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At least 181 records · Page 10

Nanomechanics of Carbon and CxByNz Nanotubes: Via a Quantum Molecular Dynamics Method

Nanomechanics of single-wall C, BN and BC$_3$ and B doped C nanotubes under axial compression and tension are investigated through a generalized tight-binding molecular dynamics (GTBMD) and {\it ab-initio} electronic structure methods. The dynamic strength of BN, BC$_3$ and B doped C nanotubes for small axial strain are comparable to each other. The main difference is in the critical strain at which structural collapse occurs. For example, even a shallow doping with B lowers the value of critical strain for C nanotubes. The critical strain for BN nanotube is found to be more than that for the similar C nanotube. Once the structural collapse starts to occur we find that carbon nanotubes irreversibly go into plastic deformation regime via the formation of tetrahedral (four-fold coordinated) bonds at the location of sharp pinches or kinks. This finding is considerably different from the classical MD (molecular dynamics) simulation results known so far. The energetics and electronic densities of states of the collapsed structures, investigated with {\it ab-initio) methods, will also be discussed.

Srivastava, Deepak↗

The Structure, Anharmonic Vibrational Frequencies, and Intensities of NNHNN+

A semi-global potential energy surface (PES) and quartic force field (QFF) based on fitting high-level electronic structure energies are presented to describe the structures and spectroscopic properties of NNHNN+. The equilibrium structure of NNHNN+ is linear with the proton equidistant between the two nitrogen groups and thus of D(sub ∞h) symmetry. Vibrational second-order perturbation theory (VPT2) calculations based on the QFF fails to describe the proton “rattle” motion, i.e., the antisymmetric proton stretch, due to the very flat nature of PES around the global minimum, but performs properly for other modes with sharper potential wells. Vibrational self-consistent field/virtual state configuration interaction (VSCF/VCI) calculations using a version of MULTIMODE without angular momentum terms successfully describe this motion and predict the fundamental to be at 759 cm(exp -1). This is in good agreement with the value of 746 cm(exp -1) from a fixed-node diffusion Monte Carlo calculation and the experimental Ar-tagged result of 743 cm(exp -1). Other VSCF/VCI energies are in good agreement with other experimentally reported ones. Both double-harmonic intensity and rigorous MULTIMODE intensity calculations show the proton transfer fundamental has a very strong intensity.

Astrochemistry↗

High Electron Mobility Transistor Structures on Sapphire Substrates Using CMOS Compatible Processing Techniques

System-on-a-chip (SOC) processes are under intense development for high-speed, high frequency transceiver circuitry. As frequencies, data rates, and circuit complexity increases, the need for substrates that enable high-speed analog operation, low-power digital circuitry, and excellent isolation between devices becomes increasingly critical. SiGe/Si modulation doped field effect transistors (MODFETs) with high carrier mobilities are currently under development to meet the active RF device needs. However, as the substrate normally used is Si, the low-to-modest substrate resistivity causes large losses in the passive elements required for a complete high frequency circuit. These losses are projected to become increasingly troublesome as device frequencies progress to the Ku-band (12 - 18 GHz) and beyond. Sapphire is an excellent substrate for high frequency SOC designs because it supports excellent both active and passive RF device performance, as well as low-power digital operations. We are developing high electron mobility SiGe/Si transistor structures on r-plane sapphire, using either in-situ grown n-MODFET structures or ion-implanted high electron mobility transistor (HEMT) structures. Advantages of the MODFET structures include high electron mobilities at all temperatures (relative to ion-implanted HEMT structures), with mobility continuously improving to cryogenic temperatures. We have measured electron mobilities over 1,200 and 13,000 sq cm/V-sec at room temperature and 0.25 K, respectively in MODFET structures. The electron carrier densities were 1.6 and 1.33 x 10(exp 12)/sq cm at room and liquid helium temperature, respectively, denoting excellent carrier confinement. Using this technique, we have observed electron mobilities as high as 900 sq cm/V-sec at room temperature at a carrier density of 1.3 x 10(exp 12)/sq cm. The temperature dependence of mobility for both the MODFET and HEMT structures provides insights into the mechanisms that allow for enhanced electron mobility as well as the processes that limit mobility, and will be presented.

Mueller, Carl↗

Dense simple plasmas as high-temperature liquid simple metals

The thermodynamic properties of dense plasmas considered as high-temperature liquid metals are studied. An attempt is made to show that the neutral pseudoatom picture of liquid simple metals may be extended for describing plasmas in ranges of densities and temperatures where their electronic structure remains 'simple'. The primary features of the model when applied to plasmas include the temperature-dependent self-consistent calculation of the electron charge density and the determination of a density and temperature-dependent ionization state.

Perrot, F.↗

Efficient Implementation for Unitary Coupled Cluster State Preparation for Near-Term Quantum Computers

Unitary coupled cluster theory (UCC) is a common wave function ansatz for quantum simulation of molecular electronic structure using the variational quantum eigenvalue solver (VQE). Even for small molecules using a double-ζ basis, the number of variational parameters required to minimize the electronic energy (i.e., optimize the circuit) is large and beyond the reach of current quantum computers. For example, a circuit simulating C2 using the UCCSD ansatz and the cc-pVDZ basis set with frozen-core will require over 10,000 variational parameters and a Hilbert space of over 10^8 determinants. To make progress on simulating such molecular systems on near-term quantum computers, we explore how much of the optimization can be approximately prepared with classical simulation while reducing the number of optimization steps performed on a quantum device. Recently, Chen, Cheng, and Freericks [J. Chem. Theory Comput. 2021, 17, 841-847] presented an algorithm for the factorized form of the UCC ansatz that allows for efficient UCC optimizations on classical hardware. We flip the algorithm around and use it to prepare approximate quantum circuits for systems that require a large number of qubits to represent. We will present results from our implementation and discuss strategies for incorporating this implementation for algorithms involving near-term quantum computers.

J Wayne Mullinax↗

Efficient Implementation for Unitary Coupled Cluster State Preparation for Near-Term Quantum Computers

Unitary coupled cluster theory (UCC) is a common wave function ansatz for quantum simulation of molecular electronic structure using the variational quantum eigenvalue solver (VQE). Even for small molecules using a double-ζ basis, the number of variational parameters required to minimize the electronic energy (i.e., optimize the circuit) is large and beyond the reach of current quantum computers. For example, a circuit simulating C2 using the UCCSD ansatz and the cc-pVDZ basis set with frozen-core will require over 10,000 variational parameters and a Hilbert space of over 10^(8) determinants. To make progress on simulating such molecular systems on near-term quantum computers, we explore how much of the optimization can be approximately prepared with classical simulation while reducing the number of optimization steps performed on a quantum device. Recently, Chen, Cheng, and Freericks [J. Chem. Theory Comput. 2021, 17, 841-847] presented an algorithm for the factorized form of the UCC ansatz that allows for efficient UCC optimizations on classical hardware. We flip the algorithm around and use it to prepare approximate quantum circuits for systems that require a large number of qubits to represent. We will present results from our implementation and discuss strategies for incorporating this implementation for algorithms involving near-term quantum computers.

Quantum Computing↗

Efficient Implementation for Unitary Coupled Cluster State Preparation for Near-Term Quantum Computers

Unitary coupled cluster theory (UCC) is a common wave function ansatz for quantum simulation of molecular electronic structure using the variational quantum eigenvalue solver (VQE). Even for small molecules using a double-ζ basis, the number of variational parameters required to minimize the electronic energy (i.e., optimize the circuit) is large and beyond the reach of current quantum computers. For example, a circuit simulating C2 using the UCCSD ansatz and the cc-pVDZ basis set with frozen-core will require over 10,000 variational parameters and a Hilbert space of over 10^(8) determinants. To make progress on simulating such molecular systems on near-term quantum computers, we explore how much of the optimization can be approximately prepared with classical simulation while reducing the number of optimization steps performed on a quantum device. Recently, Chen, Cheng, and Freericks [J. Chem. Theory Comput. 2021, 17, 841-847] presented an algorithm for the factorized form of the UCC ansatz that allows for efficient UCC optimizations on classical hardware. We flip the algorithm around and use it to prepare approximate quantum circuits for systems that require a large number of qubits to represent. We will present results from our implementation and discuss strategies for incorporating this implementation for algorithms involving near-term quantum computers.

Quantum Computing↗

Study of the production of some superconducting and magnetic materials by solidification in the drop tube and drop tower

A systematic study on the relationship between the microstructure and physical properties of several superconducting materials prepared by solidification in low gravity was conducted. Further study of the materials, such as the applications of hydrostatic pressure which is known to be an effective mean to vary the electronic structure of materials, in conjunction with the detailed microstructure analysis of the samples was also performed to better understand the low gravity effects on the enhancement of the electronic properties. Results of the studies on the directionally solidified AlInSn alloys processed in the KC-135 aircraft and immiscible GaBi alloy prepared during free fall in the Marshall Space Flight Center Drop Tower are presented.

Wu, M. K.↗

Substorm effects observed in the auroral plasma

The effects of substorm temporal development on high-latitude particle precipitation and ionospheric convection patterns near midnight were studied with the aid of data from Atmosphere Explorer C. During quiet periods generally Maxwellian electron precipitation is observed from the central plasma sheet, which is completely contained within the sunward flow region. As substorms grow and begin to recover, a strong sunward flow appears within the high latitude ionospheric electron trough, equatorward of the central plasma sheet electron precipitation. Intense inverted-V electron structures consistent with strong electrostatic acceleration appear near the Harang discontinuity and extend poleward to the polar cap boundary. Then the trough flow weakens, the Harang discontinuity becomes a gradual reversal, and the electron inverted-V precipitation becomes localized at the polar cap boundary.

Burch, J. L.↗

A Synthesis of Fluid Dynamics and Quantum Chemistry for the Design of Nanoelectronics

In 1959, during a famous lecture entitled "There's Plenty of Room at the Bottom", Richard Feynman focused on the startling technical possibilities that would exist at the limit of miniaturization, that being atomically precise devices with dimensions in the nanometer range. A nanometer is both a convenient unit of length for medium to large sized molecules, and the root of the name of the new interdisciplinary field of "nanotechnology". Essentially, "nanoelectronics" denotes the goal of shrinking electronic devices, such as diodes and transistors, as well as integrated circuits of such devices that can perform logical operations, down to dimensions in the range of 100 nanometers. The thirty-year hiatus in the development of nanotechnology can figuratively be seen as a period of waiting for the bottom-up and atomically precise construction skills of synthetic chemistry to meet the top-down reductionist aspirations of device physics. The sub-nanometer domain of nineteenth-century classical chemistry has steadily grown, and state-of-the-art supramolecular chemistry can achieve atomic precision in non-repeating molecular assemblies of the size desired for nanotechnology. For nanoelectronics in particular, a basic understanding of the electron transport properties of molecules must also be developed. Quantum chemistry provides powerful computational methods that can accurately predict the properties of small to medium sized molecules on a desktop workstation, and those of large molecules if one has access to a supercomputer. Of the many properties of a molecule that quantum chemistry routinely predicts, the ability to carry a current is one that had not even been considered until recently. "Currently", there is a controversy over just how to define this key property. Reminiscent of the situation in high-Tc superconductivity, much of the difficulty arises from the different models that are used to simplify the complex electronic structure of real materials. A model-independent approach has been proposed, that sacrifices the plentiful molecular orbitals and Bloch functions of conventional approaches, for a single three-dimensional observable quantity, the electron momentum density Pi(sub rho). This quantity is simply the probability of any electron having momentum rho, multiplied by the total number of electrons in the system (the position of the electron is uncertain). We have explored the utility of this new approach in providing a fundamental understanding of the electron transport properties of molecules that have provi been nominated as candidates for components in the design of nanoelectronics; phenylene-ethynylene oligomers. Some of the molecular systems that have been studied are sketched below.

MacDougall, Preston J.↗

The effects of molecular structure on the electrical conductivity of polymers

The role of Quantum Theoretical Methods is both predictive and supportive of experimental results in Chemistry. Present day methods are able to calculate vibrational spectra and stereochemical interactions for molecules of moderate size (up to 20 atoms). As for the predictive side, the electronic structure of molecules and polymers can be calculated in order to narrow down the field of many potential candidates, which would have the novel properties looked for. The following has been accomplished at the Rutgers Camden Chemistry Department as results of calculations on molecular and polymeric systems of interest to the Polymers Branch of the NASA Lewis Research Center, under Grant NAG3-956.

Burke, Luke A.↗

Ab initio characterization of ClOOH - Implications for atmospheric chemistry

The equilibrium structure, dipole moment, harmonic vibrational frequencies, and infrared intensities of ClOOH are determined using the CCSD(T) (singles and doubles coupled-cluster theory plus a perturbational estimate of the effects of connected triple excitations) electronic structure method in conjunction with a TZ2P (triple xi plus double polarization) basis set. The heat of formation of CIOOH is determined (using two different isodesmic reactions) to be +1.5 +/- 1 kcal/mol at 0 K or +0.2 +/- 1 kcal/mol at 298.15 K. Using the computed heat of formation, we examined the stability of ClOOH with respect to the ClO + OH, ClOO + H, and HOO + Cl dissociation limits. Since ClOOH is found to be quite stable, it is argued that the chemistry of ClOOH should be included in any accurate modeling of the stratosphere.

Lee, Timothy J.↗

Electrodynamic patterns in the polar region during periods of extreme magnetic quiescence

Using data from the DE 2 satellite, the electrodynamic patterns in the polar region during periods of extreme magnetic and auroral quiescence are analyzed for the existence of region-1 and region-2 field-aligned current systems, convection patterns, and electron-precipitation boundaries. The large-scale region-1 and region-2 currents were found to be usually absent during quiet periods, except in the cusp region. Field-aligned currents continue to be present, but as small-scale structures distributed through the auroral oval and over the entire polar cap. Convection patterns were always found in the summer hemisphere, but not always in the winter hemisphere, while structured electron precipitation was found to extend over the entire polar region independent of season.

Hoffman, R. A.↗

Energetics of Oxygen Interstitials in Cr and V

Dissolved oxygen in group IIIA-VA (Nb, Ti, Zr, Y) based alloys is a fundamental problem, affecting both mechanical properties and oxidation resistance, yet details of the phenomenon are poorly understood. In these alloys, oxygen is more stable dissolved in the metal than as an oxide-compound. In contrast, alloys based on Ni, Fe, Al and Cr exhibit almost no oxygen solubility. To improve the performance of Nb and Ti based alloys it is necessary to understand the differences in oxygen solubility between these two groups of metals. As a first step we considered the energetics of interstitial oxygen in alpha-V and alpha-Cr. Both of these metals have a BCC structure, yet the oxygen solubility in V is much higher than that in Cr. We obtain total energies, densities of states and population analyses using the CASTEP plane-wave pseudopotential density functional computer code. The differences in the energetics and electronic structures of the two materials, particularly the partial densities of states associated with the interstitial oxygen, are discussed.

Good, Brian S.↗

Vibrational and Rovibrational Spectroscopy Applied to Astrochemistry

The detection of molecules in astrophysical environments almost always requires remote sensing. While radioastronomical observation and associated rotational spectroscopy are powerful astronomical tools, infrared spectral analysis provides a unique means of examining the observable universe, especially for molecules where permanent dipole moments are small or even non-existent. The molecular vibrations of small molecules are now able to be modeled via quantum chemistry and electronic structure theory conjoined to vibrational analysis to within spectroscopic accuracy in many cases. This chapter will showcase this success and build upon it to show how such advances are now being leveraged to describe molecular vibrations for molecules containing dozens of atoms, electronically excited states, "hot bands," exoplanetary atmospheric opacity data, and even emission of polycyclic aromatic hydrocarbons. All of these are required to prune the interstellar spectral garden of its "weeds" in search of "flowers" that will provide the necessary fingerprints for astronomers to be able to probe the heavens for its past, present, and future secrets.

Ryan C. Fortenberry↗

Li-Doped Ionic Liquid Electrolytes: From Bulk Phase to Interfacial Behavior

Ionic liquids have been proposed as candidate electrolytes for high-energy density, rechargeable batteries. We present an extensive computational analysis supported by experimental comparisons of the bulk and interfacial properties of a representative set of these electrolytes as a function of Li-salt doping. We begin by investigating the bulk electrolyte using quantum chemistry and ab initio molecular dynamics to elucidate the solvation structure of Li(+). MD simulations using the polarizable force field of Borodin and coworkers were then performed, from which we obtain an array of thermodynamic and transport properties. Excellent agreement is found with experiments for diffusion, ionic conductivity, and viscosity. Combining MD simulations with electronic structure computations, we computed the electrochemical window of the electrolytes across a range of Li(+)-doping levels and comment on the role of the liquid environment. Finally, we performed a suite of simulations of these Li-doped electrolytes at ideal electrified interfaces to evaluate the differential capacitance and the equilibrium Li(+) distribution in the double layer. The magnitude of differential capacitance is in good agreement with our experiments and exhibits the characteristic camel-shaped profile. In addition, the simulations reveal Li(+) to be highly localized to the second molecular layer of the double layer, which is supported by additional computations that find this layer to be a free energy minimum with respect to Li(+) translation.

molecular dynamics↗

Electric Potential and Electric Field Imaging with Applications

The technology and techniques for remote quantitative imaging of electrostatic potentials and electrostatic fields in and around objects and in free space is presented. Electric field imaging (EFI) technology may be applied to characterize intrinsic or existing electric potentials and electric fields, or an externally generated electrostatic field may be used for (illuminating) volumes to be inspected with EFI. The baseline sensor technology, electric field sensor (e-sensor), and its construction, optional electric field generation (quasistatic generator), and current e-sensor enhancements (ephemeral e-sensor) are discussed. Demonstrations for structural, electronic, human, and memory applications are shown. This new EFI capability is demonstrated to reveal characterization of electric charge distribution, creating a new field of study that embraces areas of interest including electrostatic discharge mitigation, crime scene forensics, design and materials selection for advanced sensors, dielectric morphology of structures, inspection of containers, inspection for hidden objects, tether integrity, organic molecular memory, and medical diagnostic and treatment efficacy applications such as cardiac polarization wave propagation and electromyography imaging.

Generazio, Ed↗