Kozinenko, Vitaly P. ; Kiryutin, Alexey S. ; Knecht, Stephan ; Buntkowsky, Gerd ; Vieth, Hans-Martin ; Yurkovskaya, Alexandra V. ; Ivanov, Konstantin L. (2023)
Spin dynamics in experiments on orthodeuterium induced polarization (ODIP).
In: The Journal of Chemical Physics, 2020, 153 (11)
doi: 10.26083/tuprints-00024227
Artikel, Zweitveröffentlichung, Verlagsversion
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Kurzbeschreibung (Abstract)
A comprehensive description of the spin dynamics underlying the formation of Ortho-Deuterium Induced Polarization (ODIP) is presented. ODIP can serve as a tool for enhancing Nuclear Magnetic Resonance (NMR) signals of ²H nuclei, being important probes of molecular structure and dynamics. To produce ODIP, in the first step, the D₂ gas is brought to thermal equilibrium at low temperature, here 30 K, so that the ortho-component, corresponding to the total spin of the ²H nuclei equal to 0 and 2, is enriched, here to 92%. In the second step, the orthodeuterium molecule is attached to a substrate molecule using a suitable hydrogenation catalyst such that the symmetry of the two ²H nuclei is broken. As a result, the non-thermal spin order of orthodeuterium is converted into enhancement of observable NMR signals. In this work, we perform a theoretical study of ODIP and calculate the shape of ODIP spectra and their dependence on the magnetization flip angle. These results are compared with experiments performed for a number of substrates; good agreement between experimental and calculated ODIP spectra is found. We also discuss the performance of NMR techniques for converting anti-phase ODIP spectral patterns into in-phase patterns, which are more suitable for signal detection and for transferring ODIP to heteronuclei, here to ¹³C spins. Experimental procedures reported here allowed us to reach signal enhancement factors of more than 1000 for ²H nuclei in the liquid phase. These results are useful for extending the scope of spin hyperpolarization to the widely used ²H nuclei.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2023 |
| Autor(en): | Kozinenko, Vitaly P. ; Kiryutin, Alexey S. ; Knecht, Stephan ; Buntkowsky, Gerd ; Vieth, Hans-Martin ; Yurkovskaya, Alexandra V. ; Ivanov, Konstantin L. |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | Spin dynamics in experiments on orthodeuterium induced polarization (ODIP) |
| Sprache: | Englisch |
| Publikationsjahr: | 2023 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 2020 |
| Verlag: | American Institute of Physics |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | The Journal of Chemical Physics |
| Jahrgang/Volume einer Zeitschrift: | 153 |
| (Heft-)Nummer: | 11 |
| Kollation: | 13 Seiten |
| DOI: | 10.26083/tuprints-00024227 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/24227 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| Kurzbeschreibung (Abstract): | A comprehensive description of the spin dynamics underlying the formation of Ortho-Deuterium Induced Polarization (ODIP) is presented. ODIP can serve as a tool for enhancing Nuclear Magnetic Resonance (NMR) signals of ²H nuclei, being important probes of molecular structure and dynamics. To produce ODIP, in the first step, the D₂ gas is brought to thermal equilibrium at low temperature, here 30 K, so that the ortho-component, corresponding to the total spin of the ²H nuclei equal to 0 and 2, is enriched, here to 92%. In the second step, the orthodeuterium molecule is attached to a substrate molecule using a suitable hydrogenation catalyst such that the symmetry of the two ²H nuclei is broken. As a result, the non-thermal spin order of orthodeuterium is converted into enhancement of observable NMR signals. In this work, we perform a theoretical study of ODIP and calculate the shape of ODIP spectra and their dependence on the magnetization flip angle. These results are compared with experiments performed for a number of substrates; good agreement between experimental and calculated ODIP spectra is found. We also discuss the performance of NMR techniques for converting anti-phase ODIP spectral patterns into in-phase patterns, which are more suitable for signal detection and for transferring ODIP to heteronuclei, here to ¹³C spins. Experimental procedures reported here allowed us to reach signal enhancement factors of more than 1000 for ²H nuclei in the liquid phase. These results are useful for extending the scope of spin hyperpolarization to the widely used ²H nuclei. |
| Freie Schlagworte: | Nuclear magnetic resonance spectroscopy, Hydrogenation process, Density-matrix |
| ID-Nummer: | 114202 (2020) |
| Status: | Verlagsversion |
| URN: | urn:nbn:de:tuda-tuprints-242275 |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 530 Physik 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie |
| Hinterlegungsdatum: | 17 Jul 2023 08:30 |
| Letzte Änderung: | 02 Aug 2024 12:54 |
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- Spin dynamics in experiments on orthodeuterium induced polarization (ODIP). (deposited 17 Jul 2023 08:30) [Gegenwärtig angezeigt]
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