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arXiv:2310.18822

Donor-acceptor recombination emission in hydrogen-terminated nanodiamond: Novel single-photon source for room-temperature quantum photonics

Dmitrii G. Pasternak, Alexey M. Romshin, R. Kh. Bagramov, A. I. Galimov, Alexey A. Toropov, Dmitry A. Kalashnikov, Victor Leong, Сатанин Аркадий Михайлович, Oleg S. Kudryavtsev, Andrey L. Chernev, Vladimir P. Filonenko, Igor I. Vlasov

Published Oct 28, 2023• 0 citations
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Abstract

In fluorescence spectra of nanodiamonds (NDs) synthesized at high pressure from adamantane and other organic compounds, very narrow (~1 nm) lines of unknown origin are observed in a wide spectroscopic range from ~500 to 800 nm. Here, we propose and experimentally substantiate the hypothesis that these mysterious lines arise from radiative recombination of donor-acceptor pairs (DAPs). To confirm our hypothesis, we study the fluorescence spectra of undoped and nitrogen-doped NDs of different sizes, before and after thermal oxidation of their surface. The results obtained with a high degree of confidence allowed us to conclude that the DAPs are formed through the interaction of donor-like substitutional nitrogen present in the diamond lattice, and a 2D layer of acceptors resulting from the transfer doping effect on the surface of hydrogen-terminated NDs. A specific behavior of the DAP-induced lines was discovered in the temperature range of 100-10 K: their energy increases and most lines are split into 2 or more components with decreasing temperature. It is shown that the majority of the studied DAP emitters are sources of single photons, with an emission rate of up to >1 million counts/s at room temperature, which significantly surpasses that of nitrogen-vacancy and silicon-vacancy centers under the same detection conditions. Despite an observed temporal instability in the emission, the DAP emitters of H-terminated NDs represent a powerful room-temperature single-photon source for quantum optical technologies.

DOI
10.48550/arxiv.2310.18822

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In fluorescence spectra of nanodiamonds (NDs) synthesized at high pressure from adamantane and other organic compounds, very narrow (~1 nm) lines of unknown origin are observed in a wide spectroscopic range from ~500 to 800 nm. Here, we propose and experimentally substantiate the hypothesis that these mysterious lines arise from radiative recombination of donor-acceptor pairs (DAPs). To confirm our hypothesis, we study the fluorescence spectra of undoped and nitrogen-doped NDs of different sizes, before and after thermal oxidation of their surface. The results obtained with a high degree of confidence allowed us to conclude that the DAPs are formed through the interaction of donor-like substitutional nitrogen present in the diamond lattice, and a 2D layer of acceptors resulting from the transfer doping effect on the surface of hydrogen-terminated NDs. A specific behavior of the DAP-induced lines was discovered in the temperature range of 100-10 K: their energy increases and most lines are split into 2 or more components with decreasing temperature. It is shown that the majority of the studied DAP emitters are sources of single photons, with an emission rate of up to >1 million counts/s at room temperature, which significantly surpasses that of nitrogen-vacancy and silicon-vacancy centers under the same detection conditions. Despite an observed temporal instability in the emission, the DAP emitters of H-terminated NDs represent a powerful room-temperature single-photon source for quantum optical technologies.
Hydrogen-terminated diamond is known for its p-type surface conductivity, which arises from a near-surface hole accumulation layer induced by adsorbed acceptor species. Here, we demonstrate that these surface acceptors also form optically active donor–acceptor pairs (DAPs) with substitutional nitrogen donors in diamond. The insertion of a nominally undoped CVD interlayer between a nitrogen-rich high-pressure high-temperature substrate and a hydrogen-terminated surface enables the precise tuning of the donor–acceptor separation with nanometer precision. Radiative DAP recombination appears as bright, spectrally narrow lines whose intensity, energy, and decay dynamics depend systematically on interlayer thickness. Individual lines show single-photon statistics, while ensembles exhibit strong polarization anisotropy reflecting the planar donor–acceptor geometry. These findings reveal an optical counterpart of hydrogen-induced surface transfer doping in diamond and establish a surface-defined, nanometer-tunable platform for engineering DAP-based quantum emitters.
Hydrogen-terminated diamond is known for its p-type surface conductivity, which arises from a near-surface hole accumulation layer induced by adsorbed acceptor species. Here, we demonstrate that these surface acceptors also form optically active donor-acceptor pairs (DAP) with substitutional nitrogen donors in diamond. The insertion of a nominally undoped CVD interlayer between a nitrogen-rich HPHT substrate and a hydrogen-terminated surface enables the precise tuning of the donor-acceptor separation with nanometer precision. Radiative DAP recombination appears as bright, spectrally narrow lines whose intensity, energy, and decay dynamics depend systematically on interlayer thickness. Individual lines show single-photon statistics, while ensembles exhibit strong polarization anisotropy reflecting the planar donor-acceptor geometry. These findings reveal an optical counterpart of hydrogen-induced surface transfer doping in diamond and establish a surface-defined, nanometer-tunable platform for engineering DAP-based quantum emitters.
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.
Abstract Single photon sources (SPSs) are one of the key components in quantum communication technology. Here we report on the development of a new approach to the controlled formation of SPSs in nanodiamonds synthesized from hydrocarbons at high pressure and high temperature (HPHT). The conditions of HPHT synthesis were determined, allowing for the highly efficient production of scalable single-photon emitters based on single silicon-vacancy (SiV) centers in individual diamond particles of 250-300 nm in size. A new type of SPSs, emitting in a wide spectral range (500-800 nm) at room temperature, was found in hydrogen-terminated nanodiamonds. The recorded rate of the SPS emission exceeds 1 million photons per second. The HPHT nanodiamonds containing both SiV and the new emitters are a promising material for quantum photonics applications.
Fluorescent emitters in nanodiamonds are considered to be a valuable resource for emerging fields such as quantum communication, quantum photonics and biological imaging. In this paper we report a wide range of narrow bandwidth spectral emission lines arising from different color centers at room temperature. We associate the zero phonon lines, observed using confocal microscopy, with previously identified nickel-related centers in high pressure high temperature diamond, with a Si/Ni complex and silicon vacancy defects. In particular we show the first observation of a 850 nm emission in diamond with single photon signature, indicating the potential for diamond to harbor infrared single-photon sources. Index Terms diamond defects, single-photon emission, confocal microscopy.
The prospects of using individual nanodiamond particles as a source of single photons were studied for diamonds of various origin. It was shown that the single photon emitters could be produced on a base of "nitrogen-vacancy" centers in detonation nanodiamond synthesized from graphite-hexogen mixture. Studying meteoritic NDs we have found that single photon emitters based on "silicon-vacancy" centers could be realized even in molecular-sized diamond (less than 2 nm). Currently we are developing a new class of diamond materials, nanodiamonds synthesized from organic compounds at high pressure. In particular, we have demonstrated the possibility of synthesis of nanodiamond from its molecular analogue adamantane, controlling the size of crystallites in a wide range by changing synthesis temperature. A minimum size of obtained diamond particles about 3 nm was reached. Crystal structure of such diamonds is the most perfect in comparison with other classes of diamond materials, therefore they are the most promising material platform for production of single photon emitters.