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.
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.
Nitrogen vacancy (NV) centers in diamond have been identified over the past few years as promising systems for a variety of applications, ranging from quantum information science to magnetic sensing. This relies on the unique optical and spin properties of the negatively charged NV. Many of these applications require shallow NV centers, i.e., NVs that are close (a few nm) to the diamond surface. In recent years there has been increasing interest in understanding the spin and charge dynamics of NV centers under various illumination conditions, specifically under infrared (IR) excitation, which has been demonstrated to have significant impact on the NV centers' emission and charge state. Nevertheless, a full understanding of all experimental data is still lacking, with further complications arising from potential differences between the photodynamics of bulk and shallow NVs. Here we suggest a generalized quantitative model for NV center spin- and charge-state dynamics under both green and IR excitation. We experimentally extract the relevant transition rates, providing a comprehensive model which reconciles all existing experimental results in the literature, except for highly nonlinear regimes. Moreover, we identify key differences between the photodynamics of bulk and shallow NVs, and use them to significantly enhance the initialization fidelity of shallow NVs to the useful negatively charged state.
High spatial resolution quantum sensing of near-surface nitrogen vacancy (NV) centers in diamond has enabled detection of magnetic, electrical, and thermal signals at the nanoscale. At depths of just a few nanometers, NV centers serve as localized quantum probes for external spins or low-dimensional materials, but their proximity to the surface also enhances decoherence caused by fluctuating nuclear spins. While advances in surface engineering have stabilized the charge state of NV centers at depths of tens of nanometers, achieving both ultra-shallow implantation (0.5-2 nm) and long-term spin coherence remains a central challenge. In this work, we show using first-principles modeling that, by exploiting the interaction of surface-induced strain and weak dc magnetic fields, the spin coherence times of 1-nm-deep NV centers can be greatly improved near the spin-phonon-confined regime at room temperature in 12C-rich diamonds. We also demonstrate that this protocol benefits ~ 10-nm-deep NV centers in natural diamond, enabling vector magnetometry at the nanoscale. Shallow NV centers in diamond are advantageous for quantum sensing but suffer from surface magnetic noise. Using first-principles simulations supported by experiments, the authors show that a combination of small magnetic fields and surface strain can significantly enhance spin coherence of 1 nm-deep NV centers.
We utilize nonlinear absorption to design all-optical protocols that improve both charge-state initialization and spin readout for the nitrogen-vacancy (NV) center in diamond. Nonmonotonic variations in the equilibrium charge state as a function of visible and near-infrared optical power are attributed to competing multiphoton absorption processes. In certain regimes, multicolor illumination enhances the steady-state population of the NV's negative charge state above 90%. At higher NIR intensities, selective ionization of the singlet manifold facilitates a protocol for spin-to-charge conversion that dramatically enhances the spin readout fidelity. We demonstrate a sixfold increase in the signal-to-noise ratio for single-shot spin measurements and demonstrate a pathway towards single-shot electron spin readout at room temperature.
Abstract High-fidelity projective readout of a qubit’s state in a single experimental repetition is a prerequisite for various quantum protocols of sensing and computing. Achieving single-shot readout is challenging for solid-state qubits. For Nitrogen-Vacancy (NV) centers in diamond, it has been realized using nuclear memories or resonant excitation at cryogenic temperature. All of these existing approaches have stringent experimental demands. In particular, they require a high efficiency of photon collection, such as immersion optics or all-diamond micro-optics. For some of the most relevant applications, such as shallow implanted NV centers in a cryogenic environment, these tools are unavailable. Here we demonstrate an all-optical spin readout scheme that achieves single-shot fidelity even if photon collection is poor (delivering less than 10 3 clicks/second). The scheme is based on spin-dependent resonant excitation at cryogenic temperature combined with spin-to-charge conversion, mapping the fragile electron spin states to the stable charge states. We prove this technique to work on shallow implanted NV centers, as they are required for sensing and scalable NV-based quantum registers.
A functioning qubit must be able to be initialized and measured. The fidelity of these operations is essential for all quantum applications, including quantum sensing, communication, and computation. The diamond nitrogen-vacancy (NV) center is a point defect in the lattice with an optical interface to a coherent ground-state spin, which makes the NV center one of the few spin qubits operable at room temperature. While the NV center spin state can be initialized and read out optically, the fidelity of these operations are far from perfect due to the charge and orbital dynamics. In typical conditions, the NV center is in the proper charge state 75% of the time, and measuring the spin state results in a non-zero signal only 1% of the time. These inefficient mechanisms make many measurements practically intractable. This thesis focuses on improving the preparation and measurement fidelities of NV centers through precise all-optical control of the charge, orbital, and spin dynamics. I first discuss an improved spin readout mechanism which relies on spin-to-charge conversion (SCC) and discuss the potential for single-shot spin readout. Following, I present how charge readout and SCC can be implemented in ensembles of NV centers within nanodiamonds and demonstrate that it provides improvements for spin-relaxometry studies. Finally, I develop a method for initializing a single NV center's charge state with real-time control and show that this capability improves spin readout performance for sensing. To conclude, I discuss how these improved initialization and readout capabilities can be applied to detecting and controlling coupled nuclear spins in the diamond lattice and consider other applications of real-time control.
We propose and experimentally demonstrate a method to strongly increase the sensitivity of spin measurements on nitrogen-vacancy (NV) centers in diamond, which can be readily implemented in existing quantum sensing experiments. While charge state transitions of this defect are generally considered a parasitic effect to be avoided, we show here that these can be used to significantly increase the NV center's spin contrast, a key quantity for high sensitivity magnetometry and high fidelity state readout. The protocol consists of a two-step procedure, in which the charge state of the defect is first purified by a strong laser pulse, followed by weak illumination to obtain high spin polarization. We observe a relative improvement of the readout contrast by 17 %, and infer a reduction of the initialization error of more than 50 %. The contrast enhancement is accompanied by a beneficial increase of the readout signal. For long sequence durations, typically encountered in high-resolution magnetometry, a measurement speedup by a factor of >1.5 is extracted, and we find that the technique is beneficial for sequences of any duration. Additionally, our findings give detailed insight into the charge and spin polarization dynamics of the NV center, and provide actionable insights for direct optical, spin-to-charge, and electrical readout of solid-state spin centres.