Longitudinal relaxation in dipole-coupled homonuclear three-spin systems: Distinct correlations and odd spectral densities.
(2015) In Journal of Chemical Physics 143(23).- Abstract
- A system of three dipole-coupled spins exhibits a surprisingly intricate relaxation behavior. Following Hubbard's pioneering 1958 study, many authors have investigated different aspects of this problem. Nevertheless, on revisiting this classic relaxation problem, we obtain several new results, some of which are at variance with conventional wisdom. Most notably from a fundamental point of view, we find that the odd-valued spectral density function influences longitudinal relaxation. We also show that the effective longitudinal relaxation rate for a non-isochronous three-spin system can exhibit an unusual inverted dispersion step. To clarify these and other issues, we present a comprehensive theoretical treatment of longitudinal relaxation... (More)
- A system of three dipole-coupled spins exhibits a surprisingly intricate relaxation behavior. Following Hubbard's pioneering 1958 study, many authors have investigated different aspects of this problem. Nevertheless, on revisiting this classic relaxation problem, we obtain several new results, some of which are at variance with conventional wisdom. Most notably from a fundamental point of view, we find that the odd-valued spectral density function influences longitudinal relaxation. We also show that the effective longitudinal relaxation rate for a non-isochronous three-spin system can exhibit an unusual inverted dispersion step. To clarify these and other issues, we present a comprehensive theoretical treatment of longitudinal relaxation in a three-spin system of arbitrary geometry and with arbitrary rotational dynamics. By using the Liouville-space formulation of Bloch-Wangsness-Redfield theory and a basis of irreducible spherical tensor operators, we show that the number of relaxation components in the different cases can be deduced from symmetry arguments. For the isochronous case, we present the relaxation matrix in analytical form, whereas, for the non-isochronous case, we employ a computationally efficient approach based on the stochastic Liouville equation. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/8503875
- author
- Chang, Zhiwei LU and Halle, Bertil LU
- organization
- publishing date
- 2015
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Chemical Physics
- volume
- 143
- issue
- 23
- article number
- 234201
- publisher
- American Institute of Physics (AIP)
- external identifiers
-
- pmid:26696052
- scopus:84951165691
- wos:000369806500015
- pmid:26696052
- ISSN
- 0021-9606
- DOI
- 10.1063/1.4937377
- language
- English
- LU publication?
- yes
- id
- 9fd58d78-b70c-479a-81fe-a9e8c25106a5 (old id 8503875)
- date added to LUP
- 2016-04-01 11:14:30
- date last changed
- 2022-03-12 20:55:00
@article{9fd58d78-b70c-479a-81fe-a9e8c25106a5, abstract = {{A system of three dipole-coupled spins exhibits a surprisingly intricate relaxation behavior. Following Hubbard's pioneering 1958 study, many authors have investigated different aspects of this problem. Nevertheless, on revisiting this classic relaxation problem, we obtain several new results, some of which are at variance with conventional wisdom. Most notably from a fundamental point of view, we find that the odd-valued spectral density function influences longitudinal relaxation. We also show that the effective longitudinal relaxation rate for a non-isochronous three-spin system can exhibit an unusual inverted dispersion step. To clarify these and other issues, we present a comprehensive theoretical treatment of longitudinal relaxation in a three-spin system of arbitrary geometry and with arbitrary rotational dynamics. By using the Liouville-space formulation of Bloch-Wangsness-Redfield theory and a basis of irreducible spherical tensor operators, we show that the number of relaxation components in the different cases can be deduced from symmetry arguments. For the isochronous case, we present the relaxation matrix in analytical form, whereas, for the non-isochronous case, we employ a computationally efficient approach based on the stochastic Liouville equation.}}, author = {{Chang, Zhiwei and Halle, Bertil}}, issn = {{0021-9606}}, language = {{eng}}, number = {{23}}, publisher = {{American Institute of Physics (AIP)}}, series = {{Journal of Chemical Physics}}, title = {{Longitudinal relaxation in dipole-coupled homonuclear three-spin systems: Distinct correlations and odd spectral densities.}}, url = {{http://dx.doi.org/10.1063/1.4937377}}, doi = {{10.1063/1.4937377}}, volume = {{143}}, year = {{2015}}, }