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Quantum Size Effects on the Chemical Sensing Performance of Two-Dimensional Semiconductors

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 Added by Hui Fang
 Publication date 2012
  fields Physics
and research's language is English




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We investigate the role of quantum confinement on the performance of gas sensors based on two-dimensional InAs membranes. Pd-decorated InAs membranes configured as H2 sensors are shown to exhibit strong thickness dependence, with ~100x enhancement in the sensor response as the thickness is reduced from 48 to 8 nm. Through detailed experiments and modeling, the thickness scaling trend is attributed to the quantization of electrons which favorably alters both the position and the transport properties of charge carriers; thus making them more susceptible to surface phenomena.



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The resonance energy and the transition rate of atoms, molecules and solids were understood as their intrinsic properties in classical electromagnetism. With the development of quantum electrodynamics, it is realized that these quantities are linked to the coupling of the transition dipole and the quantum vacuum. Such effects can be greatly amplified in macroscopic many-body systems from virtual photon exchange between dipoles, but are often masked by inhomogeneity and pure dephasing, especially in solids. Here, we observe an exceptionally large renormalization of exciton resonance and radiative decay rate in transition metal dichalcogenides monolayers due to interactions with the vacuum in both absorption and emission spectroscopy. Tuning the vacuum energy density near the monolayer, we demonstrate control of cooperative Lamb shift, radiative decay, and valley polarization as well as control of the charged exciton emission. Our work establishes a simple and robust experimental system for vacuum engineering of cooperative matter-light interactions.
The elementary optical excitations of a two-dimensional electron or hole system have been identified as exciton-Fermi-polarons. Nevertheless, the connection between the bound state of an exciton and an electron, termed trion, and exciton-polarons is subject of ongoing debate. Here, we use an analogy to the Tavis-Cummings model of quantum optics to show that an exciton-polaron can be understood as a hybrid quasiparticle -- a coherent superposition of a bare exciton in an unperturbed Fermi sea and a bright collective excitation of many trions. The analogy is valid to the extent that the Chevy Ansatz provides a good description of dynamical screening of excitons and provided the Fermi energy is much smaller than the trion binding energy. We anticipate our results to bring new insight that could help to explain the striking differences between absorption and emission spectra of two-dimensional semiconductors.
We theoretically study quantum size effects in the magnetic response of a spherical metallic nanoparticle (e.g. gold). Using the Jellium model in spherical coordinates, we compute the induced magnetic moment and the magnetic susceptibility for a nanoparticle in the presence of a static external magnetic field. Below a critical magnetic field the magnetic response is diamagnetic, whereas above such field the magnetization is characterized by sharp, step-like increases of several tenths of Bohr magnetons, associated with the Zeeman crossing of energy levels above and below the Fermi sea. We quantify the robustness of these regimes against thermal excitations and finite linewidth of the electronic levels. Finally, we propose two methods for experimental detection of the quantum size effects based on the coupling to superconducting quantum interference devices.
Electrical contact resistance to two-dimensional (2D) semiconductors such as monolayer MoS_{2} is a key bottleneck in scaling the 2D field effect transistors (FETs). The 2D semiconductor in contact with three-dimensional metal creates unique current crowding that leads to increased contact resistance. We developed a model to separate the contribution of the current crowding from the intrinsic contact resistivity. We show that current crowding can be alleviated by doping and contact patterning. Using Landauer-Buttiker formalism, we show that van der Waals (vdW) gap at the interface will ultimately limit the electrical contact resistance. We compare our models with experimental data for doped and undoped MoS_{2} FETs. Even with heavy charge-transfer doping of > 2x10^{13} cm^{-2}, we show that the state-of-the-art contact resistance is 100 times larger than the ballistic limit. Our study highlights the need to develop efficient interface to achieve contact resistance of < 10 {Omega}.{mu}m, which will be ideal for extremely scaled devices.
We analyze the low-energy properties of two-dimensional direct-gap semiconductors, such as for example the transition-metal dichalcogenides MoS$_2$, WS$_2$, and their diselenide analogues MoSe$_2$, WSe$_2$, etc., which are currently intensively investigated. In general, their electrons have a mixed character -- they can be massive Dirac fermions as well as simple Schrodinger particles. We propose a measure (Diracness) for the degree of mixing between the two characters and discuss how this quantity can in principle be extracted experimentally, within magneto-transport measurements, and numerically via ab initio calculations.
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