Using paramagnetism to slow down nuclear relaxation in protein
NMR
Using paramagnetism to slow down nuclear relaxation in protein
NMR
Paramagnetic metal ions accelerate nuclear spin relaxation; this effect is widely used for distance measurement and called paramagnetic relaxation enhancement (PRE). Theoretical predictions established that, under special circumstances, it is also possible to achieve a reduction in nuclear relaxation rates (negative PRE). This situation would occur if the mechanism of nuclear relaxation in the diamagnetic state is counterbalanced by a paramagnetic relaxation mechanism caused by the metal ion. Here we report the first experimental evidence for such a cross-correlation effect. Using a uniformly 15N-labeled mutant of calbindin D9k loaded with either Tm3+ or Tb3+, reduced R1 and R2 relaxation rates of backbone 15N spins were observed compared with the diamagnetic reference (the same protein loaded with Y3+). The effect arises from the compensation of the chemical shift anisotropy tensor by the anisotropic dipolar shielding generated by the unpaired electron spin.
4815-4818
Orton, Henry W.
525b435e-b74d-4ca7-8edc-86b911d5a340
Kuprov, Ilya
bb07f28a-5038-4524-8146-e3fc8344c065
Loh, Choy-Theng
4398b090-e294-48a2-850f-fc97be0f5c2c
Otting, Gottfried
cbeb327f-5bfd-454e-b20c-1ccb1ae2fb3a
1 December 2016
Orton, Henry W.
525b435e-b74d-4ca7-8edc-86b911d5a340
Kuprov, Ilya
bb07f28a-5038-4524-8146-e3fc8344c065
Loh, Choy-Theng
4398b090-e294-48a2-850f-fc97be0f5c2c
Otting, Gottfried
cbeb327f-5bfd-454e-b20c-1ccb1ae2fb3a
Orton, Henry W., Kuprov, Ilya, Loh, Choy-Theng and Otting, Gottfried
(2016)
Using paramagnetism to slow down nuclear relaxation in protein
NMR.
The Journal of Physical Chemistry Letters, 7 (23), .
(doi:10.1021/acs.jpclett.6b02417).
Abstract
Paramagnetic metal ions accelerate nuclear spin relaxation; this effect is widely used for distance measurement and called paramagnetic relaxation enhancement (PRE). Theoretical predictions established that, under special circumstances, it is also possible to achieve a reduction in nuclear relaxation rates (negative PRE). This situation would occur if the mechanism of nuclear relaxation in the diamagnetic state is counterbalanced by a paramagnetic relaxation mechanism caused by the metal ion. Here we report the first experimental evidence for such a cross-correlation effect. Using a uniformly 15N-labeled mutant of calbindin D9k loaded with either Tm3+ or Tb3+, reduced R1 and R2 relaxation rates of backbone 15N spins were observed compared with the diamagnetic reference (the same protein loaded with Y3+). The effect arises from the compensation of the chemical shift anisotropy tensor by the anisotropic dipolar shielding generated by the unpaired electron spin.
Text
s1-ln2259534-2048588417-1939656818Hwf-515887740IdV-19536911012259534PDF_....pdf
- Accepted Manuscript
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15Nxcorr_supp6.pdf
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Accepted/In Press date: 9 November 2016
e-pub ahead of print date: 9 November 2016
Published date: 1 December 2016
Organisations:
Faculty of Natural and Environmental Sciences
Identifiers
Local EPrints ID: 405553
URI: http://eprints.soton.ac.uk/id/eprint/405553
ISSN: 1948-7185
PURE UUID: 53c2b6e3-8c01-4f37-bfc7-d23d2e9b9357
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Date deposited: 07 Feb 2017 15:33
Last modified: 16 Mar 2024 04:11
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Contributors
Author:
Henry W. Orton
Author:
Choy-Theng Loh
Author:
Gottfried Otting
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