Research output: Contribution to journal › Article › peer-review
Theoretical description of hyperpolarization formation in the SABRE-relay method. / Knecht, Stephan; Barskiy, Danila A.; Buntkowsky, Gerd et al.
In: Journal of Chemical Physics, Vol. 153, No. 16, 164106, 28.10.2020, p. 164106.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Theoretical description of hyperpolarization formation in the SABRE-relay method
AU - Knecht, Stephan
AU - Barskiy, Danila A.
AU - Buntkowsky, Gerd
AU - Ivanov, Konstantin L.
N1 - Funding Information: K.L.I. acknowledges support from the Russian Science Foundation (Project No. 19-43-04116), and G.B. acknowledges financial support from the Deutsche Forschungsgemeinschaft under Contract No. Bu-911-29-1. Publisher Copyright: © 2020 Author(s). Copyright: Copyright 2020 Elsevier B.V., All rights reserved.
PY - 2020/10/28
Y1 - 2020/10/28
N2 - SABRE (Signal Amplification By Reversible Exchange) has become a widely used method for hyper-polarizing nuclear spins, thereby enhancing their Nuclear Magnetic Resonance (NMR) signals by orders of magnitude. In SABRE experiments, the non-equilibrium spin order is transferred from parahydrogen to a substrate in a transient organometallic complex. The applicability of SABRE is expanded by the methodology of SABRE-relay in which polarization can be relayed to a second substrate either by direct chemical exchange of hyperpolarized nuclei or by polarization transfer between two substrates in a second organometallic complex. To understand the mechanism of the polarization transfer and study the transfer efficiency, we propose a theoretical approach to SABRE-relay, which can treat both spin dynamics and chemical kinetics as well as the interplay between them. The approach is based on a set of equations for the spin density matrices of the spin systems involved (i.e., SABRE substrates and complexes), which can be solved numerically. Using this method, we perform a detailed study of polarization formation and analyze in detail the dependence of the attainable polarization level on various chemical kinetic and spin dynamic parameters. We foresee the applications of the present approach for optimizing SABRE-relay experiments with the ultimate goal of achieving maximal NMR signal enhancements for substrates of interest.
AB - SABRE (Signal Amplification By Reversible Exchange) has become a widely used method for hyper-polarizing nuclear spins, thereby enhancing their Nuclear Magnetic Resonance (NMR) signals by orders of magnitude. In SABRE experiments, the non-equilibrium spin order is transferred from parahydrogen to a substrate in a transient organometallic complex. The applicability of SABRE is expanded by the methodology of SABRE-relay in which polarization can be relayed to a second substrate either by direct chemical exchange of hyperpolarized nuclei or by polarization transfer between two substrates in a second organometallic complex. To understand the mechanism of the polarization transfer and study the transfer efficiency, we propose a theoretical approach to SABRE-relay, which can treat both spin dynamics and chemical kinetics as well as the interplay between them. The approach is based on a set of equations for the spin density matrices of the spin systems involved (i.e., SABRE substrates and complexes), which can be solved numerically. Using this method, we perform a detailed study of polarization formation and analyze in detail the dependence of the attainable polarization level on various chemical kinetic and spin dynamic parameters. We foresee the applications of the present approach for optimizing SABRE-relay experiments with the ultimate goal of achieving maximal NMR signal enhancements for substrates of interest.
KW - HYDROGEN INDUCED POLARIZATION
KW - DISSOCIATION REACTION STAGES
KW - INTEGRAL ENCOUNTER THEORY
KW - REVERSIBLE EXCHANGE
KW - N-15 HYPERPOLARIZATION
KW - HIGH-FIELD
KW - SPIN HYPERPOLARIZATION
KW - SIGNAL AMPLIFICATION
KW - MULTISTAGE REACTIONS
KW - NMR
UR - http://www.scopus.com/inward/record.url?scp=85094808323&partnerID=8YFLogxK
U2 - 10.1063/5.0023308
DO - 10.1063/5.0023308
M3 - Article
C2 - 33138423
AN - SCOPUS:85094808323
VL - 153
SP - 164106
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 16
M1 - 164106
ER -
ID: 25992473