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Anomalously Rapid Tunneling: Charge Transport across Self-Assembled Monolayers of Oligo(ethylene glycol).

hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorBAGHBANZADEH, Mostafa
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorBOWERS, Carleen M.
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorRAPPOPORT, Dmitrij
hal.structure.identifierSmoluchowski Institute of Physics
dc.contributor.authorŻABA, Tomasz
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorYUAN, Li
dc.contributor.authorKANG, Kyungtae
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorLIAO, Kung-Ching
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorGONIDEC, Mathieu
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorROTHEMUND, Philipp
hal.structure.identifierSmoluchowski Institute of Physics
dc.contributor.authorCYGANIK, Piotr
hal.structure.identifierDepartment of Chemistry and Chemical Biology
dc.contributor.authorASPURU-GUZIK, Alan
hal.structure.identifierDepartment of Chemistry and Chemical Biology
hal.structure.identifierWyss Institute for Biologically Inspired Engineering [Harvard University]
hal.structure.identifierKavli Institute for Bionano Science & Technology [Harvard University] [KIBST]
dc.contributor.authorWHITESIDES, George M.
dc.date.issued2017-06-07
dc.identifier.issn0002-7863
dc.description.abstractEnThis paper describes charge transport by tunneling across self-assembled monolayers (SAMs) of thiol-terminated derivatives of oligo(ethylene glycol) (HS(CH2CH2O)nCH3; HS(EG)nCH3); these SAMs are positioned between gold bottom electrodes and Ga2O3/EGaIn top electrodes. Comparison of the attenuation factor (β of the simplified Simmons equation) across these SAMs with the corresponding value obtained with length-matched SAMs of oligophenyls (HS(Ph)nH) and n-alkanethiols (HS(CH2)nH) demonstrates that SAMs of oligo(ethylene glycol) have values of β (β(EG)n = 0.29 ± 0.02 natom(-1) and β = 0.24 ± 0.01 Å(-1)) indistinguishable from values for SAMs of oligophenyls (β(Ph)n = 0.28 ± 0.03 Å(-1)), and significantly lower than those of SAMs of n-alkanethiolates (β(CH2)n = 0.94 ± 0.02 natom(-1) and 0.77 ± 0.03 Å(-1)). There are two possible origins for this low value of β. The more probable involves hole tunneling by superexchange, which rationalizes the weak dependence of the rate of charge transport on the length of the molecules of HS(EG)nCH3 using interactions among the high-energy, occupied orbitals associated with the lone-pair electrons on oxygen. Based on this mechanism, SAMs of oligo(ethylene glycol)s are good conductors (by hole tunneling) but good insulators (by electron and/or hole drift conduction). This observation suggests SAMs derived from these or electronically similar molecules are a new class of electronic materials. A second but less probable mechanism for this unexpectedly low value of β for SAMs of S(EG)nCH3 rests on the possibility of disorder in the SAM and a systematic discrepancy between different estimates of the thickness of these SAMs.
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.title.enAnomalously Rapid Tunneling: Charge Transport across Self-Assembled Monolayers of Oligo(ethylene glycol).
dc.typeArticle de revue
dc.identifier.doi10.1021/jacs.7b02770
dc.subject.halChimie/Matériaux
bordeaux.journalJournal of the American Chemical Society
bordeaux.page7624-7631
bordeaux.volume139
bordeaux.issue22
bordeaux.peerReviewedoui
hal.identifierhal-01550337
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-01550337v1
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