Multi-Gaussian Monte Carlo Analysis of PELDOR Data in the Frequency Domain

Multi-Gaussian Monte Carlo Analysis of PELDOR Data in the Frequency Domain Научная публикация

Журнал

Zeitschrift fur Physikalische Chemie
ISSN: 0942-9352

Вых. Данные

Год: 2017, Том: 231, Номер: 3, Страницы: 671-688 Страниц : 18 DOI: 10.1515/zpch-2016-0830

Ключевые слова

biradicals; DEER; DNA; Fredholm equation regularization; Monte Carlo fitting; peptide antibiotics; RNA; spin labels; Trolox

Авторы

Matveeva Anna G. ^1,2 , Yushkova Yulia V. ³ , Morozov Sergei V. ^2,3 , Grygor'ev Igor A. ³ , Dzuba Sergei A. ^1,2

Организации

1	(Данные Web of science) Voevodsky Inst Chem Kinet & Combust, Novosibirsk 630090, Russia
2	(Данные Web of science) Novosibirsk State Univ, Novosibirsk 630090, Russia
3	(Данные Web of science) Vorozhtsov Novosibirsk Inst Organ Chem, Novosibirsk 630090, Russia

Pulsed double electron-electron resonance technique (PELDOR or DEER) is often applied to study conformations and aggregation of spin-labelled macromolecules. Because of the ill-posed nature of the integral equation determining the distance distribution function, a regularization procedure is required to restrict the smoothness of the solution. In this work, we performed PELDOR measurements for new flexible nitroxide biradicals based on trolox, which is the synthetic analogue of a-tocopherol; spin-labelled trolox derivatives are investigated as potential anti-cancer drugs. We use regularization by an approximation of the solution with a sum of limited number of Gaussians, by varying their positions, widths and amplitudes. Their best-fitted values were found by a completely random Monte Carlo process. The use of the frequency-domain PELDOR data allowed diminution of the artifacts induced by spin-spin electron-nuclear and intermolecular electron-electron interactions. It was found that for the all biradicals studied, the use of three Gaussians was enough for good agreement with the experiments. The number of trials for obtaining satisfactory result was found to be quite reasonable, which is explained by presence of the singularity in the core of integral equation. The maxima of inter-spin distance distribution for different biradicals were found to vary between 1.5 and 2.3 nm, depending on the linkers between the Trolox core and nitroxides. The distance distributions around these positions reflect flexibility of the biradicals.

Matveeva A.G. , Yushkova Y.V. , Morozov S.V. , Grygor'ev I.A. , Dzuba S.A.
Multi-Gaussian Monte Carlo Analysis of PELDOR Data in the Frequency Domain
Zeitschrift fur Physikalische Chemie. 2017. V.231. N3. P.671-688. DOI: 10.1515/zpch-2016-0830 WOS Scopus РИНЦ

Опубликована online:	26 окт. 2016 г.
Опубликована в печати:	1 янв. 2017 г.

Web of science	WOS:000393583200018
Scopus	2-s2.0-85012285843
РИНЦ	29480541
OpenAlex	W2542358108