A Versatile Approach to Attachment of Triarylmethyl Labels to DNA for Nanoscale Structural EPR Studies at Physiological Temperatures

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A Versatile Approach to Attachment of Triarylmethyl Labels to DNA for Nanoscale Structural EPR Studies at Physiological Temperatures. / Shevelev, Georgiy Yu; Gulyak, Evgeny L.; Lomzov, Alexander A. et al.

In: Journal of Physical Chemistry B, Vol. 122, No. 1, 11.01.2018, p. 137-143.

Research output: Contribution to journal › Article › peer-review

BibTeX

@article{a63905b852584015b9921cbe15dab560,

title = "A Versatile Approach to Attachment of Triarylmethyl Labels to DNA for Nanoscale Structural EPR Studies at Physiological Temperatures",

abstract = "Triarylmethyl (trityl, TAM) radicals are a promising class of spin labels for nanometer-scale distance measurements in biomolecules at physiological temperatures. However, to date, existing approaches to site-directed TAM labeling of DNA have been limited to label attachment at the termini of oligonucleotides, thus hindering a majority of demanded applications. Herein, we report a new versatile strategy for TAM attachment at arbitrary sites of nucleic acids. It utilizes an achiral non-nucleoside phosphoramidite monomer for automated solid-phase synthesis of oligonucleotides, which are then postsynthetically functionalized with TAM. We demonstrate a synthesis of a set of oligonucleotide complexes that are TAM-labeled at internal or terminal sites, as well as the possibility of measuring interspin distances up to ∼5-6 nm at 298 K using double quantum coherence electron paramagnetic resonance (EPR). Implementation of the developed approach strongly broadens the scope of nucleic acids and nucleoprotein complexes available for nanoscale structural EPR studies at room temperatures.",

keywords = "ELECTRON-PARAMAGNETIC-RESONANCE, NANOMETER DISTANCE MEASUREMENTS, SPIN LABELS, ROOM-TEMPERATURE, NUCLEIC-ACIDS, IN-VITRO, SPECTROSCOPY, RNA, RELAXATION, PROTEINS",

author = "Shevelev, {Georgiy Yu} and Gulyak, {Evgeny L.} and Lomzov, {Alexander A.} and Kuzhelev, {Andrey A.} and Krumkacheva, {Olesya A.} and Kupryushkin, {Maxim S.} and Tormyshev, {Victor M.} and Fedin, {Matvey V.} and Bagryanskaya, {Elena G.} and Pyshnyi, {Dmitrii V.}",

year = "2018",

month = jan,

day = "11",

doi = "10.1021/acs.jpcb.7b10689",

language = "English",

volume = "122",

pages = "137--143",

journal = "Journal of Physical Chemistry B",

issn = "1520-6106",

publisher = "American Chemical Society",

number = "1",

}

RIS

TY - JOUR

T1 - A Versatile Approach to Attachment of Triarylmethyl Labels to DNA for Nanoscale Structural EPR Studies at Physiological Temperatures

AU - Shevelev, Georgiy Yu

AU - Gulyak, Evgeny L.

AU - Lomzov, Alexander A.

AU - Kuzhelev, Andrey A.

AU - Krumkacheva, Olesya A.

AU - Kupryushkin, Maxim S.

AU - Tormyshev, Victor M.

AU - Fedin, Matvey V.

AU - Bagryanskaya, Elena G.

AU - Pyshnyi, Dmitrii V.

PY - 2018/1/11

Y1 - 2018/1/11

N2 - Triarylmethyl (trityl, TAM) radicals are a promising class of spin labels for nanometer-scale distance measurements in biomolecules at physiological temperatures. However, to date, existing approaches to site-directed TAM labeling of DNA have been limited to label attachment at the termini of oligonucleotides, thus hindering a majority of demanded applications. Herein, we report a new versatile strategy for TAM attachment at arbitrary sites of nucleic acids. It utilizes an achiral non-nucleoside phosphoramidite monomer for automated solid-phase synthesis of oligonucleotides, which are then postsynthetically functionalized with TAM. We demonstrate a synthesis of a set of oligonucleotide complexes that are TAM-labeled at internal or terminal sites, as well as the possibility of measuring interspin distances up to ∼5-6 nm at 298 K using double quantum coherence electron paramagnetic resonance (EPR). Implementation of the developed approach strongly broadens the scope of nucleic acids and nucleoprotein complexes available for nanoscale structural EPR studies at room temperatures.

AB - Triarylmethyl (trityl, TAM) radicals are a promising class of spin labels for nanometer-scale distance measurements in biomolecules at physiological temperatures. However, to date, existing approaches to site-directed TAM labeling of DNA have been limited to label attachment at the termini of oligonucleotides, thus hindering a majority of demanded applications. Herein, we report a new versatile strategy for TAM attachment at arbitrary sites of nucleic acids. It utilizes an achiral non-nucleoside phosphoramidite monomer for automated solid-phase synthesis of oligonucleotides, which are then postsynthetically functionalized with TAM. We demonstrate a synthesis of a set of oligonucleotide complexes that are TAM-labeled at internal or terminal sites, as well as the possibility of measuring interspin distances up to ∼5-6 nm at 298 K using double quantum coherence electron paramagnetic resonance (EPR). Implementation of the developed approach strongly broadens the scope of nucleic acids and nucleoprotein complexes available for nanoscale structural EPR studies at room temperatures.

KW - ELECTRON-PARAMAGNETIC-RESONANCE

KW - NANOMETER DISTANCE MEASUREMENTS

KW - SPIN LABELS

KW - ROOM-TEMPERATURE

KW - NUCLEIC-ACIDS

KW - IN-VITRO

KW - SPECTROSCOPY

KW - RNA

KW - RELAXATION

KW - PROTEINS

UR - http://www.scopus.com/inward/record.url?scp=85040553706&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcb.7b10689

DO - 10.1021/acs.jpcb.7b10689

M3 - Article

C2 - 29206458

AN - SCOPUS:85040553706

VL - 122

SP - 137

EP - 143

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

SN - 1520-6106

IS - 1

ER -

ID: 9266270