109 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
A composite light-harvesting layer from photoactive polymer and halide perovskite for planar heterojunction solar cells
A new route for fabrication of photoactive materials in organic-inorganic hybrid solar cells is presented in this report. Photoactive materials by blending a semiconductive conjugated polymer with an organolead halide perovskite were fabricated for the first time. The composite active layer was then used to make planar heterojunction solar cells with the PCBM film as the electron-acceptor. Photovoltaic performance of solar cells was investigated by J-V curves and external quantum efficiency spectra. We demonstrated that the incorporation of the conjugated photoactive polymer into organolead halide perovskites did not only contribute to the generation of charges, but also enhance stability of solar cells by providing a barrier protection to halide perovskites. It is expected that versatile of conjugated semi-conductive polymers and halide perovskites in photoactive properties enables to create various combinations, forming composites with advantages offered by both types of photoactive materials
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
Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3 +; X = Br– or I–) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 109 to 1010 per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations
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
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
Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals
Methylammonium lead iodide perovskite (MAPbI_3) exhibits long charge carrier lifetimes that are linked to its high efficiency in solar cells. Yet, the mechanisms governing these unusual carrier dynamics are not completely understood. A leading hypothesis—disproved in this work—is that a large, static bulk Rashba effect slows down carrier recombination. Here, using second harmonic generation rotational anisotropy measurements on MAPbI_3 crystals, we demonstrate that the bulk structure of tetragonal MAPbI_3 is centrosymmetric with I4/mcmspace group. Our calculations show that a significant Rashba splitting in the bandstructure requires a non-centrosymmetric lead iodide framework, and that incorrect structural relaxations are responsible for the previously predicted large Rashba effect. The small Rashba splitting allows us to compute effective masses in excellent agreement with experiment. Our findings rule out the presence of a large static Rashba effect in bulk MAPbI_3, and our measurements find no evidence of dynamic Rashba effects
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