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At least 307 records · Page 17

Charge density waves on a half-filled decorated honeycomb lattice

Tight binding models like the Hubbard Hamiltonian are most often explored in the context of uniform intersite hopping $\textit{t}$. The electron-electron interactions, if sufficiently large compared to this translationally invariant $\textit{t}$, can give rise to ordered magnetic phases and Mott insulator transitions, especially at commensurate filling. The more complex situation of nonuniform $\textit{t}$ has been studied within a number of situations, perhaps most prominently in multiband geometries where there is a natural distinction of hopping between orbitals of different degree of overlap. In this paper we explore related questions arising from the interplay of multiple kinetic energy scales and electron-phonon interactions. Specifically, we use determinant quantum Monte Carlo (DQMC) to solve the half-filled Holstein Hamiltonian on a “decorated honeycomb lattice,” consisting of hexagons with internal hopping $\textit{t}$ coupled together by $\textit{t'}$. This modulation of the hopping introduces a gap in the Dirac spectrum and affects the nature of the topological phases. Here, we determine the range of $\textit{t/t'}$ values which support a charge density wave phase about the Dirac point of uniform hopping $\textit{t = t'}$, as well as the critical transition temperature $T_c$. The QMC simulations are compared with the results of mean field theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ab initio calculations in atoms, molecules, and solids, treating spin–orbit coupling and electron interaction on an equal footing

We incorporate explicit, non-perturbative treatment of spin–orbit coupling into ab initio auxiliary-field quantum Monte Carlo (AFQMC) calculations. The approach allows a general computational framework for molecular and bulk systems in which material specificity, electron correlation, and spin–orbit coupling effects can be captured accurately and on an equal footing, with favorable computational scaling vs system size. We adopt relativistic effective-core potentials that have been obtained by fitting to fully relativistic data and that have demonstrated a high degree of reliability and transferability in molecular systems. This results in a two-component spin-coupled Hamiltonian, which is then treated by generalizing the ab initio AFQMC approach. We demonstrate the method by computing the electron affinity in Pb, the bond dissociation energy in Br 2 and I 2 , and solid Bi.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the Electronic Structure of [B 10 H 10 ] 2– Dianion Encapsulated by an Octamethylcalix[4]pyrrole Molecule

Despite being an important closo-borate in the condensed phase boron chemistry, isolated B 10 H 10 2- is electronically unstable and has never been detected in the gas phase. Herein, we report a successful capture of this fleeting species through binding with an octamethylcalix[4]pyrrole (omC4P) molecule to form a stable gaseous omC4P·[B 10 H 10 ] 2- complex and its characterizations utilizing negative ion photoelectron spectroscopy (NIPES). The recorded NIPE spectrum, contributed from both omC4P and [B 10 H 10 ] 2- , is deconvoluted by subtracting the omC4P contribution to yield a [B 10 H 10 ] 2- spectrum. The obtained [B 10 H 10 ] 2- spectrum consists of four major bands spanning electron binding energy (EBE) range from 1 to 5 eV with the EBE gaps matching excellently with the energy intervals of computed highly lying occupied molecular orbitals of the B 10 H 10 2- dianion. Finally, this study showcases a generic method to utilize omC4P to capture unstable multiply charged anions in the gas phase for experimental determination of their electronic structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Determination of the spin and parity of all-charm tetraquarks

The traditional quark model accounts for the existence of baryons, such as protons and neutrons, which consist of three quarks, as well as mesons, composed of a quark–antiquark pair. Only recently has substantial evidence started to accumulate for exotic states composed of four or five quarks and antiquarks. The exact nature of their internal structure remains uncertain. Here we report the first measurement of quantum numbers of the recently discovered family of three all-charm tetraquarks, using data collected by the CMS experiment at the Large Hadron Collider from 2016 to 2018 . The angular analysis techniques developed for the discovery and characterization of the Higgs boson have been applied to the new exotic states. Here we show that the quantum numbers for parity P and charge conjugation C symmetries are found to be +1. The spin J of these exotic states is determined to be consistent with 2ħ, while 0ħ and 1ħ are excluded at 95% and 99% confidence levels, respectively. The J PC = 2 ++ assignment implies particular configurations of constituent spins and orbital angular momenta, which constrain the possible internal structure of these tetraquarks.

Physics↗

Using Geophysical Technologies Deployed in Inexpensive Monitoring Wells to Monitor the Evolution of a CO 2 Plume: Potential Benefits and R&D Needs

This report demonstrates the potential benefits of an R&D program designed to substantially decrease the cost of drilling monitoring wells. The study determines the costs of monitoring a commercial-scale CO 2 storage project's CO 2 plume using a vertical seismic profile (VSP) array. The VSP array consists of permanent surface orbital vibrator (SOV) seismic sources and distributed acoustic sensing (DAS) fiber optic cable receivers permanently installed in shallow monitoring wells. Several scenarios are assessed varying the costs of drilling monitoring wells for DAS to evaluate the potential benefits of an R&D program to lower well costs. The monitoring costs of VSP are compared against those of 4-D seismic surveys which deploy temporary seismic sources and receivers. If the cost of monitoring wells can be lowered about 50%, VSP monitoring is a more attractive cost option than 4-D seismic for CO 2 plume monitoring, warranting future R&D efforts to lower these costs.

58 GEOSCIENCES↗

Beam dynamics corrections to the Run-1 measurement of the muon anomaly $a_{\mu}$ at Fermilab

The Fermi National Accelerator Laboratory (FNAL) Muon $g\!-\!2$ Experiment has measured the positive muon magnetic anomaly $a_{\mu} \equiv (g_{\mu}-2)/2$ with a precision of 0.46 parts per million, with data collected during its first physics run in 2018. The experimental result combined with the measurement from the former experiment at Brookhaven National Laboratory increases the tension with the Standard Model expectation to $4.2\sigma$, thus strengthening evidence for new physics.The magnetic anomaly is determined from the precision measurements of the muon spin precession frequency, relative to the muon momentum, and the average magnetic field seen by the beam. In an ideal case with muons orbiting in a horizontal plane with a uniform vertical magnetic field, the anomalous precession frequency $\omega_a$ is given by the difference between the spin ($s$) and cyclotron ($c$) frequencies, $\omega_a = \omega_s - \omega_c$. The observable $\omega_a$ is proportional to $a_{\mu}$.This proceeding presents the beam dynamics systematic corrections that are required to adjust the measured muon precession frequency $\omega^{m}_{a}$ to its true physical value $\omega_{a}$.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A warm super-Neptune around the G-dwarf star TOI-1710 revealed with TESS, SOPHIE, and HARPS-N

We report the discovery and characterization of the transiting extrasolar planet TOI-1710 b. It was first identified as a promising candidate by the Transiting Exoplanet Survey Satellite. Its planetary nature was then established with SOPHIE and HARPS-N spectroscopic observations via the radial-velocity method. The stellar parameters for the host star are derived from the spectra and a joint Markov chain Monte-Carlo adjustment of the spectral energy distribution and evolutionary tracks of TOI-1710. A joint MCMC analysis of the TESS light curve and the radial-velocity evolution allows us to determine the planetary system properties. From our analysis, TOI 1710 b is found to be a massive warm super-Neptune (M p = 28.3 ± 4.7 M ⊕ and R p = 5.34 ± 0.11 R ⊕ ) orbiting a G5V dwarf star (T eff = 5665 ± 55 K) on a nearly circular 24.3-day orbit (e = 0.16 ± 0.08). The orbital period of this planet is close to the estimated rotation period of its host star P rot = 22.5 ± 2.0 days and it has a low Keplerian semi-amplitude K = 6.4 ± 1.0 m s -1 ; we thus performed additional analyses to show the robustness of the retrieved planetary parameters. With a low bulk density of 1.03 ± 0.23 g cm -3 and orbiting a bright host star (J = 8.3, V = 9.6), TOI-1710 b is one of the best targets in this mass-radius range (near the Neptunian desert) for atmospheric characterization via transmission spectroscopy, a key measurement in constraining planet formation and evolutionary models of sub-Jovian planets.

79 ASTRONOMY AND ASTROPHYSICS↗

Wave function analysis with a maximum flow algorithm

An efficient algorithm for computing the maximum-flow path in a network is applied to the identification of the dominant configuration state functions (CSFs) in a graphically contracted function (GCF), configuration interaction, wave function. The flow network is a space of spin-adapted CSFs represented by a Shavitt graph, wherein the nodes correspond to orbital occupations and spin quantum numbers. The graph nodes are connected by arcs, and an arc density is defined as sums of the associated squared CSF coefficients. A max-min approach determines an upper bound to the maximum possible incoming flow for each graph node. A backtracking step generates a candidate walk and is followed by a limited search of alternative branching paths for the dominant CSF. The arc density contributions are removed from the graph, and the algorithm is reapplied to the updated graph. This list of generated walks can be partitioned in order to guarantee that the dominant CSFs have been identified. All of the steps in this algorithm are computationally efficient and do not depend on the potentially large dimension of the underlying linear CSF expansion space. An analysis of low-lying valence states of C-2 illustrates the method.

74 ATOMIC AND MOLECULAR PHYSICS↗

Pseudospin-lattice coupling and electric control of the square-lattice iridate Sr2IrO4

Sr 2 IrO 4 is an archetypal spin-orbit-coupled Mott insulator and has been extensively studied in part because of a wide range of predicted states. Limited experimental characterization of these states thus far brings to light the extraordinary susceptibility of the physical properties to the lattice, particularly, the Ir-O-Ir bond angle. Here, we report a microscopic rotation of the IrO 6 octahedra below 50 K measured by single crystal neutron diffraction. Overall, this sharp lattice anomaly provides keys to understanding the anomalous low-temperature physics and a direct confirmation of a crucial role that the Ir-O-Ir bond angle plays in determining the ground state. Indeed, as also demonstrated in this study, applied electric current readily weakens the antiferromagnetic order via the straightening of the Ir-O-Ir bond angle, highlighting that even slight change in the local structure can disproportionately affect the physical properties in the spin-orbit-coupled system.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

TOI–757 b: an eccentric transiting mini–Neptune on a 17.5–d orbit

ABSTRACT We report the spectroscopic confirmation and fundamental properties of TOI$-$757 b, a mini$-$Neptune on a 17.5$-$d orbit transiting a bright star ($V\, =\, 9.7$ mag) discovered by the TESS mission. We acquired high$-$precision radial velocity measurements with the HARPS, ESPRESSO, and PFS spectrographs to confirm the planet detection and determine its mass. We also acquired space$-$borne transit photometry with the CHEOPS space telescope to place stronger constraints on the planet radius, supported with ground$-$based LCOGT photometry. WASP and KELT photometry were used to help constrain the stellar rotation period. We also determined the fundamental parameters of the host star. We find that TOI$-$757 b has a radius of $R_{\mathrm{p}} = 2.5 \pm 0.1 R_{\oplus }$ and a mass of $M_{\mathrm{p}} = 10.5^{+2.2}_{-2.1} M_{\oplus }$, implying a bulk density of $\rho _{\text{p}} = 3.6 \pm 0.8$ g cm$^{-3}$. Our internal composition modelling was unable to constrain the composition of TOI$-$757 b, highlighting the importance of atmospheric observations for the system. We also find the planet to be highly eccentric with e = 0.39$^{+0.08}_{-0.07}$, making it one of the very few highly eccentric planets among precisely characterized mini$-$Neptunes. Based on comparisons to other similar eccentric systems, we find a likely scenario for TOI$-$757 b’s formation to be high eccentricity migration due to a distant outer companion. We additionally propose the possibility of a more intrinsic explanation for the high eccentricity due to star$-$star interactions during the earlier epoch of the Galactic disc formation, given the low metallicity and older age of TOI$-$757.

Alqasim, A. (ORCID:0000000151025505)↗

TOI-481 b and TOI-892 b: Two Long-period Hot Jupiters from the Transiting Exoplanet Survey Satellite

We present the discovery of two new 10 day period giant planets from the Transiting Exoplanet Survey Satellite mission, whose masses were precisely determined using a wide diversity of ground-based facilities. TOI-481 b and TOI-892 b have similar radii (0.99 ± 0.01 R{sub J} and 1.07 ± 0.02 R{sub J}, respectively), and orbital periods (10.3311 days and 10.6266 days, respectively), but significantly different masses (1.53 ± 0.03 M{sub J} versus 0.95 ± 0.07 M{sub J}, respectively). Both planets orbit metal-rich stars ([Fe/H] = +0.26±0.05 dex and [Fe/H] = +0.24±0.05 for TOI-481 and TOI-892, respectively) but at different evolutionary stages. TOI-481 is a M{sub ⋆} = 1.14 ± 0.02 M{sub ⊙}, R{sub ⋆} = 1.66 ± 0.02 R{sub ⊙} G-type star (T{sub eff} = 5735±72 K), that with an age of 6.7 Gyr, is in the turn-off point of the main sequence. TOI-892 on the other hand, is a F-type dwarf star (T{sub eff} = 6261±80 K), which has a mass of M{sub ⋆} = 1.28 ± 0.03 M{sub ⊙} and a radius of R{sub ⋆} = 1.39 ± 0.02 R{sub ⊙}. TOI-481 b and TOI-892 b join the scarcely populated region of transiting gas giants with orbital periods longer than 10 days, which is important to constrain theories of the formation and structure of hot Jupiters.

79 ASTRONOMY AND ASTROPHYSICS↗

Joint Modeling of GD-1 and C-19 as Old Streams

DESI observational data for the GD-1 and C-19 streams are compared to stream simulations in a common evolving multi-halo potential of a Milky Way-like galaxy based on a cosmological simulation. The goal is to find the best match of the stream velocity spread and the density power spectrum stream density to simulations having either CDM or WDM subhalos. The cocoon velocity width integrated over the length of the stream is independent of orbital blurring along the stream and the power spectrum integrates over the width of the stream, sidestepping the geometric details of the streams. Streams develop from star clusters inserted at $\simeq$1 Gyr after the Big Bang and evolved for 13 Gyr to their current orbital positions. Streams in a CDM subhalo population provide the best match to the velocity width, with streams younger than 10 Gyr ruled out as insufficiently hot. The progenitor star cluster masses, which determine the fraction of stars released at late times which comprise the stream core, are found to be $\simeq 8\times 10^4 M_\odot$ for GD-1 and $\simeq 4\times 10^4 M_\odot$ for C-19, although the mass depends on the star cluster half mass radius. Stream heating leads to stream lumpiness which is measurable for the relatively large and clean GD-1 dataset. The stream density power spectrum measured along the length of the DESI GD-1 sample is in good agreement with CDM simulations, with 1.7 to 1.9 times more power than WDM 7 keV and 5.5 keV simulations.

Carlberg, Raymond G. [Toronto U.] (ORCID:000000027↗

Strong Electronic and Magnetic Coupling in M 4 (M = Ni, Cu) Clusters via Direct Orbital Interactions between Low-Coordinate Metal Centers

In this report we present an extensive study of tetranuclear transition-metal cluster compounds M 4 (NP t Bu 3 ) 4 and [M 4 (NP t Bu 3 ) 4 ][B(C 6 F 5 ) 4 ] (M = Ni, Cu; t Bu = tert -butyl), which feature low-coordinate metal centers and direct metal-metal orbital overlap. X-ray diffraction, electrochemical, magnetic, spectroscopic, and computational analysis elucidate the nature of the bonding interactions in these clusters and the impact of these interactions on the electronic and magnetic properties. Direct orbital overlap results in strongly coupled, large-spin ground states in the [Ni 4 (NP t Bu 3 ) 4 ] +/0 clusters and fully delocalized, spin-correlated electrons. Correlated electronic structure calculations confirm the presence of ferromagnetic ground states that arise from direct exchange between magnetic orbitals, and, in the case of the neutral cluster, itinerant electron magnetism similar to that in metallic ferromagnets. The cationic nickel cluster also possesses large magnetic anisotropy exemplified by a large, positive axial zero-field splitting parameter of D = +7.95 or +9.2 cm -1 , as determined by magnetometry or electron paramagnetic resonance spectroscopy, respectively. The [Ni 4 (NP t Bu 3 ) 4 ] + cluster is also the first molecule with easy-plane magnetic anisotropy to exhibit zero-field slow magnetic relaxation, and under a small applied field, it exhibits relaxation exclusively through an Orbach mechanism with a spin relaxation barrier of 16 cm -1 . The S = 1 / 2 complex [Cu 4 (NP t Bu 3 ) 4 ] + exhibits slow magnetic relaxation via a Raman process on the millisecond time scale, supporting the presence of slow relaxation via an Orbach process in the nickel analogue. Overall, this work highlights the unique electronic and magnetic properties that can be realized in metal clusters featuring direct metal-metal orbital interactions between low-coordinate metal centers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chemical Understanding of Actinide Separations

This work provides a broad overview of the separation processes used to isolate actinides and the experimentally and computationally determined chemical characteristics that define those separations. The redox chemistry of the actinides plays a pivotal role in both aqueous and pyrochemical processing separations. The near-overlapping energies of the 6d and 5f orbitals in the light actinides allow for facile adjustment of actinide oxidation states, which is used in many established separation methods. In contrast, the stable, generally 3+ oxidation states of the mid- and heavy actinides can make it difficult to separate them from the similarly lanthanides(III). In aqueous separations, the tendency of the actinides to form anionic and neutral aqueous complexes with a variety of complexants (especially soft donors) is used to achieve high separation factors between chemically similar elements in both solid–liquid separations and liquid–liquid extraction. This selectivity can be further tuned through the use of specialized organic or solid-phase ligands. Pyroprocessing separations utilize the unique redox behavior of the actinides to adjust their distribution between a molten salt electrolyte and either a solid electrode or molten metal phase. Atomic-level insights into the mechanisms underlying actinide separation processes, with the ultimate goal of predicting separation behavior, can be provided by electronic structure and statistical mechanical-based calculation methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

How do super concentrated electrolytes push the Li-ion batteries and supercapacitors beyond their thermodynamic and electrochemical limits?

Increasing the energy density of energy storage devices is currently the key target of many battery and supercapacitor research activities. For both types of devices, the electrochemical stability window (ESW) determines the effective energy density of the device. ESWs are defined by the effective oxidation and reduction potentials of the electrolyte, which are controlled by many various factors, including the HOMO/LUMO (highest/lowest unoccupied molecular orbital) energies of the electrolyte molecules, the nature of the electrode/electrolyte interphases, and other physicochemical properties. The concentration of the electrolyte would affect the HOMO/ LUMO levels thus also change the ESW. A higher concentration of salt induces specific arrangements among the anion, cation, and solvent molecules of an electrolyte, altering the bulk behavior of the electrolyte, resulting in drastic change in the electrode interfaces. These uniquely modified physicochemical properties extend the ESW in several different ways, including the enhancement in the kinetic stability of the electrodes, as well as the thermodynamic and Nernst shifts of the oxidation/reduction potentials of the electrolyte. For organic electrolytes, it is the reduced amount of free solvent molecules that plays the key role in such changes; whereas for aqueous electrolytes, it is the scarcity of free water molecules and the reduced water activity that control the key properties of the electrolyte. Here, we focus on elucidating the fundamental structural changes occurring within an electrolyte system with increasing salt concentrations. The underlying mechanisms which not only facilitates the extension of the ESW, but also enables higher rate capabilities and mitigates aluminum dissolution for batteries with organic electrolytes, are meticulously explained. Further, we thoroughly discuss the importance of high-voltage stability in aqueous battery systems by exploiting the changed properties observed with higher concentrations of salts. To finish, high-voltage supercapacitors enabled by superconcentrated electrolytes are also explored.

25 ENERGY STORAGE↗

High-resolution infrared spectroscopy of jet cooled CH 2 Br radicals: The symmetric CH stretch manifold and absence of nuclear spin cooling

Direct laser absorption of a slit supersonic discharge expansion provides the first high-resolution spectroscopic results on the symmetric CH stretch excitation (ν 1 ) of the bromomethyl (CH 2 Br) radical in the ground electronic state. Narrowband (<1 MHz) mid-infrared radiation is produced by difference-frequency generation of two visible laser beams, with the open shell halohydrocarbon radical generated by electron dissociative attachment of CH 2 Br 2 in a discharge and rapidly cooled to T rot = 18 ± 1 K in the subsequent slit-jet supersonic expansion. A rovibrational structure in the radical spectrum is fully resolved, as well as additional splittings due to spin-rotation effects and 79 Br/ 81 Br isotopologues in natural abundance. Spectroscopic constants and band origins are determined by fitting the transition frequencies to a non-rigid Watson Hamiltonian, yielding results consistent with a vibrationally averaged planar radical and an unpaired electron in the out-of-plane p π orbital. Additionally, extensive satellite band structure from a vibrational hot band is observed and analyzed. The hot band data is compared to CFOUR/VPT2 (CCSD(T)cc-pVQZ) ab initio anharmonic predictions of the vibration rotation alpha matrix, which permits unambiguous assignment to CH 2 symmetric-stretch excitation built on the singly excited CH 2 out-of-plane bending mode (ν 1 + ν 4 ← ν 4 ). Longitudinal cooling of the Doppler width in the slit-jet expansion geometry also reveals partially resolved hyperfine structure on transitions out of the lowest angular momentum states in excellent agreement with predictions based on microwave studies. High level ab initio MOLPRO calculations [CCSD(T)-f12b/VnZ-f12 (n = 3, 4, CBS)] are also performed with explicitly correlated f12 electron methods for the out-of-plane CH 2 bending mode over the halogen series CH 2 X (X = F, Cl, Br, I), which clearly reveals a non-planar geometry for X = F (with a ΔE ≈ 0.3 kcal/mol barrier) and yet planar equilibrium geometries for X = Cl, Br, and I. Finally, a detailed Boltzmann analysis of the transition intensities provides support for negligible collisional equilibration of the entangled H atom nuclear spin states on the few hundred microsecond time scale and high collision densities of a slit supersonic expansion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A hybrid optoelectronic Mott insulator

The coupling of electronic degrees of freedom in materials to create “hybridized functionalities” is a holy grail of modern condensed matter physics that may produce versatile mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition (MIT) is technologically attractive due to the large changes in resistance, tunable by doping, strain, electric fields, and orbital occupancy but not, in and of itself, controllable with light. Here, an alternate approach is presented to produce optical functionalities using a properly engineered photoconductor/strongly correlated hybrid heterostructure. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the intimate proximity between the two materials, the heterostructure exhibits giant volatile and nonvolatile, photoinduced resistivity changes with substantial shifts in the MIT transition temperatures. This approach can be extended to other judicious combinations of strongly correlated materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Role of orbital selectivity on crystal structures and electronic states in BiMnO 3 and LaMnO 3 perovskites

Correlated oxides, such as BiMnO 3 and LaMnO 3 , show a complex interplay of electronic correlations and crystal structure exhibiting multiple first-order phase transitions, some without a clear order parameter. The quantitative theoretical description of this temperature-dependent electronic-structural interplay in the vicinity of a Mott transition is still a challenge. Here we address this issue by simultaneously considering both structural and electronic degrees of freedom, within a self-consistent density functional theory with embedded dynamical mean field theory. Our results show the existence of novel electronic states characterized by the coexistence of insulating, semimetallic, and metallic orbitals. This state is in agreement with resonant x-ray scattering. Here we also show that electronic entropy plays a decisive role in both electronic and structural phase transitions. By self-consistent determination of both the electronic state and the corresponding crystal structure, we show that the temperature evolution of these phases can be quantitatively explained from first principles, thus demonstrating the predictive power of the theoretical method for both the structural and the electronic properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗