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ACS Applied Nano Materials

Photoluminescence of Germanium-Vacancy Centers in Nanocrystalline Diamond Films: Implications for Quantum Sensing Applications

Rani Mary Joy, Paulius Pobedinskas, Emilie Bourgeois, Tanmoy Chakraborty, Johannes Goerlitz, Dennis Herrmann, Céline Noël, Julia Heupel, Daen Jannis, Nicolas Gauquelin, Jan D’Haen, Johan Verbeeck, Cyril Popov, Laurent Houssiau, Christoph Becher, Miloš Nesládek, Ken Haenen

Published Feb 15, 2024• 7 citations
Publisher

Abstract

Point defects in diamond, promising candidates for nanoscale pressure- and temperature-sensing applications, are potentially scalable in polycrystalline diamond fabricated using the microwave plasma-enhanced chemical vapor deposition (MW PE CVD) technique. However, this approach introduces residual stress in the diamond films, leading to variations in the characteristic zero phonon line (ZPL) of the point defect in diamond. Here, we report the effect of residual stress on germanium-vacancy (GeV) centers in MW PE CVD nanocrystalline diamond (NCD) films fabricated using single crystal Ge as the substrate and solid dopant source. GeV ensemble formation indicated by the zero phonon line (ZPL) at ∼602 nm is confirmed by room temperature (RT) photoluminescence (PL) measurements. PL mapping results show spatial nonuniformity in GeV formation along with other defects, including silicon-vacancy centers in the diamond films. The residual stress in NCD results in shifts in the PL peak positions. By estimating a stress shift coefficient of (2.9 ± 0.9) nm/GPa, the GeV PL peak position in the NCD film is determined to be between 598.7 and 603.2 nm. A larger ground state splitting due to the strain on a GeV-incorporated NCD pillar at a low temperature (10 K) is also reported. We also report the observation of intense ZPLs at RT that in some cases could be related to low Ge concentration and the surrounding crystalline environment. In addition, we also observe thicker microcrystalline diamond (MCD) films delaminate from the Ge substrate due to film residual stress and graphitic phase at the diamond/Ge substrate interface (confirmed by electron energy loss spectroscopy). Using this approach, a free-standing color center incorporated MCD film with dimensions up to 1 × 1 cm 2 is fabricated. Qualitative analysis using time-of-flight secondary ion mass spectroscopy reveals the presence of impurities, including Ge and silicon, in the MCD film. Our experimental results will provide insights into the scalability of GeV fabrication using the MW PE CVD technique and effectively implement NCD-based nanoscale-sensing applications.

DOI
10.1021/acsanm.3c05491

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•Jan 1, 2025•0 citations
Point defects in diamond, promising candidates for nanoscale pressure- and temperature-sensing applications, are potentially scalable in polycrystalline diamond fabricated using the microwave plasma-enhanced chemical vapor deposition (MW PE CVD) technique. However, this approach introduces residual stress in the diamond films, leading to variations in the characteristic zero phonon line (ZPL) of the point defect in diamond. Here, we report the effect of residual stress on germanium-vacancy (GeV) centers in MW PE CVD nanocrystalline diamond (NCD) films fabricated using single crystal Ge as the substrate and solid dopant source. GeV ensemble formation indicated by the zero phonon line (ZPL) at ∼602 nm is confirmed by room temperature (RT) photoluminescence (PL) measurements. PL mapping results show spatial nonuniformity in GeV formation along with other defects, including silicon-vacancy centers in the diamond films. The residual stress in NCD results in shifts in the PL peak positions. By estimating a stress shift coefficient of (2.9 ± 0.9) nm/GPa, the GeV PL peak position in the NCD film is determined to be between 598.7 and 603.2 nm. A larger ground state splitting due to the strain on a GeV-incorporated NCD pillar at a low temperature (10 K) is also reported. We also report the observation of intense ZPLs at RT that in some cases could be related to low Ge concentration and the surrounding crystalline environment. In addition, we also observe thicker microcrystalline diamond (MCD) films delaminate from the Ge substrate due to film residual stress and graphitic phase at the diamond/Ge substrate interface (confirmed by electron energy loss spectroscopy). Using this approach, a free-standing color center incorporated MCD film with dimensions up to 1 × 1 cm 2 is fabricated. Qualitative analysis using time-of-flight secondary ion mass spectroscopy reveals the presence of impurities, including Ge and silicon, in the MCD film. Our experimental results will provide insights into the scalability of GeV fabrication using the MW PE CVD technique and effectively implement NCD-based nanoscale-sensing applications.
Group IV color centers in diamond are promising single-photon emitters for quantum information processing and networking. Among them, the tin-vacancy (SnV) center stands out due to its long spin coherence times at cryogenic temperatures above 1 K. While SnV centers have been realized using various fabrication routes, their in situ formation via microwave plasma-enhanced chemical vapor deposition (MW PE CVD) remains relatively unexplored. In this study, SnV centers, identified by a zero-phonon line (ZPL) near 620 nm, were synthesized in nanocrystalline diamond and free-standing microcrystalline diamond using tin oxide (SnO 2 ) as a dopant source at substrate temperatures of 750°C and 850°C. Photoluminescence measurements reveal that lowering the substrate temperature enhances both the ZPL intensity and spatial uniformity of SnV centers. These results highlight substrate temperature as a key parameter for controlling SnV incorporation during MW PE CVD growth and provide insights into optimizing fabrication strategies for diamond-based quantum technologies.
Atomic-sized fluorescent defects in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. In this study, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.
Diamonds with impurity color centers are a novel class of functional materials with potential for various photonics applications such as quantum optics, metrology, sensorics, and life sciences. When introducing defect centers, a broad range of questions arises about the nature of the photophysical processes in the new materials, in particular regarding the relationship between spectral and morphological properties. Here we present results of comprehensive spectroscopic studies on diamond films with germanium-vacancy (GeV – ) centers, synthesized by chemical vapor deposition from gaseous germane (GeH 4 ). The combination of different techniques (emission and fluorescence excitation spectroscopy, epi-microscopy, and nanoscopy up to the single-emitter level) at room and cryogenic temperatures has shed light onto the spatial distribution of the spectral properties of the GeV – centers in different microregions of the diamond crystal and its relation to local strain/stress. We demonstrate a clear correlation between inhomogeneous broadening and morphological heterogeneities of the sample. Ultranarrow (tens of MHz) stable zero-phonon lines have been observed, which are a prerequisite for various applications.
Color centers in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. Here, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.
Tin-Vacancy (Sn-V) colour centres in diamond have a spin coherence time in the millisecond range at temperatures of 2 K, so they are promising to be used in diamond-based quantum optical devices. However, the incorporation of large Sn atoms into a dense diamond lattice is a non-trivial problem. The objective of our work is to use microwave plasma-assisted chemical vapour deposition (CVD) to grow Sn-doped diamond with submicron SnO 2 particles as a solid-state source of impurity. Well-faceted diamond microcrystals with sizes of a few micrometres were formed on AlN substrates. The photoluminescence (PL) signal with zero-phonon line (ZPL) peak for Sn-V centre at ≈620 nm was measured at room temperature (RT) and at 7 K. The peak width (full width at half-maximum) was measured to be 1.1–1.7 nm at RT and ≈0.05 nm at 7 K. The observed variations of ZPL shape and position, in particular, narrowing of PL peak at RT and formation of single-line fine structure at low- T , are attributed to strain in the crystallites. The diamond doping with Sn via CVD process offers a new route to from Sn-V colour centre in the bulk of the diamond crystallites. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.