamonds.

Recent advances in fluorescence microscopy have enabled spatial resolution below the diffraction limit by localizing multiple temporally or spectrally distinguishable fluorophores. Here, we introduce a super-resolution technique that deterministically controls the brightness of uniquely addressable, photostable emitters. We modulate the fluorescence brightness of negatively charged nitrogen-vacancy (NV(-)) centers in nanodiamonds through magnetic resonance techniques. Using a CCD camera, this "deterministic emitter switch microscopy" (DESM) technique enables super-resolution imaging with localization down to 12 nm across a 35 × 35 µm(2) area. DESM is particularly well suited for biological applications such as multispectral particle tracking since fluorescent nanodiamonds are not only cytocompatible but also nonbleaching and bright. We observe fluorescence count rates exceeding 1.5 × 10(6) photons per second from single NV(-) centers at saturation. When combined with emerging NV(-)-based techniques for sensing magnetic and electric fields, DESM opens the door to rapid, super-resolution imaging for tracking and sensing applications in the life and physical sciences.

Polarization-induced tunability of localized surface plasmon resonances in arrays of sub-wavelength cruciform apertures.

We demonstrate experimentally that by engineering the structural asymmetry of the primary unit cell of a symmetrically nanopatterned metallic film the optical transmission becomes strongly dependent on the polarization of the incident wave. By considering a specific plasmonic structure consisting of square arrays of nanoscale asymmetric cruciform apertures we show that the enhanced optical anisotropy is induced by the excitation inside the apertures of localized surface plasmon resonances. The measured transmission spectra of these plasmonic arrays show a transmission maximum whose spectral location can be tuned by almost 50% by simply varying the in-plane polarization of the incident photons. Comprehensive numerical simulations further prove that the maximum of the transmission spectra corresponds to polarization-dependent surface plasmon resonances tightly confined in the two arms of the cruciform aperture. Despite this, there are isosbestic points where the transmission, reflection, and absorption spectra are polarization-independent, regardless of the degree of asymmetry of the apertures.