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Register a new userHigh-resolution spectroscopy of single nuclear spins via sequential weak measurements
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Quantum sensors have recently achieved to detect the magnetic moment of few or single nuclear spins and measure their magnetic resonance (NMR) signal. However, the spectral resolution, a key feature of NMR, has been limited by relaxation of the sensor to a few kHz at room temperature. The spectral resolution of NMR signals from single nuclear spins can be improved by, e.g., using quantum memories, however at the expense of sensitivity. Classical signals on the other hand can be measured with exceptional spectral resolution by using continuous measurement techniques, without compromising sensitivity. To apply these techniques to single-spin NMR, it is critical to overcome the impact of back action inherent of quantum measurements. Here we report sequential weak measurements on a single $^{13}$C nuclear spin. The back-action of repetitive weak measurements causes the spin to undergo a quantum dynamics phase transition from coherent trapping to coherent oscillation. Single-spin NMR at room-temperature with a spectral resolution of 3.8 Hz is achieved. These results enable the use of measurement-correlation schemes for the detection of very weakly coupled single spins.
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Nuclear magnetic resonance (NMR) spectroscopy is a powerful technique for analyzing the structure and function of molecules, and for performing three-dimensional imaging of the spin density. At the heart of NMR spectrometers is the detection of electromagnetic radiation, in the form of a free induction decay (FID) signal, generated by nuclei precessing around an applied magnetic field. While conventional NMR requires signals from 1e12 or more nuclei, recent advances in sensitive magnetometry have dramatically lowered this number to a level where few or even individual nuclear spins can be detected. It is natural to ask whether continuous FID detection can still be applied at the single spin level, or whether quantum back-action modifies or even suppresses the NMR response. Here we report on tracking of single nuclear spin precession using periodic weak measurements. Our experimental system consists of carbon-13 nuclear spins in diamond that are weakly interacting with the electronic spin of a nearby nitrogen-vacancy center, acting as an optically readable meter qubit. We observe and minimize two important effects of quantum back-action: measurement-induced decoherence and frequency synchronization with the sampling clock. We use periodic weak measurements to demonstrate sensitive, high-resolution NMR spectroscopy of multiple nuclear spins with a priori unknown frequencies. Our method may provide the optimum route for performing single-molecule NMR at atomic resolution.
We report on precise localization spectroscopy experiments of individual 13C nuclear spins near a central electronic sensor spin in a diamond chip. By detecting the nuclear free precession signals in rapidly switchable external magnetic fields, we retrieve the three-dimensional spatial coordinates of the nuclear spins with sub-Angstrom resolution and for distances beyond 10 Angstroms. We further show that the Fermi contact contribution can be constrained by measuring the nuclear g-factor enhancement. The presented method will be useful for mapping the atomic-scale structure of single molecules, an ambitious yet important goal of nanoscale nuclear magnetic resonance spectroscopy.
The understanding of weak measurements and interaction-free measurements has greatly expanded the conceptual and experimental toolbox to explore the quantum world. Here we demonstrate single-shot variable-strength weak measurements of the electron and the nuclear spin states of a single $^{31}$P donor in silicon. We first show how the partial collapse of the nuclear spin due to measurement can be used to coherently rotate the spin to a desired pure state. We explicitly demonstrate that phase coherence is preserved throughout multiple sequential single-shot weak measurements, and that the partial state collapse can be reversed. Second, we use the relation between measurement strength and perturbation of the nuclear state as a physical meter to extract the tunneling rates between the $^{31}$P donor and a nearby electron reservoir from data, conditioned on observing no tunneling events. Our experiments open avenues to measurement-based state preparation, steering and feedback protocols for spin systems in the solid state, and highlight the fundamental connection between information gain and state modification in quantum mechanics.
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses has still remained a challenge. Here, we analyze two-dimensional Fourier spectra for resonant optical excitation of resident electrons to localized trions or donor-bound excitons in semiconductor nanostructures subject to a transverse magnetic field. Particular attention is devoted to Raman coherence spectra which allow one to accurately evaluate tiny splittings of the electron ground state and to determine the relaxation times in the electron spin ensemble. A stimulated step-like Raman process induced by a sequence of two laser pulses creates a coherent superposition of the ground state doublet which can be retrieved only optically due to selective excitation of the same sub-ensemble with a third pulse. This provides the unique opportunity to distinguish between different complexes that are closely spaced in energy in an ensemble. The related experimental demonstration is based on photon echo measurements in an n-type CdTe/(Cd,Mg)Te quantum well structure detected by a heterodyne technique. The difference in the sub-$mu$eV range between the Zeeman splittings of donor-bound electrons and electrons localized at potential fluctuations can be resolved even though the homogeneous linewidth of the optical transitions is larger by two orders of magnitude.
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal resolution optimisation and also outline paths to greater sensitivity. In addition, the method is suitable for application in low and relatively inhomogeneous background magnetic fields in contrast to both conventional liquid and solid state NMR spectroscopy.
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