Interstrand Charge Transport within Metallo-DNA: the Effect Due to Hg(II)- and Ag(I)-Mediated Base Pairs

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F20%3A00524100" target="_blank" >RIV/61388963:_____/20:00524100 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61388971:_____/20:00524100 RIV/00216208:11320/20:10414564

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acs.jpcc.9b12020" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.jpcc.9b12020</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcc.9b12020" target="_blank" >10.1021/acs.jpcc.9b12020</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Interstrand Charge Transport within Metallo-DNA: the Effect Due to Hg(II)- and Ag(I)-Mediated Base Pairs

Popis výsledku v původním jazyce

Metallo-DNA is considered promising in regard to functional molecular electronic elements. From this perspective, the longitudinal charge transport within metallo-DNA is usually studied. By contrast, this work was aimed at the transversal conductance of metallo-DNA, particularly at the effect of Hg and Ag metals on the conductance of base pairs. The charge transport through metal-mediated base pairs involving Hg(II) and Ag(I) metals, deoxythymidine (T) and 4-deoxythiothymidine (Ts), was studied by means of density functional theory (DFT) calculations employing the non-equilibrium Green's function (NEGF) method and electronic coupling calculations. The calculations showed that the conductance along the base-to-base charge transport pathway was significantly enhanced mainly due to the Hg(II)-mediated linkage. This work further showed that not only the metals within the metallo-base pair but also the substitution of the O4 atom in deoxythymidine by sulfur (the Ts nucleoside) enhanced molecular conductance as in the case of Ts-Ag(I)(2)-Ts. The bias charge transport for T-Ag(I)(2)-T was less effective than the transport for a TT mismatched base pair. The Ag orbitals participated in the highest occupied molecular orbital (HOMO) of T-Ag(I)(2)-T and Ts-Ag(I)(2)-Ts in contrast to negligible participation of Hg orbitals in the HOMO of T-Hg(II)-T. Therefore, a Coulomb blockade effect can be assumed particularly for Ag-mediated base pairs as was apparent from the plateau obtained for the calculated I/V dependencies. The Ag-mediated base pairs can, thus, be potentially utilized as molecular transistors. In addition, the metallo-base pairs anchored to gold electrodes mediated by sulfur preferred hole transport against the electron transport mechanism. This work highlighted the importance of electronic compatibility between the organic DNA scaffold and a particular metal that is essential for effective charge transport through metallo-base pairs (M-base pairs).

Název v anglickém jazyce

Interstrand Charge Transport within Metallo-DNA: the Effect Due to Hg(II)- and Ag(I)-Mediated Base Pairs

Popis výsledku anglicky

Metallo-DNA is considered promising in regard to functional molecular electronic elements. From this perspective, the longitudinal charge transport within metallo-DNA is usually studied. By contrast, this work was aimed at the transversal conductance of metallo-DNA, particularly at the effect of Hg and Ag metals on the conductance of base pairs. The charge transport through metal-mediated base pairs involving Hg(II) and Ag(I) metals, deoxythymidine (T) and 4-deoxythiothymidine (Ts), was studied by means of density functional theory (DFT) calculations employing the non-equilibrium Green's function (NEGF) method and electronic coupling calculations. The calculations showed that the conductance along the base-to-base charge transport pathway was significantly enhanced mainly due to the Hg(II)-mediated linkage. This work further showed that not only the metals within the metallo-base pair but also the substitution of the O4 atom in deoxythymidine by sulfur (the Ts nucleoside) enhanced molecular conductance as in the case of Ts-Ag(I)(2)-Ts. The bias charge transport for T-Ag(I)(2)-T was less effective than the transport for a TT mismatched base pair. The Ag orbitals participated in the highest occupied molecular orbital (HOMO) of T-Ag(I)(2)-T and Ts-Ag(I)(2)-Ts in contrast to negligible participation of Hg orbitals in the HOMO of T-Hg(II)-T. Therefore, a Coulomb blockade effect can be assumed particularly for Ag-mediated base pairs as was apparent from the plateau obtained for the calculated I/V dependencies. The Ag-mediated base pairs can, thus, be potentially utilized as molecular transistors. In addition, the metallo-base pairs anchored to gold electrodes mediated by sulfur preferred hole transport against the electron transport mechanism. This work highlighted the importance of electronic compatibility between the organic DNA scaffold and a particular metal that is essential for effective charge transport through metallo-base pairs (M-base pairs).

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA18-14990S" target="_blank" >GA18-14990S: Páry bazí s vazbou zprostředkovanou kovem; modifikace DNA pro budoucí aplikace v molekulární elektronice</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2020

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Physical Chemistry C

ISSN

1932-7447

e-ISSN

—

Svazek periodika

124

Číslo periodika v rámci svazku

13

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

7477-7486

Kód UT WoS článku

000526328500052

EID výsledku v databázi Scopus

2-s2.0-85083742873