Engineering topics

Kosina, Hans

Publications and source records attributed to Kosina, Hans.

6 records

DOE OSTI2016

The effect of oxide shell thickness on the structural, electronic, and optical properties of Si-SiO{sub 2} core-shell nano-crystals: A (time dependent)density functional theory study

Due to their tunable properties, silicon nano-crystals (NC) are currently being investigated. Quantum confinement can generally be employed for size-dependent band-gap tuning at dimensions smaller than the Bohr radius (∼5 nm for silicon). At the nano-meter scale, however, increased surface-to-volume ratio makes the surface effects dominant. Specifically, in Si-SiO{sub 2} core-shell semiconductor NCs the interfacial transition layer causes peculiar electronic and optical properties, because of the co-existence of intermediate oxidation states of silicon (Si{sup n+}, n = 0–4). Due to the presence of the many factors involved, a comprehensive understanding of the optical properties of these NCs has not yet been achieved. In this work, Si-SiO{sub 2} NCs with a diameter of 1.1 nm and covered by amorphous oxide shells with thicknesses between 2.5 and 4.75 Å are comprehensively studied, employing density functional theory calculations. It is shown that with increased oxide shell thickness, the low-energy part of the optical transition spectrum of the NC is red shifted and attenuated. Moreover, the absorption coefficient is increased in the high-energy part of the spectrum which corresponds to SiO{sub 2} transitions. Structural examinations indicate a larger compressive stress on the central silicon cluster with a thicker oxide shell. Examination of the local density of states reveals the migration of frontier molecular orbitals from the oxide shell into the silicon core with the increase of silica shell thickness. The optical and electrical properties are explained through the analysis of the density of states and the spatial distribution of silicon sub-oxide species.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

The influence of non-idealities on the thermoelectric power factor of nanostructured superlattices

Cross-plane superlattices composed of nanoscale layers of alternating potential wells and barriers have attracted great attention for their potential to provide thermoelectric power factor improvements and higher ZT figure of merit. Previous theoretical works have shown that the presence of optimized potential barriers could provide improvements to the Seebeck coefficient through carrier energy filtering, which improves the power factor by up to 40%. However, experimental corroboration of this prediction has been extremely scant. In this work, we employ quantum mechanical electronic transport simulations to outline the detrimental effects of random variation, imperfections, and non-optimal barrier shapes in a superlattice geometry on these predicted power factor improvements. Thus, we aim to assess either the robustness or the fragility of these theoretical gains in the face of the types of variation one would find in real material systems. We show that these power factor improvements are relatively robust against: overly thick barriers, diffusion of barriers into the body of the wells, and random fluctuations in barrier spacing and width. However, notably, we discover that extremely thin barriers and random fluctuation in barrier heights by as little as 10% is sufficient to entirely destroy any power factor benefits of the optimized geometry. Our results could provide performance optimization routes for nanostructured thermoelectrics and elucidate the reasons why significant power factor improvements are not commonly realized in superlattices, despite theoretical predictions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

On the role of spatial position of bridged oxygen atoms as surface passivants on the ground-state gap and photo-absorption spectrum of silicon nano-crystals

Silicon nano-crystals (NCs) are potential candidates for enhancing and tuning optical properties of silicon for optoelectronic and photo-voltaic applications. Due to the high surface-to-volume ratio, however, optical properties of NC result from the interplay of quantum confinement and surface effects. In this work, we show that both the spatial position of surface terminants and their relative positions have strong effects on NC properties as well. This is accomplished by investigating the ground-state HOMO-LUMO band-gap, the photo-absorption spectra, and the localization and overlap of HOMO and LUMO orbital densities for prototype ∼1.2 nm Si{sub 32–x}H{sub 42–2x}O{sub x} hydrogenated silicon NC with bridged oxygen atoms as surface terminations. It is demonstrated that the surface passivation geometry significantly alters the localization center and thus the overlap of frontier molecular orbitals, which correspondingly modifies the electronic and optical properties of NC.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

Diagonal-transition quantum cascade detector

We demonstrate the concept of diagonal transitions for quantum cascade detectors (QCD). Different to standard, vertical QCDs, here the active transition takes place between two energy levels in adjacent wells. Such a scheme has versatile advantages. Diagonal transitions generally yield a higher extraction efficiency and a higher resistance than vertical transitions. This leads to an improved overall performance, although the absorption strength of the active transition is smaller. Since the extraction is not based on resonant tunneling, the design is more robust, with respect to deviations from the nominal structure. In a first approach, a peak responsivity of 16.9 mA/W could be achieved, which is an improvement to the highest shown responsivity of a QCD for a wavelength of 8 μm at room-temperature by almost an order of magnitude.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Gated Si nanowires for large thermoelectric power factors

We investigate the effect of electrostatic gating on the thermoelectric power factor of p-type Si nanowires (NWs) of up to 20 nm in diameter in the [100], [110], and [111] crystallographic transport orientations. We use atomistic tight-binding simulations for the calculation of the NW electronic structure, coupled to linearized Boltzmann transport equation for the calculation of the thermoelectric coefficients. We show that gated NW structures can provide ∼5× larger thermoelectric power factor compared to doped channels, attributed to their high hole phonon-limited mobility, as well as gating induced bandstructure modifications which further improve mobility. Despite the fact that gating shifts the charge carriers near the NW surface, surface roughness scattering is not strong enough to degrade the transport properties of the accumulated hole layer. The highest power factor is achieved for the [111] NW, followed by the [110], and finally by the [100] NW. As the NW diameter increases, the advantage of the gated channel is reduced. We show, however, that even at 20 nm diameters (the largest ones that we were able to simulate), a ∼3× higher power factor for gated channels is observed. Our simulations suggest that the advantage of gating could still be present in NWs with diameters of up to ∼40 nm.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2014

Anomalous diameter dependence of thermal transport in ultra-narrow Si nanowires

We present atomistic valence force field calculations of thermal transport in Si nanowires of diameters from 12 nm down to 1 nm. We show that as the diameter is reduced, the phonon density-of-states and transmission function acquire a finite value at low frequency, in contrast to approaching zero as in the bulk material. It turns out that this effect results in what Ziman described as the “problem of long longitudinal waves” [J. M. Ziman, Electrons and Phonons: The Theory of Transport Phenomena in Solids (Clarendon, Oxford, 1962)], which states that the thermal conductivity of a material increases as its length is increased due to the vanishing scattering for long-wavelength phonons. We show that this thermal transport improvement also appears in nanowires as their diameter is decreased below D = 5 nm (not only as the length increases), originating from the increase in the density of the long wavevector modes. The observation is present under ballistic transport conditions, and further enhanced with the introduction of phonon-phonon scattering. Because of this, in such ultra-narrow nanowires, as the diameter is reduced, phonon transport is dominated more and more by lower energy phonons with longer mean-free paths. We show that ∼80% of the heat is carried by phonons with energies less than 5 meV, most with mean-free paths of several hundreds of nanometers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗