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Photonics

Study on Diamond NV Centers Excited by Green Light Emission from Upconversion Luminescence

Yangyang Guo, Fuwen Shi, Bo Li

Published Nov 26, 2025• 2 citations
Publisher

Abstract

The NV center in diamonds has been widely employed in quantum sensing, quantum computing, and bioimaging due to its controllable ground-state spin, detectable magnetic resonance, excellent photostability, favorable biocompatibility, and chemical inertness. However, conventional excitation using 532 nm green light still exhibits certain limitations in practical applications. To address this, we propose a novel NV center excitation method based on the upconversion of near-infrared light to green emission. Through the synthesis of molybdenum-doped NaYF4: 20% Yb3+, 1.5% Er3+ upconversion materials, efficient excitation of NV centers has been achieved. Both UC-LED luminescence spectroscopy and ODMR measurements confirm that the green light generated via the upconversion process exhibits sufficient intensity to effectively excite NV centers. Meanwhile, the characteristic sharp emission peaks of rare-earth upconversion materials eliminate the need for optical filters, facilitating device miniaturization, and a miniaturized UC-LED sensor has been developed.

DOI
10.3390/photonics12121163

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The NV center in diamonds has been widely employed in quantum sensing, quantum computing, and bioimaging due to its controllable ground-state spin, detectable magnetic resonance, excellent photostability, favorable biocompatibility, and chemical inertness. However, conventional excitation using 532 nm green light still exhibits certain limitations in practical applications. To address this, we propose a novel NV center excitation method based on the upconversion of near-infrared light to green emission. Through the synthesis of molybdenum-doped NaYF4: 20% Yb3+, 1.5% Er3+ upconversion materials, efficient excitation of NV centers has been achieved. Both UC-LED luminescence spectroscopy and ODMR measurements confirm that the green light generated via the upconversion process exhibits sufficient intensity to effectively excite NV centers. Meanwhile, the characteristic sharp emission peaks of rare-earth upconversion materials eliminate the need for optical filters, facilitating device miniaturization, and a miniaturized UC-LED sensor has been developed.
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The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV−^-− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
Nitrogen vacancy (NV) centers in diamond exhibit long spin coherence times, optical initialization, and optical spin readout under ambient conditions, making them excellent quantum sensors. However, the conventional scheme for charge state initialization based on off-resonant green excitation results in significant state preparation errors, typically around 30%. One method for improving charge state initialization fidelity is to use multicolor excitation, which has been demonstrated to achieve a near-unity preparation fidelity for bulk NV centers by using a few milliseconds of near-infrared (5 mW) and green (10 μW) excitation. The translation of such schemes to NV centers near the diamond surface with higher efficiency optical pumping would enable myriad tasks in nanoscale sensing. Here, we demonstrate a protocol for efficient charge initialization of shallow NV centers between 5 nm and 15 nm from the diamond surface. By carefully studying the charge dynamics of shallow NV centers, we identify a region of parameter space that allows for near-unity (95%) charge initialization within 300 μs of near-infrared (1 mW) and green (10 μW) excitation. The time to 90% charge initialization can be as fast as 10 μs for 4 mW of near-infrared and 39 μW of green illumination. This fast, efficient charge initialization protocol will enable nanoscale sensing applications where state preparation errors currently prohibit scaling, such as measuring higher-order multi-point correlators.
The photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated, but is still not fully understood. In contrast to previous work, we find that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ via absorption of 1064-nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from both charge states of the NV center under low power 1064-nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064-nm laser is spin dependent.
The nitrogen-vacancy (NV) center is a defect in the structure of diamond, roughly the size of a single atom, that possesses properties that make it applicable to quantum information processing, high-resolution magnetic resonance imaging, and probing biological systems. When an NV center is excited by green light of wavelength 523 nm, it emits red light of in the range from 600-800 nm tens of nanoseconds later. A confocal microscope can be used to excite and collect emitted photons from NV centers. By detecting the intensity of the emitted red photons, we can determine the quantum state of a single NV center, which is needed to build various quantum computing, sensing and imaging devices. The autocorrelation method is used to detect antibunching in the emission of red photons and ascertain that the observed photons are being emitted from a single NV center. We have built an autocorrelation device that measures, with sub-nanosecond accuracy, the statistical distribution of the arrival times of the red photons emitted from a diamond sample at a photon counter. The device can measure fixed time values with a time resolution of 120 ps FWHM. For uncorrelated sources measured for 120 seconds at the TAC full range of 100 ns, the average counts in each histogram bin were about 0.01% of the predicted value. The autocorrelation device that we have built costs about 10 times less than commercial units used by other NV researchers.
We demonstrate that a recently introduced family of direct-emitting green laser diodes is a simple yet efficient light source for excitation of NV centers in diamond. Thanks to their fast (sub-ns) response time, these sources are suitable for a broad variety of measurements, including pulsed optically detected magnetic resonance (ODMR) and fluorescence lifetime imaging. This feature, together with a drastically simplified design, is a significant advantage over the traditional excitation system comprising an Nd: YAG laser switched by an acousto-optic modulator. We introduce a simple design for such a compact laser system and experimentally verify that it enables simultaneous lifetime and ODMR measurements on NV centers. In particular, we find that the NV(-) charge state remains stable in spite of the short excitation wavelength of the new source.