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Using the Gemini Planet Imager located at Gemini South, we measured the near-infrared (1.0–2.4 μm) spectrum of the planetary companion to the nearby, young star β Pictoris. We compare the spectrum obtained with currently published model grids and with known substellar objects and present the best matching models as well as the best matching observed objects. Comparing the empirical measurement of the bolometric luminosity to evolutionary models, we find a mass of 12.9 ± 0.2 M{sub Jup}, an effective temperature of 1724 ± 15 K, a radius of 1.46 ± 0.01 R{sub Jup}, and a surface gravity of logg=4.18±0.01 [dex] (cgs). The stated uncertainties are statistical errors only, and do not incorporate any uncertainty on the evolutionary models. Using atmospheric models, we find an effective temperature of 1700–1800 K and a surface gravity of logg=3.5–4.0 [dex] depending upon the model. These values agree well with other publications and with “hot-start” predictions from planetary evolution models. Further, we find that the spectrum of β Pic b best matches a low surface gravity L2 ± 1 brown dwarf. Finally, comparing the spectrum to field brown dwarfs, we find the the spectrum best matches 2MASS J04062677–381210 and 2MASS J03552337+1133437.
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We report the synthesis and structural characterization of the new Ir holladite, Rb{sub 0.17}IrO{sub 2}. Rb{sub 0.17}IrO{sub 2} crystallizes in the tetragonal hollandite structure. In contrast to the previously reported monoclinic Ir hollandite K{sub 0.25}IrO{sub 2}, we do not observe a difference in Ir–O bond lengths in Rb{sub 0.17}IrO{sub 2} and thus find Ir in an average oxidation state of + 3.83. We also report and compare the electronic and magnetic properties of Rb{sub 0.17}IrO{sub 2} and K{sub 0.25}IrO{sub 2}, finding that they are both metallic and Pauli paramagnets further supporting that the electrons are delocalized in the Ir 5d states. - Graphical abstract: Crystal structure of Rb{sub 0.17}IrO{sub 2} (right), and the SEM image of Rb{sub 0.17}IrO{sub 2}, showing the growth of thin needles (left). Display Omitted - Highlights: • New iridium hollandite. • Naturally grows in very thin wires. • Elementary physical properties of Ir holladites reported for the first time metallic conductor and paramagnetic.
The performance of catalysts depends on their nanoscale properties, and local variations in structure and composition can have a dramatic impact on the catalytic reactivity. Therefore, probing the localized reactivity of catalytic surfaces using high spatial resolution vibrational spectroscopy, such as infrared (IR) nanospectroscopy and tip-enhanced Raman spectroscopy, is essential for mapping their reactivity pattern. Two fundamentally different scanning probe IR nanospectroscopy techniques, namely, scattering-type scanning near-field optical microscopy (sSNOM) and atomic force microscopy-infrared spectroscopy (AFM-IR), provide the capabilities for mapping the reactivity pattern of catalytic surfaces with a spatial resolution of ~20 nm. Herein, we compare these two techniques with regard to their applicability for probing the vibrational signature of reactive molecules on catalytic nanoparticles. For this purpose, we use chemically addressable self-assembled molecules on Au nanoparticles as model systems. We identified significant spectral differences depending on the measurement technique, which originate from the fundamentally different working principles of the applied methods. While AFM-IR spectra provided information from all the molecules that were positioned underneath the tip, the s-SNOM spectra were more orientation-sensitive. Due to its field-enhancement factor, the s-SNOM spectra showed higher vibrational signals for dipoles that were perpendicularly oriented to the surface. The s-SNOM sensitivity to the molecular orientation influenced the amplitude, position, and signal-to-noise ratio of the collected spectra. Ensemble-based IR measurements verified that differences in the localized IR spectra stem from the enhanced sensitivity of s-SNOM measurements to the adsorption geometry of the probed molecules.
Rare-earth pyrochlore iridates ( RE 2 Ir 2 O 7 ) consist of two interpenetrating cation sublattices, the RE with highly frustrated magnetic moments, and the iridium with extended conduction orbitals significantly mixed by spin-orbit interactions. The coexistence and coupling of these two sublattices create a landscape for discovery and manipulation of quantum phenomena such as the topological Hall effect, massless conduction bands, and quantum criticality. Thin films allow extended control of the material system via symmetry-lowering effects such as strain. While bulk Pr 2 Ir 2 O 7 shows a spontaneous hysteretic Hall effect below 1.5 K, we observe the effect at elevated temperatures up to 15 K in epitaxial thin films on (111) yttria-stabilized zirconia (YSZ) substrates synthesized via solid-phase epitaxy. Similar to the bulk, the lack of observable long-range magnetic order in the thin films points to a topological origin. We use synchrotron-based element-specific x-ray diffraction and x-ray magnetic circular dichroism to compare powders and thin films to attribute the spontaneous Hall effect in the films to localization of the Ir moments. Further, we link the thin-film Ir local moments to lattice distortions absent in the bulklike powders. We conclude that the elevated-temperature spontaneous Hall effect is caused by the topological effect originating either from the Ir or Pr sublattice, with interaction strength enhanced by the Ir local moments. This spontaneous Hall effect with weak net moment highlights the effect of vanishingly small lattice distortions as a means to discover topological phenomena in metallic frustrated magnetic materials.
Two pellets of iridium salt were irradiated at the center of the Flattop critical assembly, one at low neutron flux and the other at high flux. After that two counting samples were prepared from each pellet following a given chemical procedure. Measurements of the four counting samples were carried out with two high-resolution silicon drift detectors for over a year. Pulse height spectra of the L→M X-rays from 193 m Ir and 192 Ir were approximated with a Voigt function and the ratio of produced 193 m Ir and 192 Ir nuclei obtained. The 193 m Ir/ 192 Ir ratios from each measured spectrum are compared to identify possible systematic deviations.
A highly accurate CO 2 ab initio dipole moment surface (DMS), Ames-2021, is reported along with 12 C 16 O 2 infrared (IR) intensity comparisons approaching a 1–4‰ level of agreement and uncertainty. The Ames-2021 DMS was accurately fitted from CCSD(T) finite-field dipoles computed with the aug-cc-pVXZ (X = T, Q, 5) basis for C atom and the d-aug-cc-pVXZ (X = T, Q, 5) basis for O atoms, and extrapolated to the one particle basis set limit. Fitting σ(rms) is 3.8 × 10^(–7) au for 4443 geometries below 15 000 per cm . The corresponding IR intensity, S Ames-2021 , are computed using the Ames-2 potential energy surface (PES), which is the best PES available for CO 2 . Compared to high accuracy IR studies for 2001i–00001 and 3001i–00001 bands, S Ames-2021 matches NIST experiment-based intensities [S NIST-HIT16 or S HIT20 ] to −1.0 ± 1.3‰, or matches DLR experiment-based intensities [S DLR-HIT16/UCL/Ames ] to 1.9 ± 3.7‰. This indicates the systematic deviations and uncertainties have been significantly reduced in S Ames-2021 . The S UCL2015 (or S HITRAN2016 ) have larger deviations (vs S DLR ) and uncertainties (vs S DLR , S NIST ) which are attributed to the less accurate Ames-1 PES adopted in UCL-296 line list calculation. The S Ames-2021 intensity of 12 C 16 O 2 and 13 C 16 O 2 is utilized to derive new absolute 13 C/ 12 C ratios for Vienna PeeDee Belemnite (VPDB) with uncertainty reduced by 1/3 or 2/3. Further evaluation of S Ames-2021 are carried out on those CO 2 bands discussed in the HITRAN2020 update paper. Consistent improvements and better accuracies are found in band-by-band analysis, except for those bands strongly affected by Coriolis couplings, or very weak bands measured with relatively larger experimental uncertainties. The Ames-2021 296 K IR line lists are generated for 13 CO 2 isotopologues, with 18,000 per and S 296K > 1E–31) cm/molecule cutoff and then combined with CDSD line positions (except 14 C 16 O 2 ). The Ames-2021 DMS and 296 K IR line lists represent a major improvement over previous CO 2 theoretical IR intensity studies, including Ames-2016, UCL-296, and recent UCL DMS 2021 update. A real 1 permille level of agreement and uncertainty will definitely require both more accurate PES and more accurate DMS.
Abstract We report a novel dual‐IR window/electrode operando infrared (IR) spectroscopy method for battery research. In addition to keeping all the features of the in‐situ/operando IR spectroscopic methodologies for batteries reported in the literature so far, the dual‐IR window/electrode configuration reported herein offers a unique advantage of accessing both, anode and cathode processes quasi‐simultaneously by rotating the dual‐window/electrode IR battery cell 180° step‐wise in the same operando real‐battery‐like cell. The proof‐of‐concept studies demonstrated clearly its investigative advantages in gaining broader insights into the chemistry of batteries during charging/discharging and beyond.
Dynamics of imidazole (IM) and 1-methylimidazole (1-MeIM) in the liquid phase at 95 °C were studied by IR polarization selective pump-probe (PSPP) and two-dimensional IR (2D IR) spectroscopies. The two molecules are very similar structurally except that IM can be simultaneously a hydrogen bond donor and acceptor and therefore forms extended hydrogen bonded networks. The broader IR absorption spectrum and shorter vibrational lifetime of the vibrational probe, selenocyanate anion (SeCN – ), in IM vs. 1-MeIM indicate that stronger hydrogen bonding exists between SeCN – and IM. Molecular dynamics (MD) simulations support the strong hydrogen bond formation between SeCN – and IM via the HN moiety. SeCN – makes two H-bonds with IM; it is inserted in the IM H-bonded chains rather than being a chain terminator. The strong hydrogen bonding influenced the reorientation dynamics of SeCN – in IM, leading to more restricted short time angular sampling (wobbling-in-a-cone). The complete orientational diffusion time in IM is 1.7 times slower than in 1-MeIM, but the slowdown is less than expected, considering the 3-fold larger viscosity of IM. The jump reorientation mechanism accounts for the anomalously fast orientational relaxation in IM, and the MD simulations determined the average jump angle of the probe between hydrogen bonding sites. Spectral diffusion time constants obtained from the 2D IR experiments are only modestly slower in IM than in 1-MeIM in spite of the significant increase in viscosity. Here, the results indicate that the spectral diffusion sensed by the SeCN – has IM hydrogen bond dynamics contributions not present in 1-MeIM.
LRLL 54361 is an infrared source located in the star-forming region IC 348 SW. Remarkably, its infrared luminosity increases by a factor of 10 over roughly one week every 25.34 days. To understand the origin of these remarkable periodic variations, we obtained sensitive 3.3 cm JVLA radio continuum observations of LRLL 54361 and its surroundings in six different epochs: three of them during the IR-on state and three during the IR-off state. The radio source associated with LRLL 54361 remained steady and did not show a correlation with the IR variations. We suggest that the IR is tracing the results of fast (with a timescale of days) pulsed accretion from an unseen binary companion, while the radio traces an ionized outflow with an extent of ∼100 AU that smooths out the variability over a period of the order of a year. The average flux density measured in these 2014 observations, 27 ± 5 μJy, is about a factor of two less than that measured about 1.5 years before, 53 ± 11 μJy, suggesting that variability in the radio is present, but over larger timescales than in the IR. We discuss other sources in the field, in particular two infrared/X-ray stars that show rapidly varying gyrosynchrotron emission.
One of the main degradation mechanisms of hydrous iridium oxide acidic oxygen evolution reaction (OER) catalysts is dissolution and loss into the acidic membrane. While degradation models have been proposed, there is a gap in understanding the potential and time dependence of the iridium dissolution reaction and its mechanistic underpinnings. In this work, Ir dissolution rates measured as a function of time and potential via time-resolved inductively-coupled plasma mass spectrometry (ICP-MS) in aqueous acidic electrolyte are used to establish a mathematical model for Ir dissolution. The mathematical model is generated using proposed formation and dissolution reactions for Ir species. Through comparison with the ICP-MS data and existing information on the potential-dependent Ir phase, we find that the potential and time-dependence of dissolution can be modeled as dissolution of an oxide phase, here represented as IrO 2 , with potential dependent kinetics and formation of a passivating species, a process with a rate-limiting step that is not potential dependent. This understanding of the potential dependence of dissolution and passivation kinetics using aqueous electrolyte half-cell measurements can be used to predict the degradation of Ir oxide in operating energy conversion devices relying on the OER, such as proton-exchange membrane water electrolyzers.
We perform a systematic investigation on the effects of Ba and La doping on the lattice and transport properties of Sr{sub 2}IrO{sub 4}, which is theoretically predicted to be a host compound of high-temperature superconductivity. We observe a drastic straightening of the Ir–O–Ir bond angle in the Ba-doped samples. The straightening of the bond angle is much weaker in the La-doped samples. It is found that the La doping leads to the introduction of electron-type charge carriers, while the charge carrier concentration does not change too much in the Ba-doped samples. As a result, both the resistivity and the magnetic moments decrease much faster in the La-doped samples, compared to those in the Ba-doped samples. The present results suggest that it is the charge carrier density rather than the Ir–O–Ir bond angle that dominates the magnetic and transport properties of the Sr{sub 2}IrO{sub 4} system.
In this review fundamentals of optical parametric oscillator and different phase matching situation have been discussed. Requirement of nonlinear crystal and properties of some mid-IR and IR transmitting crystal have been discussed. Present status of generation of tunable radiation in mid-IR to IR spectral range by OPO based on ZnGeP{sub 2} crystal and other techniques and its applications has been discussed.
Here in this paper we report an IR-IR double resonance study of the structural landscape present in the Na + (glucose) complex. Our experimental approach involves minimal modifications to a typical IR predissociation setup, and can be carried out via ion-dip or isomer-burning methods, providing additional flexibility to suit different experimental needs. In the current study, the single-laser IR predissociation spectrum of Na + (glucose), which clearly indicates contributions from multiple structures, was experimentally disentangled to reveal the presence of three α-conformers and five β-conformers. Comparisons with calculations show that these eight conformations correspond to the lowest energy gas-phase structures with distinctive Na+ coordination.