title: DNP by thermal mixing under optimized conditions yields >60,000-fold enhancement of 89Y NMR signal.
abstract: Hyperpolarized (89)Y complexes are attractive NMR spectroscopy and MR imaging probes due to the exceptionally long spin-lattice relaxation time (T(1) ≈ 10 min) of the (89)Y nucleus. However, in vivo imaging of (89)Y has not yet been realized because of the low NMR signal enhancement levels previously achieved for this ultra low-γ(n) nucleus. Here, we report liquid-state (89)Y NMR signal enhancements over 60,000 times the thermal signal at 298 K in a 9.4 T magnet, achieved after the dynamic nuclear polarization (DNP) of Y(III) complex of 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) samples at 3.35 T and 1.4 K. The (89)Y DNP was shown to proceed by thermal mixing and the liquid state (89)Y NMR signal enhancement was maximized by (i) establishing the optimal microwave irradiation frequency, (ii) optimizing the glassing matrix, (iii) choosing a radical with negligible inhomogeneous line broadening contribution to the ESR linewidth, and (iv) addition of an electron T(1e) relaxation agent. The highest enhancements were achieved using a trityl OX063 radical combined with a gadolinium relaxation agent in water-glycerol matrix. Co-polarization of (89)YDOTA and sodium [1-(13)C]pyruvate showed that both (89)Y and (13)C nuclear species acquired the same spin temperature, consistent with thermal mixing theory of DNP. This methodology may be applicable for the optimization of DNP of other low-γ(n) nuclei.
authors.affiliation: Advanced Imaging Research Center, University of Texas Southwestern Medical Center, 5323 Harry Hines Boulevard, Dallas, Texas 75390, USA.
authors.forename: Lloyd
authors.initials: L
authors.lastname: Lumata
authors.forename: Ashish K
authors.initials: AK
authors.lastname: Jindal
authors.forename: Matthew E
authors.initials: ME
authors.lastname: Merritt
authors.forename: Craig R
authors.initials: CR
authors.lastname: Malloy
authors.forename: A Dean
authors.initials: AD
authors.lastname: Sherry
authors.forename: Zoltan
authors.initials: Z
authors.lastname: Kovacs
mesh_terms: D006573:Heterocyclic Compounds, 1-Ring / Q000737:chemistry*; D009682:Magnetic Resonance Spectroscopy / Q000379:methods*; D008280:Magnetics; D015394:Molecular Structure; D009942:Organometallic Compounds / Q000737:chemistry*; D015020:Yttrium Isotopes / Q000737:chemistry
chemical_list: D006573:Heterocyclic Compounds, 1-Ring; D009942:Organometallic Compounds; D015020:Yttrium Isotopes; C071349:1,4,7,10-tetraazacyclododecane- 1,4,7,10-tetraacetic acid