TY - JOUR

T1 - Quantitative quantum mechanical approach to SABRE hyperpolarization at high magnetic fields

AU - Knecht, Stephan

AU - Ivanov, Konstantin L.

PY - 2019/3/28

Y1 - 2019/3/28

N2 - A theoretical approach is proposed for quantitative modeling of SABRE (Signal Amplification by Reversible Exchange) experiments performed using an NMR spectrometer at a high magnetic field. SABRE is a method that exploits the spin order of parahydrogen (the H 2 molecule in its nuclear singlet state) for hyper-polarizing the spins of various substrates to enhance their NMR signals. An important feature of SABRE is that the substrate is not modified chemically; instead, spin order transfer takes place in a transient complex with parahydrogen. In high-field SABRE experiments, such a transfer is achieved by using suitable NMR excitation schemes. The approach presented here can explicitly treat the spin dynamics in the SABRE complex as well as the kinetics of substrate exchange (between the free and bound form) and complex interplay of spin evolution and chemical processes. One more important effect included in the model is the alteration of the spin state of parahydrogen giving rise to the formation of anti-phase spin order from the initial singlet order. Such a treatment enables a detailed analysis of known high-field SABRE schemes, quantitative comparison with experiments, and elucidation of the key factors that limit the resulting NMR signal enhancement.

AB - A theoretical approach is proposed for quantitative modeling of SABRE (Signal Amplification by Reversible Exchange) experiments performed using an NMR spectrometer at a high magnetic field. SABRE is a method that exploits the spin order of parahydrogen (the H 2 molecule in its nuclear singlet state) for hyper-polarizing the spins of various substrates to enhance their NMR signals. An important feature of SABRE is that the substrate is not modified chemically; instead, spin order transfer takes place in a transient complex with parahydrogen. In high-field SABRE experiments, such a transfer is achieved by using suitable NMR excitation schemes. The approach presented here can explicitly treat the spin dynamics in the SABRE complex as well as the kinetics of substrate exchange (between the free and bound form) and complex interplay of spin evolution and chemical processes. One more important effect included in the model is the alteration of the spin state of parahydrogen giving rise to the formation of anti-phase spin order from the initial singlet order. Such a treatment enables a detailed analysis of known high-field SABRE schemes, quantitative comparison with experiments, and elucidation of the key factors that limit the resulting NMR signal enhancement.

KW - PARAHYDROGEN INDUCED POLARIZATION

KW - PARA-HYDROGEN

KW - N-15 HYPERPOLARIZATION

KW - NMR-SPECTROSCOPY

KW - TRACE ANALYSIS

KW - MIXTURES

KW - KINETICS

KW - ENHANCEMENT

UR - http://www.scopus.com/inward/record.url?scp=85063484533&partnerID=8YFLogxK

U2 - 10.1063/1.5084129

DO - 10.1063/1.5084129

M3 - Article

C2 - 30927897

AN - SCOPUS:85063484533

VL - 150

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 12

M1 - 124106

ER -