Plasmonic nanostructures can induce a number of interesting responses in devices. Here we show that hot electrons can be extracted from plasmonic particles and directed into a molecular electronic device, which represents a new mechanism of transfer from light to electronic transport. To isolate this phenomenon from alternative and sometimes simultaneous mechanisms of plasmon-exciton interactions, we designed a family of hybrid nanostructure devices consisting of Au nanoparticles and optoelectronically functional porphyin molecules that enable precise control of electronic and optical properties. Temperature- and wavelength-dependent transport measurements are analyzed in the context of optical absorption spectra of the molecules, the Au particle arrays, and the devices. Enhanced photocurrent associated with exciton generation in the molecule is distinguished from enhancements due to plasmon interactions. Mechanisms of plasmon-induced current are examined, and it is found that hot electron generation can be distinguished from other possibilities.
Temperature-dependent transport of hybrid structures consisting of gold nanoparticle arrays functionalized by conjugated organic molecules [(4'-thiophenyl)ethynyl-terminated meso-to-meso ethyne-bridged (porphinato)zinc(II) complexes] that possess exceptional optical and electronic properties was characterized. Differential conductance analysis distinguished the functional forms of the temperature and voltage dependences for a range of sample particles and molecular attachments. Thermally assisted tunneling describes transport for all cases and the associated mechanistic parameters can be used to determine the relative roles of activation energy, work function, and so forth. These results provide the basis on which to examine plasmon-influenced conduction in hybrid systems.
We report the synthesis of ultrathin silver sulfide (AgS) nanoplatelets (NPLs) synthesized via a one-pot method in ethylene glycol with 3-mercaptopropionic acid serving as both the sulfur precursor and the platelet ligand. The colloidally synthesized nanoplatelets are exceptionally thin, with a thickness of only 3.5 ± 0.2 Å and a 1S exciton Bohr diameter to confinement ratio of ∼12.6. The NPL growth is shown to be quantized by layer thickness using absorption and photoluminescence (PL) spectroscopy. Transmission electron microscopy, atomic force microscopy, and X-ray diffraction analyses of the NPLs show that they correspond to the (202) plane of the β-AgS structure. The PL quantum yield of these NPLs is ∼30%, suggesting their potential use in biomedical imaging. Optoelectronic properties were evaluated via sensitized photocurrent spectroscopy with the resulting spectra closely matching the distinctive absorption spectral shape of the AgS NPLs.
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