Gaussian Approximation Potential: an interatomic potential derived from first principles Quantum Mechanics

Simulation of materials at the atomistic level is an important tool in studying microscopic structure and processes. The atomic interactions necessary for the simulation are correctly described by Quantum Mechanics. However, the computational resources required to solve the quantum mechanical equations limits the use of Quantum Mechanics at most to a few hundreds of atoms and only to a small fraction of the available configurational space. This thesis presents the results of my research on the development of a new interatomic potential generation scheme, which we refer to as Gaussian Approximation Potentials. In our framework, the quantum mechanical potential energy surface is interpolated between a set of predetermined values at different points in atomic configurational space by a non-linear, non-parametric regression method, the Gaussian Process. To perform the fitting, we represent the atomic environments by the bispectrum, which is invariant to permutations of the atoms in the neighbourhood and to global rotations. The result is a general scheme, that allows one to generate interatomic potentials based on arbitrary quantum mechanical data. We built a series of Gaussian Approximation Potentials using data obtained from Density Functional Theory and tested the capabilities of the method. We showed that our models reproduce the quantum mechanical potential energy surface remarkably well for the group IV semiconductors, iron and gallium nitride. Our potentials, while maintaining quantum mechanical accuracy, are several orders of magnitude faster than Quantum Mechanical methods.

QM/MM simulation of liquid water with an adaptive quantum region.

The simulation of complex chemical systems often requires a multi-level description, in which a region of special interest is treated using a computationally expensive quantum mechanical (QM) model while its environment is described by a faster, simpler molecular mechanical (MM) model. Furthermore, studying dynamic effects in solvated systems or bio-molecules requires a variable definition of the two regions, so that atoms or molecules can be dynamically re-assigned between the QM and MM descriptions during the course of the simulation. Such reassignments pose a problem for traditional QM/MM schemes by exacerbating the errors that stem from switching the model at the boundary. Here we show that stable, long adaptive simulations can be carried out using density functional theory with the BLYP exchange-correlation functional for the QM model and a flexible TIP3P force field for the MM model without requiring adjustments of either. Using a primary benchmark system of pure water, we investigate the convergence of the liquid structure with the size of the QM region, and demonstrate that by using a sufficiently large QM region (with radius 6 Å) it is possible to obtain radial and angular distributions that, in the QM region, match the results of fully quantum mechanical calculations with periodic boundary conditions, and, after a smooth transition, also agree with fully MM calculations in the MM region. The key ingredient is the accurate evaluation of forces in the QM subsystem which we achieve by including an extended buffer region in the QM calculations. We also show that our buffered-force QM/MM scheme is transferable by simulating the solvated Cl(-) ion.

Coexistence of high-bit-rate quantum key distribution and data on optical fiber

Quantum key distribution (QKD) uniquely allows distribution of cryptographic keys with security verified by quantum mechanical limits. Both protocol execution and subsequent applications require the assistance of classical data communication channels. While using separate fibers is one option, it is economically more viable if data and quantum signals are simultaneously transmitted through a single fiber. However, noise-photon contamination arising from the intense data signal has severely restricted both the QKD distances and secure key rates. Here, we exploit a novel temporal-filtering effect for noise-photon rejection. This allows high-bit-rate QKD over fibers up to 90 km in length and populated with error-free bidirectional Gb/s data communications. With high-bit rate and range sufficient for important information infrastructures, such as smart cities and 10 Gbit Ethernet, QKD is a significant step closer towards wide-scale deployment in fiber networks.

Dynamical behavior of damped driven coupled single electron simple harmonic oscillators

Coherent coupling between a large number of qubits is the goal for scalable approaches to solid state quantum information processing. Prototype systems can be characterized by spectroscopic techniques. Here, we use pulsed-continuous wave microwave spectroscopy to study the behavior of electrons trapped at defects within the gate dielectric of a sol-gel-based high-k silicon MOSFET. Disorder leads to a wide distribution in trap properties, allowing more than 1000 traps to be individually addressed in a single transistor within the accessible frequency domain. Their dynamical behavior is explored by pulsing the microwave excitation over a range of times comparable to the phase coherence time and the lifetime of the electron in the trap. Trap occupancy is limited to a single electron, which can be manipulated by resonant microwave excitation and the resulting change in trap occupancy is detected by the change in the channel current of the transistor. The trap behavior is described by a classical damped driven simple harmonic oscillator model, with the phase coherence, lifetime and coupling strength parameters derived from a continuous wave (CW) measurement only. For pulse times shorter than the phase coherence time, the energy exchange between traps, due to the coupling, strongly modulates the observed drain current change. This effect could be exploited for 2-qubit gate operation. The very large number of resonances observed in this system would allow a complex multi-qubit quantum mechanical circuit to be realized by this mechanism using only a single transistor.

Solid-state memories based on ferroelectric tunnel junctions.

Ferroic-order parameters are useful as state variables in non-volatile information storage media because they show a hysteretic dependence on their electric or magnetic field. Coupling ferroics with quantum-mechanical tunnelling allows a simple and fast readout of the stored information through the influence of ferroic orders on the tunnel current. For example, data in magnetic random-access memories are stored in the relative alignment of two ferromagnetic electrodes separated by a non-magnetic tunnel barrier, and data readout is accomplished by a tunnel current measurement. However, such devices based on tunnel magnetoresistance typically exhibit OFF/ON ratios of less than 4, and require high powers for write operations (>1 × 10(6) A cm(-2)). Here, we report non-volatile memories with OFF/ON ratios as high as 100 and write powers as low as ∼1 × 10(4) A cm(-2) at room temperature by storing data in the electric polarization direction of a ferroelectric tunnel barrier. The junctions show large, stable, reproducible and reliable tunnel electroresistance, with resistance switching occurring at the coercive voltage of ferroelectric switching. These ferroelectric devices emerge as an alternative to other resistive memories, and have the advantage of not being based on voltage-induced migration of matter at the nanoscale, but on a purely electronic mechanism.

Solid-state memories based on ferroelectric tunnel junctions

Ferroic-order parameters are useful as state variables in non-volatile information storage media because they show a hysteretic dependence on their electric or magnetic field. Coupling ferroics with quantum-mechanical tunnelling allows a simple and fast readout of the stored information through the influence of ferroic orders on the tunnel current. For example, data in magnetic random-access memories are stored in the relative alignment of two ferromagnetic electrodes separated by a non-magnetic tunnel barrier, and data readout is accomplished by a tunnel current measurement. However, such devices based on tunnel magnetoresistance typically exhibit OFF/ON ratios of less than 4, and require high powers for write operations (>1 × 10 6 A cm -2). Here, we report non-volatile memories with OFF/ON ratios as high as 100 and write powers as low as ∼1 × 10 4A cm -2 at room temperature by storing data in the electric polarization direction of a ferroelectric tunnel barrier. The junctions show large, stable, reproducible and reliable tunnel electroresistance, with resistance switching occurring at the coercive voltage of ferroelectric switching. These ferroelectric devices emerge as an alternative to other resistive memories, and have the advantage of not being based on voltage-induced migration of matter at the nanoscale, but on a purely electronic mechanism. © 2012 Macmillan Publishers Limited. All rights reserved.

A numerical simulation of AFR switch of SI engines

A novel mechanical method of achieving a rapid switch between stoichiometric and lean conditions for SI engines is explored. Two and three throttle configurations, a switch strategy which employs a standard intake manifold and an assembly of pipes and throttle(s), are investigated numerically by using a one-dimensional engine simulation program based on the method of characteristics. The results indicate that it is possible to achieve rapid AFR switch without a torque jump, i.e. unperceptible to the driver. © 1998 Society of Automotive Engineers, Inc.

First principles interatomic potential for tungsten based on Gaussian process regression

An accurate description of atomic interactions, such as that provided by first principles quantum mechanics, is fundamental to realistic prediction of the properties that govern plasticity, fracture or crack propagation in metals. However, the computational complexity associated with modern schemes explicitly based on quantum mechanics limits their applications to systems of a few hundreds of atoms at most. This thesis investigates the application of the Gaussian Approximation Potential (GAP) scheme to atomistic modelling of tungsten - a bcc transition metal which exhibits a brittle-to-ductile transition and whose plasticity behaviour is controlled by the properties of $\frac{1}{2} \langle 111 \rangle$ screw dislocations. We apply Gaussian process regression to interpolate the quantum-mechanical (QM) potential energy surface from a set of points in atomic configuration space. Our training data is based on QM information that is computed directly using density functional theory (DFT). To perform the fitting, we represent atomic environments using a set of rotationally, permutationally and reflection invariant parameters which act as the independent variables in our equations of non-parametric, non-linear regression. We develop a protocol for generating GAP models capable of describing lattice defects in metals by building a series of interatomic potentials for tungsten. We then demonstrate that a GAP potential based on a Smooth Overlap of Atomic Positions (SOAP) covariance function provides a description of the $\frac{1}{2} \langle 111 \rangle$ screw dislocation that is in agreement with the DFT model. We use this potential to simulate the mobility of $\frac{1}{2} \langle 111 \rangle$ screw dislocations by computing the Peierls barrier and model dislocation-vacancy interactions to QM accuracy in a system containing more than 100,000 atoms.

A coupled hydro-mechanical analysis for prediction of hydraulic fracture propagation in saturated porous media using EFG mesh-less method

The details of the Element Free Galerkin (EFG) method are presented with the method being applied to a study on hydraulic fracturing initiation and propagation process in a saturated porous medium using coupled hydro-mechanical numerical modelling. In this EFG method, interpolation (approximation) is based on nodes without using elements and hence an arbitrary discrete fracture path can be modelled.The numerical approach is based upon solving two governing partial differential equations of equilibrium and continuity of pore water simultaneously. Displacement increment and pore water pressure increment are discretized using the same EFG shape functions. An incremental constrained Galerkin weak form is used to create the discrete system of equations and a fully implicit scheme is used for discretization in the time domain. Implementation of essential boundary conditions is based on the penalty method. In order to model discrete fractures, the so-called diffraction method is used.Examples are presented and the results are compared to some closed-form solutions and FEM approximations in order to demonstrate the validity of the developed model and its capabilities. The model is able to take the anisotropy and inhomogeneity of the material into account. The applicability of the model is examined by simulating hydraulic fracture initiation and propagation process from a borehole by injection of fluid. The maximum tensile strength criterion and Mohr-Coulomb shear criterion are used for modelling tensile and shear fracture, respectively. The model successfully simulates the leak-off of fluid from the fracture into the surrounding material. The results indicate the importance of pore fluid pressure in the initiation and propagation pattern of fracture in saturated soils. © 2013 Elsevier Ltd.

Room temperature magnetic quantum cellular automata

All computers process information electronically. A processing method based on magnetism is reported here, in which networks of interacting submicrometer magnetic dots are used to perform logic operations and propagate information at room temperature. The logic states are signaled by the magnetization direction of the single-domain magnetic dots; the dots couple to their nearest neighbors through magnetostatic interactions. Magnetic solitons carry information through the networks, and an applied oscillating magnetic field feeds energy into the system and serves as a clock. These networks offer a several thousandfold increase in integration density and a hundredfold reduction in power dissipation over current microelectronic technology.