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arXiv:2207.07217 · Laser & Photonics Review

Modeling of Radiative Emission from Shallow Color Centers in Single Crystalline Diamond

Maryam Zahedian, Jietian Liu, Ricardo Vidrio, Shimon Kolkowitz, Jennifer T. Choy

Published Feb 9, 2023• 10 citations
arXivHTMLPDF

Abstract

Abstract Optically active defects in diamond are widely used as bright single‐photon sources for quantum sensing, computing, and communication. For many applications, it is useful to place the emitter close to the diamond surface, where the radiative properties of the emitter are strongly modified by its dielectric environment. It is well‐known that the radiative power from an electric dipole decreases as the emitter approaches an interface with a lower‐index dielectric, leading to an increase in the radiative lifetime. For emitters in crystalline solids, modeling of this effect needs to take into account the crystal orientation and direction of the surface cut, which can greatly impact the emission characteristics. In this paper, a framework for analyzing the emission rates of shallow (<100 nm) defects is provided, in which optical transitions are derived from electric dipoles in a plane perpendicular to their spin axis. The calculations for the depth‐dependent radiative lifetime for color centers in (100)‐, (110)‐, and (111)‐cut diamond are presented, which can be extended to other vacancy defects in diamond.

DOI
10.1002/lpor.202200529

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Abstract Optically active defects in diamond are widely used as bright single‐photon sources for quantum sensing, computing, and communication. For many applications, it is useful to place the emitter close to the diamond surface, where the radiative properties of the emitter are strongly modified by its dielectric environment. It is well‐known that the radiative power from an electric dipole decreases as the emitter approaches an interface with a lower‐index dielectric, leading to an increase in the radiative lifetime. For emitters in crystalline solids, modeling of this effect needs to take into account the crystal orientation and direction of the surface cut, which can greatly impact the emission characteristics. In this paper, a framework for analyzing the emission rates of shallow (<100 nm) defects is provided, in which optical transitions are derived from electric dipoles in a plane perpendicular to their spin axis. The calculations for the depth‐dependent radiative lifetime for color centers in (100)‐, (110)‐, and (111)‐cut diamond are presented, which can be extended to other vacancy defects in diamond.
ABSTRACT The negatively charged nitrogen‐vacancy (NV) center in diamond is a leading solid‐state quantum emitter, offering spin‐photon interfaces over a wide temperature range with applications from electromagnetic sensing to bioimaging. While NV centers in bulk diamond are well understood, embedding them in nanodiamond (ND) introduces complexities from size, NV location, and NV polarizations. NVs in ND show altered fluorescence properties, including longer lifetimes, lower quantum efficiency, and higher sensitivity to dielectric surroundings, which arise from radiative suppression, surface‐induced non‐radiative decay, and escape inefficiency at the diamond‐background interface. Prior models typically addressed isolated aspects, such as dielectric contrast or surface quenching, without integrating full quantum‐optical NV behavior with classical electrodynamics. We present a hybrid framework coupling rigorous electromagnetic simulations with a quantum‐optical NV model including phonon sideband dynamics. NV emission is found to depend strongly on ND size, NV position, and surrounding refractive index. Our results explain observations such as shallow NVs in water‐coated ND appearing brighter than deeper ones in air. This integrated model provides a unified framework for realistic NV in ND emission scenarios and informs the design of efficient NV‐based sensors and quantum devices, advancing understanding of quantum emitter photophysics in nanoscale crystals.
The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.
Color centers in diamond—especially group IV defects—have been advanced as a viable solid-state platform for quantum photonics and information technologies. We investigate the photodynamics and characteristics of germanium-vacancy (GeV) centers hosted in high-pressure high-temperature diamond nanocrystals. Through back-focal plane imaging, we analyze the far-field radiation pattern of the investigated emitters and derive a crossed-dipole emission, which is strongly aligned along one axis. We use this information in combination with lifetime measurements to extract the decay rate statistics of the GeV emitters and determine their quantum efficiency, which we estimated to be ∼ ( 22 ± 2 ) % . Our results offer further insight into the photodynamic properties of the GeV center in nanodiamonds and confirm its suitability as a desirable system for quantum technologies.
The recently demonstrated electroluminescence of color centers in diamond makes them one of the best candidates for room temperature single-photon sources.However, the reported emission rates are far off what can be achieved by state-of-the-art electrically driven epitaxial quantum dots.Since the electroluminescence mechanism has not yet been elucidated, it is not clear to what extent the emission rate can be increased.Here we develop a theoretical framework to study single-photon emission from color centers in diamond under electrical pumping.The proposed model comprises electron and hole trapping and releasing, transitions between the ground and excited states of the color center as well as structural transformations of the center due to carrier trapping.It provides the possibility to predict both the photon emission rate and the wavelength of emitted photons.Self-consistent numerical simulations of the single-photon emitting diode based on the proposed model show that the photon emission rate can be as high as 100 kcounts s -1 at standard conditions.In contrast to most optoelectronic devices, the emission rate steadily increases with the device temperature achieving of more than 100 Mcount s -1 at 500 K, which is highly advantageous for practical applications.These results demonstrate the potential of color centers in diamond as electrically driven non-classical light emitters and provide a foundation for the design and development of single-photon sources for optical quantum computation and quantum communication networks operating at room and higher temperatures.
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.
Colour centres in diamond are promising candidates as a platform for quantum technologies and biomedical imaging based on spins and/or photons. Controlling the emission properties of colour centres in diamond is a key requirement for the development of efficient single-photon sources having high collection efficiency. A number of groups have achieved an enhancement in the emission rate over narrow wavelength ranges by coupling single emitters in nanodiamond crystals to resonant electromagnetic structures. In this paper, we characterize in detail the spontaneous emission rates of nitrogen-vacancy centres at various locations on a structured substrate. We found a factor of 1.5 average enhancement of the total emission rate when nanodiamonds are on an opal photonic crystal surface, and observed changes in the lifetime distribution. We present a model for explaining these observations and associate the lifetime properties with dipole orientation and polarization effects.