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Physical review. B./Physical review. B

Photophysics of single LX centers in high pressure–high temperature microdiamonds

Arthur Yu. Neliubov, Aleksandr O. Tarasevich, Margarita Pavlenko, Евгений Алексеевич Екимов, А. В. Наумов, Ivan Yu. Eremchev

Published Apr 16, 2025• 1 citation
Publisher

Abstract

LX centers are a recently discovered class of impurity centers in diamonds, which are characterized by nearly phononfree, spectral narrowband, and intense fluorescence at room temperature. Such a set of properties pave the way for a variety of applications, including sensing and single-photon emission. The latter requires a detailed study of photophysical processes of single emitters, which is the focus of this paper. The study of the luminescence dynamics of single LX centers in microdiamonds, synthesized by the high pressure-high temperature method, is performed by means of second-order cross-correlation function (${g}^{(2)}$) analysis. Even though the blinking is not observed directly in the measurements, the presence of photon bunching indicates that the fluorescence of a single emitter is intermittent at microsecond scale. The three-level system that is commonly used to describe intermittency of dye molecules is not consistent with the observed power dependences. We suggest a four-level energy system model with two metastable states to describe the results and perform numerical simulations to validate the model. Finally, we discuss the four-level model in the form of fluctuations of photophysical parameters.

DOI
10.1103/physrevb.111.155420

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LX centers are a recently discovered class of impurity centers in diamonds, which are characterized by nearly phononfree, spectral narrowband, and intense fluorescence at room temperature. Such a set of properties pave the way for a variety of applications, including sensing and single-photon emission. The latter requires a detailed study of photophysical processes of single emitters, which is the focus of this paper. The study of the luminescence dynamics of single LX centers in microdiamonds, synthesized by the high pressure-high temperature method, is performed by means of second-order cross-correlation function (g(2){g}^{(2)}g(2)) analysis. Even though the blinking is not observed directly in the measurements, the presence of photon bunching indicates that the fluorescence of a single emitter is intermittent at microsecond scale. The three-level system that is commonly used to describe intermittency of dye molecules is not consistent with the observed power dependences. We suggest a four-level energy system model with two metastable states to describe the results and perform numerical simulations to validate the model. Finally, we discuss the four-level model in the form of fluctuations of photophysical parameters.
Microdiamonds with color centers have unique photophysical properties. We discover extremely narrow spectral lines with full width at half maximum down to 0.5 nm (\ensuremath{\approx}390 GHz at wavelength 630.15 nm) at room temperature in photoluminescence of numerous high-pressure--high-temperature microdiamonds. Correlation spectroscopy proves that these lines originate from single photon emitters. Comprehensive experimental characterization of the emitters is performed by means of complementary scanning electron and fluorescence microscopy that allows morphological characterization and in time monitoring of the same labeled emitters. Study of photoluminescence and photoluminescence excitation spectra of single emitters showed negligible phonon sideband and narrowband excitation. Temperature sensitivity, stable photoluminescence, brightness, linear polarization, and fluorescence lifetime \ensuremath{\approx}1.5--2.5 ns are demonstrated. The results show great potential of the discovered ``enigmatic'' emitters for applications in quantum optics, fluorescence labeling, and high-resolution thermometry.
A detailed study of the photophysical properties of several chromium-related color centers produced within chemical vapor deposition diamond is presented. These emitters show narrow luminescence lines in the range of $740\ensuremath{-}770$ nm. Single-photon emission was verified with continuous and pulsed excitation with detected emission rates at saturation in the range of ($2\ensuremath{-}3$) $\ifmmode\times\else\texttimes\fi{}$ 106{10}^{6}106 counts/s, while direct lifetime measurements reveal excited state lifetimes for the distinct centers ranging $1\ensuremath{-}14$ ns. In addition, a number of quantum emitters demonstrate two-level behavior with no bunching present in the second-order correlation function. The three-level systems revealed typically photoluminescence lines with width half-maximum of  4~4 4 nm while the two-level emitters have full width half-maximum of  10~10 10 nm at room temperature. In addition, the quantum efficiency of the two-level system was measured to be four times higher than that of the three-level system.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size 50 nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.
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.
Single silicon vacancy (SiV) color centers in diamond have recently shown the ability for high brightness, narrow bandwidth, room temperature single photon emission. This work develops a model describing the three level population dynamics of single SiV centers in diamond nanocrystals on iridium surfaces including an intensity dependent de-shelving process. Furthermore, we investigate the brightness and photostability of single centers and find maximum single photon rates of 6.2 Mcps under continuous excitation. We investigate the collection efficiency of the fluorescence and estimate quantum efficiencies of the SiV centers.
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.