First-principles informed phenomenological models of optical and lattice response in materials

In this dissertation, we present work on the first-principles informed phenomenological modeling of the optical properties of materials. We use density functional theory and time-dependent density functional theory calculations to inform parameterized models of the response to light in materials. We include the effect of ultrafast nonequilibrium effects, as well as the importance of quantum mechanical lattice vibrations. Using these models, we validate the approaches, and predict the effect of both ultrafast phenomena as well as quantum mechanical vibrations on the optical properties of bulk and 2D materials. Such modeling opens up avenues for efficient phenomenological approaches to describing optical phenomena in materials while keeping the accuracy of first-principles simulations

Compact Broadband Low-Loss Taper for Coupling to a Silicon Nitride Photonic Wire

We demonstrate an ultra-compact waveguide taper in Silicon Nitride platform. The proposed taper provides a coupling-efficiency of 95% at a length of 19.5 um in comparison to the standard linear taper of length 50 um that connects a 10 um wide waveguide to a 1 um wide photonic wire. The taper has a spectral response > 75% spanning over 800 nm and resilience to fabrication variations; >200 nm change in taper and end waveguide width varies transmission by <5%. We experimentally demonstrate taper insertion loss of <0.1 dB/transition for a taper as short as 19.5 um, and reduces the footprint of the photonic device by 50.8% compared to the standard adiabatic taper. To the best of our knowledge, the proposed taper is the shortest waveguide taper ever reported in Silicon Nitride

Ultra-compact low-loss broadband waveguide taper in silicon-on-insulator

A novel design of large bandwidth, fabrication tolerant, CMOS-compatible compact tapers (15 um) have been proposed and experimentally demonstrated in silicon-on-insulator. The proposed taper along with linear grating couplers for spot-size conversion exhibits no degradation in the coupling efficiency compared to a standard focusing grating in 1550 nm band. A single taper design has a broadband operation over 600 nm that can be used in O, C and L-band. The proposed compact taper is highly tolerant to fabrication variations; 80 nm change in the taper width and 200 nm in end waveguide width varies the taper transmission by <0.4 dB. The footprint of the device i.e. taper along with the linear gratings is ~ 250 {\mu}m2; this is 20X smaller than the adiabatic taper and 2X smaller than the focusing grating coupler

Illumination protocols for non-linear phononics in bismuth and antimony

We study the optical generation and control of coherent phonons in elemental bismuth (Bi) and antimony (Sb) using a classical equation of motion informed by first-principles calculations of the potential energy surface and the frequency-dependent macroscopic dielectric function along the zone-centered optical phonons coordinates. Using this approach, we demonstrate that phonons with the largest optomechanical couplings, also have the strongest degree of anharmonicity, a result of the broken symmetry structural ground state of Bi and Sb. We show how this anharmonicity, explaining the light-induced phonon softening observed in experiments, prevents the application of standard phonon-amplification and annihilation protocols. We introduce a simple linearization protocol that extends the use of such protocols to the case of anharmonic phonons in broken symmetry materials, and demonstrate its efficiency at high displacement amplitudes. Our formalism and results provide a path for improving optical control in non-linear phononics

GPAW: open Python package for electronic-structure calculations

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE) providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation (BSE), variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support of GPU acceleration has been achieved with minor modifications of the GPAW code thanks to the CuPy library. We end the review with an outlook describing some future plans for GPAW

Spectroscopic Study of the Reversible Chemical Reduction and Reoxidation of Substitutional Cr Ions in Sr₂TiO₄

The solid-state synthesis and controllable speciation of Cr dopants in the layered perovskite Sr₂TiO₄ is reported. We employed a chemical reduction procedure with NaBH₄ at relatively mild temperatures (<450 °C) to impart sensitive control over the relative concentration of Cr³⁺ dopants, the charge-state of oxygen-vacancy defects, and presence of Ti³⁺ defects in highly reduced Cr-doped Sr₂TiO₄. The electron paramagnetic resonance (EPR) spectra of the reduced powder samples reveal a 12-fold increase in the Cr³⁺ concentration within the axially compressed Ti⁴⁺-site of the Sr₂TiO₄ host. The increase in Cr³⁺ content is achieved through the reduction of higher-valence Cr ions that are either EPR silent or diamagnetic. The spin-Hamiltonian parameters for Cr³⁺ substituted at the B-site of Sr₂TiO₄ were refined to <i>D</i> = −201 × 10^–4 cm^–1, <i>g</i>_⊥ = 1.980, and <i>g</i>_∥ = 1.978. In addition, the Cr³⁺ ion exhibits a temperature-dependent axial component to the zero-field splitting of the ⁴A₂ ground term that is accounted for by ligand field theory and an isotropic contraction of the Sr₂TiO₄ lattice with decreasing temperature. The observed changes to the electronic structure upon reduction are quantitatively reversible upon reoxidation of the sample under aerobic annealing at the same temperature and duration as the reduction conditions. This temperature dependence of the Cr³⁺ content in the Cr-doped Sr₂TiO₄ powders is discussed and contrasted to our recent study on Cr-doped SrTiO₃