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Spectroscopy and Application of Quantum Emitters for Quantum Technologies

Pablo Tieben

Published Jan 1, 2026• 0 citations
Publisher

Abstract

Sources of single photons are integral to a number of applications in the emerging field of quantum technologies. For any practical implementation of single-photon sources, a variety of different properties and an overall comprehensive characterization of the sources are required. Color centers in hBN and group IV color centers in diamond are promising candidate sources due to their favorable properties and rich internal level structure. Both of these candidates, however, also present some serious challenges. Although bright and spectrally narrow, defects in hBN suffer from emission instabilities. Furthermore, limited knowledge about their atomic composition leads to behaviour, which is often unpredictable. Meanwhile, Group IV centers generally exhibit low extraction efficiencies due to total internal reflection inside the high-index diamond host material. In this thesis, several large-scale series of experiments are conducted to investigate both types of emitters in a confocal fluorescence microscope at room temperature. The excitation characteristics of a large number of single-photon emitters in hBN from a narrow spectral window are investigated using a fully automated procedure. The results are compared to theoretical predictions for several carbon defects from the literature to gain further knowledge of the atomic nature of the underlying defects. Based on this approach, the CB, CN, CBVN, and CNVB centers are confidently ruled out as possible origins of the observed emission. Some uncertainty remains about the assignment of the carbon trimer C2CN as well as carbon-based donor-acceptor pairs. In a separate series of experiments, emission instabilities of hBN emitters from the same spectral region are studied. The detected fluctuations in brightness were conclusively attributed to spectral diffusion of the emission. Furthermore, optical stabilization of these effects via short-wavelength irradiation favors an explanation of the observed behavior via nearby charge carriers and the resulting Stark effect. Tin-vacancies, as representatives of group IV centers, are studied in a novel type of diamond waveguide structure for light collection enhancement. A center with sharp zero-phonon emission around 619 nm, a g(2)(0) value of 0.32, and simultaneous stable count rate of 3.4 Mcps was found. By restricting the collection to the zero-phonon line, g(2)(0) = 0.1 could be achieved. In a widespread characterization of the sample, it was found that most structures contain more than one negatively charged SnV center, which leaves an opportunity to improve the implantation parameters. In additional experiments on single tin-vacancy centers, a possible transition to a higher excited state as well as the charge-state transitions of the defects were probed. The results of these measurements contribute to the growing body of research on tin-vacancies and other group IV centers.

DOI
10.15488/21199

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Sources of single photons are integral to a number of applications in the emerging field of quantum technologies. For any practical implementation of single-photon sources, a variety of different properties and an overall comprehensive characterization of the sources are required. Color centers in hBN and group IV color centers in diamond are promising candidate sources due to their favorable properties and rich internal level structure. Both of these candidates, however, also present some serious challenges. Although bright and spectrally narrow, defects in hBN suffer from emission instabilities. Furthermore, limited knowledge about their atomic composition leads to behaviour, which is often unpredictable. Meanwhile, Group IV centers generally exhibit low extraction efficiencies due to total internal reflection inside the high-index diamond host material. In this thesis, several large-scale series of experiments are conducted to investigate both types of emitters in a confocal fluorescence microscope at room temperature. The excitation characteristics of a large number of single-photon emitters in hBN from a narrow spectral window are investigated using a fully automated procedure. The results are compared to theoretical predictions for several carbon defects from the literature to gain further knowledge of the atomic nature of the underlying defects. Based on this approach, the CB, CN, CBVN, and CNVB centers are confidently ruled out as possible origins of the observed emission. Some uncertainty remains about the assignment of the carbon trimer C2CN as well as carbon-based donor-acceptor pairs. In a separate series of experiments, emission instabilities of hBN emitters from the same spectral region are studied. The detected fluctuations in brightness were conclusively attributed to spectral diffusion of the emission. Furthermore, optical stabilization of these effects via short-wavelength irradiation favors an explanation of the observed behavior via nearby charge carriers and the resulting Stark effect. Tin-vacancies, as representatives of group IV centers, are studied in a novel type of diamond waveguide structure for light collection enhancement. A center with sharp zero-phonon emission around 619 nm, a g(2)(0) value of 0.32, and simultaneous stable count rate of 3.4 Mcps was found. By restricting the collection to the zero-phonon line, g(2)(0) = 0.1 could be achieved. In a widespread characterization of the sample, it was found that most structures contain more than one negatively charged SnV center, which leaves an opportunity to improve the implantation parameters. In additional experiments on single tin-vacancy centers, a possible transition to a higher excited state as well as the charge-state transitions of the defects were probed. The results of these measurements contribute to the growing body of research on tin-vacancies and other group IV centers.
This thesis decay rate enhancement and photophysics of nitrogen vacancy (NV) centers in diamond and quantum emitters in hexagonal boron nitride (hBN). The NV center in diamond is a unique physical system that finds use in many quantum technologies such as quantum sensing, quantum information processing and single photon generation. Consisting of a substitutional nitrogen atom next to a vacant lattice site, the NV center introduces discrete electronic energy levels within the wide bandgap of diamond. The NV center can be optically excited and will emit single photons upon relaxation that hold information of the spin state of the NV center. In this thesis, we use metallic structures to modify and enhance the decay rate of NV centers in bulk and nano diamonds in three different experiments. Such an enhancement is a way to improve the usability of NV as a single photon source. Using TiN films with metamaterial properties we observe a 2-fold decrease of the total excited state lifetime of NV centers in nano diamonds, when comparing to similar NV centers not influenced by the TiN films. For shallow implanted NV centers in bulk diamond we experimentally investigate how a decay rate enhancement influences the signal-to-noise ratio (SNR) in spin readout measurements. In this experiment we perform spin state readout before and after introducing a rate enhancement and find a 30 % drop in spin contrast. We model the spin readout measurements using a five-level model and use that to predict the SNR under higher rate enhancement. In the last NV related experiment we use a curved metallic mirror on top of shallow implanted NV centers, to measure the continuous lifetime modification as a function of distances to the mirror. This allows us to determine the internal quantum efficiency (IQE) by fitting the experimental data with a model that includes calculating the expected Purcell factor. We find IQE values of 0.70±0.07 and 0.82±0.08 for implantation depths of 4.5±1 and 8±2 nm, respectively. Last but not least, newly discovered bright single photon emitters in two dimensional hBN were investigated. Similar to the NV center they are believed to be crystal defects, but the defect configuration is not fully known. In this thesis, the photophysics of quantum emitters in hBN nano flakes are investigated. Intensity autocorrelation measurements indicate the presence of at least two metastable states, seen by distinct photon bunching levels on long time scales in the g(2)(τ)-functions. We also observe blinking behaviour, which we show can be explained by changes in the IQE. From rate equation fitting we find that transition rates scale linearly with excitation power. Based on the transition rates we estimate the IQE to be close to unity for excitation powers below saturation.
Abstract We report on the creation and characterization of Pb-related color centers in diamond upon ion implantation and subsequent thermal annealing. Their optical emission in the photoluminescence (PL) regime consists of an articulated spectrum with intense emission peaks at 552.1 and 556.8 nm, accompanied by a set of additional lines in the 535–700 nm range. The attribution of the PL emission to stable Pb-based defects is corroborated by the correlation of its intensity with the implantation fluence of Pb ions. PL measurements performed as a function of sample temperature (in the 143–300 K range) and under different excitation wavelengths (i.e., 532, 514, 405 nm) suggest that the complex spectral features observed in Pb-implanted diamond might be related to a variety of different defects and/or charge states. The emission of the 552.1 and 556.8 nm lines is reported at the single-photon emitter level, demonstrating that they originate from the same individual defect. This work follows from previous reports on optically active centers in diamond based on group-IV impurities, such as Si, Ge, and Sn. In perspective, a comprehensive study of this set of defect complexes could bring significant insight on the common features involved in their formation and opto-physical properties, thus offering a basis for the development of a new generation of quantum-optical devices.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
Fluorescent emitters in diamond are considered to be a valuable resource for fields such as quantum communication, quantum photonics, and biological imaging. In this paper, we report a wide range of narrow bandwidth ( ~ 1.5 nm) spectral emission lines arising from different color centers at room temperature. The defects were created by chemical vapor deposition of thin diamond films grown on silica substrates seeded with nanoparticles of diamond and nickel. These fluorescent lines also possess single or few centers photon statistics. We correlate the zero-phonon lines, observed using confocal microscopy, with previously identified nickel-related centers which have been observed in high-pressure high-temperature diamond, with a Si/Ni complex and silicon vacancy defects. We compare our findings with recent results demonstrating single-photon emission in diamond associated with nickel-related centers to clarify and summarize previous studies concerning this specific dopant. The great variety of emission lines observed in the synthesized material, mainly associated with nickel-related centers, could be an important resource for applications relying on the presence of several emitters of single photons in the same sample. Moreover, the possibility of mass production of these centers in nanodiamonds in colloidal suspension may provide an important resource for biomarking and microscopy.
Quantum communication and quantum metrology established a demand for an accessible solid state systems which can generate a stream of single photons on demand [1]. Although single photon emission has been demonstrated from quantum dots (QD)[1,2], single molecules [3] and nanowires [4], their practical operation is limited by the temperature or photostability. Diamond crystals, however, are the most promising platform for generation of robust, photo-stable, single photons at room temperature [5,6]. Nevertheless, out of more than 500 existing optical centers in diamond only three known centers demonstrated a clear single photon emission: the nitrogen-vacancy complex [6,7], the silicon-vacancy complex [8] and the nickel-nitrogen complex [9,10]. Recent progress in materials science and fabrication techniques of diamond color centers unveiled novel quantum emitters with photo-physical properties surpassing the current mainstream [11,12,13]. Consequently, the versatility of the diamond lattice to host various impurities which give luminescence signals lead to a dramatic discovery of ultra bright single photon emitters operating in the MHz regime [14]. These new centers, comparable with QD in terms of brightness [1], but have the tremendous advantage of their room temperature operation and photo-stability. Furthermore, it opened a new avenue to investigate essentially an unknown group of single photon emitters. A brief description of the fabrication methods and a detailed quantum optical characterization of this class of diamond emitters is the subject of this presentation. In particular we will present the photo-physical properties of a novel family of single photon emitters, most likely originated from Cr impurities within the chemical vapor deposition grown nano-diamond crystals. We concentrate on the typical emission lines in the range of 740 - 790 nm, which exhibit single photon emission with count rate in the range of 0.8-3.2 106 counts/s at the limit of infinite optical excitation power, and life time as short as 1 ns. Even more, some of the emitters exhibit a photon statistics without any photon bunching, indicating a two-level system with unitary quantum efficiency. We will also show preliminary results of a resonant excitation at 4 K. We will highlight future directions to optimize these sources and avenues to investigate the fundamental properties of these centers.
Quantum emitters in diamond are a promising candidate for quantum network applications. Here, we show basic properties of tin-vacancy (SnV) centers in diamond, which we recently discovered. The SnV center shows a sharp zero phonon line and a high fluorescence intensity. The SnV center has a possibility to have a long spin coherence time in the Kelvin temperature range, in contrast to other group-IV color centers, i.e. silicon-vacancy and germanium-vacancy centers. We discuss important experiments regarding spin and optical properties of the SnV quantum emitter for further development towards quantum network.