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arXiv:1904.00883 · Nano Letters

Optically Coherent Nitrogen-Vacancy Centers in Micrometer-Thin Etched Diamond Membranes

Maximilian Ruf, Mark IJspeert, Suzanne B. van Dam, Nick de Jong, Hans van den Berg, Guus Evers, Ronald Hanson

Published May 28, 2019• 104 citations
arXivHTMLPDF

Abstract

Abstract Diamond membrane devices containing optically coherent nitrogen-vacancy (NV) centers are key to enable novel cryogenic experiments such as optical ground-state cooling of hybrid spin-mechanical systems and efficient entanglement distribution in quantum networks. Here, we report on the fabrication of a (3.4 ± 0.2) μm thin, smooth (surface roughness rq < 0.4 nm over an area of 20 μm by 30 μm) diamond membrane containing individually resolvable, narrow linewidth (< 100 MHz) NV centers. We fabricate this sample via a combination of high-energy electron irradiation, high-temperature annealing, and an optimized etching sequence found via a systematic study of the diamond surface evolution on the microscopic level in different etch chemistries. Although our particular device dimensions are optimized for cavity-enhanced entanglement generation between distant NV centers in open, tunable microcavities, our results have implications for a broad range of quantum experiments that require the combination of narrow optical transitions and micrometer-scale device geometry.

DOI
10.1021/acs.nanolett.9b01316

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Abstract Diamond membrane devices containing optically coherent nitrogen-vacancy (NV) centers are key to enable novel cryogenic experiments such as optical ground-state cooling of hybrid spin-mechanical systems and efficient entanglement distribution in quantum networks. Here, we report on the fabrication of a (3.4 ± 0.2) μm thin, smooth (surface roughness rq < 0.4 nm over an area of 20 μm by 30 μm) diamond membrane containing individually resolvable, narrow linewidth (< 100 MHz) NV centers. We fabricate this sample via a combination of high-energy electron irradiation, high-temperature annealing, and an optimized etching sequence found via a systematic study of the diamond surface evolution on the microscopic level in different etch chemistries. Although our particular device dimensions are optimized for cavity-enhanced entanglement generation between distant NV centers in open, tunable microcavities, our results have implications for a broad range of quantum experiments that require the combination of narrow optical transitions and micrometer-scale device geometry.
Abstract Micrometer-scale thin diamond devices are key components for various quantum sensing and networking experiments, including the integration of color centers into optical microcavities. In this work, we introduce a laser-cutting method for patterning microdevices from millimeter-sized diamond membranes. The method can be used to fabricate devices with micrometer thicknesses and edge lengths of typically 10–100 µm. We compare this method with an established nanofabrication process based on electron-beam lithography, a two-step transfer pattern utilizing a silicon nitride hard mask material, and reactive ion etching. Microdevices fabricated using both methods are bonded to a cavity Bragg mirror and characterized using scanning cavity microscopy. We record two-dimensional cavity finesse maps over the devices, revealing insights about the variation in diamond thickness, surface quality, and strain. The scans demonstrate that devices fabricated by laser-cutting exhibit similar properties to devices obtained by the conventional method. Finally, we show that the devices host optically coherent Tin- and Nitrogen-Vacancy centers suitable for applications in quantum networking.
Deploying nitrogen vacancy (NV) centers in diamond as nanoscale quantum sensors for condensed matter and materials physics requires placing the NV centers close to the sensing target. One solution is to fabricate diamond nanostructures and integrate them with materials and devices. However, diamond etching and ion milling can introduce subsurface damage and surface defects that degrade the charge stability and spin coherence of NV centers near the surface. Here we report a procedure for fabricating low-damage nanostructured diamond membranes, and we show that this fabrication scheme preserves the optical and spin properties of state-of-the-art shallow NV center quantum sensors, within nanometers of the diamond surface, while providing significant photonic enhancement. Furthermore, we demonstrate a pick-and-place transfer method, which enables integration with diverse sensing targets.
A quantumnetwork would allow the distribution of a quantum state over many spatially separated quantum nodes which individually possess the ability to generate, process and store quantum information. Connecting these nodes through quantum communication channels would enable sending quantum information over arbitrarily long distances, secret key distribution with guaranteed secure communication and distributed quantum computing. An appealing platform for implementation of quantum networks is the nitrogen-vacancy (NV) center in diamond. An NV center is an optically active defect in diamond created by the substitution of two adjacent carbon atoms in the diamond crystal matrix by a nitrogen atom and a neighboring vacancy. The NV center fits remarkably well in the described quantum network framework. Its electronic spin can be optically initialized, read out in a single shot, coherently manipulated and coupled to the nearby carbon-13 nuclear spins. These properties represent necessary ingredients of a multi-qubit quantum node. The possibility of the entanglement between the state of the NV center spin and a photon establishes a photonic quantum link which can enable the entanglement of the quantum nodes, forming a quantum network. First building blocks of the proposed quantum networks based on NV centers were demonstrated by performing entanglement between two distant NV centers separated by more than a kilometer. However, the current success rate of the entangling protocols is greatly reduced due to the low emission probability of the NV center photons into the resonant zero phonon line (ZPL) and the inefficient photon extraction from the diamond. This is the central problem which prevents promoting our experiments beyond proof-of-principle demonstration towards practical implementation of the proposed quantumnetworks. The goal of this thesis is tackling these issues by coupling NV centers to optical cavities which would greatly increase the rate of generation and collection of the ZPL photons through themechanism of Purcell enhancement. The design and the fabrication of the components constituting a diamond-basedFabry-Perot microcavity, as used in this thesis, are described in Chapter 4. For large enhancement of the NV center resonant emission, a low cavity mode volume is necessary. This is achieved by inserting a micrometers thin diamond slab into the cavity architecture; we present the fabrication details of such samples. Chapter 5 describes the fabrication of an integrated platform for microwave signal delivery to the NV centers within a diamond membrane in the cavity architecture. Microwave striplines and arrays of unique markers are embedded in the mirror onto which the diamond is bonded. We investigate the mirror optical properties post fabrication and find that the fabrication method preserves the mirror optical performance. We describe the diamond bonding method and demonstrate addressing of the NV center spin. In Chapter 6 we probe the properties of the cavity with the embedded diamond membrane through measurements of the cavity finesse. We investigate the cavity finesse dependence on length, mode structure and temperature. We further explore the operation at cryogenic temperatures by probing the effect of cryostation vibration on the cavity linewidth. Finally, in Chapter 7 we discuss ways of improving the existing experimental capabilities, outline the first steps for demonstrating enhancement of the NV center resonant emission and suggest future experiments that can be performed with this system. We conclude that coupling of the NV centers to the cavities developed in this research could lead to an increase of remote entanglement success rates by more than three orders of magnitude.
Abstract The nitrogen-vacancy (NV) center in diamond is a promising quantum system for magnetometry applications exhibiting optical readout of minute energy shifts in its spin sub-levels. Key material requirements for NV ensembles are a high NV − concentration, a long spin coherence time and a stable charge state. However, these are interdependent and can be difficult to optimize during diamond growth and subsequent NV creation. In this work, we systematically investigate the NV center formation and properties in bulk chemical vapor deposition (CVD) diamond. The nitrogen flow during growth is varied by over four orders of magnitude, resulting in a broad range of single substitutional nitrogen concentrations of 0.2–20 parts per million. For a fixed nitrogen concentration, we optimize electron-irradiation fluences with two different accelerated electron energies, and we study defect formation via optical characterizations. We discuss a general approach to determine the optimal irradiation conditions, for which an enhanced NV concentration and an optimum of NV charge states can both be satisfied. We achieve spin–spin coherence times T 2 ranging from 45.5 to 549 μ s for CVD diamonds containing 168 to 1 parts per billion NV − centers, respectively. This study shows a pathway to engineer properties of NV-doped CVD diamonds for improved sensitivity.
A key requirement for many applications in solid-state quantum sciences is a high fluence of indistinguishable photons. The spontaneous emission of these photons is governed by the coupling of an excited quantum system to electromagnetic vacuum fluctuations. In our experiment, we enhance this coupling by engineering a tunable Fabry-Perot microcavity. The quantum system we study is the nitrogen-vacancy (NV) center in diamond, a workhorse for quantum science and engineering, due to its optical transitions and the coherent electron spin system it hosts. Our device consists of a high-quality, nano-fabricated, single-crystalline diamond membrane bonded to a planar mirror; the cavity is completed by a second, concave mirror. Using piezo positioners, we achieve full spectral and spatial tunability and freedom in selecting NVs with favorable emission properties in our low-temperature (4 Kelvin) experiments. Upon tuning of the cavity into resonance, we find significant enhancement of the 637 nm zero phonon line for several individual NVs which is accompanied by a strong reduction of the overall photoluminescence (PL) lifetime. We infer a 30-fold enhancement of the zero-phonon transition rate at best. The fraction of the PL emission associated to this resonant transition is thereby increased from 3% to 46%. Our results constitute a significant leap on the route towards the implementation of fast long-distance quantum networks, which are currently limited by the photon emission rate in their nodes. Furthermore, our versatile design is readily applicable to other solid-state quantum emitters like color centers in silicon carbide.
Nitrogen-vacancy (NV) centers in diamond with coherent optical transitions are a promising candidate for quantum science and technology protocols. A widely used strategy for their creation is nitrogen-ion implantation and high-temperature annealing. The data presented in this work show that while low-strain, narrow-optical-linewidth NV centers are formed from naturally occurring 14{}^{14}14N atoms, NV centers formed from the implanted 15{}^{15}15N atoms show broadened optical transitions and experience higher strain. These results have immediate implications for the positioning accuracy of current NV center creation protocols.