57 research outputs found
Spin states of the first four holes in a silicon nanowire quantum dot
We report measurements on a silicon nanowire quantum dot with a clarity that
allows for a complete understanding of the spin states of the first four holes.
First, we show control of the hole number down to one. Detailed measurements at
perpendicular magnetic fields reveal the Zeeman splitting of a single hole in
silicon. We are able to determine the ground-state spin configuration for one
to four holes occupying the quantum dot and find a spin filling with
alternating spin-down and spin-up holes, which is confirmed by
magnetospectroscopy up to 9T. Additionally, a so far inexplicable feature in
single-charge quantum dots in many materials systems is analyzed in detail. We
observe excitations of the zero-hole ground-state energy of the quantum dot,
which cannot correspond to electronic or Zeeman states. We show that the most
likely explanation is acoustic phonon emission to a cavity between the two
contacts to the nanowire.Comment: 24 pages, 8 figures, both including supporting informatio
Numerical study of the thermoelectric power factor in ultra-thin Si nanowires
Low dimensional structures have demonstrated improved thermoelectric (TE)
performance because of a drastic reduction in their thermal conductivity,
{\kappa}l. This has been observed for a variety of materials, even for
traditionally poor thermoelectrics such as silicon. Other than the reduction in
{\kappa}l, further improvements in the TE figure of merit ZT could potentially
originate from the thermoelectric power factor. In this work, we couple the
ballistic (Landauer) and diffusive linearized Boltzmann electron transport
theory to the atomistic sp3d5s*-spin-orbit-coupled tight-binding (TB)
electronic structure model. We calculate the room temperature electrical
conductivity, Seebeck coefficient, and power factor of narrow 1D Si nanowires
(NWs). We describe the numerical formulation of coupling TB to those transport
formalisms, the approximations involved, and explain the differences in the
conclusions obtained from each model. We investigate the effects of cross
section size, transport orientation and confinement orientation, and the
influence of the different scattering mechanisms. We show that such methodology
can provide robust results for structures including thousands of atoms in the
simulation domain and extending to length scales beyond 10nm, and point towards
insightful design directions using the length scale and geometry as a design
degree of freedom. We find that the effect of low dimensionality on the
thermoelectric power factor of Si NWs can be observed at diameters below ~7nm,
and that quantum confinement and different transport orientations offer the
possibility for power factor optimization.Comment: 42 pages, 14 figures; Journal of Computational Electronics, 201
Understanding how excess lead iodide precursor improves halide perovskite solar cell performance
The presence of excess lead iodide in halide perovskites has been key for surpassing 20% photon-to-power conversion efficiency. To achieve even higher power conversion efficiencies, it is important to understand the role of remnant lead iodide in these perovskites. To that end, we explored the mechanism facilitating this effect by identifying the impact of excess lead iodide within the perovskite film on charge diffusion length, using electron-beam-induced current measurements, and on film formation properties, from grazing-incidence wide-angle X-ray scattering and high-resolution transmission electron microscopy. Based on our results, we propose that excess lead iodide in the perovskite precursors can reduce the halide vacancy concentration and lead to formation of azimuthal angle-oriented cubic alpha-perovskite crystals in-between 0 degrees and 90 degrees. We further identify a higher perovskite carrier concentration inside the nanostructured titanium dioxide layer than in the capping layer. These effects are consistent with enhanced lead iodide-rich perovskite solar cell performance and illustrate the role of lead iodide
Reversible Modulation of Spontaneous Emission by Strain in Silicon Nanowires
We computationally study the effect of uniaxial strain in modulating the spontaneous emission of photons in silicon nanowires. Our main finding is that a one to two orders of magnitude change in spontaneous emission time occurs due to two distinct mechanisms: (A) Change in wave function symmetry, where within the direct bandgap regime, strain changes the symmetry of wave functions, which in turn leads to a large change of optical dipole matrix element. (B) Direct to indirect bandgap transition which makes the spontaneous photon emission to be of a slow second order process mediated by phonons. This feature uniquely occurs in silicon nanowires while in bulk silicon there is no change of optical properties under any reasonable amount of strain. These results promise new applications of silicon nanowires as optoelectronic devices including a mechanism for lasing. Our results are verifiable using existing experimental techniques of applying strain to nanowires
Photo absorption enhancement in strained silicon nanowires: An atomistic study
The absorption spectra of silicon nanowires are calculated using semi-empirical sp(3) d(5) s* tight binding and Density Functional Theory methods. The roles of diameter, wave function symmetry, strain, and crystallographic direction in determining the absorption are discussed. We find that compressive strain can change the band edge absorption by more than one order of magnitude due to the change in wave function symmetry. In addition, photon polarization with respect to the nanowire axis significantly alters the band edge absorption. Overall, the band edge absorption of [ 110] and [100] silicon nanowires can differ by as much as three orders of magnitude. We find that compared to bulk Silicon, a strained Silicon nanowire array can absorb infrared photons (1.1 eV) approximately one hundred times better. Finally, we compare a fully numerical and a computationally efficient semi-analytical method, and find that they both yield satisfactory values of the band edge absorption
Perovskite Quantum Dots Modeled Using ab Initio and Replica Exchange Molecular Dynamics
Organometal
halide perovskites have recently attracted tremendous attention at
both the experimental and theoretical levels. Much of this work has
been dedicated to bulk material studies, yet recent experimental work
has shown the formation of highly efficient quantum-confined nanocrystals
with tunable band edges. Here we investigate perovskite quantum dots
from theory, predicting an upper bound of the Bohr radius of 45 Å
that agrees well with literature values. When the quantum dots are
stoichiometric, they are trap-free and have nearly symmetric contributions
to confinement from the valence and conduction bands. We further show
that surface-associated conduction bandedge states in perovskite nanocrystals
lie below the bulk states, which could explain the difference in Urbach
tails between mesoporous and planar perovskite films. In addition
to conventional molecular dynamics (MD), we implement an enhanced
phase-space sampling algorithm, replica exchange molecular dynamics
(REMD). We find that in simulation of methylammonium orientation and
global minima, REMD outperforms conventional MD. To the best of our
knowledge, this is the first REMD implementation for realistic-sized
systems in the realm of DFT calculations
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