No / In this paper, a compact microstrip band-pass filter (BPF) covering the 3.4 to 3.8 GHz spectrum bandwidth for 5G wireless communications is presented. The planar filter uses three resonators, each terminated by a via to hole ground at one end and a capacitor at the other end with 50 Ω transmission line impedances for input and output terminals. The coupling between the lines is adjusted to resonate at the centre frequency with third-order band-pass Butterworth properties. The proposed combline filter is designed on an alumina substrate with a relative dielectric constant of 9.8 and a very small size of 9×5×1.2 mm3. The proposed filter is simulated and optimized using CST microwave studio software. / European Union’s Horizon 2020 research and innovation programme under grant agreement H2020-MSCA-ITN-2016 SECRET-722424, UK Engineering and Physical Sciences Research Council (EPSRC) under grant EP/E022936/1

We give an overview of quantum chemical methods with a particular emphasis on the development of high-accuracy quantum chemical models. The reliability of these methods often hinges on whether enough electron correlation is included in the truncated wave function. As an example, we investigate the structures of m-benzyne and its fluorinated derivative, tetrafluoro-m-benzyne where the inclusion of triple excitations is paramount to correctly describe through-bond delocalization of the monocyclic form. At the CCSDT/6-31G** level of theory, the C1–C3 distance of the minimum energy form of m-benzyne is 2.0°A and the profile of the PES along the C1–C3 distance is that of an asymmetric, single-well, in agreement with previous density-functional theory and coupled cluster studies. In addition, the calculated CCSD(T) fundamental frequencies are in excellent agreement with the measured infrared frequencies, thus confirming the monocyclic form of m-benzyne. For tetrafluoro-m-benzyne, however, the increased eclipsing strain between the ring-external Câ X bonds stabilizes the bicyclo[3.1.0]hexatriene form: the C1–C3 distance is calculated at the CCSD(T)/cc-pVTZ level to be approximately 1.75 °A, which is in the range of elongated CC bonds. Computed harmonic vibrational frequencies compare reasonably well with the experimental neon-matrix difference spectrum and provide further evidence for the existence of a bicyclic form. We also report an extension of the coupled cluster iterative-triples model, CC3, to excited states of open-shell molecules, including radicals. We define the method for both spin-unrestricted Hartree-Fock (UHF) and spin-restricted open-shell Hartree-Fock (ROHF) reference determinants and discuss its efficient implementation in the PSI3 program package. The program is streamlined to use at most O(N7) computational steps and avoids storage of the triple-excitation amplitudes for both the ground-and excited-state calculations. The excitation-energy program makes use of a Lowdin projection formalism (comparable to that of earlier implementations) that allows computational reduction of the Davidson algorithm to only the single- and double-excitation space, but limits the calculation to only one excited state at a time. However, a root-following algorithm may be used to compute energies for multiple states of the same symmetry. Benchmark applications of the new methods to the lowest valence 2B1 state of the allyl radical, low-lying states of the CH and CO+ diatomics, and the nitromethyl radical show substantial improvement over ROHF- and UHF-based CCSD excitation energies for states with strong double-excitation character or cases suffering from significant spin contamination. For the allyl radical, CC3 adiabatic excitation energies differ from experiment by less than 0.02 eV, while for the 2§+ state of CH, significant errors of more than 0.4 eV remain. Finally, ground- and excited-state dipole moments are derived diagramatically and were recently developed within the PSI3 quantum chemistry package. However, convergence problems with computing the left-hand excited-state has prevented us from reporting any meaningful results. Thus, future work includes solving this convergence problem before the effects of triple excitations on one-electron properties can be reported with certainty. / Ph. D.

One of the most promising methods for surmounting the high-degree polynomial scaling wall associated with electron correlating wave function methods is the local correlation technique of Pulay and Saebø. They have proposed using a set of localized occupied and virtual orbitals free of the canonical constraint commonly employed in quantum chemistry, resulting in a method that scales linearly (in the asymptotic limit) with molecular size. Pulay and Saeb$oslash; first applied their methods to configuration interaction and later to M$oslash;ller-Plesset perturbation theory. Werner et al. have have extended the local correlation scheme of Pulay and Saeb$oslash; to coupled-cluster theory. One of the pitfalls of the local correlation methods developed by Pulay and Saeb$oslash; is the dependence of domain selection on the molecular geometry. In other words, as the geometry changes the domain structure of the local correlation calculation can change also, leading to discontinuities in the potential energy surface. We have examined the size of these discontinuities for the homolytic bond cleavage of fluoromethane and the heterolytic bond dissociation of singlet ketene and propadienone. Properties such as polarizabilities and optical rotation are realized through linear response theory, where the Hamiltonian is subject to an external perturbation and the wave function is allowed to respond to the applied perturbation. Within the context of local correlation it is necessary to understand how the domain structure alters in response to an applied perturbation. We have proposed using solutions to the CPHF equations (coupled-perturbed Hartree-Fock) in order to predict the correlation response to an applied perturbation. We have applied this technique to the calculation of polarizabilities, with very favorable results, and also to optical rotation, with mixed results. / Ph. D.

Coupled cluster (CC) and density functional theory (DFT) are highly regarded as robust quantum chemical methods for accurately predicting a wide variety of properties, such as molecular structures, thermochemical data, vibrational spectra, etc., but there has been little focus on the theoretical prediction of optical rotation. This property, also referred to as circular birefringence, is inherent to all chiral molecules and occurs because such samples exhibit different refractive indices for left- and right- circularly polarized light. This thesis focuses on the theoretical prediction of this chiroptic property using CC and DFT quantum chemical models. Several small chiral systems have been studied, including (S)-methyloxirane, (R)-epichlorohydrin, (R)-methylthiirane, and the conformationally flexible molecules, (R)-3-chloro-1-butene and (R)-2-chlorobutane. All predicted results have been compared to recently published gas-phase cavity ringdown polarimetry data. When applicable, well-converged Gibbs free energy differences among confomers were determined using complete-basis-set extrapolations of CC energies in order to obtain Boltzmann-averaged specific rotations. The overall results indicate that the theoretical rotation is highly dependent on the choice of optimized geometry and basis set (diffuse functions are shown to be extremely important), and that there is a large difference between the CC and DFT predicted values, with DFT usually predicting magnitudes that are larger than those of coupled cluster theory. / Ph. D.

Spontaneous order happens in non-equilibrium systems composed of interacting elements. This phenomenon manifests in both the formation of space-time patterns in reaction-diffusion systems and collective rhythmic behaviors in coupled oscillators. In this thesis, we present the results of two studies: 1) The response of a multi-species predator-prey system to perturbation. 2) The features of a rich attractor space in a system of repulsively coupled Kuramoto oscillators. In the first part, we address this question: how does a complex coarsening system with non-trivial in-domain dynamics respond to perturbations? We choose a cyclic predator-prey model with six species each attacking three others. As a result of this interaction network, two competing domains form, while inside each domain three species play a rock-paper-scissors game which results in the formation of spirals inside the domains. We perturb the system by changing the interaction scheme which leads to a change of alliances and therefore a different spatial pattern. As expected, perturbing a complex space-time pattern results in a complex response. In the second part, we explore the attractor space of a system of repulsively coupled oscillators with non-homogeneous natural frequencies on a hexagonal lattice. Due to the negative coupling and the particular choice of geometry, some of the links between oscillators become frustrated. Coupled oscillators with frustration show similar features as frustrated magnetic systems. We use the parameters of the system like the coupling constant and the width of the frequency distribution to understand the system's attractor space. Further, we study the effects of external noise on the system. We also identify the breaking of time-translation invariance in the absence of external noise, in our system. / Doctor of Philosophy / Spontaneous ordering is a ubiquitous phenomenon observed in natural systems containing many interacting elements. In some systems the order is observed in the form of spatial patterns. It also can be seen in a population of coupled oscillators in the form of collective rhythmic behaviors. In this thesis, we present the results of two studies. For the first study, we choose a cyclic predator-prey system that shows a non-trivial space-time pattern. The system consists of six species each attacking three others, cyclically. By choosing such an interaction network, two competing domains form, while inside each domain three species play a rock-paper-scissors game. As a result of the inner competition, spirals form inside the domains. We study the response of the system to a perturbation. To perturb the system, we change the interaction scheme which leads to a change of alliances and therefore, a different spatial pattern. In the second study, we explore the patterns of clustering and synchronization in a system of repulsively coupled oscillators with non-homogeneous natural frequencies. Due to the negative coupling and the particular choice of geometry, some of the links between oscillators become frustrated. We use the parameters of the system such as the coupling constant and the width of the frequency distribution to understand the system’s attractor space. Further, we examine the effect of external noise on the system.

The variational quantum eigensolver (VQE) approach is currently one of the most promising strategies for simulating chemical systems on quantum hardware. In this work, I will describe a new quantum algorithm and a new set of classical algorithms based on VQE. The quantum algorithm, ADAPT-VQE, shows promise in mitigating many of the known limitations of VQEs: Ansatz ambiguity, local minima, and barren plateaus are all addressed to varying degrees by ADAPT-VQE. The classical algorithm family, O2DX-UCCSD, draws inspiration from VQEs, but is classically solvable in polynomial time. This group of algorithms yields equations similar to those of the linearized coupled cluster theory (LCCSD) but is more systematically improvable and, for X = 3 or X = ∞, can break single bonds, which LCCSD cannot do. The overall aim of this work is to showcase the richness of the VQE algorithm and the breadth of its derivative applications. / Doctor of Philosophy / A core goal of quantum chemistry is to compute accurate ground-state energies for molecules. Quantum computers promise to simulate quantum systems in ways that classical computers cannot. It is believed that quantum computers may be able to characterize molecules that are too large for classical computers to treat accurately. One approach to this is the variational quantum eigensolver, or VQE. The idea of a VQE is to use a quantum computer to measure the molecular energy associated with a quantum state which is parametrized by some classical set of parameters. A classical computer will use a classical optimization scheme to update those parameters before the quantum computer measures the energy again. This loop is expected to minimize the quantum resources needed for a quantum computer to be useful, since much of the work is outsourced to classical computers. In this work, I describe two novel algorithms based on the VQE which solve some of its problems.

The efficient computation of dynamic (time-dependent) molecular properties is a broad field with numerous applications in aiding molecular synthesis and design, with a particular preva- lence in spectroscopic predictions. Typical methods for computing the response of a molecu- lar system to an electromagnetic field (EMF) considers a quantum mechanical description of the molecule and a classical approximation for the EMF. Methods for describing light-matter interactions with high-accuracy electronic structure methods, such as coupled cluster (CC), are discussed, with a focus on improving the efficiency of such methods. The CC method suffers from high-degree polynomial scaling. In addition to the ground-state calculation, computing dynamic properties requires the description of sensitive excited-state effects. The cost of such methods often prohibits the accurate calculation of response prop- erties for systems of significant importance, such as large-molecule drug candidates or chiral species present in biological systems. While the literature is ripe with reduced-scaling meth- ods for CC ground-state calculations, considerably fewer approaches have been applied to excited-state properties, with even fewer still providing adequate results for realistic systems. This work presents three studies on the reduction of the cost of molecular property evalu- ations, in the hopes of closing this gap in the literature and widening the scope of current theoretical methods. There are two main ways of simulating time-dependent light-matter interactions: one may consider these effects in the frequency domain, where the response of the system to an EMF is computed directly; or, the response may be considered explicitly in the time domain, where wave function (or density) parameters can be propagated in time and examined in detail. Each methodology has unique advantages and computational bottlenecks. The first two studies focus on frequency-domain calculations, and employ fragmentation and machine- learning techniques to reduce the cost of single-molecule calculations or sets of calculations across a series of geometric conformations. The third study presents a novel application of the local correlation technique to real-time CC calculations, and highlights deficiencies and possible solutions to the approach. / Doctor of Philosophy / Theoretical chemistry plays a key role in connecting experimental results with physical inter- pretation. Paramount to the success of theoretical methods is the ability to predict molecular properties without the need for costly high-throughput synthesis, aiding in the determina- tion of molecular structure and the design of new materials. Light-matter interactions, which govern spectroscopic techniques, are particularly complicated, and sensitive to the theoreti- cal tools employed in their prediction. Compounding the issue of accuracy is one of efficiency — accurate theoretical methods typically incur steep scaling of computational cost (memory and processor time) with respect to the size of the system. An important aspect in improving the efficiency of these methods is understanding the nature of light-matter interactions at a quantum level. Many unanswered questions still remain, such as, "Can light-matter interactions be thought of as a sum of interactions be- tween smaller fragments of the system?" and "Can conventional methods of accelerating ground-state calculations be expected to perform well for spectroscopic properties?" The present work seeks to answer these questions through three studies, focusing on improving the efficiency of these techniques, while simultaneously addressing their fundamental flaws and providing reasonable alternatives.

Yes / Large amount of sediment deposits in the reservoir area can cause dam break, which not only leads to an immeasurable loss to the society, but also the sediments from the reservoir can be transported to generate further problems in the downstream catchment. This study aims to investigate the short-to-long term sediment transport and channel meandering process under such a situation. A coupled explicit-implicit technique based on the Euler-Lagrangian method (ELM) is used to solve the hydrodynamic equations, in which both the small and large time steps are used separately for the fluid and sediment marching. The main feature of the model is the use of the Characteristic-Based Split (CBS) method for the local time step iteration to correct the ELM traced lines. Based on the solved flow field, a standard Total Variation Diminishing (TVD) finite volume scheme is applied to solve the sediment transportation equation. The proposed model is first validated by a benchmark dambreak water flow experiment to validate the efficiency and accuracy of ELM modelling capability. Then an idealized engineering dambreak flow is used to investigate the long-term downstream channel meandering process with nonuniform sediment transport. The results showed that both the hydrodynamic and morphologic features have been well predicted by the proposed coupled model. / This research work is supported by Sichuan Science and Technology Support Plan (2014SZ0163), Start-up Grant for the Young Teachers of Sichuan University (2014SCU11056), and Open Research Fund of the State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University (SKLH 1409; 1512).

An investigation of the effect of the coupling value and the structural perturbation parameter is conducted on coupled systems. The analysis of a coupled pendulums system results in the analytical expression of the natural frequencies of the system. The response of the system for harmonic excitation and random input is developed. Two single Euler-Bemouilli beams coupled by a torsional spring constitute the multi degree of freedom extension of the study. Special care is given to show the variation of the natural frequencies \with the two parameters and modal overlapping is shown. The study of the response to harmonic excitation makes the localization phenomenon apparent. For the special case where one of the beam is excited by a rain-on-the roof load, the estimates of the amplitude for each beam and the power flow between the beams are analytically expressed. The power flow is proved to be concentrated around the natural frequencies, stronger for a tuned system and sensitive to the number of modes, especially v:hen modal overlapping occurs. A Monte Carlo simulation considering the perturbation parameter as a Gaussian random variable points out that the mean value of the power decreases rapidly with higher frequency. The power flow is also calculated using the theory of the Statistical Energy Analysis. / Master of Science

Quantum mechanical methods are becoming increasingly useful and applicable tools to complement and support experiment. Nonetheless, some barriers to further applications of theoretical models still remain. A coupled cluster singles and doubles (CCSD) calculation, a reliable ab initio method, scales approximately on the order of 𝑂(𝑁⁶), where 𝑁 is a measure of the system size. This unfortunately limits the use of such high-accuracy methods to relatively small systems. Coupled cluster property calculations must be used in conjunction with reduced-scaling methods in order to broaden the range of applications to larger systems. In this work, we introduce some of the underlying theory behind such calculations and test the performance of several local correlation techniques for polarizabilities, optical rotations, and excited state properties. In general, when the computational cost is significantly reduced, the necessary accuracy is lost. Polarizabilities are less sensitive to the truncation schemes than optical rotations, and the excitation data is often only in agreement with the canonical result for the first few excited states. Additionally, we present a novel application of equation-of-motion coupled cluster singles and doubles to simulated circularly polarized luminescence spectra of eight chiral ketones. Both the absorption in the ground state and emission from the excited states were examined. Extensive geometry analyses were performed, revealing that optimized structures at the density functional theory were adequate for the calculation accurate coupled cluster excitation data. / Ph. D.