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Nanotechnology

Fluorescence dynamics of color centers in diamond needles

Филоненко Елена Михайловна, P. Kuzhir, Sergei Malykhin

Published Mar 25, 2025• 1 citation
Publisher

Abstract

Abstract This study presents a detailed investigation into the fluorescence properties of color centers in single-crystal diamond needles (SCDNs) synthesized via chemical vapor deposition. Using steady-state and time-resolved photoluminescence (PL) techniques, we identified color centers with zero-phonon lines at 389 nm, 468 nm, 575 nm (NV0), 637 nm (NV–), and 738 nm (SiV–). PL excitation spectroscopy conducted at room temperature revealed the complex electronic structure of some of these centers, paving the way for further investigation into their fluorescence properties. Lifetime measurements were performed for each center, with the 389 nm one exhibiting the longest decay time (∼30 ns), which is advantageous for enhancing quantum coherence, improving photon emission efficiency, and reducing power consumption. Altogether, these findings highlight the potential of SCDNs for quantum applications and confirm their promise as a platform for next-generation photonic and quantum devices.

DOI
10.1088/1361-6528/adc4f1

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Abstract This study presents a detailed investigation into the fluorescence properties of color centers in single-crystal diamond needles (SCDNs) synthesized via chemical vapor deposition. Using steady-state and time-resolved photoluminescence (PL) techniques, we identified color centers with zero-phonon lines at 389 nm, 468 nm, 575 nm (NV0), 637 nm (NV–), and 738 nm (SiV–). PL excitation spectroscopy conducted at room temperature revealed the complex electronic structure of some of these centers, paving the way for further investigation into their fluorescence properties. Lifetime measurements were performed for each center, with the 389 nm one exhibiting the longest decay time (∼30 ns), which is advantageous for enhancing quantum coherence, improving photon emission efficiency, and reducing power consumption. Altogether, these findings highlight the potential of SCDNs for quantum applications and confirm their promise as a platform for next-generation photonic and quantum devices.
Atomic-sized fluorescent defects in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. In this study, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
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.
Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~10 3 ) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.
Color centers in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. Here, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.
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.