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arXiv:1602.07418 · Nature Communications

Stimulated emission from nitrogen-vacancy centres in diamond

Jan Jeske, Desmond W. M. Lau, Xavier Vidal, Liam Paul McGuinness, Philipp Reineck, Brett C. Johnson, Marcus W. Doherty, Jeffrey Colin McCallum, Shinobu Onoda, Fedor Jelezko, Takeshi Ohshima, Thomas Volz, Jared H. Cole, Brant C. Gibson, Andrew D. Greentree

Published Jan 27, 2017• 96 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/ncomms14000

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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.
Negatively charged nitrogen-vacancy (NV) centers in diamond are promising magnetic field quantum sensors. Laser threshold magnetometry theory predicts improved NV center ensemble sensitivity via increased signal strength and magnetic field contrast. Here, we experimentally demonstrate laser threshold magnetometry. We use a macroscopic high-finesse laser cavity containing a highly NV-doped and low absorbing diamond gain medium that is pumped at 532 nm and resonantly seeded at 710 nm. This enables a 64% signal power amplification by stimulated emission. We test the magnetic field dependency of the amplification and thus demonstrate magnetic field-dependent stimulated emission from an NV center ensemble. This emission shows an ultrahigh contrast of 33% and a maximum output power in the milliwatt regime. The coherent readout of NV centers pave the way for novel cavity and laser applications of quantum defects and diamond NV magnetic field sensors with substantially improved sensitivity for the health, research, and mining sectors.
Negatively charged nitrogen-vacancy centres in diamond are promising quantum magnetic field sensors. Laser threshold magnetometry has been a theoretical approach for the improvement of NV-centre ensemble sensitivity via increased signal strength and magnetic field contrast. In this work we experimentally demonstrate laser threshold magnetometry. We use a macroscopic high-finesse laser cavity containing a highly NV-doped and low absorbing diamond gain medium that is pumped at 532nm and resonantly seeded at 710nm. This enables amplification of the signal power by stimulated emission of 64%. We show the magnetic-field dependency of the amplification and thus, demonstrate magnetic-field dependent stimulated emission from an NV-centre ensemble. This emission shows a record contrast of 33% and a maximum output power in the mW regime. These advantages of coherent read-out of NV-centres pave the way for novel cavity and laser applications of quantum defects as well as diamond NV magnetic field sensors with significantly improved sensitivity for the health, research and mining sectors.
Nitrogen vacancy (NV) centres are a type of defect in diamond that exhibit a number of interesting properties. NV centres can be optically excited around 450-650 nm and emit fluorescence at around 550-800 nm [1]. The optical excitation also spin polarises the negatively charged NV centres, permitting optical detection of magnetic resonance [2]. This allows nanotesla scale sensitive magnetometry to be performed with nanometre scale spatial resolution [3].To date, a direct measurement of stimulated emission from ensembles of NV centres in diamond has yet to be demonstrated experimentally. Despite this, stimulated emission depletion microscopy has been utilised in superresolution imaging that relies on the stimulated emission of single NV centres to quench fluorescence [4]. Recently, there has also been similar indirect experimental evidence of stimulated emission in NV ensembles [5]. We thus aimed to show both optical gain of a probe beam in a pumped NV-rich diamond sample and a modulation of this gain via microwave excitation of its ground level spin transitions. The experimental set-up consisted of a pump (532 nm) and probe (723-950 nm) laser beam combined with a dichroic mirror and focused into a bulk diamond specimen to a spot-size of around 90 microns. Pump excitation powers of up to 3 W and probe powers up to 0.5 W were used. The beams were then collimated and separated with a prism and the probe power measured with a photodiode. The diamond specimen was placed on an antenna to allow simultaneous excitation with microwaves. A double modulation scheme was employed to measure either the change in probe power due to the pump laser or the microwave excitation during any one experiment.
Laser threshold magnetometry using the negatively charged nitrogen-vacancy (NV−) centre in diamond as a gain medium has been proposed as a technique to dramatically enhance the sensitivity of room-temperature magnetometry. We experimentally explore a diamond-loaded open tunable fibre-cavity system as a potential contender for the realisation of lasing with NV− centres. We observe amplification of the transmission of a cavity-resonant seed laser at 721 nm when the cavity is pumped at 532 nm and attribute this to stimulated emission. Changes in the intensity of spontaneously emitted photons accompany the amplification, and a qualitative model including stimulated emission and ionisation dynamics of the NV− centre captures the dynamics in the experiment very well. These results highlight important considerations in the realisation of an NV− laser in diamond.
We report on the spectroscopic and laser characterization of negatively charged nitrogen-vacancy (NV−) centers in diamond. Spectroscopic properties such as absorption and emission spectra as well as kinetics were studied, and parameters such as cross-sections and lifetimes were estimated. A vibronic band of NV0 with zero phonon line (ZPL) at 575 nm was detected under 532 nm pulsed excitation due to the photoionization of NV−. Transmission of 532 nm pump pulses saturate around ∼10%, which is much smaller than the theoretical level. Δk/k0 kinetics revealed slow recovery of NV− centers after photoionization under 532 nm pumping, which involved different relaxation channels depending on the probe beam wavelengths. Localization of the electrons in the metastable state of NV0 centers resulted in higher saturated transmission of 632 nm pump.
Abstract The neutral nitrogen‐vacancy (NV0) defects in diamond are photostable color centers, suitable for a wide range of applications in science and engineering. However, the photophysical properties of the centers have not yet been fully characterized. This work measured the stimulated emission cross sections of NV0 in a single‐crystal diamond by two‐photon excitation of its matrix at 344 nm. From the measured photoluminescence spectrum and the fluorescence lifetime of 20 ± 1 ns, we determined a peak stimulated emission cross section of 1.43 ± 0.07 × 10−17 cm2 at 650 nm for the NV0 centers. In addition, we have also examined the thermal shifts of the zero‐phonon line of NV0 centers in nanoscale diamonds (~100 nm in diameter) over the temperature range of 30–120°C. A temperature measurement sensitivity of 0.2 K·Hz−1/2 was achieved, which is about two‐fold better than that of NV−, despite that the fluorescence intensity of NV0 is about six‐fold lower than that of NV− in the same nanoparticles. The result is attributed to the smaller electron–phonon coupling strength of the neutral center, compared with its negatively charged counterpart.