Precise distance measurements in DNA G-quadruplex dimers and sandwich complexes by pulsed dipolar EPR spectroscopy
| dc.contributor.author | Stratmann, Lukas M. | |
| dc.contributor.author | Kutin, Yury | |
| dc.contributor.author | Kasanmascheff, Müge | |
| dc.contributor.author | Clever, Guido H. | |
| dc.date.accessioned | 2021-07-14T15:27:27Z | |
| dc.date.available | 2021-07-14T15:27:27Z | |
| dc.date.issued | 2020-10-16 | |
| dc.description.abstract | DNA G-quadruplexes show a pronounced tendency to form higher-order structures, such as π-stacked dimers and aggregates with aromatic binding partners. Reliable methods for determining the structure of these non-covalent adducts are scarce. Here, we use artificial square-planar Cu(pyridine)4 complexes, covalently incorporated into tetramolecular G-quadruplexes, as rigid spin labels for detecting dimeric structures and measuring intermolecular Cu2+–Cu2+ distances via pulsed dipolar EPR spectroscopy. A series of G-quadruplex dimers of different spatial dimensions, formed in tail-to-tail or head-to-head stacking mode, were unambiguously distinguished. Measured distances are in full agreement with results of molecular dynamics simulations. Furthermore, intercalation of two well-known G-quadruplex binders, PIPER and telomestatin, into G-quadruplex dimers resulting in sandwich complexes was investigated, and previously unknown binding modes were discovered. Additionally, we present evidence that free G-tetrads also intercalate into dimers. Our transition metal labeling approach, combined with pulsed EPR spectroscopy, opens new possibilities for examining structures of non-covalent DNA aggregates. | en |
| dc.identifier.uri | http://hdl.handle.net/2003/40311 | |
| dc.identifier.uri | http://dx.doi.org/10.17877/DE290R-22186 | |
| dc.language.iso | en | de |
| dc.relation.ispartofseries | Angewandte chemie international edition;Vol. 60. 2021, Issue 9, 4939-4947 | |
| dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | |
| dc.subject | DNA | de |
| dc.subject | G-quadruplexes | en |
| dc.subject | Metal base-pairing | en |
| dc.subject | p-stacking | en |
| dc.subject | EPR spectroscopy | en |
| dc.subject.ddc | 540 | |
| dc.title | Precise distance measurements in DNA G-quadruplex dimers and sandwich complexes by pulsed dipolar EPR spectroscopy | en |
| dc.type | Text | de |
| dc.type.publicationtype | article | de |
| dcterms.accessRights | open access | |
| eldorado.secondarypublication | true | de |
| eldorado.secondarypublication.primarycitation | Angewandte chemie international edition. Vol. 60. 2021, Issue 9, 4939-4947 | de |
| eldorado.secondarypublication.primaryidentifier | 10.1002/anie.202008618 | de |