2016
DOI: 10.1039/c5sc03097h
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Transition voltages respond to synthetic reorientation of embedded dipoles in self-assembled monolayers

Abstract: Transition voltages respond to the collective action of dipole moments embedded in self-assembled monolayers.

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Cited by 50 publications
(100 citation statements)
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“…5 Likewise, SAMs exhibit collective effects that cannot be observed at the single-molecule level; for example, odd-even effects driven by the conformation of close-packed alkyl chains [6][7][8] and the collective action of molecular dipoles affecting transition voltages (V trans ) by shiing vacuum levels. 9,10 Although single-molecule junctions are generally studied in greater detail, the technological relevance of SAM-junctions is more apparent and mature. 11 Here, we report the asymmetric conduction in tunneling junctions using eutectic Ga-In (EGaIn) top-contacts 12 that is driven by the collective action of dipole moments embedded in a SAM comprising molecules of identical empirical formula, frontier orbital energies (for isolated molecules) and interfaces with the electrodes (Fig.…”
mentioning
confidence: 99%
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“…5 Likewise, SAMs exhibit collective effects that cannot be observed at the single-molecule level; for example, odd-even effects driven by the conformation of close-packed alkyl chains [6][7][8] and the collective action of molecular dipoles affecting transition voltages (V trans ) by shiing vacuum levels. 9,10 Although single-molecule junctions are generally studied in greater detail, the technological relevance of SAM-junctions is more apparent and mature. 11 Here, we report the asymmetric conduction in tunneling junctions using eutectic Ga-In (EGaIn) top-contacts 12 that is driven by the collective action of dipole moments embedded in a SAM comprising molecules of identical empirical formula, frontier orbital energies (for isolated molecules) and interfaces with the electrodes (Fig.…”
mentioning
confidence: 99%
“…We previously observed this effect experimentally in SAMs of three series of compounds as a shi in the work function (WF) of the bottom electrode 16 and characterized its impact on tunneling charge-transport. 9,10 Thus, the compounds used to form the SAMs in this study are regioisomers with nearly identical frontier orbitals ( Fig. S7 †) that form tunneling junctions of nearly identical geometries (Table 1).…”
mentioning
confidence: 99%
“…Without detailed knowledge of the packing of the molecules in the SAM and atomistic detail of the Ga 2 O 3 electrode and SAM//Ga 2 O 3 EGaIn interface, none of which are available, it is impossible to construct an accurate model capable of predicting these effects. The principal limitations of using a model Au/molecule/Au junction is that we cannot reliably estimate the Fermi level E f and the relative level-alignments will not reflect any collective effects such as broadening or electrostatic shifts31 (for example, the 0.4–0.5 eV shift induced by S–Au bonds in SAMs32). However, we can still compare (similar) molecular structures and draw meaningful (qualitative) conclusions in combination with experimental data from Au TS /SAM//EGaIn junctions9.…”
Section: Discussionmentioning
confidence: 99%
“…However, we can still compare (similar) molecular structures and draw meaningful (qualitative) conclusions in combination with experimental data from Au TS /SAM//EGaIn junctions9. We estimated E f by adding the calculated highest-occupied π state (HOPS) to the experimentally derived transition voltages3133 V trans for each Au TS /SAM//EGaIn junction (see Supplementary Table 3) to establish the relative level-alignment between related structures (that is, OPE3 and PCP; AH and AC).…”
Section: Discussionmentioning
confidence: 99%
“…Such an approach has recently been suggested for manipulating the electronic states within graphene and semiconducting self‐assembled monolayers (SAMs) on metal substrates . First proof of principle experiments on SAMs have already confirmed the induced potential step within the monolayer and its significant impact on ballistic charge transport through the SAMs …”
mentioning
confidence: 99%