Scott J. Seltzer

Optical hyperpolarization and NMR detection of 129 Xe on a microfluidic chip

Optically hyperpolarized (129)Xe gas has become a powerful contrast agent in nuclear magnetic resonance (NMR) spectroscopy and imaging, with applications ranging from studies of the human lung to the targeted detection of biomolecules. Equally attractive is its potential use to enhance the sensitivity of microfluidic NMR experiments, in which small sample volumes yield poor sensitivity. Unfortunately, most (129)Xe polarization systems are large and non-portable. Here we present a microfabricated chip that optically polarizes (129)Xe gas. We have achieved (129)Xe polarizations >0.5% at flow rates of several microlitres per second, compatible with typical microfluidic applications. We employ in situ optical magnetometry to sensitively detect and characterize the (129)Xe polarization at magnetic fields of 1 μT. We construct the device using standard microfabrication techniques, which will facilitate its integration with existing microfluidic platforms. This device may enable the implementation of highly sensitive (129)Xe NMR in compact, low-cost, portable devices.

Sensitive magnetic control of ensemble nuclear spin hyperpolarization in diamond

Dynamic nuclear polarization, which transfers the spin polarization of electrons to nuclei, is routinely applied to enhance the sensitivity of nuclear magnetic resonance. This method is particularly useful when spin hyperpolarization can be produced and controlled optically or electrically. Here we show complete polarization of nuclei located near optically polarized nitrogen-vacancy centres in diamond. Close to the ground-state level anti-crossing condition of the nitrogen-vacancy electron spins, (13)C nuclei in the first shell are polarized in a pattern that depends sensitively upon the magnetic field. Based on the anisotropy of the hyperfine coupling and of the optical polarization mechanism, we predict and observe a reversal of the nuclear spin polarization with only a few millitesla change in the magnetic field. This method of magnetic control of high nuclear polarization at room temperature can be applied in sensitivity enhanced nuclear magnetic resonance of bulk nuclei, nuclear-based spintronics, and quantum computation in diamond.

Room-temperature operation of a radiofrequency diamond magnetometer near the shot-noise limit

1 and T � 1 2 , where T1 and T2 are the longitudinal and transverse relaxation times of the electron spin during optical irradiation. We measured a maximum detection bandwidth of � 1.6 MHz with optical excitation intensity of � 2.3 MW/cm 2 , limited by the available optical power. The sensitivity of the NV ensemble for continuous-wave magnetometry in the presence of photon shot noise is analyzed. Two detection schemes are compared, one involving modulation of the fluorescence by an oscillating magnetic field while the microwave frequency is held constant, and the other involving double modulation of the fluorescence when the microwave frequency is modulated during the detection. For the first of these methods, we measure a sensitivity of 4.6 6 0.3 nT/Hz, unprecedented in a detector with this active volume of � 10lm 3 and close to the photonshot-noise limit of our experiment. The measured bandwidth and sensitivity of our device should allow detection of micro-scale NMR signals with microfluidic devices. V C 2012 American Institute

Ultra-Low-Field NMR Relaxation and Diffusion Measurements Using an Optical Magnetometer†

Nuclear magnetic resonance (NMR) relaxometry and diffusometry are important tools for the characterization of heterogeneous materials and porous media, with applications including medical imaging, food characterization and oil-well logging. These methods can be extremely effective in applications where high-resolution NMR is either unnecessary, impractical, or both, as is the case in the emerging field of portable chemical characterization. Here, we present a proof-of-concept experiment demonstrating the use of high-sensitivity optical magnetometers as detectors for ultra-low-field NMR relaxation and diffusion measurements.

Optically detected nuclear quadrupolar interaction ofN14in nitrogen-vacancy centers in diamond

We report sensitive detection of the nuclear quadrupolar interaction of the 14N nuclear spin of the nitrogen-vacancy (NV) center using the electron spin echo envelope modulation technique. We applied a weak transverse magnetic field to the spin system so that certain forbidden transitions became weakly allowed due to second-order effects involving the nonsecular terms of the hyperfine interaction. The weak transitions cause modulation of the electron spin-echo signal, and a theoretical analysis suggests that the modulation frequency is primarily determined by the nuclear quadrupolar frequency; numerical simulations confirm the analytical results and show excellent quantitative agreement with experiments. This is an experimentally simple method of detecting quadrupolar interactions, and it can be used to study spin systems with an energy structure similar to that of the nitrogen vacancy center.

An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129 Xe

Low thermal-equilibrium nuclear spin polarizations and the need for sophisticated instrumentation render conventional nuclear magnetic resonance (NMR) spectroscopy and imaging (MRI) incompatible with small-scale microfluidic devices. Hyperpolarized 129Xe gas has found use in the study of many materials but has required very large and expensive instrumentation. Recently a microfabricated device with modest instrumentation demonstrated all-optical hyperpolarization and detection of 129Xe gas. This device was limited by 129Xe polarizations less than 1%, 129Xe NMR signals smaller than 20 nT, and transport of hyperpolarized 129Xe over millimeter lengths. Higher polarizations, versatile detection schemes, and flow of 129Xe over larger distances are desirable for wider applications. Here we demonstrate an ultra-sensitive microfabricated platform that achieves 129Xe polarizations reaching 7%, NMR signals exceeding 1 μT, lifetimes up to 6 s, and simultaneous two-mode detection, consisting of a high-sensitivity in situ channel with signal-to-noise of 105 and a lower-sensitivity ex situ detection channel which may be useful in a wider variety of conditions. 129Xe is hyperpolarized and detected in locations more than 1 cm apart. Our versatile device is an optimal platform for microfluidic magnetic resonance in particular, but equally attractive for wider nuclear spin applications benefitting from ultra-sensitive detection, long coherences, and simple instrumentation.