skip to main content

This content will become publicly available on October 4, 2023

Title: Assigning quantum labels and improving accuracy for the ro-vibrational eigenstates of H3+ calculated using ScalIT
In a recent article [AIP Adv. 11, 045033 (2021)], we carried out exact quantum dynamical calculations and computed ro-vibrational energy levels and wave functions for the H 3 + molecular ion up to the dissociation threshold (at J = 46) using a recently developed potential energy surface (PES) [Mol. Phys. 117, 1663 (2019)]—arguably, the most accurate to date —together with the ScalIT suite of parallel codes. In this work, we further improved the convergence accuracy and range of our ScalIT calculations for all J values up to J = 20 to a few 10 –5  cm −1 (or better). In addition, we performed an ab initio assignment of the ro-vibrational energy levels, providing vibrational ‘ v 1 , v 2 , | l |’ and rotational ‘ J , G , U , K ’ quantum labels for more than 2,200 ro-vibrational states, including every single 0 ≤ J ≤ 20 state up to and above the barrier to linearity at 10,000 cm −1 . The main underlying motivation of our work is to provide a list of reliably labeled, spectroscopically accurate energy levels in a format that can be used in spectroscopic line lists, which are based on both experimental more » and theoretical levels. Such line lists are of huge importance in various astrochemical and astrophysical contexts. « less
Award ID(s):
Publication Date:
Journal Name:
Frontiers in Physics
Sponsoring Org:
National Science Foundation
More Like this
  1. Resonant tunneling diodes (RTDs) have come full-circle in the past 10 years after their demonstration in the early 1990s as the fastest room-temperature semiconductor oscillator, displaying experimental results up to 712 GHz and fmax values exceeding 1.0 THz [1]. Now the RTD is once again the preeminent electronic oscillator above 1.0 THz and is being implemented as a coherent source [2] and a self-oscillating mixer [3], amongst other applications. This paper concerns RTD electroluminescence – an effect that has been studied very little in the past 30+ years of RTD development, and not at room temperature. We present experiments and modeling of an n-type In0.53Ga0.47As/AlAs double-barrier RTD operating as a cross-gap light emitter at ~300K. The MBE-growth stack is shown in Fig. 1(a). A 15-μm-diam-mesa device was defined by standard planar processing including a top annular ohmic contact with a 5-μm-diam pinhole in the center to couple out enough of the internal emission for accurate free-space power measurements [4]. The emission spectra have the behavior displayed in Fig. 1(b), parameterized by bias voltage (VB). The long wavelength emission edge is at  = 1684 nm - close to the In0.53Ga0.47As bandgap energy of Ug ≈ 0.75 eV at 300 K.more »The spectral peaks for VB = 2.8 and 3.0 V both occur around  = 1550 nm (h = 0.75 eV), so blue-shifted relative to the peak of the “ideal”, bulk InGaAs emission spectrum shown in Fig. 1(b) [5]. These results are consistent with the model displayed in Fig. 1(c), whereby the broad emission peak is attributed to the radiative recombination between electrons accumulated on the emitter side, and holes generated on the emitter side by interband tunneling with current density Jinter. The blue-shifted main peak is attributed to the quantum-size effect on the emitter side, which creates a radiative recombination rate RN,2 comparable to the band-edge cross-gap rate RN,1. Further support for this model is provided by the shorter wavelength and weaker emission peak shown in Fig. 1(b) around = 1148 nm. Our quantum mechanical calculations attribute this to radiative recombination RR,3 in the RTD quantum well between the electron ground-state level E1,e, and the hole level E1,h. To further test the model and estimate quantum efficiencies, we conducted optical power measurements using a large-area Ge photodiode located ≈3 mm away from the RTD pinhole, and having spectral response between 800 and 1800 nm with a peak responsivity of ≈0.85 A/W at  =1550 nm. Simultaneous I-V and L-V plots were obtained and are plotted in Fig. 2(a) with positive bias on the top contact (emitter on the bottom). The I-V curve displays a pronounced NDR region having a current peak-to-valley current ratio of 10.7 (typical for In0.53Ga0.47As RTDs). The external quantum efficiency (EQE) was calculated from EQE = e∙IP/(∙IE∙h) where IP is the photodiode dc current and IE the RTD current. The plot of EQE is shown in Fig. 2(b) where we see a very rapid rise with VB, but a maximum value (at VB= 3.0 V) of only ≈2×10-5. To extract the internal quantum efficiency (IQE), we use the expression EQE= c ∙i ∙r ≡ c∙IQE where ci, and r are the optical-coupling, electrical-injection, and radiative recombination efficiencies, respectively [6]. Our separate optical calculations yield c≈3.4×10-4 (limited primarily by the small pinhole) from which we obtain the curve of IQE plotted in Fig. 2(b) (right-hand scale). The maximum value of IQE (again at VB = 3.0 V) is 6.0%. From the implicit definition of IQE in terms of i and r given above, and the fact that the recombination efficiency in In0.53Ga0.47As is likely limited by Auger scattering, this result for IQE suggests that i might be significantly high. To estimate i, we have used the experimental total current of Fig. 2(a), the Kane two-band model of interband tunneling [7] computed in conjunction with a solution to Poisson’s equation across the entire structure, and a rate-equation model of Auger recombination on the emitter side [6] assuming a free-electron density of 2×1018 cm3. We focus on the high-bias regime above VB = 2.5 V of Fig. 2(a) where most of the interband tunneling should occur in the depletion region on the collector side [Jinter,2 in Fig. 1(c)]. And because of the high-quality of the InGaAs/AlAs heterostructure (very few traps or deep levels), most of the holes should reach the emitter side by some combination of drift, diffusion, and tunneling through the valence-band double barriers (Type-I offset) between InGaAs and AlAs. The computed interband current density Jinter is shown in Fig. 3(a) along with the total current density Jtot. At the maximum Jinter (at VB=3.0 V) of 7.4×102 A/cm2, we get i = Jinter/Jtot = 0.18, which is surprisingly high considering there is no p-type doping in the device. When combined with the Auger-limited r of 0.41 and c ≈ 3.4×10-4, we find a model value of IQE = 7.4% in good agreement with experiment. This leads to the model values for EQE plotted in Fig. 2(b) - also in good agreement with experiment. Finally, we address the high Jinter and consider a possible universal nature of the light-emission mechanism. Fig. 3(b) shows the tunneling probability T according to the Kane two-band model in the three materials, In0.53Ga0.47As, GaAs, and GaN, following our observation of a similar electroluminescence mechanism in GaN/AlN RTDs (due to strong polarization field of wurtzite structures) [8]. The expression is Tinter = (2/9)∙exp[(-2 ∙Ug 2 ∙me)/(2h∙P∙E)], where Ug is the bandgap energy, P is the valence-to-conduction-band momentum matrix element, and E is the electric field. Values for the highest calculated internal E fields for the InGaAs and GaN are also shown, indicating that Tinter in those structures approaches values of ~10-5. As shown, a GaAs RTD would require an internal field of ~6×105 V/cm, which is rarely realized in standard GaAs RTDs, perhaps explaining why there have been few if any reports of room-temperature electroluminescence in the GaAs devices. [1] E.R. Brown,et al., Appl. Phys. Lett., vol. 58, 2291, 1991. [5] S. Sze, Physics of Semiconductor Devices, 2nd Ed. 12.2.1 (Wiley, 1981). [2] M. Feiginov et al., Appl. Phys. Lett., 99, 233506, 2011. [6] L. Coldren, Diode Lasers and Photonic Integrated Circuits, (Wiley, 1995). [3] Y. Nishida et al., Nature Sci. Reports, 9, 18125, 2019. [7] E.O. Kane, J. of Appl. Phy 32, 83 (1961). [4] P. Fakhimi, et al., 2019 DRC Conference Digest. [8] T. Growden, et al., Nature Light: Science & Applications 7, 17150 (2018). [5] S. Sze, Physics of Semiconductor Devices, 2nd Ed. 12.2.1 (Wiley, 1981). [6] L. Coldren, Diode Lasers and Photonic Integrated Circuits, (Wiley, 1995). [7] E.O. Kane, J. of Appl. Phy 32, 83 (1961). [8] T. Growden, et al., Nature Light: Science & Applications 7, 17150 (2018).« less
  2. Abstract
    Site description. This data package consists of data obtained from sampling surface soil (the 0-7.6 cm depth profile) in black mangrove (Avicennia germinans) dominated forest and black needlerush (Juncus roemerianus) saltmarsh along the Gulf of Mexico coastline in peninsular west-central Florida, USA. This location has a subtropical climate with mean daily temperatures ranging from 15.4 °C in January to 27.8 °C in August, and annual precipitation of 1336 mm. Precipitation falls as rain primarily between June and September. Tides are semi-diurnal, with 0.57 m median amplitudes during the year preceding sampling (U.S. NOAA National Ocean Service, Clearwater Beach, Florida, station 8726724). Sea-level rise is 4.0 ± 0.6 mm per year (1973-2020 trend, mean ± 95 % confidence interval, NOAA NOS Clearwater Beach station). The A. germinans mangrove zone is either adjacent to water or fringed on the seaward side by a narrow band of red mangrove (Rhizophora mangle). A near-monoculture of J. roemerianus is often adjacent to and immediately landward of the A. germinans zone. The transition from the mangrove to the J. roemerianus zone is variable in our study area. An abrupt edge between closed-canopy mangrove and J. roemerianus monoculture may extend for up to several hundred metersMore>>
  3. By combining a newly developed two-color laser pulsed field ionization-photoion (PFI-PI) source and a double-quadrupole–double-octopole (DQDO) mass spectrometer, we investigated the integral cross sections ( σ s) of the vanadium cation (V + ) toward the activation of CO 2 in the center-of-mass kinetic energy ( E cm ) range from 0.1 to 10.0 eV. Here, V + was prepared in single spin–orbit levels of its lowest electronic states, a 5 D J ( J = 0–4), a 5 F J ( J = 1–5), and a 3 F J ( J = 2–4), with well-defined kinetic energies. For both product channels VO + + CO and VCO + + O identified, V + (a 3 F 2,3 ) is found to be greatly more reactive than V + (a 5 D 0,2 ) and V + (a 5 F 1,2 ), suggesting that the V + + CO 2 reaction system mainly proceeds via a “weak quintet-to-triplet spin-crossing” mechanism favoring the conservation of total electron spins. In addition, no J -state dependence was observed. The distinctive structures of the quantum electronic state selected integral cross sections observed as a function of E cm and the electronic state of themore »V + ion indicate that the difference in the chemical reactivity of the title reaction originated from the quantum-state instead of energy effects. Furthermore, this work suggests that the selection of the quantum electronic states a 3 F J ( J = 2–4) of the transition metal V + ion can greatly enhance the efficiency of CO 2 activation.« less
  4. We present a multiline survey of the interstellar medium (ISM) in two z  > 6 quasar host galaxies, PJ231−20 ( z  = 6.59) and PJ308−21 ( z  = 6.23), and their two companion galaxies. Observations were carried out using the Atacama Large (sub-)Millimeter Array (ALMA). We targeted 11 transitions including atomic fine-structure lines (FSLs) and molecular lines: [NII] 205 μm , [CI] 369 μm , CO ( J up  = 7, 10, 15, 16), H 2 O 3 12  − 2 21 , 3 21  − 3 12 , 3 03  − 2 12 , and the OH 163 μm doublet. The underlying far-infrared (FIR) continuum samples the Rayleigh-Jeans tail of the respective dust emission. By combining this information with our earlier ALMA [CII] 158 μm observations, we explored the effects of star formation and black hole feedback on the ISM of the galaxies using the CLOUDY radiative transfer models. We estimated dust masses, spectral indexes, IR luminosities, and star-formation rates from the FIR continuum. The analysis of the FSLs indicates that the [CII] 158 μm and [CI] 369 μm emission arises predominantly from the neutral medium in photodissociation regions (PDRs). We find that line deficits agree with those of local luminous IR galaxies. The CO spectral line energy distributions (SLEDs) reveal significant high- J COmore »excitation in both quasar hosts. Our CO SLED modeling of the quasar PJ231−20 shows that PDRs dominate the molecular mass and CO luminosities for J up  ≤ 7, while the J up  ≥ 10 CO emission is likely driven by X-ray dissociation regions produced by the active galactic nucleus (AGN) at the very center of the quasar host. The J up  > 10 lines are undetected in the other galaxies in our study. The H 2 O 3 21  − 3 12 line detection in the same quasar places this object on the L H 2 O  −  L TIR relation found for low- z sources, thus suggesting that this water vapor transition is predominantly excited by IR pumping. Models of the H 2 O SLED and of the H 2 O-to-OH 163 μm ratio point to PDR contributions with high volume and column density ( n H  ∼ 0.8 × 10 5 cm −3 , N H  = 10 24 cm −2 ) in an intense radiation field. Our analysis suggests a less highly excited medium in the companion galaxies. However, the current data do not allow us to definitively rule out an AGN in these sources, as suggested by previous studies of the same objects. This work demonstrates the power of multiline studies of FIR diagnostics in order to dissect the physical conditions in the first massive galaxies emerging from cosmic dawn.« less
  5. Direct detection of gravitational waves (GWs) on 17 August 2017, propagating from a binary neutron star merger, or a “kilonova”, opened the era of multimessenger astronomy. The ejected material from neutron star mergers, or “kilonova”, is a good candidate for optical and near infrared follow-up observations after the detection of GWs. The kilonova from the ejecta of GW1780817 provided the first evidence for the astrophysical site of the synthesis of heavy nuclei through the rapid neutron capture process or r-process. Since properties of the emission are largely affected by opacities of the ejected material, enhancements in the available r-process data is important for neutron star merger modeling. However, given the complexity of the electronic structure of these heavy elements, considerable efforts are still needed to converge to a reliable set of atomic structure data. The aim of this work is to alleviate this situation for low charge state elements in the Os-like isoelectronic sequence. In this regard, the general-purpose relativistic atomic structure packages (GRASP0 and GRASP2K) were used to obtain energy levels and transition probabilities (E1 and M1). We provide line lists and expansion opacities for a range of r-process elements. We focus here on the Os isoelectronic sequence (Osmore »I, Ir II, Pt III, Au IV, Hg V). The results are benchmarked against existing experimental data and prior calculations, and predictions of emission spectra relevant to kilonovae are provided. Fine-structure (M1) lines in the infrared potentially observable by the James Webb Space Telescope are highlighted.« less