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

Abstract

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 10 5 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 simplemore » instrumentation.« less

Authors:
 [1];  [1];  [2];  [1];  [3];  [4];  [4];  [4];  [1];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Time and Frequency Division; Univ. of Colorado, Boulder, CO (United States). Dept. of Physics
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  4. National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Time and Frequency Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1408421
Grant/Contract Number:
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; imaging and sensing; microfluidics; NMR spectroscopy; optical sensors

Citation Formats

Kennedy, Daniel J., Seltzer, Scott J., Jiménez-Martínez, Ricardo, Ring, Hattie L., Malecek, Nicolas S., Knappe, Svenja, Donley, Elizabeth A., Kitching, John, Bajaj, Vikram S., and Pines, Alexander. An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe. United States: N. p., 2017. Web. doi:10.1038/srep43994.
Kennedy, Daniel J., Seltzer, Scott J., Jiménez-Martínez, Ricardo, Ring, Hattie L., Malecek, Nicolas S., Knappe, Svenja, Donley, Elizabeth A., Kitching, John, Bajaj, Vikram S., & Pines, Alexander. An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe. United States. doi:10.1038/srep43994.
Kennedy, Daniel J., Seltzer, Scott J., Jiménez-Martínez, Ricardo, Ring, Hattie L., Malecek, Nicolas S., Knappe, Svenja, Donley, Elizabeth A., Kitching, John, Bajaj, Vikram S., and Pines, Alexander. Tue . "An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe". United States. doi:10.1038/srep43994. https://www.osti.gov/servlets/purl/1408421.
@article{osti_1408421,
title = {An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe},
author = {Kennedy, Daniel J. and Seltzer, Scott J. and Jiménez-Martínez, Ricardo and Ring, Hattie L. and Malecek, Nicolas S. and Knappe, Svenja and Donley, Elizabeth A. and Kitching, John and Bajaj, Vikram S. and Pines, Alexander},
abstractNote = {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.},
doi = {10.1038/srep43994},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {Tue Mar 07 00:00:00 EST 2017},
month = {Tue Mar 07 00:00:00 EST 2017}
}

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  • Purpose: Radiation induced lung injury (RILI) is a common side effect for patients undergoing thoracic radiation therapy (RT). RILI can lead to temporary or permanent loss of lung function and in extreme cases, death. Combining functional lung imaging information with conventional radiation treatment plans may lead to more desirable treatment plans that reduce lung toxicity and improve the quality of life for lung cancer survivors. Magnetic Resonance Imaging of the lung following inhalation of hyperpolarized{sup 129}Xe may provide a useful nonionizing approach for probing changes in lung function and structure associated with RILI before, during, or after RT (early andmore » late time-points). Methods: In this study, dynamic{sup 129}Xe MR spectroscopy was used to measure whole-lung gas transfer time constants for lung tissue and red blood cells (RBC), respectively (T{sub Tr-tissue} and T{sub Tr-RBC}) in groups of rats at two weeks and six weeks following 14 Gy whole-lung exposure to radiation from a {sup 60}Co source. A separate group of six healthy age-matched rats served as a control group. Results: T{sub Tr-tissue} values at two weeks post-irradiation (51.6 ± 6.8 ms) were found to be significantly elevated (p < 0.05) with respect to the healthy control group (37.2 ± 4.8 ms). T{sub Tr-RBC} did not show any significant changes between groups. T{sub Tr-tissue} was strongly correlated with T{sub Tr-RBC} in the control group (r = 0.9601 p < 0.05) and uncorrelated in the irradiated groups. Measurements of arterial partial pressure of oxygen obtained by arterial blood sampling were found to be significantly decreased (p < 0.05) in the two-week group (54.2 ± 12.3 mm Hg) compared to those from a representative control group (85.0 ± 10.0 mm Hg). Histology of a separate group of similarly irradiated animals confirmed the presence of inflammation due to radiation exposure with alveolar wall thicknesses that were significantly different (p < 0.05). At six weeks post-irradiation, T{sub Tr-tissue} returned to values (35.6 ± 9.6 ms) that were not significantly different from baseline. Conclusions: Whole-lung tissue transfer time constants for{sup 129}Xe (T{sub Tr-tissue}) can be used to detect the early phase of RILI in a rat model involving 14 Gy thoracic {sup 60}Co exposure as early as two weeks post-irradiation. This knowledge combined with more sophisticated models of gas exchange and imaging techniques, may allow functional lung avoidance radiation therapy planning to be achievable, providing more beneficial treatment plans and improved quality of life for recovering lung cancer patients.« less
  • We present a design for a spin-exchange optical pumping system to produce large quantities of highly polarized {sup 129}Xe. Low xenon concentrations in the flowing gas mixture allow the laser to maintain high Rb polarization. The large spin-exchange rate between Rb and {sup 129}Xe through the long-lived van der Waals molecules at low pressure, combined with a high flow rate, results in large production rates of hyperpolarized xenon. We report a maximum polarization of 64% achieved for a 0.3 l/h Xe flow rate, and maximum magnetization output of 6 l/h at 22% polarization. Our findings regarding the polarization dependence onmore » temperature, nitrogen partial pressure, and gas mixture flow velocity are also reported.« less
  • The major obstacle to the use of 129-xenon (I = {1/2}) as a new source of contrast in magnetic resonance is its low sensitivity. The hyperpolarized {sup 129}Xe-MRI technique using laser optical pumping of rubidium promises to resolve this problem. The potential of xenon-based MRI for the body tissues other than the lung air spaces depends on the {sup 129}Xe polarization lifetime (T1) in the blood at a magnetic field of commonly available clinical MRI systems. Xenon with natural abundance of {sup 129}Xe (26%) was dissolved in human blood and studied at 36{degrees}C in a 2.35 T 40 cm boremore » MRI spectrometer (27.6 MHz). Zeeman relaxation (T1) of six blood samples was measured by the progressive saturation method for periods of 4-8 h each. NMR spectra revealed two peaks at 216.0 ppm (A) and 194.0 ppm (B) relative to the xenon gas above the blood volume. Assignment and {sup 129}Xe T1 values were 4.5 {+-} 1 s for red blood cells (A), 0.6 {+-} 2 s for plasma (B) and 11.9 {+-} 1.6 s for xenon gas at atmospheric oxygen pressure. Xenon dissolved in distilled water appears at 189.8 ppm and has T1 = 26.3 {+-} 1.4 s. These relaxation times, though shorter than expected, are comparable to the transport time of blood, and are long enough to encourage use of hyperpolarized xenon for MRI studies in tissues, in addition to lung. 18 refs., 2 figs.« less
  • Studies of hyperpolarized xenon-129 in media such as liquid crystals and cell suspensions are in demand for applications ranging from biomedical imaging to materials engineering but have been hindered by the inability to bubble Xe through the desired media as a result of viscosity or perturbations caused by bubbles. This research reports on a device that can be reliably used to dissolve hp- 129 Xe into viscous aqueous and organic samples without bubbling. This method is robust, requires small sample volumes ( < 60 μL), is compatible with existing NMR hardware, and is made from readily available materials. Experiments showmore » that Xe can be introduced into viscous and aligned media without disrupting molecular order. We detected dissolved xenon in an aqueous liquid crystal that is disrupted by the shear forces of bubbling, and we observed liquid-crystal phase transitions in (MBBA). This tool allows an entirely new class of samples to be investigated by hyperpolarized-gas NMR spectroscopy. Blending into the crowd: A new device that facilitates the direct dissolution of hyperpolarized 129 Xe into viscous liquid-crystalline media is presented. 129 Xe and 2 H NMR spectra show the nondisruptive dissolution of xenon, the presence of ordered phases, and, in the case of the thermotropic liquid crystal N-(4-methoxybenzylidene)-4-butylaniline, a nematic-isotropic phase transition.« less
  • Purpose: To assess the feasibility of hyperpolarized (HP) {sup 129}Xe MRI for detection of early stage radiation-induced lung injury (RILI) in a rat model involving unilateral irradiation by assessing differences in gas exchange dynamics between irradiated and unirradiated lungs. Methods: The dynamics of gas exchange between alveolar air space and pulmonary tissue (PT), PT and red blood cells (RBCs) was measured using single-shot spiral iterative decomposition of water and fat with echo asymmetry and least-squares estimation images of the right and left lungs of two age-matched cohorts of Sprague Dawley rats. The first cohort (n = 5) received 18 Gymore » irradiation to the right lung using a {sup 60}Co source and the second cohort (n = 5) was not irradiated and served as the healthy control. Both groups were imaged two weeks following irradiation when radiation pneumonitis (RP) was expected to be present. The gas exchange data were fit to a theoretical gas exchange model to extract measurements of pulmonary tissue thickness (L{sub PT}) and relative blood volume (V{sub RBC}) from each of the right and left lungs of both cohorts. Following imaging, lung specimens were retrieved and percent tissue area (PTA) was assessed histologically to confirm RP and correlate with MRI measurements. Results: Statistically significant differences in L{sub PT} and V{sub RBC} were observed between the irradiated and non-irradiated cohorts. In particular, L{sub PT} of the right and left lungs was increased approximately 8.2% and 5.0% respectively in the irradiated cohort. Additionally, V{sub RBC} of the right and left lungs was decreased approximately 36.1% and 11.7% respectively for the irradiated cohort compared to the non-irradiated cohort. PTA measurements in both right and left lungs were increased in the irradiated group compared to the non-irradiated cohort for both the left (P < 0.05) and right lungs (P < 0.01) confirming the presence of RP. PTA measurements also correlated with the MRI measurements for both the non-irradiated (r = 0.79, P < 0.01) and irradiated groups (r = 0.91, P < 0.01). Conclusions: Regional RILI can be detected two weeks post-irradiation using HP {sup 129}Xe MRI and analysis of gas exchange curves. This approach correlates well with histology and can potentially be used clinically to assess radiation pneumonitis associated with early RILI to improve radiation therapy outcomes.« less