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ACS Photonics

Sub-GHz Linewidth Ensembles of SiV Centers in a Diamond Nanopyramid Revealed by Charge State Conversion

Louis Nicolas, Tom Delord, Paul H. Huillery, Clément Pellet-Mary, Gabriel Hetet

Published Sep 18, 2019• 13 citations
Publisher

Abstract

Producing nanostructures with embedded bright ensembles of lifetime-limited emitters is a challenge with potential high impact in a broad range of physical sciences. In this work, we demonstrate controlled charge transfer to and from dark states exhibiting very long lifetimes in high-density ensembles of SiV centers hosted in a diamond nanopyramid grown by chemical vapor deposition. Further, using a combination of resonant photoluminescence excitation and a frequency-selective persistent hole-burning technique that exploits this charge state transfer, we could demonstrate close to lifetime-limited linewidths from the SiV centers. Such a nanostructure with thousands of bright narrow linewidth emitters in a volume much below λ 3 will be useful for coherent light–matter coupling, biological sensing, and nanoscale thermometry.

DOI
10.1021/acsphotonics.9b00262

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physica status solidi (a)•Jul 25, 2020•18 citations
Producing nanostructures with embedded bright ensembles of lifetime-limited emitters is a challenge with potential high impact in a broad range of physical sciences. In this work, we demonstrate controlled charge transfer to and from dark states exhibiting very long lifetimes in high-density ensembles of SiV centers hosted in a diamond nanopyramid grown by chemical vapor deposition. Further, using a combination of resonant photoluminescence excitation and a frequency-selective persistent hole-burning technique that exploits this charge state transfer, we could demonstrate close to lifetime-limited linewidths from the SiV centers. Such a nanostructure with thousands of bright narrow linewidth emitters in a volume much below λ 3 will be useful for coherent light–matter coupling, biological sensing, and nanoscale thermometry.
Producing nano-structures with embedded bright ensembles of lifetime-limited emitters is a challenge with potential high impact in a broad range of physical sciences. In this work, we demonstrate controlled charge transfer to and from dark states exhibiting very long lifetimes in high density ensembles of SiV centers hosted in a CVD-grown diamond nano-pyramid. Further, using a combination of resonant photoluminescence excitation and a frequency-selective persistent hole burning technique that exploits such charge state transfer, we could demonstrate close to lifetime-limited linewidths from the SiV centers. Such a nanostructure with thousands of bright narrow linewidth emitters in a volume much below λ3λ^3λ3 will be useful for coherent light-matter coupling, for biological sensing, and nanoscale thermometry.
Silicon-vacancy (SiV) centers in diamond are promising systems for quantum information applications due to their bright single-photon emission and optically accessible spin states. Furthermore, SiV centers in low-strain diamond are insensitive to perturbations of the dielectric environment; i.e., they show very weak spectral diffusion. This property renders ensembles of SiV centers interesting for sensing applications. We here report on photoluminescence excitation (PLE) spectroscopy on an SiV ensemble in a low strain, chemical vapor deposition-grown high-quality diamond layer, where we measure the fine structure with high resolution and obtain the line widths and splittings of the SiV centers. We investigate the temperature dependence of the width and position of the fine structure peaks. Our measurements reveal line widths of about 10 GHz as compared to a lifetime limited width on the order of 0.1 GHz. This difference arises from the inhomogeneous broadening of the transitions caused by residual strain. To overcome inhomogeneous broadening we use spectral hole burning spectroscopy, which enables us to measure a nearly lifetime limited homogeneous line width of 279 MHz. Furthermore, we demonstrate evidence of coherent interaction in the system by driving a $\mathrm{\ensuremath{\Lambda}}$ scheme. Additional measurements on single emitters created by ion implantation confirm the homogeneous line widths seen in the spectral hole burning experiments and relate the ground-state splitting to the decoherence rate.
High Resolution Image Download MS PowerPoint Slide The negatively charged silicon vacancy center (SiV – ) in diamond is a promising, yet underexplored candidate for single-spin quantum sensing at sub-kelvin temperatures and tesla-range magnetic fields. A key ingredient for such applications is the ability to perform all-optical, coherent addressing of the electronic spin of near-surface SiV – centers. We present a robust and scalable approach for creating individual, ∼50 nm deep SiV – with lifetime-limited optical linewidths in diamond nanopillars through an easy-to-realize and persistent optical charge-stabilization scheme. The latter is based on single, prolonged 445 nm laser illumination that enables continuous photoluminescence excitation spectroscopy without the need for any further charge stabilization or repumping. Our results constitute a key step toward the use of near-surface, optically coherent SiV – for sensing under extreme conditions, and offer a powerful approach for stabilizing the charge-environment of diamond color centers for quantum technology applications.
Color centers in diamond are versatile solid state atomic-like systems suitable for quantum technological applications. In particular, the negatively charged silicon vacancy center (SiV) exhibits a narrow photoluminescence (PL) line and lifetime-limited linewidth in a bulk at cryogenic temperature. We present a low-temperature study of chemical vapour deposition (CVD)-grown diamond nano-pyramids containing SiV centers. The PL spectra feature a bulk-like zero-phonon line with ensembles of SiV centers, with a linewidth below 10 GHz which demonstrates very low crystal strain for such a nano-object.
Diamond nanoparticles with optically active color centers can be used in nanoscale devices for quantum networking and sensing. A particular interest is focused on nanodiamonds (NDs) containing a small ensemble of negatively charged silicon‐vacancy (SiV) centers. Such NDs can be integrated with on‐chip optical structures. Here, chemical vapor deposition (CVD) is used to synthesize diamond particles of less than 100 nm in size containing 10–20 centers per ND. Two types of NDs grown on a Si substrate are studied, seeded with detonation NDs and without any seeding. The SiV luminescence under off‐resonant and resonant laser excitation at the temperature of 15 K is investigated. The emission lines of SiVs of individual NDs are well resolved and found to be spread in the range of 730–750 nm. The typical SiV linewidth is within 1–2 GHz for spontaneous NDs, which is only a factor of 2.5–5 broader than the lifetime limited linewidth of the SiV at 15 K. The emission of a single SiV is highly stable for both types of samples. This work is a critical step toward the synthesis of SiVs suitable for the realization of integrated quantum photonic devices.