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.
Journal reference
Phys. Rev. Research 5, 013014, Vol. 5, Iss. 1, 2023
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.
We demonstrate the optical readout of ensembles of nitrogen-vacancy (NV) center spins in a bulk diamond sample via spin-to-charge conversion. A high power 594 nm laser is utilized to selectively ionize these paramagnetic defects in the mS=0 spin state with a contrast of up to 12%. In comparison to the conventional 520 nm spin readout, the spin-to-charge-conversion-based readout provides a higher signal-to-noise ratio, with tenfold sensing measurement speedup for millisecond long pulse sequences. This level of performance was achieved for an NV− ionization of only 25%, limited by the ionization and readout laser powers. These observations pave the way to a range of high-sensitivity metrology applications where the use of NV− ensembles in bulk diamond has proven useful, including sensing and imaging of target materials overlaid on the diamond surface.
Nanodiamonds containing nitrogen-vacancy (NV) centers offer a versatile platform for sensing applications spanning from nanomagnetism to in vivo monitoring of cellular processes. In many cases, however, weak optical signals and poor contrast demand long acquisition times that prevent the measurement of environmental dynamics. Here, we demonstrate the ability to perform fast, high-contrast optical measurements of charge distributions in ensembles of NV centers in nanodiamonds and use the technique to improve the spin-readout signal-to-noise ratio through spin-to-charge conversion. A study of 38 nanodiamonds with sizes ranging between 20 and 70 nm, each hosting a small ensemble of NV centers, uncovers complex, multiple time scale dynamics due to radiative and nonradiative ionization and recombination processes. Nonetheless, the NV-containing nanodiamonds universally exhibit charge-dependent photoluminescence contrasts and the potential for enhanced spin readout using spin-to-charge conversion. We use the technique to speed up a T 1 relaxometry measurement by a factor of 5.
In recent years, defect centers in wide band gap semiconductors such as diamond, have received significant attention. Defects offer great utility as single photon emitters, nanoscale sensors, and quantum memories and registers for quantum computation. Critical to the utility of these defects, is their charge state. In this dissertation, experiments surrounding the charge state dynamics and the carrier dynamics are performed and analyzed. Extensive studies of the ionization and recombination processes of defects in diamond, specifically, the Nitrogen Vacancy (NV) center, have been performed. Diffusion of ionized charge carriers has been imaged indirectly through the recapture of said carriers by optically active defects such as the NV center and the Silicon Vacancy (SiV) center. With proper understanding of the carrier dynamics, diamond stands to be a strong competitor in the field of spintronics for quantum information processing. Additionally, the understanding of these charge state dynamics is utilized in a novel proof of principle experiment, showing that the NV center defect’s charge state could serve as an ultra-dense 3D memory platform. The NV center has also been used as a nanoscale magnetometer. The high degree of spin polarization and the ease of manipulation of the NV allows us to transfer this polarization to other spins in the diamond and assists in the detection of spins outside of the diamond. Ensembles of Nitrogen Vacancy centers can be used to perform NMR spectroscopy of sample volumes not achievable through traditional methods. The operating mechanisms of the magnetic resonance aspects of the NV center will be discussed in depth. Work surrounding the control and polarization of the NV center’s host nitrogen spin will be covered. The topic of sensitivity and methods to improve that sensitivity will be covered as well.
The nitrogen-vacancy (NV) center in diamond is a heavily studied defect due to its potential applications to quantum metrology and computation, particularly in ambient conditions. The key mechanism to using the NV in any application lies in the ability to read out the spin state of the defect which is typically done optically. The optical contrast is then the key metric for electron spin readout fidelity and one of the key limiting factors in the NV's overall performance. We present a mechanism for high contrast readout using the spin-to-charge conversion mechanism in conjunction with an electrode to improve the spin contrast by altering the NV energy levels relative to the diamond conduction band. Theoretical modeling predicts an optical spin contrast at 42% which would be the highest optical contrast for the NV at room temperature and the technique opens up a range of alternative research pathways for the NV which are discussed.
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.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.