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Advanced Optical Materials

Observation of Binary Spectral Jumps in Color Centers in Diamond

Zhao Mu, Yu Zhou, Disheng Chen, Johannes E. Fröch, Jianqun Yang, Xingji Li, Igor Aharonovich, Weibo Gao

Published Jul 15, 2020• 6 citations
Publisher

Abstract

Abstract Optical “blinking” normally refers to a switching behavior of fluorescence for quantum emissions between “ON” and “OFF” state. For quantum dots, single molecules, and nitrogen‐vacancy centers in diamond, it usually stems from conversions between two different charge states, with one emitting strong and bright fluorescence while the other scattering weak or no fluorescence. Here, a different type of blinking from single emitters in ion implanted diamond is reported, with both blinking states exhibiting detectable photoluminescence under nonresonant excitation. Thanks to the low jumping rates, the dynamics of the emission can be directly monitored. The quadratic power dependence of the conversion rates suggests the possibility of two‐photon ionization process in quantum jumps. This work provides extra insights into the photodynamics of the spectral jumps on defect‐based single‐photon emitters hosted in wide‐bandgap semiconductors.

DOI
10.1002/adom.202000495

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Abstract Optical “blinking” normally refers to a switching behavior of fluorescence for quantum emissions between “ON” and “OFF” state. For quantum dots, single molecules, and nitrogen‐vacancy centers in diamond, it usually stems from conversions between two different charge states, with one emitting strong and bright fluorescence while the other scattering weak or no fluorescence. Here, a different type of blinking from single emitters in ion implanted diamond is reported, with both blinking states exhibiting detectable photoluminescence under nonresonant excitation. Thanks to the low jumping rates, the dynamics of the emission can be directly monitored. The quadratic power dependence of the conversion rates suggests the possibility of two‐photon ionization process in quantum jumps. This work provides extra insights into the photodynamics of the spectral jumps on defect‐based single‐photon emitters hosted in wide‐bandgap semiconductors.
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.
A systematic photoluminescence (PL) investigation of the spectral emission properties of individual optical defects fabricated in diamond upon ion implantation and annealing is reported. Three spectral lines at 620, 631, and 647 nm are identified and attributed to the SnV center due to their occurrence in the PL spectra of the very same single‐photon emitting defects. It is shown that the relative occurrence of the three spectral features can be modified by oxidizing the sample surface following thermal annealing. The relevant emission properties of each class of individual emitters, including the excited state emission lifetime and the emission intensity saturation parameters are reported.
Single-photon emitters with stable and uniform photoluminescence properties are important for quantum technology. However, in many cases, colour centres in diamond exhibit spectral diffusion and photoluminescence intensity fluctuation. It is therefore essential to investigate the dynamics of colour centres at the single defect level in order to enable the on-demand manipulation and improved applications in quantum technology. Here we report the polarization switching, intensity jumps and spectral shifting observed on a negatively charged single silicon-vacancy colour centre in diamond. The observed phenomena elucidate the single emitter dynamics induced by photoionization of nearby electron donors in the diamond.
Spectral diffusion is the phenomenon of random jumps in the emission wavelength of narrow lines. This phenomenon is a major hurdle for applications of solid state quantum emitters like quantum dots, molecules, or diamond defect centers in an integrated quantum optical technology. Here, we provide further insight into the underlying processes of spectral diffusion of the zero-phonon line of single nitrogen vacancy centers in nano-size diamond by using a novel method based on photon correlation interferometry. The method works although the spectral diffusion rate is several orders of magnitude higher than the photon detection rate and thereby improves the time resolution of previous experiments with nano-size diamond by 6 orders of magnitude. We study the dependency of the spectral diffusion rate on the excitation power, temperature, and excitation wavelength under off-resonant excitation. Our results bring insight into the mechanism of spectral diffusion and suggest a strategy to increase the number of spectrally indistinguishable photons emitted by diamond nanocrystals.
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.
Optical sources that deliver single photons on demand play a key role in quantum cryptography and optical quantum computations. At present, color centers in wide-bandgap semiconductors, such as the nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers in diamond, are considered to be the most promising candidates for practical quantum information applications owing to their unique emission properties at room temperature. However, for practical reasons, single-photon sources should be pumped electrically, which is required for integrability, scalability, and energy efficiency. However, diamond and related wide-bandgap semiconductor materials are at the interface between insulators and semiconductors, which makes electrical excitation of color centers very challenging. Here, we report on our progress in the understanding of single-photon electroluminescence of color centers in diamond, discuss different factors affecting the brightness of these emitter under electrical excitation, and study how to improve the performance of electrically- pumped single-photon sources based on color centers in diamond.