This growing collection consists of scholarly works authored by ASU-affiliated faculty, students, and community members, and it contains many open access articles. ASU-affiliated authors are encouraged to Share Your Work in KEEP.

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Contrasting the Material Chemistry of Cu2ZnSnSe4 and Cu2ZnSnS(4–x)Sex

Description

Earth-abundant sustainable inorganic thin-film solar cells, independent of precious elements, pivot on a marginal material phase space targeting specific compounds. Advanced materials characterization efforts are necessary to expose the roles

Earth-abundant sustainable inorganic thin-film solar cells, independent of precious elements, pivot on a marginal material phase space targeting specific compounds. Advanced materials characterization efforts are necessary to expose the roles of microstructure, chemistry, and interfaces. Herein, the earth-abundant solar cell device, Cu[subscript 2]ZnSnS[subscript (4–x)]Se[subscript x], is reported, which shows a high abundance of secondary phases compared to similarly grown Cu[subscript 2]ZnSnSe[subscript 4].

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  • 2016-02-02

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Damage-free vibrational spectroscopy of biological materials in the electron microscope

Description

Vibrational spectroscopy in the electron microscope would be transformative in the study of biological samples, provided that radiation damage could be prevented. However, electron beams typically create high-energy excitations that

Vibrational spectroscopy in the electron microscope would be transformative in the study of biological samples, provided that radiation damage could be prevented. However, electron beams typically create high-energy excitations that severely accelerate sample degradation. Here this major difficulty is overcome using an ‘aloof’ electron beam, positioned tens of nanometres away from the sample: high-energy excitations are suppressed, while vibrational modes of energies <1 eV can be ‘safely’ investigated. To demonstrate the potential of aloof spectroscopy, we record electron energy loss spectra from biogenic guanine crystals in their native state, resolving their characteristic C–H, N–H and C=O vibrational signatures with no observable radiation damage. The technique opens up the possibility of non-damaging compositional analyses of organic functional groups, including non-crystalline biological materials, at a spatial resolution of ∼10 nm, simultaneously combined with imaging in the electron microscope.

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Date Created
  • 2016-03-10

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Unusual lattice vibration characteristics in whiskers of the pseudo-one-dimensional titanium trisulfide TiS3

Description

Transition metal trichalcogenides form a class of layered materials with strong in-plane anisotropy. For example, titanium trisulfide (TiS[subscript 3]) whiskers are made out of weakly interacting TiS[subscript 3] layers, where

Transition metal trichalcogenides form a class of layered materials with strong in-plane anisotropy. For example, titanium trisulfide (TiS[subscript 3]) whiskers are made out of weakly interacting TiS[subscript 3] layers, where each layer is made of weakly interacting quasi-one-dimensional chains extending along the b axis. Here we establish the unusual vibrational properties of TiS[subscript 3] both experimentally and theoretically. Unlike other two-dimensional systems, the Raman active peaks of TiS[subscript 3] have only out-of-plane vibrational modes, and interestingly some of these vibrations involve unique rigid-chain vibrations and S–S molecular oscillations. High-pressure Raman studies further reveal that the A[subscript g][superscript S–S] S-S molecular mode has an unconventional negative pressure dependence, whereas other peaks stiffen as anticipated. Various vibrational modes are doubly degenerate at ambient pressure, but the degeneracy is lifted at high pressures. These results establish the unusual vibrational properties of TiS[subscript 3] with strong in-plane anisotropy, and may have relevance to understanding of vibrational properties in other anisotropic two-dimensional material systems.

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  • 2016-09-22

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Unusual dimensionality effects and surface charge density in 2D Mg(OH)2

Description

We present two-dimensional Mg(OH)[subscript 2] sheets and their vertical heterojunctions with CVD-MoS[subscript 2] for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties.

We present two-dimensional Mg(OH)[subscript 2] sheets and their vertical heterojunctions with CVD-MoS[subscript 2] for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties. New hydrothermal crystal growth technique enabled isolation of environmentally stable monolayer Mg(OH)[subscript 2] sheets. Raman spectroscopy and vibrational calculations reveal that the lattice vibrations of Mg(OH)[subscript 2] have fundamentally different signature peaks and dimensionality effects compared to other 2D material systems known to date. Sub-wavelength electron energy-loss spectroscopy measurements and theoretical calculations show that Mg(OH)[subscript 2] is a 6 eV direct-gap insulator in 2D, and its optical band gap displays strong band renormalization effects from monolayer to bulk, marking the first experimental confirmation of confinement effects in 2D insulators. Interestingly, 2D-Mg(OH)[subscript 2] sheets possess rather strong surface polarization (charge) effects which is in contrast to electrically neutral h-BN materials. Using 2D-Mg(OH)[subscript 2] sheets together with CVD-MoS[subscript 2] in the vertical stacking shows that a strong change transfer occurs from n-doped CVD-MoS[subscript 2] sheets to Mg(OH)[subscript 2], naturally depleting the semiconductor, pushing towards intrinsic doping limit and enhancing overall optical performance of 2D semiconductors. Results not only establish unusual confinement effects in 2D-Mg(OH)[subscript 2], but also offer novel 2D-insulating material with unique physical, vibrational, and chemical properties for potential applications in flexible optoelectronics.

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Date Created
  • 2016-02-05

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Electroluminescence from GeSn heterostructure pin diodes at the indirect to direct transition

Description

The emission properties of GeSn heterostructure pin diodes have been investigated. The devices contain thick (400–600 nm) Ge [subscript 1− y] Sn [subscript y] i-layers spanning a broad compositional range below

The emission properties of GeSn heterostructure pin diodes have been investigated. The devices contain thick (400–600 nm) Ge [subscript 1− y] Sn [subscript y] i-layers spanning a broad compositional range below and above the crossover Sn concentration y [subscript c] where the Ge [subscript 1− y] Sn [subscript y] alloy becomes a direct-gap material. These results are made possible by an optimized device architecture containing a single defected interface thereby mitigating the deleterious effects of mismatch-induced defects. The observed emission intensities as a function of composition show the contributions from two separate trends: an increase in direct gap emission as the Sn concentration is increased, as expected from the reduction and eventual reversal of the separation between the direct and indirect edges, and a parallel increase in non-radiative recombination when the mismatch strains between the structure components is partially relaxed by the generation of misfit dislocations. An estimation of recombination times based on the observed electroluminescence intensities is found to be strongly correlated with the reverse-bias dark current measured in the same devices.

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  • 2015-03-02

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Ge1-ySny (y=0.01-0.10) alloys on Ge-buffered Si: Synthesis, microstructure, and optical properties

Description

Novel hydride chemistries are employed to deposit light-emitting Ge [subscript 1- y] Sn [subscript y] alloys with y ≤ 0.1 by Ultra-High Vacuum Chemical Vapor Deposition (UHV-CVD) on Ge-buffered Si wafers. The

Novel hydride chemistries are employed to deposit light-emitting Ge [subscript 1- y] Sn [subscript y] alloys with y ≤ 0.1 by Ultra-High Vacuum Chemical Vapor Deposition (UHV-CVD) on Ge-buffered Si wafers. The properties of the resultant materials are systematically compared with similar alloys grown directly on Si wafers. The fundamental difference between the two systems is a fivefold (and higher) decrease in lattice mismatch between film and virtual substrate, allowing direct integration of bulk-like crystals with planar surfaces and relatively low dislocation densities. For y ≤ 0.06, the CVD precursors used were digermane Ge [subscript 2]H[subscript 6] and deuterated stannane SnD[subscript 4]. For y ≥ 0.06, the Ge precursor was changed to trigermane Ge [subscript 3]H[subscript 8], whose higher reactivity enabled the fabrication of supersaturated samples with the target film parameters. In all cases, the Ge wafers were produced using tetragermane Ge [subscript 4]H[subscript 10] as the Ge source. The photoluminescence intensity from Ge [subscript 1− y] Sn [subscript y] /Ge films is expected to increase relative to Ge [subscript 1− y] Sn [subscript y] /Si due to the less defected interface with the virtual substrate. However, while Ge [subscript 1− y] Sn [subscript y] /Si films are largely relaxed, a significant amount of compressive strain may be present in the Ge [subscript 1− y] Sn [subscript y] /Ge case. This compressive strain can reduce the emission intensity by increasing the separation between the direct and indirect edges. In this context, it is shown here that the proposed CVD approach to Ge [subscript 1− y] Sn [subscript y] /Ge makes it possible to approach film thicknesses of about 1  μm, for which the strain is mostly relaxed and the photoluminescence intensity increases by one order of magnitude relative to Ge [subscript 1− y] Sn [subscript y] /Si films. The observed strain relaxation is shown to be consistent with predictions from strain-relaxation models first developed for the Si[subscript 1− x] Ge [subscript x] /Si system. The defect structure and atomic distributions in the films are studied in detail using advanced electron-microscopy techniques, including aberration corrected STEM imaging and EELS mapping of the average diamond–cubic lattice.

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Date Created
  • 2014-10-07

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Structural Evolution during Photocorrosion of Ni/NiO Core/Shell Cocatalyst on TiO2

Description

The Ni/NiO core/shell structure is one of the most efficient co-catalysts for solar water splitting when coupled with suitable semiconducting oxides. It has been shown that pretreated Ni/NiO core/shell structures

The Ni/NiO core/shell structure is one of the most efficient co-catalysts for solar water splitting when coupled with suitable semiconducting oxides. It has been shown that pretreated Ni/NiO core/shell structures are more active than pure Ni metal, pure NiO or mixed dispersion of Ni metal and NiO nanoparticles. However, Ni/NiO core/shell structures on TiO2 are only able to generate H2 but not O2 in aqueous water. The nature of the hydrogen evolution reaction in these systems was investigated by correlating photochemical H2 production with atomic resolution structure determined with aberration corrected electron microscopy. It was found that the core/shell structure plays an important role for H2 generation but the system undergoes deactivation due to a loss of metallic Ni. During the H2 evolution reaction, the metal core initially formed partial voids which grew and eventually all the Ni diffused out of the core-shell into solution leaving an inactive hollow NiO void structure. The H2 evolution was generated by a photochemical reaction involving photocorrosion of Ni metal.

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Date Created
  • 2015

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Carrier density modulation in a germanium heterostructure by ferroelectric switching

Description

The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and

The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and measurable semiconductor modulation. Here we report a true ferroelectric field effect—carrier density modulation in an underlying Ge(001) substrate by switching of the ferroelectric polarization in epitaxial c-axis-oriented BaTiO[subscript 3] grown by molecular beam epitaxy. Using the density functional theory, we demonstrate that switching of BaTiO[subscript 3] polarization results in a large electric potential change in Ge. Aberration-corrected electron microscopy confirms BaTiO[subscript 3] tetragonality and the absence of any low-permittivity interlayer at the interface with Ge. The non-volatile, switchable nature of the single-domain out-of-plane ferroelectric polarization of BaTiO[subscript 3] is confirmed using piezoelectric force microscopy. The effect of the polarization switching on the conductivity of the underlying Ge is measured using microwave impedance microscopy, clearly demonstrating a ferroelectric field effect.

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Date Created
  • 2015-01-01

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Compositional dependence of the direct and indirect band gaps in Ge1-ySny alloys from room temperature photoluminescence: implications for the indirect to direct gap crossover in intrinsic and n-type materials

Description

The compositional dependence of the lowest direct and indirect band gaps in Ge[subscript 1−y]Sn[subscript y] alloys has been determined from room-temperature photoluminescence measurements. This technique is particularly attractive for a

The compositional dependence of the lowest direct and indirect band gaps in Ge[subscript 1−y]Sn[subscript y] alloys has been determined from room-temperature photoluminescence measurements. This technique is particularly attractive for a comparison of the two transitions because distinct features in the spectra can be associated with the direct and indirect gaps. However, detailed modeling of these room temperature spectra is required to extract the band gap values with the high accuracy required to determine the Sn concentration y[subscript c] at which the alloy becomes a direct gap semiconductor. For the direct gap, this is accomplished using a microscopic model that allows the determination of direct gap energies with meV accuracy. For the indirect gap, it is shown that current theoretical models are inadequate to describe the emission properties of systems with close indirect and direct transitions. Accordingly, an ad hoc procedure is used to extract the indirect gap energies from the data. For y < 0.1 the resulting direct gap compositional dependence is given by ΔE[subscript 0] = −(3.57 ± 0.06)y (in eV). For the indirect gap, the corresponding expression is ΔE[subscript ind] = −(1.64 ± 0.10)y (in eV). If a quadratic function of composition is used to express the two transition energies over the entire compositional range 0 ≤ y ≤ 1, the quadratic (bowing) coefficients are found to be b[subscript 0] = 2.46 ± 0.06 eV (for E0) and b[subscript ind] = 1.03 ± 0.11 eV (for E[subscript ind]). These results imply a crossover concentration y[subscript c] = $0.073 [+0.007 over -0.006], much lower than early theoretical predictions based on the virtual crystal approximation, but in better agreement with predictions based on large atomic supercells.

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Date Created
  • 2014-11-01