Enhancing Spin Coherence in Optically Addressable Molecular Qubits through Host-Matrix Control
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74 ATOMIC AND MOLECULAR PHYSICS↗
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Laser-induced-fluorescence imaging of a spin-polarized ultracold neutral plasma in a magnetic field
In this work, we report Doppler-sensitive laser-induced-fluorescence (LIF) imaging of an ultracold neutral plasma in a magnetic field. Local values of ion density, hydrodynamic fluid velocity, temperature, and spin polarization are obtained using a fluorescence model based on velocity-resolved rate equations (REs) including the transfer of ions between states due to laser coupling and spontaneous emission. The RE approach captures optical pumping of ions into states that are not driven by the LIF excitation laser, and this is validated with experimental data. Combined molecular-dynamics and quantum-trajectories simulations verify that velocity-changing collisions have a negligible impact on the state population evolution for typical experimental conditions. Relative intensities of Zeeman components of the LIF spectra provide clear evidence that the ions are electron-spin-polarized when created by photoionization of magnetically trapped 88 Sr atoms. This probe opens many possibilities for studying thermal transport and the equilibration of neutral plasmas in overlapping regimes of strong coupling and magnetization.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
ASCA Observation of an "X-Ray Shadow" in the Galactic Plane
The diffuse X-ray background (DXB) emission near the Galactic plane (l,b about 25.6 deg., 0.78 deg.) has been observed with ASC.4. The observed re-ion is toward a Galactic molecular'cloud which was recently reported to cast a deep X-ray shadow in the 0.5 - 2.0 keV band DXB. The selection of this particular region is intended to provide a constraint on the spatial distribution of the DXB emission along the line of sight: i.e., the molecular cloud is optically thick at < 2 keV and so the bulk of the observed soft X-rays must originate in the foreground of the cloud, which is at about 3 kpc from the Sun. In the 0.8 - 9.0 keV band, atomic emission lines have been detected, and the observed spectrum is primarily from thermal plasmas. Although the detailed nature of the spectrum is complicated, the observed DXB emission appears to originate from the multiple components of hot plasmas including a thermal plasma of T about 10(exp 7) K, which prevails within about 3 kpc from the Sun.
Park, Sangwook↗
Downward quantum learning from element 118: Automated generation of Fermi–Löwdin orbitals for all atoms
A new algorithm based on a rigorous theorem and quantum data computationally mined from element 118 guarantees automated construction of initial Fermi–Löwdin-Orbital (FLO) starting points for all elements in the Periodic Table. It defines a means for constructing a small library of scalable FLOs for universal use in molecular and solid-state calculations. The method can be systematically improved for greater efficiency and for applications to excited states such as x-ray excitations and optically silent excitations. FLOs were introduced to recast the Perdew–Zunger self-interaction correction (PZSIC) into an explicit unitarily invariant form. The FLOs are generated from a set of N quasi-classical electron positions, referred to as Fermi-Orbital descriptors (FODs), and a set of N-orthonormal single-electron orbitals. FOD positions, when optimized, minimize the PZSIC total energy. However, creating sets of starting FODs that lead to a positive definite Fermi orbital overlap matrix has proven to be challenging for systems composed of open-shell atoms and ions. The proof herein guarantees the existence of a FLOSIC solution and further guarantees that if a solution for N electrons is found, it can be used to generate a minimum of N – 1 and a maximum of 2 N – 2 initial starting points for systems composed of a smaller number of electrons. As a result, applications to heavy and super-heavy atoms are presented. All starting solutions reported here were obtained from a solution for element 118, Oganesson.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Driven-dissipative phase transition in a Kerr oscillator: From semiclassical PT symmetry to quantum fluctuations
We study a minimal model that has a driven-dissipative quantum phase transition, namely a Kerr non-linear oscillator subject to driving and dissipation. Using mean-field theory, exact diagonalization, and the Keldysh formalism, we analyze the critical phenomena in this system, showing which aspects can be captured by each approach and how the approaches complement each other. Then critical scaling and finite-size scaling are calculated analytically using the quantum Langevin equation. Furthermore, the physics contained in this simple model is surprisingly rich: it includes a continuous phase transition, Z 2 symmetry breaking, PT symmetry, state squeezing, and critical fluctuations. Due to its simplicity and solvability, this model can serve as a paradigm for exploration of open quantum many-body physics.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Making Macroscopic Assemblies of Aligned Carbon Nanotubes
A method of aligning and assembling single-wall carbon nanotubes (SWNTs) to fabricate macroscopic structures has been invented. The method entails suspending SWNTs in a fluid, orienting the SWNTs by use of a magnetic and/or electric field, and then removing the aligned SWNTs from suspension in such a way as to assemble them while maintaining the alignment. SWNTs are essentially tubular extensions of fullerene molecules. It is desirable to assemble aligned SWNTs into macroscopic structures because the common alignment of the SWNTs in such a structure makes it possible to exploit, on a macroscopic scale, the unique mechanical, chemical, and electrical properties that individual oriented SWNTs exhibit at the molecular level. Because of their small size and high electrical conductivity, carbon nanotubes, and especially SWNTs, are useful for making electrical connectors in integrated circuits. Carbon nanotubes can be used as antennas at optical frequencies, and as probes in scanning tunneling microscopes, atomic-force microscopes, and the like. Carbon nanotubes can be used with or instead of carbon black in tires. Carbon nanotubes are useful as supports for catalysts. Ropes of SWNTs are metallic and, as such, are potentially useful in some applications in which electrical conductors are needed - for example, they could be used as additives in formulating electrically conductive paints. Finally, macroscopic assemblies of aligned SWNTs can serve as templates for the growth of more and larger structures of the same type. The great variety of tubular fullerene molecules and of the structures that could be formed by assembling them in various ways precludes a complete description of the present method within the limits of this article. It must suffice to present a typical example of the use of one of many possible variants of the method to form a membrane comprising SWNTs aligned substantially parallel to each other in the membrane plane. The apparatus used in this variant of the method (see figure) includes a reservoir containing SWNTs dispersed in a suspending agent (for example, dimethylformamide) and a reservoir containing a suitable solvent (for example, water mixed with a surfactant). By use of either pressurized gas supplied from upstream or suction from downstream, the suspension of SWNTs and the solvent are forced to mix and flow into a tank. A filter inside the tank contains pores small enough to prevent the passage of most SWNTs, but large enough to allow the passage of molecules of the solvent and suspending agent. The filter is oriented perpendicular to the flow path. A magnetic field parallel to the plane of the filter is applied. The success of the method is based on the tendency of SWNTs to become aligned with their longitudinal axes parallel to an applied magnetic field. The alignment energy of an SWNT increases with the length of the SWNT and the magnetic-field strength. In order to obtain an acceptably small degree of statistical deviation of SWNTs of a given length from alignment with a magnetic field, one must make the field strong enough so that the thermal energy associated with rotation of an SWNT away from alignment is less than the alignment energy.
Smalley, Richard E.↗
Cadmium Magnesium Telluride for Next-Generation X-Ray Free Electron Laser, Synchrotron, and Many Other Applications
We developed a picosecond photodetector based on our Bridgman-grown and specially engineered cadmium magnesium telluride (Cd 1–x MgxTe) single crystal that is sensitive to both optical and X-ray pulses for coarse timing in free-electron laser applications. Cd 1–x MgxTe is a widebandgap semiconductor with potential applications, not only in optoelectronics, but also in particle physics as an intense pulse radiation detector for bremsstrahlung, X-ray/gamma-ray radiation, thermal neutrons, and medical imaging. For femtosecond optical and X-ray crosscorrelation, the material must have a very short lifetime, a condition that is opposite to that required for nuclear spectroscopy applications. At the same time, the material also needs to have a very low bulk leakage current, in the 10–90 nA range for voltages to even 1000 V. Hence, the ability to tailor or engineer the material is very crucial. Picosecond response and the crystal growth of this specially engineered Cd 1–x MgxTe material are presented. Furthermore, other characterization and transient measurements are discussed along with room-temperature semiconductor detector performance for other nuclear radiation detection applications.
36 MATERIALS SCIENCE↗
Laser-Plasma Spatiotemporal Cyanide Spectroscopy and Applications
This article reports new measurements of laser-induced plasma hypersonic expansion measurements of diatomic molecular cyanide (CN). Focused, high-peak-power 1064 nm Q-switched radiation of the order of 1 TW/cm 2 generated optical breakdown plasma in a cell containing a 1:1 molar gas mixture of N 2 and CO 2 at a fixed pressure of 1.1 × 10 5 Pascal and in a 100 mL/min flow of the mixture. Line-of-sight (LOS) analysis of recorded molecular spectra indicated the outgoing shockwave at expansion speeds well in excess of Mach 5. Spectra of atomic carbon confirmed increased electron density near the shockwave, and, equally, molecular CN spectra revealed higher excitation temperature near the shockwave. Results were consistent with corresponding high-speed shadowgraphs obtained by visualization with an effective shutter speed of 5 nanoseconds. In addition, LOS analysis and the application of integral inversion techniques allow inferences about the spatiotemporal plasma distribution.
36 MATERIALS SCIENCE↗
Unusual Ferromagnetic Band Evolution and High Curie Temperature in Monolayer 1T‐CrTe2 on Bilayer Graphene
2D van der Waals ferromagnets hold immense promise for spintronic applications due to their controllability and versatility. Despite their significance, the realization and in-depth characterization of ferromagnetic materials in atomically thin single layers, close to the true 2D limit, has been scarce. Here, a successful synthesis of monolayer (ML) 1T-CrTe2 is reported on a bilayer graphene (BLG) substrate via molecular beam epitaxy. Using angle-resolved photoemission spectroscopy and magneto-optical Kerr effect measurements, that the ferromagnetic transition is observed at the Curie temperature (TC) of 150 K in ML 1T-CrTe2 on BLG, accompanied by unconventional temperature-dependent band evolutions. The spectroscopic analysis and first-principle calculations reveal that the ferromagnetism may arise from Goodenough-Kanamori super-exchange and double-exchange interactions, enhanced by the lattice distortion and the electron doping from the BLG substrate. These findings provide pivotal insight into the fundamental understanding of mechanisms governing 2D ferromagnetism and offer a pathway for engineering higher TC in 2D materials for future spintronic devices.
Park, Kyoungree↗
Effect of elastic anisotropy on thermally induced distortions of a laser beam in single cubic syngony crystals with radial cooling. Part I
We have studied thermally induced distortions of a beam in single cubic syngony crystals of all symmetry groups with an anisotropic elastic stiffness tensor. The arithmetic mean and the difference between the thermally induced phase incursions of eigenpolarisations, as well as the angle of incidence of these polarisations, are calculated for a long rod and a thin disk with radial cooling under uniform volume pumping of the active element. The position of the specific crystal orientations unrelated to its symmetry elements is investigated. The effective values of the thermo-optical constant Q in two specific orientations, as well as the thermo-optical constant P in an arbitrary orientation, are found. (invited paper)
36 MATERIALS SCIENCE↗
Reversible Oxidation Quantified by Optical Properties in Epitaxial Fe2CrO4+d Films on (001) MgAl2O4
We report on the structural and optical properties of Fe2CrO4+d epitaxial films grown by molecular beam epitaxy on MgAl2O4 (001) as a function of ?. The average Fe valence can be correlated with the out-of-plane lattice parameter and the extent of light absorption in the infrared spectral region. Over-oxidized films (0 < d < 0.5) exhibit reduced lattice parameters and suppressed infrared absorption. We discuss the behavior of a novel infrared transition at ~0.6 eV in stoichiometric Fe2CrO4 films deposited on MgAl2O4 (MAO) at or above 400 °C. This research provides new insight into the atomic structure, optical processes, oxidation states, electronic structure, and application potentials of Fe2CrO4+d.
ellipsometry, Epitaxy, thin film, oxidation, reduc↗
Temperature-Dependent Properties of Molten Li 2 BeF 4 Salt Using Ab Initio Molecular Dynamics
Molten lithium tetrafluoroberyllate (Li 2 BeF 4 ) salt, also known as FLiBe, with a 2:1 mixture of LiF and BeF 2 is being proposed as a coolant and solvent in advanced nuclear reactor designs, such as the molten salt reactor or the fluoride salt cooled high-temperature reactor. We present the results on the structure and properties of FLiBe over a wide range of temperatures, 0–2000 K, from high-throughput ab initio molecular dynamics simulation using a supercell model of 504 atoms. The variations in the local structures of solid and liquid FLiBe with temperature are discussed in terms of a pair distribution function, coordination number, and bond angle distribution. The temperature-dependent electronic structure and optical and mechanical properties of FLiBe are calculated. The optical and mechanical property results are reported for the first time. The results above and below the melting temperature (~732 K) are compared with the experimental data and with data for crystalline FLiBe. The electronic structure and interatomic bonding results are discussed in correlation with the mechanical strength. A novel concept of total bond order density (TBOD), an important quantum mechanical parameter, is used to characterize the internal cohesion and strength in the simulated models. The results show a variation in the rate of change in properties in solid and liquid phases with anomalous behavior across the melting region. The observed trend is the decrease in mechanical strength, band gap, and TBOD in a nonlinear fashion as a function of temperature. The refractive index shows a surprising minimum at 850 K, among the tested temperatures, which lies above the melting point. These findings provide a new platform to understand the interplay between the temperature-dependent structures and properties of FLiBe salt.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Seedless nonresonant gas-flow velocimetry with single-shot coherent Rayleigh-Brillouin scattering
We demonstrate neutral gas-flow velocimetry by exploiting the optical dipole forces exerted by precisely tailored high-intensity laser fields on polarizable particles, in the form of single-shot coherent Rayleigh-Brillouin scattering (CRBS). This enables mapping of the velocity distribution function of the particles in a single laser shot of approximately 200 ns duration, allowing us to perform spectroscopic measurements in the time, rather than the frequency, domain. Importantly, CRBS results in a coherent signal beam, which renders the technique ideal for measurements in optically noisy environments. By correlating the time shift of the resulting spectrum to the Doppler shift caused by the bulk motion of particles, we perform neutral gas-flow velocimetry without the need to seed the flow, nondestructively, for a variety of gases, atomic or molecular. We demonstrate gas-flow velocimetry at flow velocities as low as 1 m s −1 , with similar velocity resolution, while temperature and gas density can also be estimated from the same single-shot spectra. To prove the effectiveness of the measurement technique, we benchmark it against Pitot tube measurements, which show excellent agreement.
Gerakis, Alexandros [Luxembourg Institute of Scien↗
Explosions of infalling comets in Jupiter's atmosphere
In view of the expected collision of comet Shoemaker-Levy 9 (1993e) with Jupiter in 1994 July, we calculate basic properties of the initial interaction for a simplified Jovian atmosphere. The comet is expected to impact Jupiter at 60 km/sec and at an angle of 45 deg to the zenith. The shock wave generated by the bolide should be optically thick once it has penetrated to an atmospheric density approximately 10(exp -6) gr/cm(exp 3), and we calculate the post-shock conditions assuming local thermodynamic equilibrium (LTE) for shock velocities v(sub sh) in the range 10 to 60 km/sec and preshock densities rho(sub a) = 10(exp -6) to 10(exp -2) gr/cm(exp 3). Our shock calculations include molecular hydrogen, atomic hydrogen, ionized hydrogen, neutral helium, and singly ionized helium. Even at the highest shock velocity, the gas is only partially ionized and the postshock temperature rises with preshock density in order to maintain the ionization. The value of the effective shock adiabatic index gamma(sub sh) varies from 1.17 (at low v(sub sh) and rho(sub a) to 1.40 (at high v(sub sh) and rho(sub a). The ablation rate is limited by the radiative flux that reaches the bolide surface. We argue that the ablated gas does not efficiently transfer its kinetic energy to the atmosphere, and it ultimately slows in a similar fashion to the comet material. As the bolide initially falls through the atmosphere, the character of the shock emission changes. At rho(sub a) approximately 10(exp -8) gr/cm (exp 3), the gas is optically thin and we expect line emission; in the optical spectrum, Balmer emission is expected from the shocked atmosphere and low-ionization metal lines from ablated cometary material. At rho(sub a) approximately 10(exp -6) gr/m(exp 3), the shocked gas is optically thick and the shock front near the bolide produces a blackbody spectrum. The temperature is favorable for ultraviolet (1000 to 3000 A) emission and the luminosity may be approximately 5 x 10(exp 23) ergs/sec for approximately 0.6 sec for a bolide 1 km in radius. At rho(sub a) approximately 10(exp -4) gr/cm(exp 3), the bolide has passed below the ultraviolet photosphere. The shock front emits considerable ionizing radiation, but it is absorbed in a narrow preshock region. The bolometric correction for the optical luminosity is large and we expect a 3000 to 8000 A luminosity of approximately 3 x 10(exp 23) ergs/sec for approximately 1 sec. The optical emission is strongly peaked in the vicinity of the bolide. The bolide does have a somewhat less luminous, optically thick trail extending greater than or equal to 10 km, but the radiation is characterized by a temperature of 4000 to 5000 K. From the fragmentation model of Chyba, Thomas, & Zahnle (1993), the bolide deposits most of its kinetic energy at rho(sub a) approximately 10(exp -3) gr/cm(exp 3) and this is the effective explosion site. The shock wave from such an explosion can move up about one density scale height. We examine the breakout of the shock front from the Jovian atmosphere and find that the shock acceleration in the decreasing density region is slow, so that the energy flux in the shock front is small. Higher velocities might be generated by shock acceleration along the channel left by the bolide if the shock motion can occur before the channel closes off as a result of radiative cooling. Hot gas created by the explosion ultimately rises due to buoyancy on a timescale of a minute. The luminosity is highest when the bubble first rises into the optically thin part of the atmosphere and may be approximately 1 x 10(exp 25) ergs/sec in the near-infrared. Roughly 1% of the initial bolide energy may be radiated in this way; the rest of the energy is lost to sound waves from the initial explosion and to work done by the bubble on the surrounding atmosphere.
Chevalier, Roger A.↗
Excited State Phenomena in Correlated Nanostructures: Transition Metal Oxide Clusters and Nanocrystals
The primary goal of our research program was to apply advanced computational techniques to predict electronic properties of molecular species. These include transition metal monoxide and dioxide clusters and negatively charged copper oxide clusters which are important systems for their utilization in a variety of technological applications. The enhanced electron-electron interactions inherent in these systems make it challenging to model their excited state properties within a parameter-free approach. The excited state properties in question include the interaction of light with these molecules which results in ejection of electrons from the system, or the absorption of light by the molecular system resulting in a molecule in a higher-energy state. Our overall goal was to investigate the impact of various computational and theoretical approaches on such electronic and optical excitations in these systems. Comparing several variants of theoretical approaches with available experimental data, and high-level quantum chemistry computations helped us identify the level of theory and approximations that are needed to achieve a reasonable balance between accuracy and computational demand.
74 ATOMIC AND MOLECULAR PHYSICS↗
Effect of thermochemical treatments on laser-induced luminescence spectra from strontium titanate: comparison with swift ion-beam irradiation experiments
Results recently reported on the effect of thermochemical treatments on the (He-Cd) laser-excited emission spectra of strontium titanate (STO) are re-analyzed here and compared with results obtained under ion-beam irradiation. Contributing bands centered at 2.4 eV and 2.8 eV, which appear under laser excitation, present intensities dependent upon previous thermal treatments in oxidizing (O 2 ) or reducing atmosphere (H 2 ). As a key result, the emission band centered at 2.8 eV is clearly enhanced in samples exposed to a reducing atmosphere. From a comparison with the ionoluminescence data, it is concluded that the laser-excited experiments can be rationalized within a framework developed from ion-beam excitation studies. In particular, the band at 2.8 eV, sometimes attributed to oxygen vacancies, behaves as expected for optical transitions from conduction-band (CB) states to the ground state level of the self-trapped exciton center. The band at 2.0 eV reported in ion-beam irradiated STO, and attributed to oxygen vacancies, is not observed in laser-excited crystals. As a consequence of our analysis, a consistent scheme of electronic energy levels and optical transitions can now be reliably offered for strontium titanate.
74 ATOMIC AND MOLECULAR PHYSICS↗
Energetic Ion and Electron Irradiation of the Icy Galilean Satellites
Galileo Orbiter measurements of energetic ions (20 keV to 100 MeV) and electrons (20-700 keV) in Jupiter's magnetosphere are used, in conjunction with the JPL electron model (less than 40 MeV), to compute irradiation effects in the surface layers of Europa, Ganymede, and Callisto. Significant elemental modifications are produced on unshielded surfaces to approximately centimeter depths in times of less than or equal to 10(exp 6) years, whereas micrometer depths on Europa are fully processed in approximately 10 years. Most observations of surface composition are limited to optical depths of approximately 1 mm, which are indirect contact with the space environment. Incident flux modeling includes Stormer deflection by the Ganymede dipole magnetic field, likely variable over that satellite's irradiation history. Delivered energy flux of approximately 8 x 10(exp 10) keV/square cm-s at Europa is comparable to total internal heat flux in the same units from tidal and radiogenic sources, while exceeding that for solar UV energies (greater than 6 eV) relevant to ice chemistry. Particle energy fluxes to Ganymede's equator and Callisto are similar at approximately 2-3 x 10(exp 8) keV/square cm-s with 5 x 10(exp 9) at Ganymede's polar cap, the latter being comparable to radiogenic energy input. Rates of change in optical reflectance and molecular composition on Europa, and on Ganymede's polar cap, are strongly driven by energy from irradiation, even in relatively young regions. Irradiation of nonice materials can produce SO2 and CO2, detected on Callisto and Europa, and simple to complex hydrocarbons. Iogenic neutral atoms and meteoroids deliver negligible energy approximately 10(exp 4-5) keV/square cm-s but impacts of the latter are important for burial or removal of irradiation products. Downward transport of radiation produced oxidants and hydrocarbons could deliver significant chemical energy into the satellite interiors for astrobiological evolution in putative sub-surface oceans.
Cooper, John F.↗
Atomically Resolved Characterization of Optically Driven Ligand Reconfiguration on Nanoparticle Catalyst Surfaces
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99 GENERAL AND MISCELLANEOUS↗