Temperature response of 129Xe depolarization transfer and its application for ultra-sensitive NMR detection

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Temporary trapping of atomic xenon in functionalized cryptophane cages makes the high sensitivity of hyperpolarized (hp) 129Xe available for highly specific NMR detection of biomolecules like proteins in solution. Here, we study the signal transfer onto a reservoir of unbound hp xenon by gating the residence time of the nuclei in the cage through the temperature-dependent exchange rate. Temperature changes were detectable immediately as an altered reservoir signal and yielded a sensitivity of 0.6 K. The temperature response is adjustable with lower concentrations of caged xenon providing more sensitivity at higher temperatures and allows ultra-sensitive detection of such molecular cages ... continued below

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Schroeder, Leif; Schroder, Leif; Meldrum, Tyler; Smith, Monica; Lowery, Thomas J.; Wemmer, David E. et al. March 20, 2008.

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Temporary trapping of atomic xenon in functionalized cryptophane cages makes the high sensitivity of hyperpolarized (hp) 129Xe available for highly specific NMR detection of biomolecules like proteins in solution. Here, we study the signal transfer onto a reservoir of unbound hp xenon by gating the residence time of the nuclei in the cage through the temperature-dependent exchange rate. Temperature changes were detectable immediately as an altered reservoir signal and yielded a sensitivity of 0.6 K. The temperature response is adjustable with lower concentrations of caged xenon providing more sensitivity at higher temperatures and allows ultra-sensitive detection of such molecular cages at 310 K. Functionalized cryptophane could be detected at concentrations as low as 10nM which corresponds to a 4000-fold sensitivity enhancement compared to conventional detection. This sensitivity makes hp-NMR capable of detecting such constructs in concentrations far belowthe detection limit by UV-visible light absorbance.

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  • Journal Name: Physical Review Letters

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  • Report No.: LBNL-276E
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 928953
  • Archival Resource Key: ark:/67531/metadc896110

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  • March 20, 2008

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  • Sept. 27, 2016, 1:39 a.m.

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  • Sept. 30, 2016, 7:16 p.m.

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Schroeder, Leif; Schroder, Leif; Meldrum, Tyler; Smith, Monica; Lowery, Thomas J.; Wemmer, David E. et al. Temperature response of 129Xe depolarization transfer and its application for ultra-sensitive NMR detection, article, March 20, 2008; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc896110/: accessed November 20, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.