Spin dynamics of [1,2- 13 C 2 ]pyruvate hyperpolarization by parahydrogen in reversible exchange at micro Tesla fields
Spin dynamics of [1,2- 13 C 2 ]pyruvate hyperpolarization by parahydrogen in reversible exchange at micro Tesla fields
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微特斯拉场可逆交换中仲氢引起的[1,2- 13 C 2 ]丙酮酸超极化的自旋动力学
DOI：
10.1039/d3cp00843f
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发表时间：
2023
影响因子：
3.3
通讯作者：
Theis, Thomas
中科院分区：
文献类型：
--
作者：
Browning, Austin;Macculloch, Keilian;TomHon, Patrick;Mandzhieva, Iuliia;Chekmenev, Eduard Y.;Goodson, Boyd M.;Lehmkuhl, Sören;Theis, Thomas
13 C-丙酮酸通过可逆交换信号放大（SABRE）的超极化是最近的一个重要发现，因为超极化相对简单，并且丙酮酸作为生物分子探针用于体外或体内研究的中心生物相关性。本文从理论和实验上分析了[1，2 - 13 C2]双原子-SABRE自旋系统及其场依赖性。我们提供了第一性原理分析的管理4自旋二氢化物-13 C2的哈密顿量和数值自旋动力学模拟的7自旋二氢化物-13 C2-CH 3系统。的分析和数值计算结果进行了比较，匹配系统的实验。利用这些方法，我们揭示了在微特斯拉场下观察到的单重态和三重态的自旋态混合，并分析了从微特斯拉场转移到高场进行检测的动力学过程，以理解[1，2 - 13 C2]双原子-SABRE系统的光谱。
Hyperpolarization of 13C-pyruvate via Signal Amplificaton By Reversibble Exchange (SABRE) is an important recent discovery because of both the relative simplicity of hyperpolarization and the central biological relevance of pyruvate as a biomolecular probe for in vitro or in vivo studies. Here, we analyze the [1,2-13C2]pyruvate-SABRE spin system and its field dependence theoretically and experimentally. We provide first-principles analysis of the governing 4-spin dihydride-13C2 Hamiltonian and numerical spin dynamics simulations of the 7-spin dihydride-13C2–CH3 system. The analytical and the numerical results are compared to matching systematic experiments. With these methods we unravel the observed spin state mixing of singlet states and triplet states at microTesla fields and we also analyze the dynamics during transfer from micro-Tesla field to high field for detection to understand the resulting spectra from the [1,2-13C2]pyruvate-SABRE system.