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SPIE Quantum Technologies

Structural dependence of antibunching and fluorescence lifetime

Madhura Ghosh Dastidar, Praveen Hegde, Immanuel Thekkooden, Vidya Praveen Bhallamudi

Published Jun 10, 2024• 0 citations
Publisher

Abstract

The rapid growth of quantum technologies has driven the development of quantum defects for both single photon sources as well as for spin qubit and sensor applications. These artificial atoms in wide bandgap solid-state materials such as diamond and hBN offer the possibility of a truly quantum deterministic source. These single photon emitting quantum defects exhibit antibunching that can be quantified by performing the Hanbury-Brown Twiss (HBT) experiment. The HBT experiment allows one to evaluate the second-order autocorrelation (g(2)(τ )) function, which is a central measure in determining the quality of single photon emission. To enhance the various emission parameters such as intensity, wavelength, and directionality from these defects the development of photonic structures become essential. Here, we study single photon emission from a diamond nanopillar array containing Nitrogen Vacancy (NV) centers. We spatially map the g(2)(τ ) function and radiative lifetimes in these samples and correlate the two quantities. Crucially, we observe that the measured antibunching varies as a function of position of the objective relative to the nanopillar, even across the same pillar. This likely shows the dependence of the apparent antibunching to the angle of excitation and detection in such photonic structures. Our results highlight the importance of structural and geometric factors in g(2)(τ ) measurements of emitters, especially when embedded in photonic structures. These should be carefully understood in evaluating the quality of the single photon sources.

DOI
10.1117/12.3016497

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The rapid growth of quantum technologies has driven the development of quantum defects for both single photon sources as well as for spin qubit and sensor applications. These artificial atoms in wide bandgap solid-state materials such as diamond and hBN offer the possibility of a truly quantum deterministic source. These single photon emitting quantum defects exhibit antibunching that can be quantified by performing the Hanbury-Brown Twiss (HBT) experiment. The HBT experiment allows one to evaluate the second-order autocorrelation (g(2)(τ )) function, which is a central measure in determining the quality of single photon emission. To enhance the various emission parameters such as intensity, wavelength, and directionality from these defects the development of photonic structures become essential. Here, we study single photon emission from a diamond nanopillar array containing Nitrogen Vacancy (NV) centers. We spatially map the g(2)(τ ) function and radiative lifetimes in these samples and correlate the two quantities. Crucially, we observe that the measured antibunching varies as a function of position of the objective relative to the nanopillar, even across the same pillar. This likely shows the dependence of the apparent antibunching to the angle of excitation and detection in such photonic structures. Our results highlight the importance of structural and geometric factors in g(2)(τ ) measurements of emitters, especially when embedded in photonic structures. These should be carefully understood in evaluating the quality of the single photon sources.
Defects in diamond have evolved as unique object for their potential application for Optical imaging and Nano-photonics. High pressure high temperature (HPHT) grown type-Ib diamond particles were milled down to the size of ~ 80 nm and purified to remove iron & graphitic carbon impurities and irradiated with 35 KeV He+ ions to create vacancies in the diamond lattice. Vacancies diffuse close to substitutional nitrogen impurities of nano-diamond particles upon thermal treatment. Characteristic sharp emission of NV centers were observed at 575.5 nm and 637.9 nm corresponding to NV° and NV− charged states in addition to a broad emission in the range 550-750 nm. Structural and photo-physical behavior of these fluorescent diamonds was found to depend on the method of purification adopted. Samples purified through acid reflux were found suitable for bio-imaging applications while, sample purified through air oxidation shows properties desirable for Nano-photonic applications. Photon-correlation measurements of emission from individual diamond nanoparticles using Hanbury Brown and Twiss interferometer (HBT) shows anti-bunching curve with g2(t)= 0 confirming their suitability as single photon source. Such sources of indistinguishable photons are highly desirable for quantum computation and quantum optics applications.
Emitters of single photons are essential resources for emerging quantum technologies and developed within different platforms including nonlinear optics and atomic and solid-state systems. The energy-level structures of emission processes are critical for reaching and controlling high-quality sources. The most commonly applied test uses a Hanbury Brown and Twiss (HBT) setup to determine the emitter energy-level structure based on fitting temporal correlations of photon detection events. However, only partial information about the emission process is extracted from such detection, that might be followed by an inconclusive fitting of the data. This process predetermines our limited ability to quantify and understand the dynamics in the photon emission process that are of importance for the applications in communication, sensing, and computing. In this work, we present a complete analysis based on all normalized coincidences between detection and no-detection events recorded in the same HBT setup to certify expected properties of an emitted photonic state. As a proof of concept we apply our methodology to single nitrogen-vacancy centers in diamond, in which case the certification conclusively rejects a model based on a two-level emitter that radiates a photonic state mixed with any classical noise background. Published by the American Physical Society 2024
The fabrication of luminescent defects in single-crystal diamond upon Sn implantation and annealing is reported. The relevant spectral features of the optical centers (emission peaks at 593.5, 620.3, 630.7, and 646.7 nm) are attributed to Sn-related defects through the correlation of their photoluminescence (PL) intensity with the implantation fluence. Single Sn-related defects were identified and characterized through the acquisition of their second-order autocorrelation emission functions, by means of Hanbury-Brown and Twiss interferometry. The investigation of their single-photon emission regime as a function of excitation laser power revealed that Sn-related defects are based on three-level systems with a 6 ns radiative decay lifetime. In a fraction of the studied centers, the observation of a blinking PL emission is indicative of the existence of a dark state. Furthermore, absorption dependence on the polarization of the excitation radiation with ∼45% contrast was measured. This work shed light on the existence of a new optical center associated with a group-IV impurity in diamond, with similar photophysical properties to the already well-known Si–V and Ge–V emitters, thus, providing results of interest from both the fundamental and applicative points of view.
The nitrogen-vacancy (NV) center is a defect in the structure of diamond, roughly the size of a single atom, that possesses properties that make it applicable to quantum information processing, high-resolution magnetic resonance imaging, and probing biological systems. When an NV center is excited by green light of wavelength 523 nm, it emits red light of in the range from 600-800 nm tens of nanoseconds later. A confocal microscope can be used to excite and collect emitted photons from NV centers. By detecting the intensity of the emitted red photons, we can determine the quantum state of a single NV center, which is needed to build various quantum computing, sensing and imaging devices. The autocorrelation method is used to detect antibunching in the emission of red photons and ascertain that the observed photons are being emitted from a single NV center. We have built an autocorrelation device that measures, with sub-nanosecond accuracy, the statistical distribution of the arrival times of the red photons emitted from a diamond sample at a photon counter. The device can measure fixed time values with a time resolution of 120 ps FWHM. For uncorrelated sources measured for 120 seconds at the TAC full range of 100 ns, the average counts in each histogram bin were about 0.01% of the predicted value. The autocorrelation device that we have built costs about 10 times less than commercial units used by other NV researchers.
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.
For applications in Quantum Information and Quantum Key Distribution an on-demand source of single photons is desirable because absolute security is of utmost importance. Photons are quantum systems; hence encoding information onto them offers a secure alternative to classical cryptography as a measurement cannot be performed on photons without altering their properties. The Nitrogen Vacancy (NV) centre in diamond is a good source of such photons. It is photo-stable and its location in diamond offers robustness. It has zero phonon line at 637 nm and its relative short luminescence life-time of about 12 ns makes it suitable for generating single photons. This thesis covers two aspects: Firstly the characterization of defects in diamonds and subsequent selection of diamonds suitable for use in the single photon setup and secondly, the development of the experimental setup for single photon generation. This thesis sets out to describe the development of a laboratory based single photon source using the NV centre in diamond. For this purpose a suite of diamond samples were selected and subjected to various spectroscopic tests in order to characterize and classify the samples, especially the presence of the NV centres and their concentrations. The characterization of the defects was done through the use of the following spectroscopic techniques: UltravioletVisible-Near infrared spectroscopy, Infrared spectroscopy, Electron Spin Resonance and Photoluminescence. These techniques enabled us to understand the types and origins of crystal defects that were present in the diamond samples used in this study and to use this to select diamonds that are most suitable for use in generation of single photons. The experimental setup for single photon generation using the NV centre is based on a confocal microscope arrangement. Single NV centres were identified by measuring the second order autocorrelation function of the fluorescence light emitted by the sample when illuminated with a laser. This measurement was done using a Hanbury-Brown Twiss (HBT) interferometer.