# Open Access Publications

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Open access publications by faculty, postdocs, and graduate students in the Department of Physics and Astronomy.

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Item Non-minimal quartic inflation in supersymmetric SO(10)(Elsevier Science, 2016-12-16) Leontaris, George K.; Okada, Nobuchika; Shafi, Qaisar; George K. Leontaris, Nobuchika Okada, Qaisar Shafi; Shafi, QaisarWe describe how quartic (λφ4) inflation with non-minimal coupling to gravity is realized in realistic supersymmetric SO(10)models. In a well-motivated example the 16 −16Higgs multiplets, which break SO(10)to SU(5)and yield masses for the right-handed neutrinos, provide the inflaton field φ. Thus, leptogenesis is a natural outcome in this class of SO(10)models. Moreover, the adjoint (45-plet) Higgs also acquires a GUT scale value during inflation so that the monopole problem is evaded. The scalar spectral index nsis in good agreement with the observations and r, the tensor to scalar ratio, is predicted for realistic values of GUT parameters to be of order 10−3–10−2.Item Robustness of quantized transport through edge states of finite length: Imaging current density in Floquet topological versus quantum spin and anomalous Hall insulators(Physical Review Research, 2020-09-17) Bajpai, Utkarsh; Ku, Mark J. H.; Nikolić, Branislav K.The theoretical analysis of topological insulators (TIs) has been traditionally focused on infinite homogeneous crystals with band gap in the bulk and nontrivial topology of their wave functions, or infinite wires whose boundaries host surface or edge metallic states. Such infinite-length edge states exhibit quantized conductance which is insensitive to edge disorder, as long as it does not break the underlying symmetry or introduce energy scale larger than the bulk gap. However, experimental devices contain finite-size topological region attached to normal metal (NM) leads, which poses a question about how precise is quantization of longitudinal conductance and how electrons transition from topologically trivial NM leads into the edge states. This particularly pressing issue for recently conjectured two-dimensional (2D) Floquet TI where electrons flow from time-independent NM leads into time-dependent edge states, the very recent experimental realization [J. W. McIver et al., Nat. Phys. 16, 38 (2020)] of Floquet TI using graphene irradiated by circularly polarized light did not exhibit either quantized longitudinal or Hall conductance. Here, we employ a charge-conserving solution for Floquet-nonequilibrium Green functions of irradiated graphene nanoribbon to compute longitudinal two-terminal conductance, as well as spatial profiles of local current density as electrons propagate from NM leads into the Floquet TI. For comparison, we also compute conductance of graphene-based realization of 2D quantum Hall, quantum anomalous Hall, and quantum spin Hall insulators. Although zero-temperature conductance within the gap of these three conventional time-independent 2D TIs of finite length exhibits small oscillations due to reflections at the NM-lead/2D-TI interface, it remains very close to perfectly quantized plateau at 2e2/h and completely insensitive to edge disorder. This is due to the fact that inside conventional TIs there is only edge local current density which circumvents any disorder. In contrast, in the case of Floquet TI both bulk and edge local current densities contribute equally to total current, which leads to longitudinal conductance below the expected quantized plateau that is further reduced by edge vacancies. We propose two experimental schemes to detect coexistence of bulk and edge current densities within Floquet TI: (i) drilling a nanopore in the interior of irradiated region of graphene will induce backscattering of bulk current density, thereby reducing longitudinal conductance by ∼28%; (ii) imaging of magnetic field produced by local current density using diamond nitrogen-vacancy centers.Item Scattering-induced and highly tunable by gate damping-like spin-orbit torque in graphene doubly proximitized by two-dimensional magnet Cr2Ge2Te6 and monolayer WS2(Physical Review Research, 2020-10-09) Zollner, Klaus; Petrović, Marko D.; Dolui, Kapildeb; Plecháč, Petr; Nikolić, Branislav K.; Fabian, JaroslavGraphene sandwiched between semiconducting monolayers of ferromagnet Cr2Ge2Te6 and transition-metal dichalcogenide WS2 acquires both spin-orbit (SO) coupling, of valley-Zeeman and Rashba types, and exchange coupling. Using first principles combined with quantum transport calculations, we predict that such doubly proximitized graphene within van der Waals heterostructure will exhibit SO torque driven by unpolarized charge current. This system lacks spin Hall current which is putatively considered as necessary for the efficient damping-like (DL) SO torque that plays a key role in magnetization switching. Instead, it demonstrates how a DL SO torque component can be generated solely by skew scattering off spin-independent potential barrier or impurities in purely two-dimensional electronic transport due to the presence of proximity SO coupling and its spin texture tilted out of plane. This leads to current-driven nonequilibrium spin density emerging in all spatial directions, whose cross product with proximity magnetization yields DL SO torque, unlike the ballistic regime with no scatterers in which only field-like (FL) SO torque appears. In contrast to SO torque on conventional metallic ferromagnets in contact with three-dimensional SO-coupled materials, the ratio of FL and DL components of SO torque can be tuned by more than an order of magnitude via combined top and back gates.Item Bimetal–organic frameworks derived tuneable Co nanoparticles embedded in porous nitrogen-doped carbon nanorods as high-performance electromagnetic wave absorption materials(Journal of Materials Chemistry C, 2021-05-04) Pan, Jiannan; Yang, Huadong; Hong, Qu; Wen, Hui-Min; Xiao, John Q.; Hu, JunThe in situ pyrolysis of metal–organic-frameworks (MOFs) is an effective strategy to prepare magnetic metal nanoparticle (NP) doped porous carbon materials. These composite materials have shown great potential as high performance electromagnetic wave (EMW) absorption materials. So far, the precise control of composite composition and structure has remained a major challenge in constructing highly porous composites with uniformly distributed NPs. In this work, we report a facile route to synthesize tuneable Co NPs embedded in porous nitrogen-doped carbon (Co/NC) nanorods through the direct thermolysis of the bimetal–organic framework (CoZn–ZIF) precursor. By adjusting the proportion of Co2+ in the MOF precursor, the content and distribution of Co NPs in the composite absorber change accordingly. When the molar ratio between Co2+ and Zn2+ is 3 : 1, the carbonized composites exhibit the largest external surface area and the best EMW absorption performance. With a filler mass loading of merely 15 wt%, the minimum reflection loss (RLmin) reaches −52.3 dB at 10.1 GHz with a thin layer thickness of 2.5 mm. The largest effective absorption bandwidth (EAB) of 5.0 GHz (11.1–16.1 GHz) is achieved in a 2.0 mm thick sample. The qualified bandwidth can be up to 14.5 GHz (3.5–18.0 GHz) with the integrated thickness from 1.0 mm to 5.5 mm. The enhanced conductive/magnetic losses, strong interfacial/dipolar/defect polarization, hierarchical pore structure and the geometric effect endow the Co/NC absorber with improved impedance matching and enhanced attenuation of EMW. This work provides a good direction for the future study of MOF-derived lightweight and efficient EMW absorbing materials.Item Electroweak monopoles and magnetic dumbbells in grand unified theories(Physical Review D, 2021-05-20) Lazarides, G.; Shafi, Q.We use the SU(5) model to show the presence in grand unified theories of an electroweak monopole and a magnetic dumbbell (“meson”) made up of a monopole-antimonopole pair connected by a Z-magnetic flux tube. The monopole is associated with the spontaneous breaking of the weak SU(2)L gauge symmetry by the induced vacuum expectation value of a heavy scalar SU(2)L triplet with zero weak hypercharge contained in the adjoint Higgs 24-plet. This monopole carries a Coulomb magnetic charge of (3/4)(2π/e) as well as Z-magnetic charge, where 2π/e denotes the unit Dirac magnetic charge. Its total magnetic charge is √3/8(4π/e), which is in agreement with the Dirac quantization condition. The monopole weighs about 700 GeV, but because of the attached Z-magnetic tube it exists, together with the antimonopole, in a magnetic dumbbell configuration whose mass is expected to lie in the TeV range. The presence of these topological structures in SU(5) and SO(10) and in their supersymmetric extensions provides an exciting new avenue for testing these theories in high-energy colliders.Item Spintronics Meets Density Matrix Renormalization Group: Quantum Spin-Torque-Driven Nonclassical Magnetization Reversal and Dynamical Buildup of Long-Range Entanglement(Physical Review X, 2021-06-23) Petrović, Marko D.; Mondal, Priyanka; Feiguin, Adrian E.; Plecháč, Petr; Nikolić, Branislav K.We introduce the time-dependent density matrix renormalization group (tDMRG) as a solution to a long-standing problem in spintronics—how to describe spin-transfer torque (STT) between flowing spins of conduction electrons and localized spins within a magnetic material by treating the dynamics of both spin species fully quantum mechanically. In contrast to conventional Slonczewski-Berger STT, where the localized spins are viewed as classical vectors obeying the Landau-Lifshitz-Gilbert equation and where their STT-driven dynamics is initiated only when the spin polarization of flowing electrons and localized spins are noncollinear, quantum STT can occur when these vectors are collinear but antiparallel. Using tDMRG, we simulate the time evolution of a many-body quantum state of electrons and localized spins, where the former are injected as a spin-polarized current pulse while the latter comprise a quantum Heisenberg ferromagnetic metallic (FM) spin-1/2XXZ chain initially in the ground state with spin polarization antiparallel to that of injected electrons. The quantum STT reverses the direction of localized spins, but without rotation from the initial orientation, when the number of injected electrons exceeds the number of localized spins. Such nonclassical reversal, which is absent from Landau-Lifshitz-Gilbert dynamics, is strikingly inhomogeneous across the FM chain, and it can be accompanied by reduction of the magnetization associated with localized spins, even to zero at specific locations. This feature arises because quantum STT generates a highly entangled nonequilibrium many-body state of all flowing and localized spins, despite starting from the initially unentangled ground state of a mundane FM. Furthermore, the mutual information between localized spins at the FM edges remains nonzero even at infinite separation as the signature of dynamical buildup of long-range entanglement. The growth in time of entanglement entropy differentiates between the quantum and conventional (i.e., noncollinear) setups for STT, reaching a much larger asymptotic value in the former case.Item A scaling relationship for non-thermal radio emission from ordered magnetospheres: from the top of the main sequence to planets Get access Arrow(Monthly Notices of the Royal Astronomical Society, 2021-07-28) Leto, P.; Trigilio, C.; Krtička, J.; Fossati, L.; Ignace, R.; Shultz, M. E.; Buemi, C. S.; Cerrigone, L.; Umana, G.; Ingallinera, A.; Bordiu, C.; Pillitteri, I.; Bufano, F.; Oskinova, L. M.; Agliozzo, C.; Cavallaro, F.; Riggi, S.; Loru, S.; Todt, H.; Giarrusso, M.; Phillips, N. M.; Robrade, J.; Leone, F.In this paper, we present the analysis of incoherent non-thermal radio emission from a sample of hot magnetic stars, ranging from early-B to early-A spectral type. Spanning a wide range of stellar parameters and wind properties, these stars display a commonality in their radio emission which presents new challenges to the wind scenario as originally conceived. It was thought that relativistic electrons, responsible for the radio emission, originate in current sheets formed, where the wind opens the magnetic field lines. However, the true mass-loss rates from the cooler stars are too small to explain the observed non-thermal broad-band radio spectra. Instead, we suggest the existence of a radiation belt located inside the inner magnetosphere, similar to that of Jupiter. Such a structure explains the overall indifference of the broad-band radio emissions on wind mass-loss rates. Further, correlating the radio luminosities from a larger sample of magnetic stars with their stellar parameters, the combined roles of rotation and magnetic properties have been empirically determined. Finally, our sample of early-type magnetic stars suggests a scaling relationship between the non-thermal radio luminosity and the electric voltage induced by the magnetosphere’s co-rotation, which appears to hold for a broader range of stellar types with dipole-dominated magnetospheres (like the cases of the planet Jupiter and the ultracool dwarf stars and brown dwarfs). We conclude that well-ordered and stable rotating magnetospheres share a common physical mechanism for supporting the generation of non-thermal electrons.Item SU(5) × U(1)x axion model with observable proton decay(Physical Review D, 2021-09-27) Okada, Nobuchika; Raut, Digesh; Shafi, QaisarWe propose a SU(5) x U(1)x X U(1)PQ model, where U(1)x is the generalization of the B − L (baryon minus lepton number) gauge symmetry and U(1)PQ is the global Peccei-Quinn (PQ) symmetry. There are four fermions families in 5 + 10 representations of SU(5), a mirror family in 5 + 10 representations, and three SU(5) singlet Majorana fermions. The U(1)x related anomalies all cancel in the presence of the Majorana neutrinos. The SU(5) symmetry is broken at MGUT ≃ (6–9) x 10^15 GeV and the proton lifetime τp is estimated to be well within the expected sensitivity of the future hyper-Kamiokande experiment, τp ≲ 1.3 × 10^35 years. The SU(5) breaking also triggers the breaking of the PQ symmetry, resulting in axion dark matter (DM), with the axion decay constant fa of order MGUT or somewhat larger. The CASPEr experiment can search for such an axion DM candidate. The Hubble parameter during inflation must be low, Hinf ≲ 10^9 GeV, in order to successfully resolve the axion domain wall, axion DM isocurvature and SU(5) monopole problems. With the identification of the U(1)x breaking Higgs field with the inflaton field, we implement inflection-point inflation, which is capable of realizing the desired value for Hinf. The vectorlike fermions in the model are essential for achieving successful unification of the SM gauge couplings as well as the phenomenological viability of both axion DM and inflation scenario.Item von Karman Correlation Similarity of the Turbulent Interplanetary Magnetic Field(Astrophysical Journal Letters, 2021-10-01) Roy, Sohom; Chhiber, R.; Dasso, S.; Ruiz, M. E.; Matthaeus, W. H.A major development underlying much of hydrodynamic turbulence theory is the similarity decay hypothesis due to von Karman and Howarth here extended empirically to magnetic field fluctuations in the solar wind. In similarity decay the second-order correlation experiences a continuous transformation based on a universal functional form and a rescaling of energy and characteristic length. Solar wind turbulence follows many principles adapted from classical fluid turbulence, but previously this similarity property has not been examined explicitly. Here we analyze an ensemble of magnetic correlation functions computed from Advanced Composition Explorer data at 1 au, and demonstrate explicitly that the two-point correlation functions undergo a collapse to a similarity form of the type anticipated from von Karman's hypothesis. This provides for the first time a firm empirical basis for employing the similarity decay hypothesis to the magnetic field, one of the primitive variables of magnetohydrodynamics, and one frequently more accessible from spacecraft instruments. This approach is of substantial utility in space turbulence data analysis, and for adopting von Karman-type heating rates in global and subgrid-scale dynamical modeling.Item Inner shell excitation by strong field laser rescattering: optimal laser conditions for high energy recollision(Journal of the Optical Society of America B, 2021-11-15) Kelley, L.; Germain, Z.; Jones, E. C.; Milliken, D.; Walker, Barry C.We address the challenge of finding the optimal laser intensity and wavelength to drive high-energy, strong field rescattering and report the maximum yields of K-shell and LI-shell hole creation. Surprisingly, our results show laser-driven rescattering is able to create inner shell holes in all atoms from lithium to uranium with the interaction spanning from the deep IR to x-ray free electron laser sources. The calculated peak rescattering follows a simple scaling with the atomic number and laser wavelength. The results show it is possible to describe the ideal laser intensity and wavelength for general high-energy laser rescattering processes.Item Measurement of the tune-out wavelength for 133Cs at 880 nm(Physical Review A, 2021-11-22) Ratkata, Apichayaporn; Gregory, Philip D.; Innes, Andrew D.; Matthies, Jonas A.; McArd, Lewis A.; Mortlock, Jonathan M.; Safronova, M. S.; Bromley, Sarah L.; Cornish, Simon L.We perform a measurement of the tune-out wavelength, λ0, between the D1, 62S1/2→62P1/2, and D2, 62S1/2→62P3/2, transitions for 133Cs in the ground hyperfine state (F=3,mF=+3). At λ0, the frequency-dependent scalar polarizability is zero leading to a zero scalar ac Stark shift. We measure the polarizability as a function of wavelength using Kapitza-Dirac scattering of a 133Cs Bose-Einstein condensate in a one-dimensional optical lattice, and determine the tune-out wavelength to be λ0=880.21790(40)stat(8)sys nm. From this measurement we determine the ratio of reduced matrix elements to be ∣∣⟨6P3/2∥d∥6S1/2⟩∣∣2/∣∣⟨6P1/2∥d∥6S1/2⟩∣∣2=1.9808(2). This represents an improvement of a factor of 10 over previous results derived from excited-state lifetime measurements. We use the present measurement as a benchmark test of high-precision theory.Item Quantum many-body states and Green's functions of nonequilibrium electron-magnon systems: Localized spin operators versus their mapping to Holstein-Primakoff bosons(Physical Review B, 2021-11-22) Bajpai, Utkarsh; Suresh, Abhin; Nikolić, Branislav K.It is well-known that operators of localized spins within a magnetic material satisfy neither fermionic nor bosonic commutation relations. Thus, to construct diagrammatic many-body perturbation theory requiring the Wick theorem, the spin operators are usually mapped to the bosonic ones with Holstein-Primakoff (HP) transformation being the most widely used in magnonics and spintronics literature. However, to make calculations tractable, the square root of operators in the HP transformation is expanded into a Taylor series truncated to some low order. This poses a question on the range of validity of the truncated HP transformation when describing nonequilibrium dynamics of localized spins interacting with each other or with conduction electron spins—a problem frequently encountered in numerous transport phenomena in magnonics and spintronics. Here we apply exact diagonalization techniques to a Hamiltonian of fermions (i.e., electrons) interacting with HP bosons versus a Hamiltonian of fermions interacting with the original localized spin operators to compare their many-body states and one-particle equilibrium and nonequilibrium Green's functions (GFs). We employ as a test bed a one-dimensional quantum Heisenberg ferromagnetic spin-S XXX chain of N≤7 sites, where S=1 or S=5/2, and the ferromagnet can be made metallic by allowing electrons to hop between the sites while interacting with the localized spins via sd exchange interaction. For these two different versions of the Hamiltonian of this model, we compare the structure of their ground states, time evolution of excited states, spectral functions computed from the retarded GF in equilibrium, and matrix elements of the lesser GF out of equilibrium. Interestingly, magnonic spectral function can be substantially modified by acquiring additional peaks due to quasibound states of electrons and magnons once the interaction between these subsystems is turned on. The Hamiltonian of fermions interacting with HP bosons gives an incorrect ground state and electronic spectral function unless a large number of terms are retained in the truncated HP transformation. Furthermore, tracking the nonequilibrium dynamics of localized spins over longer time intervals requires a progressively larger number of terms in truncated HP transformation, even if a small magnon density is excited initially, but the required number of terms is reduced when interaction with conduction electrons is turned on. Finally, we show that recently proposed [M. Vogl et al., Phys. Rev. Res. 2, 043243 (2020); J. König et al., SciPost Phys. 10, 007 (2021)] resummed HP transformation, where spin operators are expressed as polynomials in bosonic operators, resolves the trouble with truncated HP transformation while allowing us to derive an exact quantum many-body (manifestly Hermitian) Hamiltonian consisting of a finite and fixed number of boson-boson and electron-boson interacting terms.Item Mechanical Energy Deposition in Cool Star Atmospheres: Resonant Coupling to Coronal Loops in M Dwarfs(The Astrophysical Journal, 2021-11-29) Mullan, D. J.The efficiency of coronal heating ε(cor) in a star can be quantified by LX/Lbol, i.e., the ratio of X-ray luminosity to bolometric luminosity. The efficiency of chromospheric heating in the same star ε(chr) is typically assumed to be proportional to L(Hα)/Lbol or L(Ca K)/Lbol where the lines Hα and Ca K are often the two strongest emission lines in the visible spectrum: the constant of proportionality (η = ε(chr)/[L(Hα)/Lbol] > 1) includes contributions from many other lines emitted by the chromosphere. In the case of the quiet Sun, it has been known for decades that, in the Sun, the efficiency of chromospheric heating is larger by a factor of ε(chr)/ε(cor) > 10 than the efficiency of coronal heating. Over the intervening years, data pertaining to ε(cor) and ε(chr) have been estimated for an increasingly large sample of main-sequence stars with spectral types later than the Sun. These data suggest that among M dwarfs, the efficiency ratio ε(chr)/ε(cor) may in some stars become smaller than in the solar case. The effect of this is such that the value of ε(cor) may become comparable to the value of ε(chr). Here, we seek to understand why coronal heating may be >10 times more efficient (relative to chromospheric heating) in certain M dwarfs than in the Sun. Using data on coronal loop properties in flaring stars, we examine the hypothesis that in M dwarfs, the enhanced efficiency of coronal heating may be related to resonant coupling between coronal loops and the source of mechanical energy in the convection zone.Item Light and microwave driven spin pumping across FeGaB–BiSb interface(Physical Review Materials, 2021-12-16) Sharma, Vinay; Wu, Weipeng; Bajracharya, Prabesh; To, Duy Quang; Johnson, Anthony; Janotti, Anderson; Bryant, Garnett W.; Gundlach, Lars; Jungfleisch, M. Benjamin; Budhani, Ramesh C.Three-dimensional (3D) topological insulators (TIs) with large spin Hall conductivity have emerged as potential candidates for spintronic applications. Here, we report spin to charge conversion in bilayers of amorphous ferromagnet (FM) Fe78Ga13B9 (FeGaB) and 3D TI Bi85Sb15 (BiSb) activated by two complementary techniques: spin pumping and ultrafast spin-current injection. DC magnetization measurements establish the soft magnetic character of FeGaB films, which remains unaltered in the heterostructures of FeGaB-BiSb. Broadband ferromagnetic resonance (FMR) studies reveal enhanced damping of precessing magnetization and large value of spin mixing conductance (5.03×1019m–2) as the spin angular momentum leaks into the TI layer. Magnetic field controlled bipolar DC voltage generated across the TI layer by inverse spin Hall effect is analyzed to extract the values of spin Hall angle and spin diffusion length of BiSb. The spin pumping parameters derived from the measurements of the femtosecond light-pulse-induced terahertz emission are consistent with the result of FMR. The Kubo-Bastin formula and tight-binding model calculations shed light on the thickness-dependent spin-Hall conductivity of the TI films, with predictions that are in remarkable agreement with the experimental data. Our results suggest that room temperature deposited amorphous and polycrystalline heterostructures provide a promising platform for creating novel spin orbit torque devices.Item Precision Calculation of Hyperfine Constants for Extracting Nuclear Moments of 229Th(Physical Review Letters, 2021-12-17) Porsev, S. G.; Safronova, M. S.; Kozlov, M. G.Determination of nuclear moments for many nuclei relies on the computation of hyperfine constants, with theoretical uncertainties directly affecting the resulting uncertainties of the nuclear moments. In this work, we improve the precision of such a method by including for the first time an iterative solution of equations for the core triple cluster amplitudes into the relativistic coupled-cluster method, with large-scale complete basis sets. We carried out calculations of the energies and magnetic dipole and electric quadrupole hyperfine structure constants for the low-lying states of 229Th3+ in the framework of such a relativistic coupled-cluster single double triple method. We present a detailed study of various corrections to all calculated properties. Using the theory results and experimental data, we found the nuclear magnetic dipole and electric quadrupole moments to be μ=0.366(6)μN and Q=3.11(2) eb, respectively, and reduce the uncertainty of the quadrupole moment by a factor of 3. The Bohr-Weisskopf effect of the finite nuclear magnetization is investigated, with bounds placed on the deviation of the magnetization distribution from the uniform one.Item Energy transfer in reconnection and turbulence(Physical Review E, 2021-12-21) Adhikari, S.; Parashar, T. N.; Shay, M. A.; Matthaeus, W. H.; Pyakurel, P. S.; Fordin, S.; Stawarz, J. E.; Eastwood, J. P.Reconnection and turbulence are two of the most commonly observed dynamical processes in plasmas, but their relationship is still not fully understood. Using 2.5D kinetic particle-in-cell simulations of both strong turbulence and reconnection, we compare the cross-scale transfer of energy in the two systems by analyzing the generalization of the von Kármán Howarth equations for Hall magnetohydrodynamics, a formulation that subsumes the third-order law for steady energy transfer rates. Even though the large scale features are quite different, the finding is that the decomposition of the energy transfer is structurally very similar in the two cases. In the reconnection case, the time evolution of the energy transfer also exhibits a correlation with the reconnection rate. These results provide explicit evidence that reconnection dynamics fundamentally involves turbulence-like energy transfer.Item Crystal Structure Predictions for 4-Amino-2,3,6-trinitrophenol Using a Tailor-Made First-Principles-Based Force Field(Crystal Growth and Design, 2022-01-24) Metz, Michael P.; Shahbaz, Muhammad; Song, Hongxing; Vogt-Maranto, Leslie; Tuckerman, Mark E.; Szalewicz, KrzysztofPredictions of crystal structures from first-principles electronic structure calculations and molecular simulations have been performed for an energetic molecule, 4-amino-2,3,6-trinitrophenol. This physics-based approach consists of a series of steps. First, a tailor-made two-body potential energy surface (PES) was constructed with recently developed software, autoPES, using symmetry-adapted perturbation theory based on a density-functional theory description of monomers [SAPT(DFT)]. The fitting procedure ensures asymptotic correctness of the PES by employing a rigorous asymptotic multipole expansion, which seamlessly integrates with SAPT(DFT) interaction energies. Next, crystal structure prediction (CSP) was performed by generating possible crystal structures with rigid molecules, minimizing these structures using the SAPT(DFT) force field, and running isothermal–isobaric molecular dynamics (MD) simulations with flexible molecules based on the tailor-made SAPT(DFT) intermolecular force field and a generic/SAPT(DFT) intramolecular one. This workflow led to the experimentally observed structure being identified as one of the forms with the lowest lattice energy, demonstrating the success of a first-principles, bottom-up approach to CSP. Importantly, we argue that the accuracy of the intermolecular potential, here the SAPT(DFT)-based potential, is determinative of the crystal structure, while generic/SAPT(DFT) force fields can be used to represent the intramolecular potential. This force field approach simplifies the CSP workflow, without significantly compromising the accuracy of the prediction.Item Laser spectroscopy of the y7PoJ states of Cr I(Physical Review A, 2022-03-16) Norrgard, E. B.; Barker, D. S.; Eckel, S. P.; Porsev, S. G.; Cheung, C.; Kozlov, M. G.; Tupitsyn, I. I.; Safronova, M. S.Here we report measured and calculated values of decay rates of the 3d4(5D)4s4p(3Po)y7Po2,3,4 states of Cr i. The decay rates are measured using time-correlated single-photon counting with roughly 1% total uncertainty. In addition, the isotope shifts for transitions between these states and the ground state are measured by laser induced fluorescence to roughly 0.5% uncertainty. The decay rate calculations are carried out by a hybrid approach that combines configuration interaction and the linearized coupled-cluster method (CI+all-order method). The measurements provide a much needed precision benchmark for testing the accuracy of the CI+all-order approach for such complicated systems with six valence electrons, allowing us to significantly expand its applicability. These measurements also demonstrate operation of a cryogenic buffer gas beam source for future cold molecule experiments.Item Ammonia dimer: extremely fluxional but still hydrogen bonded(Nature Communications, 2022-03-18) Aling, Jing; Szalewicz, Krzysztof; van der Avoird, AdIn the 1980s, Nelson, Fraser, and Klemperer (NFK) published an experimentally derived structure of the ammonia dimer dramatically different from the structure determined computationally, which led these authors to the question “Does ammonia hydrogen bond?". This question has not yet been answered satisfactorily. To answer it, we have developed an ab initio potential energy surface (PES) for this dimer at the limits of the current computational capabilities and performed essentially exact six-dimensional calculations of the vibration-rotation-tunneling (VRT) spectra of NH3-NH3 and ND3-ND3, obtaining an unprecedented agreement with experimental spectra. In agreement with other recent electronic structure calculations, the global minimum on the PES is in a substantially bent hydrogen-bonded configuration. Since the bottom of the PES is exceptionally flat, the dimer is extremely fluxional and the probability of finding it in configurations that are not hydrogen bonded is high. Nevertheless, the probability of hydrogen-bonded configurations is large enough to consider the ammonia dimer to be hydrogen bonded. We also show that NFK’s inference that the ammonia dimer is nearly rigid actually results from unusual cancellations between quantum effects that generate differences in spectra of different isotopologues.Item MOBSTER – VI. The crucial influence of rotation on the radio magnetospheres of hot stars(Monthly Notices of the Royal Astronomical Society, 2022-04-27) Shultz, M. E.; Owocki, S. P.; ud-Doula, A.; Biswas, A.; Bohlender, D.; Chandra, P.; Das, B.; David-Uraz, A.; Khalack, V.; Kochukhov, O.; Landstreet, J. D.; Leto, P.; Monin, D.; Neiner, C.; Rivinius, Th.; Wade, G. A.Numerous magnetic hot stars exhibit gyrosynchrotron radio emission. The source electrons were previously thought to be accelerated to relativistic velocities in the current sheet formed in the middle magnetosphere by the wind opening magnetic field lines. However, a lack of dependence of radio luminosity on the wind power, and a strong dependence on rotation, has recently challenged this paradigm. We have collected all radio measurements of magnetic early-type stars available in the literature. When constraints on the magnetic field and/or the rotational period are not available, we have determined these using previously unpublished spectropolarimetric and photometric data. The result is the largest sample of magnetic stars with radio observations that has yet been analysed: 131 stars with rotational and magnetic constraints, of which 50 are radio-bright. We confirm an obvious dependence of gyrosynchrotron radiation on rotation, and furthermore find that accounting for rotation neatly separates stars with and without detected radio emission. There is a close correlation between H α emission strength and radio luminosity. These factors suggest that radio emission may be explained by the same mechanism responsible for H α emission from centrifugal magnetospheres, i.e. centrifugal breakout (CBO), however, while the H α-emitting magnetosphere probes the cool plasma before breakout, radio emission is a consequence of electrons accelerated in centrifugally driven magnetic reconnection.