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Au 133 (SPh - t Bu) 52 Nanomolecules: X-ray Crystallography, Optical, Electrochemical, and Theoretical Analysis
Crystal structure determination has revolutionized modern science in biology, chemistry, and physics. However, the difficulty in obtaining periodic crystal lattices which are needed for X-ray crystal analysis has hindered the determination of atomic structure in nanomaterials, known as the "nanostructure problem". Here, by using rigid and bulky ligands, we have overcome this limitation and successfully solved the X-ray crystallographic structure of the largest reported thiolated gold nanomolecule, Au133S52. The total composition, Au-133(SPh-tBu)(52), was verified using high resolution electrospray ionization mass spectrometry (ESI-MS). The experimental and simulated optical spectra show an emergent surface plasmon resonance that is more pronounced than in the slightly larger Au-144(SCH2CH2Ph)(60). Theoretical analysis indicates that the presence of rigid and bulky ligands is the key to the successful crystal formation.
Nanometer resolution optical coherence tomography using broad bandwidth XUV and soft x-ray radiation
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Elucidating the optical spectra of [Au 25 (SR) 18 ] q nanoclusters
Density functional theory calculations reveal how optical spectra of [Au 25 (SR) 18 ] q nanoclusters ( q = −1, 0, +1) change with different ligands.
Integration of electrocatalysts with silicon microcone arrays for minimization of optical and overpotential losses during sunlight-driven hydrogen evolution
Microstructured photoelectrode morphologies can advantageously facilitate integration of optically absorbing electrocatalysts with semiconducting light absorbers.
Combined Plasmonic Au-nanoparticle and Conducting Metal Oxide High-temperature Optical Sensing with LSTO
<span style="color: rgba(0, 0, 0, 0.79); font-family: "Source Sans Pro", source-sans-pro, museo_sans300, museo-sans, Arial, sans-serif; font-size: 16px; background-color: rgb(255, 255, 255);">Fiber optic sensor technology offers several advantages for harsh-environment applications. However, the development of optical gas sensing layers that are stable under harsh environmental conditions is an ongoing research challenge. In this work, electronically conducting metal oxide lanthanum-doped strontium titanate (LSTO) films embedded with gold nanoparticles are examined as a sensing layer for application in reducing gas flows at high temperature (600–800 °C). A strong localized surface plasmon resonance (LSPR) based response to hydrogen is demonstrated in the visible region of the spectrum, while a Drude free electron-based response is observed in the near-IR. Characteristics of these responses are studied both on planar glass substrates and on silica fibers. Charge transfer between the oxide film and the gold nanoparticles is explored as a possible mechanism governing the Au LSPR response and is considered in terms of the corresponding properties of the conducting metal oxide-based matrix phase. Principal component analysis is applied to the combined plasmonic and free-carrier based response over a range of temperatures and hydrogen concentrations. It is demonstrated that the combined visible and near-IR response of these films provides improved versatility for multiwavelength interrogation, as well as improved discrimination of important process parameters (concentration and temperature) through application of multivariate analysis techniques.</span>
Optical Instruments Synergy in Determination of Optical Depth of Thin Clouds
Optically thin clouds have a strong radiative effect and need to be represented accurately in climate models. Cloud optical depth of thin clouds was retrieved using high resolution digital photography, lidar, and a radiative transfer model. The Doppler Lidar was operated at 1.5 μm, minimizing return from Rayleigh scattering, emphasizing return from aerosols and clouds. This approach examined cloud structure on scales 3 to 5 orders of magnitude finer than satellite products, opening new avenues for examination of cloud structure and evolution.
Effects of structure distortion on optical phonon properties of crystalline beta-BaTeMo{sub 2}O{sub 9}—A novel nonlinear optical material: Infrared and Raman spectra as well as first-principles calculations
The infrared dielectric property of monoclinic BaTeMo{sub 2}O{sub 9} single crystals is studied by polarized IR reflectance spectra from 20 to 1800 cm{sup −1}. Based on the modified Lorentz model, the frequencies, strengths, and dampings of TO modes as well as the orientations of the dipole momenta are determined, agreeing well with Raman spectra and results from First-principles calculation. The observed modes are visually assigned to the specific atoms' motions in the primitive cell based on the theory calculations. A large shift of the internal modes of the anion groups relative to free anion co-ordination polyhedra is observed, which can be used to indicate the distortions of co-ordination polyhedra related to the nonlinear optical properties. Further, the experimental results of the strengths of the oscillators support the elimination and splitting of degenerate modes in free regular polyhedrons. These results offer a way to evaluate the nonlinear optical properties by use of traditional IR reflectivity spectra.
Energy-selective optical excitation and detection in InAs/InP quantum dot ensembles using a one-dimensional optical microcavity
We demonstrate the selective optical excitation and detection of subsets of quantum dots (QDs) within an InAs/InP ensemble using a SiO{sub 2}/Ta{sub 2}O{sub 5}-based optical microcavity. The low variance of the exciton transition energy and dipole moment tied to the narrow linewidth of the microcavity mode is expected to facilitate effective qubit encoding and manipulation in a quantum dot ensemble with ease of quantum state readout relative to qubits encoded in single quantum dots.
Note: Efficient generation of optical sidebands at GHz with a high-power tapered amplifier
Two methods using a laser-diode tapered amplifier to produce high-power, high-efficiency optical frequency sidebands over a wide tunable frequency range are studied and compared. For a total output of 500 mW at 811 nm, 20% of the power can be placed in each of the first-order sidebands. Functionality and characterization are presented within the sideband frequency region of 0.8–2.3 GHz, and it is shown that both methods can be applied beyond this frequency range. These methods provide a versatile and effective tool for atomic physics experiments.
Temperature-dependent optical measurements of the dominant recombination mechanisms in InAs/InAsSb type-2 superlattices
Temperature-dependent measurements of carrier recombination rates using a time-resolved optical pump-probe technique are reported for mid-wave infrared InAs/InAs{sub 1−x}Sb{sub x} type-2 superlattices (T2SLs). By engineering the layer widths and alloy compositions, a 16 K band-gap of ∼235 ± 10 meV was achieved for five unintentionally and four intentionally doped T2SLs. Carrier lifetimes were determined by fitting lifetime models based on Shockley-Read-Hall (SRH), radiative, and Auger recombination processes to the temperature and excess carrier density dependent data. The minority carrier (MC), radiative, and Auger lifetimes were observed to generally increase with increasing antimony content and decreasing layer thickness for the unintentionally doped T2SLs. The MC lifetime is limited by SRH processes at temperatures below 200 K in the unintentionally doped T2SLs. The extracted SRH defect energy levels were found to be near mid-bandgap. Also, it is observed that the MC lifetime is limited by Auger recombination in the intentionally doped T2SLs with doping levels greater than n ∼ 10{sup 16} cm{sup −3}.
Optical-optical double resonance, laser induced fluorescence, and revision of the signs of the spin-spin constants of the boron carbide (BC) free radical
The cold boron carbide free radical (BC X {sup 4}Σ{sup −}) has been produced in a pulsed discharge free jet expansion using a precursor mixture of trimethylborane in high pressure argon. High resolution laser induced fluorescence spectra have been obtained for the B {sup 4}Σ{sup −}–X {sup 4}Σ{sup −} and E {sup 4}Π–X {sup 4}Σ{sup −} band systems of both {sup 11}BC and {sup 10}BC. An optical-optical double resonance (OODR) scheme was implemented to study the finer details of both band systems. This involved pumping a single rotational level of the B state with one laser and then recording the various allowed transitions from the intermediate B state to the final E state with a second laser by monitoring the subsequent E–X ultraviolet fluorescence. In this fashion, we were able to prove unambiguously that, contrary to previous studies, the spin-spin constant λ is negative in the ground state and positive in the B {sup 4}Σ{sup −} excited state. It has been shown that λ″ < 0 is in fact expected based on a semiempirical second order perturbation theory calculation of the magnitude of the spin-spin constant. The OODR spectra have also been used to validate our assignments of the complex and badly overlapped E {sup 4}Π–X {sup 4}Σ{sup −} 0-0 and 1-0 bands of {sup 11}BC. The E–X 0-0 band of {sup 10}BC was found to be severely perturbed. The ground state main electron configuration is …3σ{sup 2}4σ{sup 2}5σ{sup 1}1π{sup 2}2π{sup 0} and the derived bond lengths show that there is a 0.03 Å contraction in the B state, due to the promotion of an electron from the 4σ antibonding orbital to the 5σ bonding orbital. In contrast, the bond length elongates by 0.15 Å in the E state, a result of promoting an electron from the 5σ bonding orbital to the 2π antibonding orbitals.
Optical shielding of nickel nanoparticle by a bubble: Optical limiting gets limited
We have demonstrated that in a nickel nanoparticle colloid, the optical limiting action reduces if a vapor bubble forms around the nanoparticle. The energy-dependent transmission and z-scan measurements on nickel nanoparticles in toluene show the onset of an additional process. At high fluence excitation, the particle becomes less visible to the later part of the incoming pulse due to the heat generated bubble formed around it. We have proposed a simple “particle-in-bubble” model which fits the optical limiting and z-scan curves quite well. Using this model, we have also estimated that the bubble radius increases at a rate of 4.5 m/s.
Optical spectroscopy and band gap analysis of hybrid improper ferroelectric Ca{sub 3}Ti{sub 2}O{sub 7}
We bring together optical absorption spectroscopy, photoconductivity, and first principles calculations to reveal the electronic structure of the room temperature ferroelectric Ca{sub 3}Ti{sub 2}O{sub 7}. The 3.94 eV direct gap in Ca{sub 3}Ti{sub 2}O{sub 7} is charge transfer in nature and noticeably higher than that in CaTiO{sub 3} (3.4 eV), a finding that we attribute to dimensional confinement in the n = 2 member of the Ruddlesden-Popper series. While Sr substitution introduces disorder and broadens the gap edge slightly, oxygen deficiency reduces the gap to 3.7 eV and gives rise to a broad tail that persists to much lower energies.
Measurements of the effective electron density in an electron beam ion trap using extreme ultraviolet spectra and optical imaging
In an electron beam ion trap (EBIT), the ions are not confined to the electron beam, but rather oscillate in and out of the beam. As a result, the ions do not continuously experience the full density of the electron beam. To determine the effective electron density, n e,eff , experienced by the ions, the electron beam size, the nominal electron density n e , and the ion distribution around the beam, i.e., the so-called ion cloud, must be measured. We use imaging techniques in the extreme ultraviolet (EUV) and optical to determine these. The electron beam width is measured using 3 d → 3 p emission from Fe xii and xiii between 185 and 205 Å. These transitions are fast and the EUV emission occurs only within the electron beam. The measured spatial emission profile and variable electron current yield a nominal electron density range of n e ~ 10 11 –10 13 cm –3 . We determine the size of the ion cloud using optical emission from metastable levels of ions with radiative lifetimes longer than the ion orbital periods. Here, the resulting emission maps out the spatial distribution of the ion cloud. We find a typical electron beam radius of ~60 μm and an ion cloud radius of ~300 μ m. These yield a spatially averaged effective electron density, ne,eff, experienced by the ions in EBIT spanning ~ 5 × 10 9 –5 × 10 11 cm –3 .
Dynamic absorption in optical pyrometry of hot spots in plastic-bonded triaminotrinitrobenzene [Optical Pyrometry of Shock-induced Hot Spots in Plastic-bonded Triaminotrinitrobenzene]
Herein we demonstrate a methodology for measuring optical pyrometry in environments which are disadvantageous for typical pyrometery applications by introducing additional fit parameters to account for absorption or emission which convolutes the thermal spectrum. Emission spectra from a plastic-bonded formulation of triaminotrinitrobenzene (TATB) shocked by 2-4 km s -1 impacts with Al flyer plates show significant deviations from graybody behavior. To extract reliable temperatures via optical pyrometry, we fit the spectra to a combination of a graybody and either a Gaussian absorption or emission spectrum. We found that the absorption needed to fit the data corresponds well with the known pressure-dependent absorption of TATB, and that the absorption model gives temperatures and emissivities in line with other explosives. By contrast, emission gives temperatures too low and emissivities that decrease as more material reacts. We conclude the nonthermal part of the spectrum is dominated by the absorption of unreacted TATB, and accurate pyrometry of TATB must use either our graybody plus absorption model or must limit the spectral range of observation to above 650 nm.
Electronic, direct optical, and phonon-assisted optical properties of 4H Si from first principles
The cubic polytype of silicon (Si) is the most commercialized semiconductor material and finds applications in numerous electronic and optoelectronic devices, such as solar cells. However, recent reports on the synthesis of the hexagonal 4H Si polytype have attracted the attention of the scientific community to understand its functional properties. Here, we report the electronic, vibrational, and optical properties of the 4H Si polytype obtained with predictive first-principles calculations, with an emphasis of phonon-assisted absorption in the indirect regime. Compared to the cubic polytype, 4H Si shows a slightly narrower indirect gap by ∼0.05 eV. The calculated phonon-assisted optical spectra show that 4H Si exhibits a stronger absorption coefficient than cubic Si across the visible and IR spectral regions. We further evaluate the short-circuit current density of textured thin-films. We demonstrate that 4H Si can achieve the same short-circuit current density for a five times thinner film compared to the cubic polytype, which mainly resulted from absorption in the indirect gap regime. Our work demonstrates the advantages of 4H Si for thin-film silicon-based solar-cell applications.
Examining astrophysical gas cloud collapse using an optical depth-scaled, x-ray-irradiated, carbon-foam sphere
When stellar radiation interacts with a molecular cloud, the cloud's fate depends on the strength of the incident radiation and the radiation's mean-free-path within the cloud [F. Bertoldi, Astrophys. J. 346, 735–755 (1989)]. Under the right conditions, the radiation compresses the cloud and a star formation may occur. Where and when the stellar formation occurs in the cloud's collapse are open questions. Direct observation of the complete star–cloud lifecycle is nearly impossible due to the immense timescales and distances over which the interaction occurs. Laboratory astrophysics offers a way to investigate such a system by scaling the important astrophysical parameters to the laboratory. This work describes laboratory experiments to study the radiation-driven implosion of clouds, using x rays from a laser-irradiated, thin, gold foil as a surrogate star and a carbon-foam sphere as a surrogate cloud. An optically thick system, theoretically corresponding to a star-forming regime, was selected by choice of the foam density. Gold foil and sphere motions were imaged by x-ray radiography. Radiographic images show the formation of an interface between rarefied gold and carbon plasmas, a shock moving into the sphere, and a blunting of the initial sphere's shape. Measurements show that the shock moved linearly around 64 μm/ns into the sphere, and the gold–carbon interface formed by 2 ns at the sphere edge remained stationary. The deformation of the sphere was driven by the incident radiation and not by mechanical pressures applied by gold plasma. The blunting of the sphere was likely due to the geometric reduction of flux near the sphere's poles. Higher x-ray flux near the sphere's equator caused high compression and a faster shock, which flattened the sphere. We will discuss the results and implications of our observations.