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Optical Spectroscopy of Xenon-Related Defects in Diamond

Y. Dziashko

Published Jan 1, 2014• 2 citations
OpenAlex

Abstract

The work presents the results of optical studies of Xe-related defect in diamond. This defect is one of a few having narrow zero-phonon line in the near-infrared part of the photo-luminescence spectra. It appears in diamond after Xe+ ion implantation followed by thermal annealing. Given unique physical properties of diamond (hardness, optical transparency in wide spectral range, chemical inertness, high thermal conductivity, low thermal expansion coefficient) and stability of Xe-related center it can be viewed as an potential candidate for the source of single-photons, or as optically manipulated qubit, not unlike nitrogen-vacancy center. However, compared to the latter Xe-related center is not as well understood and it is necessary to gain thorough understanding of its spatial structure, symmetry, electronic states and mechanisms of interaction with the host diamond lattice. This thesis addresses several questions, in regard to Xe-related center: 1) How efficiently this center is formed in the implantation/annealing process; 2) How does it interact with the host lattice to produce both homogeneous and inhomogeneous shape of the 811.7 nm zero-phonon line; and 3) What is the type and nature of transitions responsible for the 811.7 nm zero-phonon line. In answering the first question two methods for measuring the conversion efficiency of any kind of optically active defect have been developed and applied to Xe-related center in diamond. The study of line-broadening mechanisms showed how this center interacts with the strain produced by other neighboring Xe-centers, distributed in a plane-like geometry. Also, interaction with vibrational motions of the diamond lattice localized in the vicinity of the Xe-centers is analyzed and the parameters of this pseudo-local mode are found. Finally, using the effects of optical saturation in photo-luminescence under excitation with Gaussian laser beams it has been shown that 811.7 nm zero-phonon line is due to absorption and emission by circular magnetic dipole. Also, the site symmetry of Xe-related center has been confirmed as trigonal with the threefold axis oriented alongdirection in the diamond crystal.

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The work presents the results of optical studies of Xe-related defect in diamond. This defect is one of a few having narrow zero-phonon line in the near-infrared part of the photo-luminescence spectra. It appears in diamond after Xe+ ion implantation followed by thermal annealing. Given unique physical properties of diamond (hardness, optical transparency in wide spectral range, chemical inertness, high thermal conductivity, low thermal expansion coefficient) and stability of Xe-related center it can be viewed as an potential candidate for the source of single-photons, or as optically manipulated qubit, not unlike nitrogen-vacancy center. However, compared to the latter Xe-related center is not as well understood and it is necessary to gain thorough understanding of its spatial structure, symmetry, electronic states and mechanisms of interaction with the host diamond lattice. This thesis addresses several questions, in regard to Xe-related center: 1) How efficiently this center is formed in the implantation/annealing process; 2) How does it interact with the host lattice to produce both homogeneous and inhomogeneous shape of the 811.7 nm zero-phonon line; and 3) What is the type and nature of transitions responsible for the 811.7 nm zero-phonon line. In answering the first question two methods for measuring the conversion efficiency of any kind of optically active defect have been developed and applied to Xe-related center in diamond. The study of line-broadening mechanisms showed how this center interacts with the strain produced by other neighboring Xe-centers, distributed in a plane-like geometry. Also, interaction with vibrational motions of the diamond lattice localized in the vicinity of the Xe-centers is analyzed and the parameters of this pseudo-local mode are found. Finally, using the effects of optical saturation in photo-luminescence under excitation with Gaussian laser beams it has been shown that 811.7 nm zero-phonon line is due to absorption and emission by circular magnetic dipole. Also, the site symmetry of Xe-related center has been confirmed as trigonal with the threefold axis oriented alongdirection in the diamond crystal.
Ion implantation in diamond creates optically active defects which have emission lines in broad spectral regions and may be used in advanced photonics and optical communication applications. A brief review of the photoluminescence properties of Xe+ ion implanted diamond is presented. The Xe-related center is of particular interest as this center is one of a few centers (Ni, Si, Cr) in diamond having sharp emission lines in the infrared spectral region, specifically at 813 and 794nm. The paper discusses an approach to determine the important and difficult to measure conversion efficiency of implanted ions into emitting optical centers. The method uses micro-luminescence confocal mapping and statistical analysis based on a compound Poisson distribution, accounting for both the implanted centers and the optically excited centers statistics. Results of numerical simulations and experimental measurements are presented.
Diamond is a promising platform for the development of technological applications in quantum optics and photonics. The quest for color centers with optimal photo-physical properties has led in recent years to the search for novel impurity-related defects in this material. Here, we report on a systematic investigation of the photo-physical properties of two He-related (HR) emission lines at 535.2 nm and 559.7 nm (as measured at a temperature of 25 K) created in three different diamond substrates upon implantation with 1.3 MeV He+ ions and subsequent annealing. The spectral features of the HR centers were studied in an “optical grade” diamond substrate as a function of several physical parameters, namely, the measurement temperature, the excitation wavelength, and the intensity of external electric fields. The emission lifetimes of the 535.2 nm and 559.7 nm lines were also measured by means of time-gated photoluminescence measurements. The Stark shifting of the HR centers under the application of an external electrical field was observed in a CVD diamond film equipped with buried graphitic electrodes, suggesting the lack of inversion symmetry in the defects' structure. Furthermore, the photoluminescence mapping under 405 nm excitation of a “detector grade” diamond sample implanted at a He+ ion fluence of 1 × 1010 cm−2 enabled us to identify the spectral features of both the HR emission lines from the same localized optical spots. The reported results provide an insight into the structure of He-related defects in diamond and their possible utilization in practical applications.
Abstract Optically active defects in diamond find a wide range of applications from lasers to single photon emitters essential for quantum communications. Ion implantation followed by thermal annealing is a mature technique used to create such defects. Implanted at a fixed energy, ions form a thin layer of optically active defects. Low temperature photoluminescence spectra of Xe‐related defects in pure CVD diamond show peculiar behavior: the narrow zero‐phonon line at 811.7 nm changes its shape significantly with the increase of implantation dose from 1.1 × 1011 to 5 × 1012 ion cm−2. This work investigates the possible causes of this effect: planar geometry of the defects distribution and/or the complex defect structure.
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.
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.
We report the optical observation of lead-vacancy (PbV) centers in diamond fabricated by Pb ion implantation and subsequent high-temperature annealing (2100 °C) under high pressure (7.7 GPa). Their optical properties were characterized by photoluminescence at varying temperatures down to 5.7 K. We observed intense emission peaks at 550 and 554 nm, with a large splitting of approximately 3900 GHz. The two lines are thought to correspond to the zero phonon line (ZPL) of PbV centers with split ground and excited states. A cubic trend of the ZPL width was observed while varying the temperature. We performed polarization measurements of the two lines in a single PbV center, showing nearly orthogonal dipole polarizations. These optical measurements strongly indicate that the PbV center possesses D 3 d symmetry in the diamond lattice. The observed large ground state splitting significantly suppresses the phonon-mediated transition, which causes decoherence of the electron spin state of the group IV color centers in diamond, leading to the expectation of a long spin coherence time at a temperature ∼9 K.