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The Journal of Chemical Physics

Chemical shift anisotropic mapping of a coherent optical absorber using magnetic field induced quantum beats

Andrew J. M. Kiruluta

Published Jul 14, 2006• 0 citations
Publisher

Abstract

A new method for mapping the spatial structure of optical coherent materials which relies on imposing a set of linear orthogonal gradient magnetic fields for a controlled hyperfine splitting of energy levels to create characteristic quantum beats when illuminated with a laser pulse with sufficient bandwidth to excite these levels is proposed. In this approach, a spectroscopic fingerprint of the dopant sites due to concentration and field susceptibilities in the sample is achieved through a Fourier decomposition of the radiative relaxation decay in an approach analogous to nuclear magnetic resonance spectroscopy due to the imposition of a controlled spatial-spectral encoding scheme. A three pulse sequence necessary to interrogate a gradient resolved voxel is also discussed. This three pulse approach can be combined with the conventional confocal imaging technique to provide information about the underlying chemistry of dopant distribution along each imaging plane which is useful in guiding the design and manufacturing process of optical crystals. In combination with gradient induced quantum beats, the entire inhomogeneous bandwidth can be interrogated. The proposed approach would scan this entire bandwidth at much faster rate enabling characterization of a large number of crystals than is currently possible through mechanical scanning with a confocal microscopy based spectroscopic technique as well as providing functional dopant profiling which is not currently possible with conventional approaches.

DOI
10.1063/1.2219435

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Abstract Magnetic resonance imaging is a three-dimensional imaging technique, where a gradient of the magnetic field is used to interrogate spin resonances with spatial resolution. The application of this technique to probe the coherence of atoms with good three-dimensional resolution is a challenging application. We propose and demonstrate an optical method to probe spin resonances via a two-photon Raman transition, reconstructing the 3D-structure of an atomic ensemble’s coherence, which is itself subject to external fields. Our method relies on a single time-and-space resolved heterodyne measurement, allowing the reconstruction of a complex 3D coherence profile. Owing to the optical interface, we reach a tomographic image resolution of 14 × 14 × 36 μm3. The technique allows to probe any transparent medium with a resonance structure and provides a robust diagnostic tool for atom-based quantum information protocols. As such, it is a viable technique for application to magnetometry, electrometry, and imaging of electromagnetic fields.
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We perform spectroscopy on the hyperfine splitting of 85^{85}85Rb atoms trapped in far-off-resonance optical traps. The existence of a spatially dependent shift in the energy levels is shown to induce an inherent dephasing effect, which causes a broadening of the spectroscopic line and hence an inhomogeneous loss of atomic coherence at a much faster rate than the homogeneous one caused by spontaneous photon scattering. We present here a number of approaches for reducing this inhomogeneous broadening, based on trap geometry, additional laser fields, and novel microwave pulse sequences. We then show how hyperfine spectroscopy can be used to study quantum dynamics of optically trapped atoms.
A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of 13CH^{13}\mathrm{CH}13CH3F_{3}\mathrm{F}3​F by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.
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Crystal-strain variation imposes significant limitations on many quantum sensing and information applications for solid-state defect qubits in diamond. Thus, the precision measurement and control of diamond crystal strain is a key challenge. Here, we report diamond strain measurements with a unique set of capabilities, including micron-scale spatial resolution, a millimeter-scale field of view, and a 2-order-of-magnitude improvement in volume-normalized sensitivity over previous work, reaching $5(2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}8}/\sqrt{\mathrm{Hz}\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}{\mathrm{m}}^{\ensuremath{-}3}}$ (with spin-strain coupling coefficients representing the dominant systematic uncertainty). We use strain-sensitive spin-state interferometry on ensembles of nitrogen-vacancy (N\mathrm{N}N-VVV) color centers in single-crystal bulk diamond with low strain gradients. This quantum interferometry technique provides insensitivity to magnetic-field inhomogeneity from the electronic and nuclear spin bath, thereby enabling long N\mathrm{N}N-VVV--ensemble electronic spin dephasing times and enhanced strain sensitivity, as well as broadening the potential applications of the technique beyond isotopically enriched or high-purity diamond. We demonstrate the strain-sensitive measurement protocol first on a confocal scanning laser microscope, providing quantitative measurement of sensitivity as well as three-dimensional strain mapping; and second on a wide-field-imaging quantum diamond microscope. Our strain-microscopy technique enables fast, sensitive characterization for diamond material engineering and nanofabrication; as well as diamond-based sensing of strains applied externally, as in diamond anvil cells or embedded diamond stress sensors, or internally, as by crystal damage due to particle-induced nuclear recoils.