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Excited-state spectroscopy using single-spin manipulation in diamond

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 Added by David D. Awschalom
 Publication date 2008
  fields Physics
and research's language is English




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We use single-spin resonant spectroscopy to study the spin structure in the orbital excited-state of a diamond nitrogen-vacancy center at room temperature. We find that the excited state spin levels have a zero-field splitting that is approximately half of the value of the ground state levels, a g-factor similar to the ground state value, and a hyperfine splitting ~20x larger than in the ground state. In addition, the width of the resonances reflects the electronic lifetime in the excited state. We also show that the spin-splitting can significantly differ between NV centers, likely due to the effects of local strain, which provides a pathway to control over the spin Hamiltonian and may be useful for quantum information processing.



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Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single Nitrogen-Vacancy color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3E excited state, which is invaluable for the development of diamond-based quantum information processing.
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.
We demonstrate a wide-band all-optical method of nanoscale magnetic resonance (MR) spectroscopy under ambient conditions. Our method relies on cross-relaxation between a probe spin, the electronic spin of a nitrogen-vacancy centre in diamond, and target spins as the two systems are tuned into resonance. By optically monitoring the spin relaxation time ($T_1$) of the probe spin while varying the amplitude of an applied static magnetic field, a frequency spectrum of the target spin resonances, a $T_1$-MR spectrum, is obtained. As a proof of concept, we measure $T_1$-MR spectra of a small ensemble of $^{14}$N impurities surrounding the probe spin within the diamond, with each impurity comprising an electron spin 1/2 and a nuclear spin 1. The intrinsically large bandwidth of the technique and probe properties allows us to detect both electron spin transitions -- in the GHz range -- and nuclear spin transitions -- in the MHz range -- of the $^{14}$N spin targets. The measured frequencies are found to be in excellent agreement with theoretical expectations, and allow us to infer the hyperfine, quadrupole and gyromagnetic constants of the target spins. Analysis of the strength of the resonances obtained in the $T_1$-MR spectrum reveals that the electron spin transitions are probed via dipole interactions, while the nuclear spin resonances are dramatically enhanced by hyperfine coupling and an electron-mediated process. Finally, we investigate theoretically the possibility of performing $T_1$-MR spectroscopy on nuclear spins without hyperfine interaction and predict single-proton sensitivity using current technology. This work establishes $T_1$-MR as a simple yet powerful technique for nanoscale MR spectroscopy, with broadband capability and a projected sensitivity down to the single nuclear spin level.
We propose a protocol to estimate magnetic fields using a single nitrogen-vacancy (N-V) center in diamond, where the estimate precision scales inversely with time, ~1/T$, rather than the square-root of time. The method is based on converting the task of magnetometry into phase estimation, performing quantum phase estimation on a single N-V nuclear spin using either adaptive or nonadaptive feedback control, and the recently demonstrated capability to perform single-shot readout within the N-V [P. Neumann et. al., Science 329, 542 (2010)]. We present numerical simulations to show that our method provides an estimate whose precision scales close to ~1/T (T is the total estimation time), and moreover will give an unambiguous estimate of the static magnetic field experienced by the N-V. By combining this protocol with recent proposals for scanning magnetometry using an N-V, our protocol will provide a significant decrease in signal acquisition time while providing an unambiguous spatial map of the magnetic field.
159 - H.Y. Chen , E. R. MacQuarrie , 2018
We study the resonant optical transitions of a single nitrogen-vacancy (NV) center that is coherently dressed by a strong mechanical drive. Using a gigahertz-frequency diamond mechanical resonator that is strain-coupled to an NV centers orbital states, we demonstrate coherent Raman sidebands out to the ninth order and orbital-phonon interactions that mix the two excited-state orbital branches. These interactions are spectroscopically revealed through a multi-phonon Rabi splitting of the orbital branches which scales as a function of resonator driving amplitude, and is successfully reproduced in a quantum model. Finally, we discuss the application of mechanical driving to engineering NV center orbital states.
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