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Theoretical description of hyperpolarization formation in the SABRE-relay method

Knecht, Stephan ; Barskiy, Danila A. ; Buntkowsky, Gerd ; Ivanov, Konstantin L. (2023)
Theoretical description of hyperpolarization formation in the SABRE-relay method.
In: The Journal of Chemical Physics, 2020, 153 (16)
doi: 10.26083/tuprints-00024228
Article, Secondary publication, Publisher's Version

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Item Type: Article
Type of entry: Secondary publication
Title: Theoretical description of hyperpolarization formation in the SABRE-relay method
Language: English
Date: 17 July 2023
Place of Publication: Darmstadt
Year of primary publication: 2020
Publisher: American Institute of Physics
Journal or Publication Title: The Journal of Chemical Physics
Volume of the journal: 153
Issue Number: 16
Collation: 11 Seiten
DOI: 10.26083/tuprints-00024228
Corresponding Links:
Origin: Secondary publication service

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.

Uncontrolled Keywords: Polarization, Exchange reactions, Chemical kinetics and dynamics, Density-matrix, Nuclear magnetic resonance
Identification Number: 164106 (2020)
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-242287
Classification DDC: 500 Science and mathematics > 530 Physics
500 Science and mathematics > 540 Chemistry
Divisions: 07 Department of Chemistry > Eduard Zintl-Institut > Physical Chemistry
Date Deposited: 17 Jul 2023 08:28
Last Modified: 05 Oct 2023 10:12
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/24228
PPN: 512013640
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