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Modeling electrostatic and quantum detection of molecules

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 Added by Smitha Vasudevan
 Publication date 2008
  fields Physics
and research's language is English




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We describe two different modes for electronically detecting an adsorbed molecule using a nanoscale transistor. The attachment of an ionic molecular target shifts the threshold voltage through modulation of the depletion layer electrostatics. A stronger bonding between the molecule and the channel, involving actual overlap of their quantum mechanical wavefunctions, leads to scattering by the molecular traps that creates characteristic fingerprints when scanned with a backgate. We describe a theoretical approach to model these transport characteristics.

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Electric charge detection by atomic force microscopy (AFM) with single- electron resolution (e-EFM) is a promising way to investigate the electronic level structure of individual quantum dots (QD). The oscillating AFM tip modulates the energy of the QDs, causing single electrons to tunnel between QDs and an electrode. The resulting oscillating electrostatic force changes the resonant frequency and damping of the AFM cantilever, enabling electrometry with a single-electron sensitivity. Quantitative electronic level spectroscopy is possible by sweeping the bias voltage. Charge stability diagram can be obtained by scanning the AFM tip around the QD. e-EFM technique enables to investigate individual colloidal nanoparticles and self- assembled QDs without nanoscale electrodes. e-EFM is a quantum electromechanical system where the back-action of a tunneling electron is detected by AFM; it can also be considered as a mechanical analog of admittance spectroscopy with a radio frequency resonator, which is emerging as a promising tool for quantum state readout for quantum computing. In combination with the topography imaging capability of the AFM, e-EFM is a powerful tool for investigating new nanoscale material systems which can be used as quantum bits.
Scanning tunneling microscopy (STM) can be used to detect inelastic spin transitions in magnetic nano-structures comprising only a handful of atoms. Here we demonstrate that STM can uniquely identify the electrostatic spin crossover effect, whereby the exchange interaction between two magnetic centers in a magnetic molecule changes sign as a function of an external electric field. The fingerprint of such effect is a large drop in the differential conductance as the bias increases. Crucially in the case of a magnetic dimer the spin crossover transition inverts the order between the ground state and the first excited state, but does not change their symmetry. This means that at both sides of the conductance drop associated to the spin crossover transition there are two inelastic transition between the same states. The corresponding conductance steps split identically in a magnetic field and provide a unique way to identify the electrostatic spin crossover.
In this work we theoretically study properties of electric current driven by a temperature gradient through a quantum dot/molecule coupled to the source and drain charge reservoirs. We analyze the effect of Coulomb interactions between electrons on the dot/molecule and of thermal environment on the thermocurrent. The environment is simulated by two thermal baths associated with the reservoirs and kept at different temperatures. The scattering matrix formalism is employed to compute electron transmission through the system. This approach is further developed and combined with nonequilibrium Greens functions formalism, so that scattering probabilities are expressed in terms of relevant energies including the thermal energy, strengths of coupling between the dot/molecule and charge reservoirs and characteristic energies of electron-phonon interactions. It is shown that one may bring the considered system into regime favorable for heat-to-electric energy conversion by varying the applied bias and gate voltages.
Electrostatic gating lies in the heart of modern FET-based integrated circuits. Usually, the gate electrode has to be placed very close to the conduction channel, typically a few nanometers, in order to achieve efficient tunability. However, remote control of a FET device through a gate electrode placed far away is always highly desired, because it not only reduces the complexity of device fabrication, but also enables designing novel devices with new functionalities. Here, a non-local gating effect in graphene using both near-field optical nano-imaging and electrical transport measurement is reported. With assistance of absorbed water molecules, the charge density of graphene can be efficiently tuned by a local-gate placed over 30 {mu}m away. The observed non-local gating effect is initially driven by an in-plane electric field established between graphene regions with different charge densities due to the quantum capacitance near the Dirac point in graphene. The nonlocality is further amplified and largely enhanced by absorbed water molecules through screening the in-plane electric field and expending the transition length. This research reveals novel non-local phenomenon of Dirac electrons, and paves the way for designing electronic devices with remote-control using 2D materials with small density of states.
Exciting phenomena may emerge in non-centrosymmetric two-dimensional (2D) electronic systems when spin-orbit coupling (SOC) interplays dynamically with Coulomb interactions, band topology, and external modulating forces, etc. Here, we report illuminating synergetic effects between SOC and Stark in centrosymmetric few-layer black arsenic (BAs), manifested as giant Rashba valley splitting and exotic quantum Hall states (QHS) reversibly controlled by electrostatic gating. The unusual finding is rooted in the puckering square lattice of BAs, in which heavy $4p$ orbitals form highly asymmetric $Gamma$ valley with the $p_{z}$ symmetry and $D$ valleys of the $p_{x}$ origin, located at the Brillouin zone (BZ) center and near the time reversal invariant momenta of $X$, respectively. When the structure inversion symmetry is broken by perpendicular electric field, giant Rashba SOC is activated for the $p_{x}$ bands to produce strong spin-polarized $D^{+}$ and $D^{-}$ valleys related by time-reversal symmetry, coexisting with weak $Gamma$ Rashba bands constrained by the $p_{z}$ symmetry. Intriguingly, strong Stark effect shows the same $p_{x}$-orbital selectiveness for $D$, collectively shifting the valence band maximum of $D^{pm}$ valleys to exceed the $Gamma$ pockets. Such an orchestrating effect between SOC and Stark allows us to realize gate-tunable spin valley manipulations for 2D hole gas, as revealed by unconventional magnetic field triggered even-to-odd transitions in QHS. For electron doping, the quantization of the $Gamma$ Rashba bands is characterized by peculiar density-dependent transitions in band topology from two parabolic valleys to a unique inner-outer helical structure when charge carrier concentrations increase.
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