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Physics Procedia

How far into the infrared can a colour centre in diamond emit?

Lachlan J. Rogers

Published Feb 1, 2010• 11 citations
Publisher

Abstract

Infrared emission has been observed for the nitrogen-vacancy (NV −) colour centre in diamond, in addition to the characteristic red emission of this centre [1]. However, this infrared emission zero-phonon line at 1046 nm is about four orders of magnitude weaker than the red emission. This is somewhat surprising, as a third of the population is known to decay without the red emission and the infrared emission is considered to be associated with the alternative decay path. The most obvious explanation is a competing effcient non-radiative decay. There are few reports of diamond emitting at wavelengths longer than 1000 nm. Colour centres in diamond have strong electron-phonon coupling and, of course, the phonon energies in diamond are high. These properties suggest that non-radiative decay could dominate the transition whenever the electronic energy lies in the infrared. This would be a general phenomena and would account for the weak IR emission observed for this centre. It would also account for why there are so few reports of emission from diamond in the infrared.

DOI
10.1016/j.phpro.2010.01.221

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Infrared emission has been observed for the nitrogen-vacancy (NV −) colour centre in diamond, in addition to the characteristic red emission of this centre [1]. However, this infrared emission zero-phonon line at 1046 nm is about four orders of magnitude weaker than the red emission. This is somewhat surprising, as a third of the population is known to decay without the red emission and the infrared emission is considered to be associated with the alternative decay path. The most obvious explanation is a competing effcient non-radiative decay. There are few reports of diamond emitting at wavelengths longer than 1000 nm. Colour centres in diamond have strong electron-phonon coupling and, of course, the phonon energies in diamond are high. These properties suggest that non-radiative decay could dominate the transition whenever the electronic energy lies in the infrared. This would be a general phenomena and would account for the weak IR emission observed for this centre. It would also account for why there are so few reports of emission from diamond in the infrared.
An emission band in the infrared (IR) is shown to be associated with a transition within the negative nitrogen-vacancy centre in diamond. The band has a zero-phonon line at 1046 nm, and uniaxial stress and magnetic field measurements indicate that the emission is associated with a transition between 1 E and 1 A 1 singlet levels. Inter-system crossing to these singlets causes the spin polarization that makes the NV - centre attractive for quantum information processing, and the IR emission band provides a new avenue for using the centre in such applications.
We report the photoluminescence characteristics of a colour centre in diamond grown by plasma-assisted chemical vapour deposition. The colour centre emits with a sharp zero-phonon line at 2.330 eV (λ=532 nm) and a lifetime of 3.3 ns, thus offering potential for a high-speed single-photon source with green emission. It displays a vibronic emission spectrum with a Huang–Rhys parameter of 2.48 at 77 K. Hanbury–Brown and Twiss measurements reveal that the electronic level structure of the defect includes a metastable state that can be populated from the optically excited state.
Single-photon sources are a fundamental element for developing quantum technologies, and sources based on colour centres in diamonds are among the most promising candidates. The well-known nitrogen vacancy centres are characterized by several limitations, and thus few other defects have recently been considered. In the present work, we characterize, in detail, native efficient single colour centres emitting in the near infra-red ( λ = 740–780 nm) in both standard IIa single-crystal and electronic-grade polycrystalline commercial chemical vapour deposited (CVD) diamond samples. In the former case, a high-temperature ( T > 1000 °C) annealing process in vacuum is necessary to induce the formation/activation of luminescent centres with good emission properties, while in the latter case the annealing process has marginally beneficial effects on the number and performance of native centres in commercially available samples. Although displaying significant variability in several photo-physical properties (emission wavelength, emission rate instabilities, saturation behaviours), these centres generally display appealing photophysical properties for applications as single photon sources: short lifetimes (0.7–3 ns), high emission rates (∼50–500 × 10 3 photons s −1 ) and strongly (>95%) polarized light. The native centres are tentatively attributed to impurities incorporated in the diamond crystal during the CVD growth of high-quality type-IIa samples, and offer promising perspectives in diamond-based photonics.
We study the spectroscopy of an ensemble of negatively charged nitrogen-vacancy centers in diamond at high temperatures between room temperature and 700K under high vacuum conditions. Spin resonances are studied using optical detection of magnetic resonance (ODMR), and optical spectroscopy is employed to study radiative transitions. Upon increasing the temperature, the intensity of radiative decay in visible and infrared decreased. In addition, the ODMR resonance frequencies were decreased, and the phonon line emission shifted to higher wavelengths. Density functional theory calculation of the zero-field splitting parameter (D) revealed that thermal expansion is not enough to explain the shift in the ODMR frequencies. Fitting the measured intensity of photo-luminescence with the theoretical predictions of the Mott–Seitz model yields the value of 0.22eV for the energy barrier associated with nonradiative decay.
Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively charged nitrogen-vacancy (NV−) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV− to date. Here we show both theoretical and experimental evidence for stimulated emission from NV− using light in the phonon sidebands around 700 nm. Furthermore, we show the transition from stimulated emission to photoionization as the stimulating laser wavelength is reduced from 700 to 620 nm. While lasing at the zero-phonon line is suppressed by ionization, our results open the possibility of diamond lasers based on NV− centres, tuneable over the phonon sideband. This broadens the applications of NV− magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system. Here Jeskeet al. show both theoretical and experimental evidence for stimulated emission from negatively charged nitrogen vacancy centres using light in the phonon sidebands around 700 nm, demonstrating its suitability as a laser medium.
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.