Charge-state dependent vibrational relaxation in a single-molecule junction

The interplay between nuclear and electronic degrees of freedom strongly influences molecular charge transport. Herein, we report on transport through a porphyrin dimer molecule, weakly coupled to graphene electrodes, that displays sequential tunneling within the Coulomb-blockade regime. The sequential transport is initiated by current-induced phonon absorption and proceeds by rapid sequential transport via a non-equilibrium vibrational distribution. We demonstrate this is possible only when the vibrational dissipation is slow relative to sequential tunneling rates, and obtain a lower bound for the vibrational relaxation time of 8 ns, a value that is dependent on the molecular charge state.Comment: 8 pages, 7 figure

Phase-Coherent Charge Transport through a Porphyrin Nanoribbon

Quantum interference in nano-electronic devices could lead to reduced-energy computing and efficient thermoelectric energy harvesting. When devices are shrunk down to the molecular level it is still unclear to what extent electron transmission is phase coherent, as molecules usually act as scattering centres, without the possibility of showing particle-wave duality. Here we show electron transmission remains phase coherent in molecular porphyrin nanoribbons, synthesized with perfectly defined geometry, connected to graphene electrodes. The device acts as a graphene Fabry-P\'erot interferometer, allowing direct probing of the transport mechanisms throughout several regimes, including the Kondo one. Electrostatic gating allows measurement of the molecular conductance in multiple molecular oxidation states, demonstrating a thousand-fold increase of the current by interference, and unravelling molecular and graphene transport pathways. These results demonstrate a platform for the use of interferometric effects in single-molecule junctions, opening up new avenues for studying quantum coherence in molecular electronic and spintronic devices.Comment: 14 pages, 3 figure

Fano resonance engineering in mirror-symmetry-broken THz metamaterials

We introduce a comprehensive approach to the design of mirror-symmetry broken terahertz (THz) metamaterials and present both the simulation and experimental results which show the desired asymmetric Fano resonances and electromagnetic induced transparency (EIT)-like windows. With a full wave simulation, we find these asymmetry-induced resonance modes possess extremely high quality factors and they broaden with increase of the structure asymmetry. This phenomenon arises from the destructive interference of a super-radiative bright mode and a sub-radiative dark mode which can’t be excited directly. Surface current and electric field distributions are analyzed to explain the emergence of these Fano resonances. An intuitive mechanical coupled oscillator model is derived to explain the unique line-shape of such Fano resonances. Moreover, large resonant frequency tuning (50 GHz) of Fano resonance has been demonstrated by temperature induced phase change in liquid crystals. We believe that the Fano resonance in THz metamaterials may serve as a strong building block for passive or active THz elements with potential applications for future detection and sensing systems and devices.The authors would like to thank the UK Engineering and Physical Sciences Research Council (EPSRC) for the support through the Platform Grant for Liquid Crystal Photonics (EP/F00897X/1). Xuefeng Li would like to acknowledge the support from Cambridge Trust.This is the author accepted manuscript. It is currently under an indefinite embargo pending publication by Springer

Large amplitude charge noise and random telegraph fluctuations in room-temperature graphene single-electron transistors

We analyze the noise in liquid-gated, room temperature, graphene quantum dots. These devices display extremely large noise amplitudes. The observed noise is explained in terms of a charge noise model by considering fluctuations in the applied source–drain and gate potentials. We show that the liquid environment and substrate have little effect on the observed noise and as such attribute the noise to charge trapping/detrapping at the disordered graphene edges. The trapping/detrapping of individual charges can be tuned by gating the device, which can result in stable two-level fluctuations in the measured current. These results have important implications for the use of electronic graphene nanodevices in single-molecule biosensing

Data and analysis scripts for: Statistical signature of electroburning in graphene nano-junctions

The electroburning trace data for all the substrates (SiO2, Al2O3, AlN, quartz) and scripts for creating the Figures in the manuscript are included in this submission

Statistical signature of electrobreakdown in graphene nanojunctions

Controlled electrobreakdown of graphene is important for the fabrication of stable nanometer-size tunnel gaps, large-scale graphene quantum dots, and nanoscale resistive switches, etc. However, owing to the complex thermal, electronic, and electrochemical processes at the nanoscale that dictate the rupture of graphene, it is difficult to generate conclusions from individual devices. We describe here a way to explore the statistical signature of the graphene electrobreakdown process. Such analysis tells us that feedback-controlled electrobreakdown of graphene in the air first shows signs of joule heating-induced cleaning followed by rupturing of the graphene lattice that is manifested by the lowering of its conductance. We show that when the conductance of the graphene becomes smaller than around 0.1 G0, the effective graphene notch width starts to decrease exponentially slower with time. Further, we show how this signature gets modified as we change the environment and or the substrate. Using statistical analysis, we show that the electrobreakdown under a high vacuum could lead to substrate modification and resistive-switching behavior, without the application of any electroforming voltage. This is attributed to the formation of a semiconducting filament that makes a Schottky barrier with the graphene. We also provide here the statistically extracted Schottky barrier threshold voltages for various substrate studies. Such analysis not only gives a better understanding of the electrobreakdown of graphene but also can serve as a tool in the future for single-molecule diagnostics