Hyperpolarized (hp)3He and 129 Xe (both nuclear spin I = 1/2), produced by alkali metal vapor spin-exchange optical pumping (SEOP), [1] enable a wide variety of unique nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) applications.[ Xe, the noble gas isotope 83 Kr (I = 9/2) can be hyperpolarized by SEOP [5,6] and thus far has yielded MR signals that are three or more orders of magnitude above those of thermally polarized krypton. [7, 8] 83 Kr differs from 3 He and 129 Xe in that its longitudinal relaxation is usually dominated by quadrupolar interactions caused by distortions to the spherical symmetry of its electric environment. [9][10][11] These interactions reduce the lifetime of the hp state and, to some extent, limit the nonequilibrium polarization. However, quadrupolar relaxation is also responsible for the sensitivity hp 83 Kr displays toward surface-to-volume ratio, [12] surface temperature, [7] and surface chemistry. [8,12] This sensitivity can be harnessed to produce T 1 contrast in gas-phase MRI, [13,14] making 83 Kr a promising agent for materials science and biomedical applications. Thus an increased understanding of the factors that contribute to the relaxation of 83 Kr could lead to improved SEOP and the development of novel surface characterization techniques.The 83 Kr longitudinal relaxation rate is known to increase linearly with gas density, [11] but an additional density-independent component was recently observed.[8] Herein, we describe investigations of this density-independent contribution by studying 83 Kr relaxation as a function of krypton density, gas composition, and surface chemistry (i.e. in either an untreated or a siliconized Pyrex detection cell) in twelve different krypton-containing gas mixtures. The krypton content in these krypton-helium and krypton-nitrogen mixtures was varied from 10 to 100 %, and the total gas density was varied from 1 to 10 amagat. (An amagat is the number density of an ideal gas at 101.325 kPa and 273.15 K and is equal to 2.6868 10 25 m
À3.) The resulting T 1 values ranged from 40 s to more than 400 s, depending on gas composition and pressure. Although these times are longer than those of most molecular species, [15,16] they are much shorter than the T 1 values of 129 Xe, which can reach 27 h in dilute mixtures [17] or 3 He, which displays T 1 values of hundred of hours in the absence of paramagnetic species.[18] An advantage of these shorter 83 Kr relaxation times is that more rapid data collection becomes possible compared to NMR data collection for noble gas isotopes with spin I = 1/2. In total, this work comprises more than 700 individual relaxation measurements.Experiments were performed on a Chemagnetics CMX II 400 NMR spectrometer in a 9.4 T, wide-bore (89 mm) superconducting magnet using a custom-built probe tuned to the 15.4 MHz 83 Kr resonance frequency. SEOP was performed as previously described [7] using research grade gases (Airgas, Radnor, PA) and natural abundance krypton (11.5 % 83 Kr). Following a SEOP period of ...