Gadolinium Effect at High-Magnetic-Field DNP: 70% 13C Polarization of [U-13C] Glucose Using Trityl

Andrea Capozzi*, Saket Patel, W. Thomas Wenckebach, Magnus Karlsson, Mathilde H. Lerche, Jan Henrik Ardenkjær-Larsen

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

We show that the trityl electron spin resonance (ESR) features, crucial for an efficient dynamic nuclear polarization (DNP) process, are sample-composition-dependent. Working at 6.7 T and 1.1 K with a generally applicable DNP sample solvent mixture such as water/glycerol plus trityl, the addition of Gd3+ leads to a dramatic increase in [U-13C] glucose polarization from 37 ± 4% to 69 ± 3%. This is the highest value reported to date and is comparable to what can be achieved on pyruvic acid. Moreover, performing ESR measurements under actual DNP conditions, we provide experimental evidence that gadolinium doping not only shortens the trityl electron spin-lattice relaxation time but also modifies the radical g-tensor. The latter yielded a considerable narrowing of the ESR spectrum line width. Finally, in the frame of the spin temperature theory, we discuss how these two phenomena affect the DNP performance.
Original languageEnglish
JournalJournal of Physical Chemistry Letters
Volume10
Pages (from-to)3420-3425
ISSN1948-7185
DOIs
Publication statusPublished - 2019

Cite this

@article{4f06943331f24b789181d7c98140e1af,
title = "Gadolinium Effect at High-Magnetic-Field DNP: 70{\%} 13C Polarization of [U-13C] Glucose Using Trityl",
abstract = "We show that the trityl electron spin resonance (ESR) features, crucial for an efficient dynamic nuclear polarization (DNP) process, are sample-composition-dependent. Working at 6.7 T and 1.1 K with a generally applicable DNP sample solvent mixture such as water/glycerol plus trityl, the addition of Gd3+ leads to a dramatic increase in [U-13C] glucose polarization from 37 ± 4{\%} to 69 ± 3{\%}. This is the highest value reported to date and is comparable to what can be achieved on pyruvic acid. Moreover, performing ESR measurements under actual DNP conditions, we provide experimental evidence that gadolinium doping not only shortens the trityl electron spin-lattice relaxation time but also modifies the radical g-tensor. The latter yielded a considerable narrowing of the ESR spectrum line width. Finally, in the frame of the spin temperature theory, we discuss how these two phenomena affect the DNP performance.",
author = "Andrea Capozzi and Saket Patel and Wenckebach, {W. Thomas} and Magnus Karlsson and Lerche, {Mathilde H.} and Ardenkj{\ae}r-Larsen, {Jan Henrik}",
year = "2019",
doi = "10.1021/acs.jpclett.9b01306",
language = "English",
volume = "10",
pages = "3420--3425",
journal = "The Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",

}

TY - JOUR

T1 - Gadolinium Effect at High-Magnetic-Field DNP: 70% 13C Polarization of [U-13C] Glucose Using Trityl

AU - Capozzi, Andrea

AU - Patel, Saket

AU - Wenckebach, W. Thomas

AU - Karlsson, Magnus

AU - Lerche, Mathilde H.

AU - Ardenkjær-Larsen, Jan Henrik

PY - 2019

Y1 - 2019

N2 - We show that the trityl electron spin resonance (ESR) features, crucial for an efficient dynamic nuclear polarization (DNP) process, are sample-composition-dependent. Working at 6.7 T and 1.1 K with a generally applicable DNP sample solvent mixture such as water/glycerol plus trityl, the addition of Gd3+ leads to a dramatic increase in [U-13C] glucose polarization from 37 ± 4% to 69 ± 3%. This is the highest value reported to date and is comparable to what can be achieved on pyruvic acid. Moreover, performing ESR measurements under actual DNP conditions, we provide experimental evidence that gadolinium doping not only shortens the trityl electron spin-lattice relaxation time but also modifies the radical g-tensor. The latter yielded a considerable narrowing of the ESR spectrum line width. Finally, in the frame of the spin temperature theory, we discuss how these two phenomena affect the DNP performance.

AB - We show that the trityl electron spin resonance (ESR) features, crucial for an efficient dynamic nuclear polarization (DNP) process, are sample-composition-dependent. Working at 6.7 T and 1.1 K with a generally applicable DNP sample solvent mixture such as water/glycerol plus trityl, the addition of Gd3+ leads to a dramatic increase in [U-13C] glucose polarization from 37 ± 4% to 69 ± 3%. This is the highest value reported to date and is comparable to what can be achieved on pyruvic acid. Moreover, performing ESR measurements under actual DNP conditions, we provide experimental evidence that gadolinium doping not only shortens the trityl electron spin-lattice relaxation time but also modifies the radical g-tensor. The latter yielded a considerable narrowing of the ESR spectrum line width. Finally, in the frame of the spin temperature theory, we discuss how these two phenomena affect the DNP performance.

U2 - 10.1021/acs.jpclett.9b01306

DO - 10.1021/acs.jpclett.9b01306

M3 - Journal article

C2 - 31181932

VL - 10

SP - 3420

EP - 3425

JO - The Journal of Physical Chemistry Letters

JF - The Journal of Physical Chemistry Letters

SN - 1948-7185

ER -