%0 Journal Article %1 WOS:000262607100031 %A Saraiva-Souza, Aldilene %A de Souza, Fabricio Macedo %A Aleixo, Vicente F P %A Girao, Eduardo Costa %A Filho, Josue Mendes %A Meunier, Vincent %A Sumpter, Bobby G %A Filho, Antonio Gomes Souza %A Nero, Jordan Del %C 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA %D 2008 %I AMER INST PHYSICS %J JOURNAL OF CHEMICAL PHYSICS %K Green's HF calculations; compounds; electric electronic electronics; fields; function initio methods; molecular organic rectification; rectifiers} states; {ab %N 20 %R 10.1063/1.3020353 %T A single molecule rectifier with strong push-pull coupling %V 129 %X We theoretically investigate the electronic charge transport in a molecular system composed of a donor group (dinitrobenzene) coupled to an acceptor group (dihydrophenazine) via a polyenic chain (unsaturated carbon bridge). Ab initio calculations based on the Hartree-Fock approximations are performed to investigate the distribution of electron states over the molecule in the presence of an external electric field. For small bridge lengths (n=0-3) we find a homogeneous distribution of the frontier molecular orbitals, while for n>3 a strong localization of the lowest unoccupied molecular orbital is found. The localized orbitals in between the donor and acceptor groups act as conduction channels when an external electric field is applied. We also calculate the rectification behavior of this system by evaluating the charge accumulated in the donor and acceptor groups as a function of the external electric field. Finally, we propose a phenomenological model based on nonequilibrium Green's function to rationalize the ab initio findings.

@article{WOS:000262607100031, abstract = {We theoretically investigate the electronic charge transport in a molecular system composed of a donor group (dinitrobenzene) coupled to an acceptor group (dihydrophenazine) via a polyenic chain (unsaturated carbon bridge). Ab initio calculations based on the Hartree-Fock approximations are performed to investigate the distribution of electron states over the molecule in the presence of an external electric field. For small bridge lengths (n=0-3) we find a homogeneous distribution of the frontier molecular orbitals, while for n>3 a strong localization of the lowest unoccupied molecular orbital is found. The localized orbitals in between the donor and acceptor groups act as conduction channels when an external electric field is applied. We also calculate the rectification behavior of this system by evaluating the charge accumulated in the donor and acceptor groups as a function of the external electric field. Finally, we propose a phenomenological model based on nonequilibrium Green's function to rationalize the ab initio findings.}, added-at = {2022-05-23T20:00:14.000+0200}, address = {1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA}, author = {Saraiva-Souza, Aldilene and de Souza, Fabricio Macedo and Aleixo, Vicente F P and Girao, Eduardo Costa and Filho, Josue Mendes and Meunier, Vincent and Sumpter, Bobby G and Filho, Antonio Gomes Souza and Nero, Jordan Del}, biburl = {https://www.bibsonomy.org/bibtex/2f4aec965db85aabceef2a57f28bbbb02/ppgfis_ufc_br}, doi = {10.1063/1.3020353}, interhash = {5df7f03a29cde996f12dc8a31f70b87a}, intrahash = {f4aec965db85aabceef2a57f28bbbb02}, issn = {0021-9606}, journal = {JOURNAL OF CHEMICAL PHYSICS}, keywords = {Green's HF calculations; compounds; electric electronic electronics; fields; function initio methods; molecular organic rectification; rectifiers} states; {ab}, number = 20, publisher = {AMER INST PHYSICS}, pubstate = {published}, timestamp = {2022-05-23T20:00:14.000+0200}, title = {A single molecule rectifier with strong push-pull coupling}, tppubtype = {article}, volume = 129, year = 2008 }