ABSTRACT
Enhancing thermopower is a key goal in organic and molecular thermoelectrics. Herein, it is shown that introducing noncovalent contact with a single-layer graphene (SLG) electrode improves the thermopower of saturated molecules as compared to the traditional gold-thiolate covalent contact. Thermoelectric junction measurements with a liquid-metal technique reveal that the value of Seebeck coefficient in large-area junctions based on n-alkylamine self-assembled monolayers (SAMs) on SLG is increased up to fivefold compared to the analogous junction based on n-alkanethiolate SAMs on gold. Experiments with Raman spectroscopy and field-effect transistor analysis indicate that such enhancements benefit from the creation of new in-gap states and electron doping through noncovalent interaction between the amine anchor and the SLG electrode, which leads to a reduced energy offset between the Fermi level and the transport channel. This work demonstrates that control of interfacial bonding nature in molecular junctions improves the Seebeck effect in saturated molecules.
ABSTRACT
Great effort has been devoted in recent years to improve the electrical conductivity of graphene for use in practical applications. Here, we demonstrate the hole carrier density of CVD graphene on a SiO2/Si substrate increases by more than one order of magnitude to n = 3 × 10(13) cm(-2) after irradiation with a high energy 5 MeV proton beam. As a result, the dc-resistance (R) of graphene is reduced significantly by 60%. Only a negligible amount of defect is created by the irradiation. Also the hole-doped low resistance state of graphene remains robust against external perturbations. This carrier doping is achieved without requiring the bias-gate voltage as is the case for other field effect devices. We make two important observations, (i) occurrence of the doping after the irradiation is turned off (ii) indispensability of the SiO2-layer in the substrate, which leads to a purely electronic mechanism for the doping where electron-hole pair creation and interlayer Coulomb attraction play a major role. A flux-dependent study predicts that an ultrahigh doping may be obtained by longer irradiation. We expect the irradiation doping method could be applied to other atomically thin solids, facilitating the fundamental study and application of the 2d materials.
ABSTRACT
High-k dielectric oxides are supposedly ideal gate-materials for ultra-high doping in graphene and other 2D-crystals. Here, we report a temperature-dependent electronic transport study on chemical vapor deposited-graphene gated with SrTiO3 (STO) thin film substrate. At carrier densities away from charge neutrality point the temperature-dependent resistivity of our graphene samples on both STO and SiO2/Si substrates show metallic behavior with contributions from Coulomb scattering and flexural phonons attributable to the presence of characteristic quasi-periodic nano-ripple arrays. Significantly, for graphene samples on STO substrates we observe an anomalous 'slope-break' in the temperature-dependent resistivity for T = 50 to 100â K accompanied by a decrease in mobility above 30â K. Furthermore, we observe an unusual decrease in the gate-induced doping-rate at low temperatures, despite an increase in dielectric constant of the substrate. We believe that a complex mechanism is at play as a consequence of the structural phase transition of the underlying substrate showing an anomalous transport behavior in graphene on STO. The anomalies are discussed in the context of Coulomb as well as phonon scattering.
ABSTRACT
Graphene charge carriers behave as massless Dirac fermions, opening the exciting possibility to observe long-range virtual tunneling of electrons in a solid. In granular metals, electron hops arising from series of virtual transitions are predicted to yield observable currents at low-enough temperatures, but to date experimental evidence is lacking. We report on electron transport in granular graphene films self-assembled by hydrogenation of suspended graphene. While the log-conductance shows a characteristic T(-1/2) temperature dependence, cooling the samples below 10â K drives a triple crossover: a slope break in log-conductance, simultaneous to a substantial increase in magneto-conductance and onset of large mesoscopic conductance fluctuations. These phenomena are signatures of virtual transitions of electrons between distant localized states, and conductance statistics reveal that the high crossover-temperature is due to the Dirac nature of granular graphene charge carriers.
