Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Applied Physics Reviews

Radiative recombination of near-surface donor–acceptor pairs in hydrogenated homoepitaxial diamond nanolayers

Alexey M. Romshin, A. P. Bolshakov, Alexander A. Zhivopistsev, Alexander V. Gritsienko, Oleg S. Kudryavtsev, Pavel Aleksandrovich Pivovarov, Victor Ralchenko, Igor I. Vlasov

Published Oct 9, 2026• 0 citations
Publisher

Abstract

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.

DOI
10.1063/5.0346046

Related papers

Near surface donor-acceptor pairs in hydrogenated homoepitaxial diamond nanolayers

A. M. Romshin, A. P. Bolshakov, A. A. Zhivopistsev +5 more

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.

quant-pharXiv:2605.29492•May 29, 2026•0 citations

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 +9 more

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.

arXiv:2310.18822•Oct 28, 2023•0 citations

Donor-acceptor pairs in wide-bandgap semiconductors for quantum technology applications

Anil Bilgin, Ian Hammock, Jeremy Estes +4 more

Abstract We propose a quantum science platform utilizing the dipole-dipole coupling between donor-acceptor pairs (DAPs) in wide bandgap semiconductors to realize optically controllable, long-range interactions between defects in the solid state. We carry out calculations based on density functional theory (DFT) to investigate the electronic structure and interactions of DAPs formed by various substitutional point-defects in diamond and silicon carbide (SiC). We determine the most stable charge states and evaluate zero phonon lines using constrained DFT and compare our results with those of simple donor-acceptor pair (DAP) models. We show that polarization differences between ground and excited states lead to unusually large electric dipole moments for several DAPs in diamond and SiC. We predict photoluminescence spectra for selected substitutional atoms and show that while B-N pairs in diamond are challenging to control due to their large electron-phonon coupling, DAPs in SiC, especially Al-N pairs, are suitable candidates to realize long-range optically controllable interactions.

arXiv:2305.05791•npj Computational Materials•Jan 6, 2024•19 citations

Spin-State Control of Shallow Single NV Centers in Hydrogen-Terminated Diamond

Taisuke Kageura, Yosuke Sasama, Tokuyuki Teraji +6 more

The ability to control the charge and spin states of nitrogen-vacancy (NV) centers near the diamond surface is of pivotal importance for quantum applications. Hydrogen-terminated diamond is promising for long spin coherence times and ease of controlling the charge states due to the low density of surface defects. However, it has so far been challenging to create negatively charged single NV centers with controllable spin states beneath a hydrogen-terminated surface because atmospheric adsorbates that act as acceptors induce surface holes. In this study, we optically detected the magnetic resonance of shallow single NV centers in hydrogen-terminated diamond through precise control of the nitrogen implantation fluence. Furthermore, we found that the probability of detecting the resonance was enhanced by reducing the surface acceptor density through passivation of the hydrogen-terminated surface with hexagonal boron nitride without air exposure. This control method opens up new opportunities for using NV centers in quantum applications.

ACS Applied Materials & Interfaces•Mar 1, 2024•4 citations

Investigating the initialization and readout of relative populations of NV− and NV0 defects in diamond

Rodrick Kuate Defo, Steven L. Richardson

The static electric dipole–dipole coupling between donor–acceptor pairs (DAPs) in wide-bandgap semiconductors has recently emerged as a means of realizing a quantum science platform through optically controllable, long-range interactions between defects in the solid state. In this work, we generalize DAPs to consider arbitrary dopant populations and demonstrate that the charge of the NV center in diamond is well suited for quantum science. Explicitly, we leverage experimental results [see Z. Yuan et al., PRR 2, 033263 (2020)] to show that shallow NV centers can be efficiently initialized to a given relative population of the negative and neutral charge states and that modulating the surface termination would allow for control of the timescale over which the initialization and subsequent computations would occur. Furthermore, we argue that the observation of electroluminescence from the neutral charge state of the NV center [see N. Mizuochi et al., Nat. Photon. 6, 299 (2012)], but not from the negative charge state, implies the ability to interface with the NV center’s charge in a manner analogous to the spin interface enabled by the spin-state dependent fluorescence of the NV center.

Journal of Applied Physics•Jun 28, 2024•3 citations

Computing Using Shallow NV-Center Charges in Diamond

Rodrick Kuate Defo, Steven L. Richardson

The static electric dipole-dipole coupling between donor-acceptor pairs (DAPs) in wide-bandgap semiconductors has recently emerged as a means of realizing a quantum science platform through optically controllable, long-range interactions between defects in the solid state. In this work, we generalize DAPs to consider arbitrary dopant populations and demonstrate that the charge of the NV center in diamond is well suited for quantum science. Explicitly, we leverage experimental results [see Z. Yuan et al., PRR 2, 033263 (2020)] to show that shallow NV centers can be efficiently initialized to a given relative population of the negative and neutral charge states and that modulating the surface termination would allow for control of the timescale over which the initialization and subsequent computations would occur. Furthermore, we argue that the observation of electroluminescence from the neutral charge state of the NV center [see N. Mizuochi et al., Nat. Photon. 6, 299 (2012)], but not from the negative charge state, implies the ability to interface with the NV center's charge in a manner analogous to the spin interface enabled by the spin-state dependent fluorescence of the NV center.

arXiv:2402.17083•Feb 26, 2024•0 citations
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.
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.
Abstract We propose a quantum science platform utilizing the dipole-dipole coupling between donor-acceptor pairs (DAPs) in wide bandgap semiconductors to realize optically controllable, long-range interactions between defects in the solid state. We carry out calculations based on density functional theory (DFT) to investigate the electronic structure and interactions of DAPs formed by various substitutional point-defects in diamond and silicon carbide (SiC). We determine the most stable charge states and evaluate zero phonon lines using constrained DFT and compare our results with those of simple donor-acceptor pair (DAP) models. We show that polarization differences between ground and excited states lead to unusually large electric dipole moments for several DAPs in diamond and SiC. We predict photoluminescence spectra for selected substitutional atoms and show that while B-N pairs in diamond are challenging to control due to their large electron-phonon coupling, DAPs in SiC, especially Al-N pairs, are suitable candidates to realize long-range optically controllable interactions.
The ability to control the charge and spin states of nitrogen-vacancy (NV) centers near the diamond surface is of pivotal importance for quantum applications. Hydrogen-terminated diamond is promising for long spin coherence times and ease of controlling the charge states due to the low density of surface defects. However, it has so far been challenging to create negatively charged single NV centers with controllable spin states beneath a hydrogen-terminated surface because atmospheric adsorbates that act as acceptors induce surface holes. In this study, we optically detected the magnetic resonance of shallow single NV centers in hydrogen-terminated diamond through precise control of the nitrogen implantation fluence. Furthermore, we found that the probability of detecting the resonance was enhanced by reducing the surface acceptor density through passivation of the hydrogen-terminated surface with hexagonal boron nitride without air exposure. This control method opens up new opportunities for using NV centers in quantum applications.
The static electric dipole–dipole coupling between donor–acceptor pairs (DAPs) in wide-bandgap semiconductors has recently emerged as a means of realizing a quantum science platform through optically controllable, long-range interactions between defects in the solid state. In this work, we generalize DAPs to consider arbitrary dopant populations and demonstrate that the charge of the NV center in diamond is well suited for quantum science. Explicitly, we leverage experimental results [see Z. Yuan et al., PRR 2, 033263 (2020)] to show that shallow NV centers can be efficiently initialized to a given relative population of the negative and neutral charge states and that modulating the surface termination would allow for control of the timescale over which the initialization and subsequent computations would occur. Furthermore, we argue that the observation of electroluminescence from the neutral charge state of the NV center [see N. Mizuochi et al., Nat. Photon. 6, 299 (2012)], but not from the negative charge state, implies the ability to interface with the NV center’s charge in a manner analogous to the spin interface enabled by the spin-state dependent fluorescence of the NV center.
The static electric dipole-dipole coupling between donor-acceptor pairs (DAPs) in wide-bandgap semiconductors has recently emerged as a means of realizing a quantum science platform through optically controllable, long-range interactions between defects in the solid state. In this work, we generalize DAPs to consider arbitrary dopant populations and demonstrate that the charge of the NV center in diamond is well suited for quantum science. Explicitly, we leverage experimental results [see Z. Yuan et al., PRR 2, 033263 (2020)] to show that shallow NV centers can be efficiently initialized to a given relative population of the negative and neutral charge states and that modulating the surface termination would allow for control of the timescale over which the initialization and subsequent computations would occur. Furthermore, we argue that the observation of electroluminescence from the neutral charge state of the NV center [see N. Mizuochi et al., Nat. Photon. 6, 299 (2012)], but not from the negative charge state, implies the ability to interface with the NV center's charge in a manner analogous to the spin interface enabled by the spin-state dependent fluorescence of the NV center.