@article {1476, title = {Optically detected cross-relaxation spectroscopy of electron spins in diamonds}, journal = {Nature Communication}, volume = {5}, year = {2014}, month = {06/2014}, pages = {4135}, doi = {10.1038/ncomms5135}, author = {Wang, H. J. and Shin, C. S. and Seltzer, S. J. and Avalos, C. E. and Pines, A. and Bajaj, V. S.} } @article {1074, title = {Sensitive magnetic control of ensemble nuclear spin hyperpolarization in diamond}, journal = {Nature Communications}, volume = {4}, year = {2013}, note = {Nature communicationsWang, Hai-JingShin, Chang SAvalos, Claudia ESeltzer, Scott JBudker, DmitryPines, AlexanderBajaj, Vikram SengEngland2013/06/06 06:00Nat Commun. 2013 Jun 5;4:1940. doi: 10.1038/ncomms2930.}, month = {June 5, 2013}, pages = {1940}, chapter = {1940}, abstract = {

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.

}, isbn = {2041-1723 (Linking)}, doi = {10.1038/ncomms2930}, url = {http://www.ncbi.nlm.nih.gov/pubmed/23736952}, author = {Wang, H. J. and Shin, C. S. and Avalos, C. E. and Seltzer, S. J. and Budker, D. and Pines, A. and Bajaj, V. S.} } @article {249, title = {Room-temperature operation of a radiofrequency diamond magnetometer near the shot-noise limit}, journal = {Journal of Applied Physics}, volume = {112}, year = {2012}, note = {J Appl Phys061ECTimes Cited:1Cited References Count:15}, month = {Dec 15, 2012}, pages = {124519}, chapter = {124519}, abstract = {

We operate a nitrogen-vacancy (NV-) diamond magnetometer at ambient temperatures and study the dependence of its bandwidth on experimental parameters including optical and microwave excitation powers. A model based on the Bloch equations is used to analyze the NV center\&$\#$39;s response time, tau, during continuous optical and microwave irradiation, and tau(-1) is shown to be a weighted average of T-1(-1) and T-2(-1), where T-1 and T-2 are the longitudinal and transverse relaxation times of the electron spin during optical irradiation. We measured a maximum detection bandwidth of similar to 1.6 MHz with optical excitation intensity of similar to 2.3MW/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 +/- 0.3 nT/root Hz, unprecedented in a detector with this active volume of similar to 10 mu m(3) and close to the photon-shot-noise limit of our experiment. The measured bandwidth and sensitivity of our device should allow detection of micro-scale NMR signals with microfluidic devices. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4771924]

}, keywords = {spin}, isbn = {0021-8979}, doi = {Doi 10.1063/1.4771924}, url = {http://link.aip.org/link/doi/10.1063/1.4771924}, author = {Shin, C. S. and Avalos, C. E. and Butler, M. C. and Trease, D. R. and Seltzer, S. J. and Mustonen, J. P. and Kennedy, D. J. and Acosta, V. M. and Budker, D. and Pines, A. and Bajaj, V. S.} } @article {257, title = {Band-selective chemical exchange saturation transfer imaging with hyperpolarized xenon-based molecular sensors}, journal = {Journal of Magnetic Resonance}, volume = {213}, year = {2011}, note = {J Magn Reson847UKTimes Cited:3Cited References Count:29}, month = {Dec}, pages = {14-21}, abstract = {

Molecular imaging based on saturation transfer in exchanging systems is a tool for amplified and chemically specific magnetic resonance imaging. Xenon-based molecular sensors are a promising category of molecular imaging agents in which chemical exchange of dissolved xenon between its bulk and agent-bound phases has been use to achieve sub-picomolar detection sensitivity. Control over the saturation transfer dynamics, particularly when multiple exchanging resonances are present in the spectra, requires saturation fields of limited bandwidth and is generally accomplished by continuous wave irradiation. We demonstrate instead how band-selective saturation sequences based on multiple pulse inversion elements can yield saturation bandwidth tuneable over a wide range, while depositing less RF power in the sample. We show how these sequences can be used in imaging experiments that require spatial-spectral and multispectral saturation. The results should be applicable to all CEST experiments and, in particular, will provide the spectroscopic control required for applications of arrays of xenon chemical sensors in microfluidic chemical analysis devices. (C) 2011 Elsevier Inc. All rights reserved.

}, keywords = {xe-129}, isbn = {1090-7807}, doi = {Doi 10.1016/J.Jmr.2011.06.027}, url = {://WOS:000296997800002}, author = {Meldrum, T. and Bajaj, V. S. and Wemmer, D. E. and Pines, A.} } @article {259, title = {Remotely Detected MRI Velocimetry in Microporous Bead Packs}, journal = {Journal of Physical Chemistry A}, volume = {115}, year = {2011}, note = {J Phys Chem A752NBTimes Cited:1Cited References Count:52}, month = {Apr 28}, pages = {4023-4030}, abstract = {

Many NAIR and MRI methods probe fluid dynamics within macro- and mesoporous materials, but with few exceptions, they report on its macroscopically averaged properties. MRI methods are generally unable to localize microscopic features of flow within macroscopic samples because the fraction of the enclosing detector volume occupied by these features is so small. We have recently overcome this problem using remotely detected MRI velocimetry, a technique in which spatial, chemical, and velocity information about elements of the flow is encoded with a conventional NMR coil and detected sensitively at the sample outflow by a volume-matched microdetector. Here, we apply this method to microporous model systems, recording MRI images that correlate local velocity, spin relaxation, and time-of-flight in microscopic resolution and three spatial dimensions. Our results illustrate that remotely detected MRI is an effective approach to elucidate flow dynamics in porous materials including bead pack microreactors and chromatography columns.

}, keywords = {gradients}, isbn = {1089-5639}, doi = {Doi 10.1021/Jp109728j}, url = {://WOS:000289697500039}, author = {Halpern-Manners, N. W. and Paulsen, J. L. and Bajaj, V. S. and Pines, A.} } @article {254, title = {Remotely Detected NMR for the Characterization of Flow and Fast Chromatographic Separations Using Organic Polymer Monoliths}, journal = {Analytical Chemistry}, volume = {83}, year = {2011}, note = {Anal Chem798ZVTimes Cited:4Cited References Count:35}, month = {Aug 1}, pages = {6004-6010}, abstract = {

An application of remotely detected magnetic resonance imaging is demonstrated for the characterization of flow and the detection of fast, small molecule separations within hypercrosslinked polymer monoliths. The hyper-cross-linked monoliths exhibited excellent ruggedness, with a transit time relative standard deviation of less than 2.1\%, even after more than 300 column volumes were pumped through at high pressure and flow. Magnetic resonance imaging enabled high. resolution intensity and velocity-encoded images of mobile phase flow through the monolith. The images confirm that the presence of a polymer monolith within the capillary disrupts the parabolic laminar flow profile that is characteristic of mobile phase flow within an open tube. As a result, the mobile phase and analytes are equally distributed in the radial direction throughout the monolith. Also, in-line monitoring of chromatographic separations of small molecules at high flow rates is shown. The coupling of monolithic chromatography columns and NMR provides both real-time peak detection and chemical shift information for small aromatic molecules. These experiments demonstrate the unique power of magnetic resonance, both direct and remote, in studying chromatographic processes.

}, keywords = {visualization}, isbn = {0003-2700}, doi = {Doi 10.1021/Ac2010108}, url = {://WOS:000293252500029}, author = {Teisseyre, T. Z. and Urban, J. and Halpern-Manners, N. W. and Chambers, S. D. and Bajaj, V. S. and Svec, F. and Pines, A.} } @article {252, title = {Ultrafast optical encoding of magnetic resonance}, journal = {Chemical Physics Letters}, volume = {503}, year = {2011}, note = {Chem Phys Lett719FWTimes Cited:0Cited References Count:19}, month = {Feb 17}, pages = {187-190}, abstract = {

Temporal resolution in magnetic resonance imaging (MRI) is limited by the time required to encode the position of spins using time-varying (10-100 ms) magnetic field gradients. Here, we demonstrate spatial encoding of MRI images in a time that is three orders of magnitude shorter than what is possible by conventional gradient encoding techniques. Our method exploits the chemically induced dynamic nuclear polarization (CIDNP) effect and is an initial example of a set of approaches that seek to combine the favorable properties of optical spectroscopy with those of NMR for polarization, encoding, and detection. (C) 2010 Elsevier B.V. All rights reserved.

}, keywords = {state}, isbn = {0009-2614}, doi = {Doi 10.1016/J.Cplett.2010.12.063}, url = {://WOS:000287187800001}, author = {Trease, D. and Bajaj, V. S. and Paulsen, J. and Pines, A.} } @article {265, title = {Magnetic resonance imaging of oscillating electrical currents}, journal = {Proceedings of the National Academy of Sciences of the United States of America}, volume = {107}, year = {2010}, note = {P Natl Acad Sci USA595DPTimes Cited:1Cited References Count:47}, month = {May 11}, pages = {8519-8524}, abstract = {

Functional MRI has become an important tool of researchers and clinicians who seek to understand patterns of neuronal activation that accompany sensory and cognitive processes. However, the interpretation of fMRI images rests on assumptions about the relationship between neuronal firing and hemodynamic response that are not firmly grounded in rigorous theory or experimental evidence. Further, the blood-oxygen-level-dependent effect, which correlates an MRI observable to neuronal firing, evolves over a period that is 2 orders of magnitude longer than the underlying processes that are thought to cause it. Here, we instead demonstrate experiments to directly image oscillating currents by MRI. The approach rests on a resonant interaction between an applied rf field and an oscillating magnetic field in the sample and, as such, permits quantitative, frequency-selective measurements of current density without spatial or temporal cancellation. We apply this method in a current loop phantom, mapping its magnetic field and achieving a detection sensitivity near the threshold required for the detection of neuronal currents. Because the contrast mechanism is under spectroscopic control, we are able to demonstrate how ramped and phase-modulated spin-lock radiation can enhance the sensitivity and robustness of the experiment. We further demonstrate the combination of these methods with remote detection, a technique in which the encoding and detection of an MRI experiment are separated by sample flow or translation. We illustrate that remotely detected MRI permits the measurement of currents in small volumes of flowing water with high sensitivity and spatial resolution.

}, keywords = {nerve}, isbn = {0027-8424}, doi = {Doi 10.1073/Pnas.1003146107}, url = {://WOS:000277591200008}, author = {Halpern-Manners, N. W. and Bajaj, V. S. and Teisseyre, T. Z. and Pines, A.} } @article {263, title = {A Xenon-Based Molecular Sensor Assembled on an MS2 Viral Capsid Scaffold}, journal = {Journal of the American Chemical Society}, volume = {132}, year = {2010}, note = {J Am Chem Soc589OATimes Cited:20Cited References Count:23}, month = {May 5}, pages = {5936-+}, abstract = {

In MRI, anatomical structures are most often differentiated by variations in their bulk magnetic properties. Alternatively, exogenous contrast agents can be attached to chemical moieties that confer affinity to molecular targets; the distribution of such contrast agents can be imaged by magnetic resonance. Xenon-based molecular sensors are molecular imaging agents that rely on the reversible exchange of hyperpolarized xenon between the bulk and a specifically targeted host-guest complex. We have incorporated similar to 125 xenon sensor molecules in the interior of an MS2 viral capsid, conferring multivalency and other properties of the viral capsid to the sensor molecule. The resulting signal amplification facilitates the detection of sensor at 0.7 pM, the lowest to date for any molecular imaging agent used in magnetic resonance. This amplification promises the detection of chemical targets at much lower concentrations than would be possible without the capsid scaffold.

}, keywords = {nmr}, isbn = {0002-7863}, doi = {Doi 10.1021/Ja100319f}, url = {://WOS:000277158500007}, author = {Meldrum, T. and Seim, K. L. and Bajaj, V. S. and Palaniappan, K. K. and Wu, W. and Francis, M. B. and Wemmer, D. E. and Pines, A.} } @article {266, title = {Zooming In on Microscopic Flow by Remotely Detected MRI}, journal = {Science}, volume = {330}, year = {2010}, note = {Science682BUTimes Cited:12Cited References Count:27}, month = {Nov 19}, pages = {1078-1081}, abstract = {

Magnetic resonance imaging (MRI) can elucidate the interior structure of an optically opaque object in unparalleled detail but is ultimately limited by the need to enclose the object within a detection coil; acquiring the image with increasingly smaller pixels reduces the sensitivity, because each pixel occupies a proportionately smaller fraction of the detector\&$\#$39;s volume. We developed a technique that overcomes this limitation by means of remotely detected MRI. Images of fluids flowing in channel assemblies are encoded into the phase and intensity of the constituent molecules\&$\#$39; nuclear magnetic resonance signals and then decoded by a volume-matched detector after the fluids flow out of the sample. In combination with compressive sampling, we thus obtain microscopic images of flow and velocity distributions similar to 10(6) times faster than is possible with conventional MRI on this hardware. Our results illustrate the facile integration of MRI with microfluidic assays and suggest generalizations to other systems involving microscopic flow.

}, keywords = {biosensor}, isbn = {0036-8075}, doi = {Doi 10.1126/Science.1192313}, url = {://WOS:000284374700036}, author = {Bajaj, V. S. and Paulsen, J. and Harel, E. and Pines, A.} }