Hyperpolarization Of Silicon Nanoparticles With Tempo Radicals, Jingzhe Hu, Nicholas Whiting, Pratip Bhattacharya
Mar 2018
Hyperpolarization Of Silicon Nanoparticles With Tempo Radicals, Jingzhe Hu, Nicholas Whiting, Pratip Bhattacharya
Nicholas Whiting
Silicon-based particles can be hyperpolarized via dynamic nuclear polarization to enhance 29Si magnetic resonance signals. Application of this technique to nanoscale silicon particles has been limited because of the low signal enhancements achieved; it is hypothesized that this is due to the low number of endogenous electronic defects inherent to the particles. We introduce a method of incorporating exogenous radicals into silicon nanoparticle suspensions in order to improve the hyperpolarization of 29Si nuclear spins to levels sufficient for in vivo MR imaging. Calibration of radical concentrations and polarization times are reported for a variety of silicon particle sizes (30−200 nm …
Hyperpolarized Porous Silicon Nanoparticles: Potential Theragnostic Material For 29si Magnetic Resonance Imaging, Hyeonglim Seo, Ikjang Choi, Nicholas Whiting, Jingzhe Hu, Quy S. Luu, Shivanand Pudakalakatti, Caitlin Mccowan, Yaewon Kim, Niki Zacharias Millward, Seunghyun Lee, Pratip Bhattacharya, Youngbok Lee
Dec 2017
Hyperpolarized Porous Silicon Nanoparticles: Potential Theragnostic Material For 29si Magnetic Resonance Imaging, Hyeonglim Seo, Ikjang Choi, Nicholas Whiting, Jingzhe Hu, Quy S. Luu, Shivanand Pudakalakatti, Caitlin Mccowan, Yaewon Kim, Niki Zacharias Millward, Seunghyun Lee, Pratip Bhattacharya, Youngbok Lee
Nicholas Whiting
Porous silicon nanoparticles have recently garnered attention as potentially-promising biomedical platforms for drug delivery and medical diagnostics. Here, we demonstrate porous silicon nanoparticles as contrast agents for 29Si magnetic resonance imaging. Size-controlled porous silicon nanoparticles were synthesized by magnesiothermic reduction of silica nanoparticles and were surface activated for further functionalization. Particles were hyperpolarized via dynamic nuclear polarization to enhance their 29Si MR signals; the particles demonstrated long 29Si spin-lattice relaxation (T1) times (~25 mins), which suggests potential applicability for medical imaging. Furthermore, 29Si hyperpolarization levels were sufficient to allow 29Si MRI in phantoms. These results underscore the potential of porous …
Using Raman Spectroscopy To Improve Hyperpolarized Noble Gas Production For Clinical Lung Imaging Techniques, Jonathan R. Birchall, Nicholas Whiting, Jason G. Skinner, Michael J. Barlow, Boyd M. Goodson
Dec 2016
Using Raman Spectroscopy To Improve Hyperpolarized Noble Gas Production For Clinical Lung Imaging Techniques, Jonathan R. Birchall, Nicholas Whiting, Jason G. Skinner, Michael J. Barlow, Boyd M. Goodson
Nicholas Whiting
Spin-exchange optical pumping (SEOP) can be used to “hyperpolarize” 129Xe for human lung MRI. SEOP involves transfer of angular momentum from light to an alkali metal (Rb) vapor, and then onto 129Xe nuclear spins during collisions; collisions between excited Rb and N2 ensure that incident optical energy is nonradiatively converted into heat. However, because variables that govern SEOP are temperature-dependent, the excess heat can complicate efforts to maximize spin polarization—particularly at high laser fluxes and xenon densities. Ultra-low frequency Raman spectroscopy may be used to perform in situ gas temperature measurements to investigate the interplay of energy thermalization and SEOP …
Developing Hyperpolarized Silicon Particles For In Vivo Mri Targeting Of Ovarian Cancer, Nicholas Whiting, Jingzhe Hu, Niki M. Zacharias, Ganesh L. R. Lokesh, David E. Volk, David G. Menter, Rajesha Rupaimoole, Rebecca Previs, Anil K. Sood, Pratip Bhattacharya
Aug 2016
Developing Hyperpolarized Silicon Particles For In Vivo Mri Targeting Of Ovarian Cancer, Nicholas Whiting, Jingzhe Hu, Niki M. Zacharias, Ganesh L. R. Lokesh, David E. Volk, David G. Menter, Rajesha Rupaimoole, Rebecca Previs, Anil K. Sood, Pratip Bhattacharya
Nicholas Whiting
Silicon-based nanoparticles are ideally suited for use as biomedical imaging agents due to their biocompatibility, biodegradability, and simple surface chemistry that facilitates drug loading and targeting. A method of hyperpolarizing silicon particles using dynamic nuclear polarization, which increases magnetic resonance imaging signals by several orders-of-magnitude through enhanced nuclear spin alignment, has recently been developed to allow silicon particles to function as contrast agents for in vivo magnetic resonance imaging. The enhanced spin polarization of silicon lasts significantly longer than other hyperpolarized agents (tens of minutes, whereas <1 min for other species at room temperature), allowing a wide range of potential …
Interrogating Metabolism In Brain Cancer, Travis Salzillo, Jingzhe Hu, Linda Nguyen, Nicholas Whiting, Jaehyuk Lee, Joseph Weygand, Prasanta Dutta, Shivanand Pudakalakatti, Niki Zacharias Millward, Seth Gammon, Frederick F. Lang, Amy B. Heimberger, Pratip Bhattacharya
Dec 2015
Interrogating Metabolism In Brain Cancer, Travis Salzillo, Jingzhe Hu, Linda Nguyen, Nicholas Whiting, Jaehyuk Lee, Joseph Weygand, Prasanta Dutta, Shivanand Pudakalakatti, Niki Zacharias Millward, Seth Gammon, Frederick F. Lang, Amy B. Heimberger, Pratip Bhattacharya
Nicholas Whiting
Many existing and emerging techniques of interrogating metabolism in brain cancer are at an early stage of development. A few clinical trials that employ these techniques are in progress in patients with brain cancer to establish the clinical efficacy of these techniques. It is likely that in vivo metabolomics and metabolic imaging is the next frontier in brain cancer diagnosis and assessing therapeutic efficacy.
Real-Time Mri-Guided Catheter Tracking Using Hyperpolarized Silicon Particles, Nicholas Whiting, Jingzhe Hu, Jay V. Shah, Maja C. Cassidy, Erik Cressman, Niki Zacharias Millward, David G. Menter, Charles M. Marcus, Pratip K. Bhattacharya
Jan 2015
Real-Time Mri-Guided Catheter Tracking Using Hyperpolarized Silicon Particles, Nicholas Whiting, Jingzhe Hu, Jay V. Shah, Maja C. Cassidy, Erik Cressman, Niki Zacharias Millward, David G. Menter, Charles M. Marcus, Pratip K. Bhattacharya
Nicholas Whiting
Visualizing the movement of angiocatheters during endovascular interventions is typically accomplished using x-ray fluoroscopy. There are many potential advantages to developing magnetic resonance imaging-based approaches that will allow three-dimensional imaging of the tissue/vasculature interface while monitoring other physiologically-relevant criteria, without exposing the patient or clinician team to ionizing radiation. Here we introduce a proof-of-concept development of a magnetic resonance imaging-guided catheter tracking method that utilizes hyperpolarized silicon particles. The increased signal of the silicon particles is generated via low-temperature, solid-state dynamic nuclear polarization, and the particles retain their enhanced signal for ≥40 minutes—allowing imaging experiments over extended time durations. The …
Spin-Exchange Optical Pumping At High Xenon Densities And Laser Fluxes: Principles And Practice, Boyd M. Goodson, Nicholas Whiting, Hayley Newton, Jason G. Skinner, Kaili Ranta, Panayiotis Nikolaou, Michael J. Barlow, Eduard Y. Chekmenev
Dec 2014
Spin-Exchange Optical Pumping At High Xenon Densities And Laser Fluxes: Principles And Practice, Boyd M. Goodson, Nicholas Whiting, Hayley Newton, Jason G. Skinner, Kaili Ranta, Panayiotis Nikolaou, Michael J. Barlow, Eduard Y. Chekmenev
Nicholas Whiting
Once limited to the realm of fundamental physics experiments, hyperpolarized (HP) noble gases have been exploited for a wide range of applications across NMR and MRI. In most cases, hyperpolarized noble gases are prepared by spin-exchange optical pumping (SEOP)...
Hyperpolarization Methods For Mrs, Boyd M. Goodson, Nicholas Whiting, Aaron M. Coffey, Panayiotis Nikolaou, Fan Shi, Brogan M. Gust, Maxwell E. Gemeinhardt, Roman Shchepin, Jason G. Skinner, Jonathan R. Birchall, Michael J. Barlow, Eduard Y. Chekmenev
Dec 2014
Hyperpolarization Methods For Mrs, Boyd M. Goodson, Nicholas Whiting, Aaron M. Coffey, Panayiotis Nikolaou, Fan Shi, Brogan M. Gust, Maxwell E. Gemeinhardt, Roman Shchepin, Jason G. Skinner, Jonathan R. Birchall, Michael J. Barlow, Eduard Y. Chekmenev
Nicholas Whiting
This article covers the fundamental principles and practice of NMR hyperpolarization techniques, which are proving useful for in vivo magnetic resonance spectroscopy (MRS) studies of metabolism in animal models, and clinical trials with hyper-enhanced sensitivity. Fundamentally, hyperpolarization methods enhance nuclear spin polarization by orders-of-magnitude, resulting in concomitant improvement in NMR detection sensitivity. The hyperpolarization methods described here – dynamic nuclear polarization (DNP), para-hydrogen induced polarization (PHIP), signal amplification by reversible exchange (SABRE), and spin-exchange optical pumping (SEOP) – are capable of achieving nuclear spin polarization approaching the theoretical maximum of unity on nuclear spin sites of molecular or atomic agents …
Xena: An Automated 'Open-Source' 129xe Hyperpolarizer For Clinical Use, Panayiotis Nikolaou, Aaron M. Coffey, Laura L. Walkup, Brogan M. Gust, Nicholas Whiting, Hayley Newton, Iga Muradyan, Mikayel Dabaghyan, Kaili Ranta, Gregory D. Moroz, Matthew S. Rosen, Samuel Patz, Michael J. Barlow, Eduard Y. Chekmenev, Boyd M. Goodson
Dec 2013
Xena: An Automated 'Open-Source' 129xe Hyperpolarizer For Clinical Use, Panayiotis Nikolaou, Aaron M. Coffey, Laura L. Walkup, Brogan M. Gust, Nicholas Whiting, Hayley Newton, Iga Muradyan, Mikayel Dabaghyan, Kaili Ranta, Gregory D. Moroz, Matthew S. Rosen, Samuel Patz, Michael J. Barlow, Eduard Y. Chekmenev, Boyd M. Goodson
Nicholas Whiting
Here we provide a full report on the construction, components, and capabilities of our consortium’s “opensource”
large-scale (~1 L/h) 129Xe hyperpolarizer for clinical, pre-clinical, and materials NMR/MRI (Nikolaou et al., Proc. Natl. Acad. Sci. USA, 110, 14150 (2013)). The ‘hyperpolarizer’ is automated and built mostly of off-the-shelf components; moreover, it is designed to be cost-effective and installed in both research laboratories and clinical settings with materials costing less than $125,000. The device runs in the xenon-rich regime (up to 1800 Torr Xe in 0.5 L) in either stopped-flow or single-batch mode—making cryo-collection of the hyperpolarized gas unnecessary for many applications. …
Near-Unity Nuclear Polarization With An Open-Source 129xe Hyperpolarizer For Nmr And Mri, Panayiotis Nikolaou, Aaron M. Coffey, Laura L. Walkup, Brogan M. Gust, Nicholas Whiting, Hayley Newton, Scott Barcus, Iga Muradyan, Mikayel Dabaghyan, Gregory D. Moroz, Matthew S. Rosen, Samuel Patz, Michael J. Barlow, Eduard Y. Chekmenev, Boyd M. Goodson
Aug 2013
Near-Unity Nuclear Polarization With An Open-Source 129xe Hyperpolarizer For Nmr And Mri, Panayiotis Nikolaou, Aaron M. Coffey, Laura L. Walkup, Brogan M. Gust, Nicholas Whiting, Hayley Newton, Scott Barcus, Iga Muradyan, Mikayel Dabaghyan, Gregory D. Moroz, Matthew S. Rosen, Samuel Patz, Michael J. Barlow, Eduard Y. Chekmenev, Boyd M. Goodson
Nicholas Whiting
The exquisite NMR spectral sensitivity and negligible reactivity of hyperpolarized xenon-129 (HP129Xe) make it attractive for a number of magnetic resonance applications; moreover, HP129Xe embodies an alternative to rare and nonrenewable 3He. However, the ability to reliably and inexpensively produce large quantities of HP129Xe with sufficiently high 129Xe nuclear spin polarization (PXe) remains a significant challenge—particularly at high Xe densities. We present results from our “open-source” large-scale (∼1 L/h) 129Xe polarizer for clinical, preclinical, and materials NMR and MRI research. Automated and composed mostly of off-the-shelf components, this “hyperpolarizer” is designed to be readily implementable in other laboratories. The device …
Using Frequency-Narrowed, Tunable Laser Diode Arrays With Integrated Volume Holographic Gratings For Spin-Exchange Optical Pumping At High Resonant Fluxes And Xenon Densities, Nicholas Whiting, Panayiotis Nikolaou, Neil A. Eschmann, Michael J. Barlow, R Lammert, J Ungar, W Hu, Laurent Vaissie, Boyd M. Goodson
Dec 2011
Using Frequency-Narrowed, Tunable Laser Diode Arrays With Integrated Volume Holographic Gratings For Spin-Exchange Optical Pumping At High Resonant Fluxes And Xenon Densities, Nicholas Whiting, Panayiotis Nikolaou, Neil A. Eschmann, Michael J. Barlow, R Lammert, J Ungar, W Hu, Laurent Vaissie, Boyd M. Goodson
Nicholas Whiting
Next-generation laser diode arrays with integrated ‘on-chip’ volume holographic gratings can provide high power with spectrally narrowed output that can be tuned about the rubidium D1 line—without causing significant changes to the laser’s flux or spectral profile. These properties were exploited to independently evaluate the effects of varying the laser centroid wavelength and power on batch-mode Rb/129Xe spin-exchange optical pumping (SEOP) as functions of xenon partial pressure and cell temperature...
Interdependence Of In-Cell Xenon Density And Temperature During Rb/129xe Spin-Exchange Optical Pumping Using Vhg-Narrowed Laser Diode Arrays, Nicholas Whiting, Panayiotis Nikolaou, Neil A. Eschmann, Michael J. Barlow, Boyd M. Goodson
Dec 2009
Interdependence Of In-Cell Xenon Density And Temperature During Rb/129xe Spin-Exchange Optical Pumping Using Vhg-Narrowed Laser Diode Arrays, Nicholas Whiting, Panayiotis Nikolaou, Neil A. Eschmann, Michael J. Barlow, Boyd M. Goodson
Nicholas Whiting
The 129Xe nuclear spin polarization (PXe) that can be achieved via spin-exchange optical pumping (SEOP) is typically limited at high in-cell xenon densities ([Xe]cell), due primarily to corresponding reductions in the alkali metal electron spin polarization (e.g. PRb) caused by increased non-spin-conserving Rb–Xe collisions. While demonstrating the utility of volume holographic grating (VHG)-narrowed lasers for Rb/129Xe SEOP, we recently reported [P. Nikolaou et al., JMR 197 (2009) 249] an anomalous dependence of the observed PXe on the in-cell xenon partial pressure (pXe), wherein PXe values were abnormally low at decreased pXe, peaked at moderate pXe (~300 torr), and remained surprisingly …
Generation Of Laser-Polarized Xenon Using Fiber-Coupled Laser-Diode Arrays Narrowed With Integrated Volume Holographic Gratings, Panayiotis Nikolaou, Nicholas Whiting, Neil A. Eschmann, Kathleen E. Chaffee, Michael J. Barlow, Boyd M. Goodson
Dec 2007
Generation Of Laser-Polarized Xenon Using Fiber-Coupled Laser-Diode Arrays Narrowed With Integrated Volume Holographic Gratings, Panayiotis Nikolaou, Nicholas Whiting, Neil A. Eschmann, Kathleen E. Chaffee, Michael J. Barlow, Boyd M. Goodson
Nicholas Whiting
Volume holographic gratings (VHGs) can be exploited to narrow the spectral output of high-power laserdiode arrays (LDAs) by nearly an order of magnitude, permitting more efficient generation of laser-polarized noble gases for various applications. A ~3-fold improvement in 129Xe nuclear spin polarization, PXe, (compared to a conventional LDA) was achieved with the VHG-LDA’s center wavelength tuned to a wing of the Rb D1 line. Additionally, an anomalous dependence of PXe on the xenon density within the OP cell is reported—including high PXe values (>10%) at high xenon partial pressures (~1000 torr).
Characterization Of Violet Emission From Rb Optical Pumping Cells Used In Laser-Polarized Xenon Nmr Experiments, Indrajit Saha, Panayiotis Nikolaou, Nicholas Whiting, Boyd M. Goodson
Dec 2005
Characterization Of Violet Emission From Rb Optical Pumping Cells Used In Laser-Polarized Xenon Nmr Experiments, Indrajit Saha, Panayiotis Nikolaou, Nicholas Whiting, Boyd M. Goodson
Nicholas Whiting
Visible emission from Rb optical pumping cells was characterized under a range of conditions relevant to the production of laserpolarized xenon (including temperature, partial pressures, and D1-resonant 795 nm laser power). Bright 421 nm (6P --> 5S) emission was consistent with energy-pooling processes of the type: Rb*(5P1/2) + Rb*(5P1/2,3/2) --> Rb*(6P1/2,3/2) + Rb(5S1/2), with processes transiting through 5D states likely contributing at higher temperatures/lower N2 partial pressures. Under such conditions a number of Rb lines may be observed, indicating population of Rb states to P9D (~31822 cm^-1). Such energies exceed those required for efficient production of laser-induced plasma.
Interactions Between Xenon And Phospholipid Bicelles Studied By 2h/129xe/131xe Nmr And Optical Pumping Of Nuclear Spins, Xiaoxia Li, Caitlin Newberry, Indrajit Saha, Panayiotis Nikolaou, Nicholas Whiting, Boyd M. Goodson
Dec 2004
Interactions Between Xenon And Phospholipid Bicelles Studied By 2h/129xe/131xe Nmr And Optical Pumping Of Nuclear Spins, Xiaoxia Li, Caitlin Newberry, Indrajit Saha, Panayiotis Nikolaou, Nicholas Whiting, Boyd M. Goodson
Nicholas Whiting
The interactions between xenon and DMPC/DHPC bicelles (q = 3.5%,7.5% w/v) were studied via 2H, 129Xe, 131Xe, and optically enhanced 129Xe NMR. The chemical shifts, linewidths, and quadrupolar couplings of the xenon/bicelle NMR signals were correlated with different regions of the bicellar phase diagram. The addition of xenon (<70 mM) was observed to reduce the temperature-onset of bicelle alignment by several degrees, in quantitative agreement with effects previously observed with chloroform; however, the stable liquid-crystalline range was not significantly reduced. Preliminary laser-polarized xenon/bicelle studies yielded 129Xe T1 values of ~120 s, long enough to permit a variety of planned experiments.
