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Register a new userDependence of Mobility on Density of Gap States in Organics by GAMEaS - Gate Modulated Activation Energy Spectroscopy
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W. So
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We develop a broadly applicable transport-based technique, GAte Modulated activation Energy Spectroscopy (GAMEaS), for determining the density of states (DOS) in the energy gap. GAMEaS is applied to field effect transistors made from different single crystal oligomer semiconductors to extract the free-carrier mobility, u_0, from the field effect mobility, u_eff. Samples with a lower DOS exhibit higher u_eff. Values of u_0 up to 100 +/- 40 cm2/Vs at 300K are observed, showing that performance can be greatly enhanced by improving sample purity and crystal quality.
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Using an electrochemically gated transistor, we achieved controlled and reversible doping of poly(p-phenylene vinylene) in a large concentration range. Our data open a wide energy-window view on the density of states (DOS) and show, for the first time, that the core of the DOS function is Gaussian, while the low-energy tail has a more complex structure. The hole mobility increases by more than four orders of magnitude when the electrochemical potential is scanned through the DOS.
CrBr$_{3}$ is a layered van der Waals material with magnetic ordering down to the 2D limit. For decades, based on optical measurements, it is believed that the energy gap of CrBr$_{3}$ is in the range of 1.68-2.1 eV. However, controversial results have indicated that the band gap of CrBr$_{3}$ is possibly smaller than that. An unambiguous determination of the energy gap is critical to the correct interpretations of the experimental results of CrBr$_{3}$. Here, we present the scanning tunneling microscopy and spectroscopy (STM/S) results of CrBr$_{3}$ thin and thick flakes exfoliated onto pyropytic graphite (HOPG) surfaces and density functional theory (DFT) calculations to reveal the small energy gap (peak-to-peak energy gap to be 0.57 eV $pm$ 0.04 eV; or the onset signal energy gap to be 0.29 $pm$ 0.05 eV from dI/dV spectra). Atomic resolution topography images show the defect-free crystal structure and the dI/dV spectra exhibit multiple peak features measured at 77 K. The conduction band - valence band peak pairs in the multi-peak dI/dV spectrum agree very well with all reported optical transitions. STM topography images of mono- and bi-layer CrBr$_{3}$ flakes exhibit edge degradation due to short air exposure (~15 min) during sample transfer. The unambiguously determined small energy gap settles the controversy and is the key in better understanding CrBr$_{3}$ and similar materials.
Because inorganic solid electrolytes are one of the key components for application to all-solid-state batteries, high-ionic-conductivity materials must be developed. Therefore, we propose a method of efficiently evaluating the activation energy of ionic diffusion by calculating a potential-energy surface (PES), searching for the optimal diffusion path by an algorithm developed using dynamic programming (DP), and calculating the corresponding activation energy by the nudged elastic band (NEB) method. Taking beta-Li3PS4 as an example, the activation energy of Li-ion diffusion was calculated as 0.43, 0.25, and 0.40 eV in the a-, b-, and c-axis directions, respectively, which is in good agreement with previously reported values. By comprehensively searching for the lowest energy path by PES-DP, the arbitrariness of the path selection can be eliminated, and the activation energy must only be calculated using the NEB method a few times, which greatly reduces the computational cost required for evaluating activation energy and enables the high-throughput screening of solid state electrolytes.
Electron energy-loss spectroscopy (EELS) performed in transmission electron microscopes is shown to directly render the photonic local density of states (LDOS) with unprecedented spatial resolution, currently below the nanometer. Two special cases are discussed in detail: (i) 2D photonic structures with the electrons moving along the translational axis of symmetry and (ii) quasi-planar plasmonic structures under normal incidence. Nanophotonics in general and plasmonics in particular should benefit from these results connecting the unmatched spatial resolution of EELS with its ability to probe basic optical properties like the photonic LDOS.
We quantify the degree of disorder in the {pi}-{pi} stacking direction of crystallites of a high performing semicrystalline semiconducting polymer with advanced X-ray lineshape analysis. Using first principles calculations, we obtain the density of states of a system of {pi}-{pi} stacked polymer chains with increasing amounts of paracrystalline disorder. We find that for an aligned film of PBTTT the paracrystalline disorder is 7.3%. This type of disorder induces a tail of trap states with a breadth of ~100 meV as determined through calculation. This finding agrees with previous device modeling and provides physical justification for the mobility edge model.
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