Research output: Contribution to journal › Article › peer-review
Quantitative quantum mechanical approach to SABRE hyperpolarization at high magnetic fields. / Knecht, Stephan; Ivanov, Konstantin L.
In: Journal of Chemical Physics, Vol. 150, No. 12, 124106, 28.03.2019.Research output: Contribution to journal › Article › peer-review
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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 -
ID: 19029192