Physical Sciences and Mathematics Commons^™

In Situ Study Of Ultrafast Carrier Transport Dynamics In Perovskite Thin-Films, Kanishka Kobbekaduwa

All Dissertations

Perovskites are a novel class of materials that have piqued the interest of researchers in photovoltaics, photodetectors, and optoelectronics. In this study, we measure and elucidate in situ ultrafast carrier dynamics in both organic and inorganic, lead, and non-lead-based halide perovskite thin films using ultrafast photocurrent spectroscopy (UPCS) with a sub-25 ps time resolution. The UPCS technique enables us to define carrier transport dynamics in spatial, temporal, and energy landscapes via measurements at different electric fields, laser intensities, and temperatures. Here we explore and analyze solution-processed bulk MAPbI₃ and nanocrystalline CsPbI₃-based devices and novel non-lead double-layered perovskite …

Pressure- And Temperature-Dependent Inelastic Neutron Scattering Study Of The Phase Transition And Phonon Lattice Dynamics In Para-Terphenyl, Qingan Cai, Michael Mcintire, Luke L. Daemen, Chen Li, Eric Chronister

Chemistry and Biochemistry Faculty Research

Inelastic neutron scattering has been performed on para-terphenyl at temperatures from 10 to 200 K and under pressures from the ambient pressure to 1.51 kbar. The temperature dependence of phonons, especially low-frequency librational bands, indicates strong anharmonic phonon dynamics. The pressure- and temperature-dependence of the phonon modes suggest a lack of phase transition in the region of 0-1.51 kbar and 10-30 K. Additionally, the overall lattice dynamics remains similar up to 200 K under the ambient pressure. The results suggest that the boundary between the ordered triclinic phase and the third solid phase, reported at lower temperatures and higher pressures, …

Investigation Of Phonon Polaritons In An Hbn Gan Heterostructure, Catherine G. O'Hearn

Graduate Theses, Dissertations, and Problem Reports

There have been many great advances in the generation and manipulation of optics in the visible and near infrared (IR) range over the past decade. This is largely due to plasmonic enhancement, which has led to new technology in biosensing and molecule detection, solid-state lighting, and solar energy harvesting. The field of plasmonics uses quanta of plasma oscillations, plasmons, formed from the interaction between electromagnetic radiation and free electrons to enhance optical near field magnitudes. However, there is still a large region of the electromagnetic spectrum, covering the mid-infrared (MIR) and terahertz (THz) regions, ranging from 3 μm to 1 …

Lattice Thermal Conductivity Of Quartz At High Pressure And Temperature From The Boltzmann Transport Equation, Xue Xiong, Eugene J. Ragasa, Aleksandr V. Chernatynskiy, Dawei Tang, Simon R. Phillpot

Physics Faculty Research & Creative Works

The thermal conductivities along the basal and hexagonal directions of α-quartz silica, the low-temperature form of crystalline SiO₂, are predicted from the solution of the Boltzmann transport equation combined with the van Beest, Kramer, and van Santen potential for the temperature up to 900 K and the pressure as high as 4 GPa. The thermal conductivities at atmospheric pressure, which show a negative and nonlinear dependence on temperature, are in reasonable agreement with the experimental data. The influence of pressure on thermal conductivity is positive and linear. The pressure (P) and temperature (T) dependences of the thermal conductivity …

Impact Of Anharmonicity On The Vibrational Entropy And Specific Heat Of Uo₂, M. S. Bryan, J. W. L. Pang, B. C. Larson, Aleksandr V. Chernatynskiy, D. L. Abernathy, K. Gofryk, M. E. Manley, For Full List Of Authors, See Publisher's Website.

Physics Faculty Research & Creative Works

The impact of anharmonicity on the vibrational entropy and heat capacity of UO2 has been investigated from 10 to 1200 K using inelastic neutron-scattering measurements of the phonon density of states (PDOS). Small changes in the PDOS are observed from 10 to 295 K, with more noticeable changes appearing in the 750- and 1200-K data. The specific heat determined from the PDOS measurements is in agreement with macroscopic specific heat measurements, and the overall impact of nondilation anharmonicity on the specific heat has been shown to be less than 2%. An analysis of the phonon measurements shows that the softening …

Large And Realistic Models Of Amorphous Silicon, Dale Ingram, Bishal Bhattarai, Parthapratim Biswas, David A. Drabold

Faculty Publications

Amorphous silicon (a-Si) models are analyzed for structural, electronic and vibrational characteristics. Several models of various sizes have been computationally fabricated for this analysis. It is shown that a recently developed structural modeling algorithm known as force-enhanced atomic refinement (FEAR) provides results in agreement with experimental neutron and X-ray diffraction data while producing a total energy below conventional schemes. We also show that a large model (∼ 500 atoms) and a complete basis is necessary to properly describe vibrational and thermal properties. We compute the density for a-Si, and compare with experimental results.

Transient Lattice Deformations Of Crystals Studied By Means Of Ultrafast Time-Resolved X-Ray And Electron Diffraction, Runze Li, Kyle Sundqvist, Jie Chen, H. E. Elsayed-Ali, Jie Zhang, Peter M. Rentzepis

Electrical & Computer Engineering Faculty Publications

Ultrafast lattice deformation of tens to hundreds of nanometer thick metallic crystals, after femtosecond laser excitation, was measured directly using 8.04 keV subpicosecond x-ray and 59 keV femtosecond electron pulses. Coherent phonons were generated in both single crystal and polycrystalline films. Lattice compression was observed within the first few picoseconds after laser irradiation in single crystal aluminum, which was attributed to the generation of a blast force and the propagation of elastic waves. The different time scales of lattice heating for tens and hundreds nanometer thick films are clearly distinguished by electron and x-ray pulse diffraction. The electron and lattice …

Progress Towards Terahertz Acoustic Phonon Generation In Doping Superlattices, Thomas E. Wilson

Thomas E. Wilson

Progress is described in experiments to generate coherent terahertz acoustic phonons in silicon doping superlattices by the resonant absorption of nanosecond-pulsed far-infrared laser radiation. Future experiments are proposed that would use the superlattice as a transducer in a terahertz cryogenic acoustic reflection microscope with sub-nanometer resolution.

Prospective Solid-State Photonic Cryocooler Based On The “Phonon-Deficit Effect”, Gurgen Melkonyan, Armen Gulian

Mathematics, Physics, and Computer Science Faculty Articles and Research

In this design microwave photons are propagating in a sapphire rod, and are being absorbed by a superconductor deposited on the surface of the rod. The frequency of the radiation is tuned to be less than the energy gap in the superconductor, so that the pair breaking is not taking place. This photon pumping redistributes the electron-hole quasiparticles: their distribution function is non-equilibrium, and the “phonon-deficit effect” takes place. There is a dielectric material deposited on top of superconductor, which serves asthe “cold finger” of the cooler. Its “acoustical density” is supposed to be smaller than that of the superconducting …

Terahertz Studies Of The Dielectric Response And Second-Order Phonons In A Gase Crystal, B. L. Yu, F. Zeng, V. Kartazayev, R. R. Alfano, K. C. Mandal

Krishna C. Mandal

No abstract provided.

Erratum: “Terahertz Studies Of The Dielectric Response And Second-Order Phonons In A Gase Crystal” [Appl. Phys. Lett.87, 182104 (2005)], B. L. Yu, F. Zeng, V. Kartazayev, R. R. Alfano, K. C. Mandal

Krishna C. Mandal

No abstract provided.

Tb3+-Doped K Pb2Br5: Low-Energy Phonon Mid-Infrared Laser Crystal, U. N. Roy, R. H. Hawrami, Y. Cui, S. Morgan, A. Burger, K. C. Mandal, C. C. Noblitt, S. A. Speakman, K. Rademaker, S. A. Payne

Krishna C. Mandal

No abstract provided.

Terahertz Studies Of The Dielectric Response And Second-Order Phonons In A Gase Crystal, B. L. Yu, F. Zeng, V. Kartazayev, R. R. Alfano, K. C. Mandal

Krishna C. Mandal

No abstract provided.

Mueller Matrix Spectroscopic Ellipsometry Of Multiferroics, Roman Basistyy

Dissertations

Multiferroics, materials which possess several ferroic orders, are the focus of research in recent years. Among these materials are oxide crystals, such as, for example, RMnO₃, RMn₂O₅, R₃Fe₅O₁₂, where R stands for rare earth ions. The most fascinating physics occurs when magnon-lattice coupling reveals itself in the far-IR spectra of multiferroics. The expected optical behavior puts multiferroics into a more general category of bi-anisotropic materials, the properties of which could be only described using anisotropic dielectric ε(ω), magnetic μ(ω), and …

Crystal Dynamics Of Zinc Chalcogenides I: An Application To Znscrystal Dynamics Of Zinc Chalcogenides I: An Application To Zns, Jay Prakash Dubey, Raj Kishor Tiwari, Kripa Shankar Upadhyaya, Pramod Kumar Pandey

Turkish Journal of Physics

A van der Waals three body force rigid shell model (VTRSM) developed earlier for NaCl and CsCl structure was expanded by us for zinc blende structure (ZBS). This model includes the effect of three body interactions and van der Waals interactions in the rigid shell model where short-range interactions were considered up to the second neighbor. Our model thus developed was applied to study the phonon dispersion curves, Debye temperature variation, two phonon Raman/IR spectra, and anharmonic elastic properties of ZnS. Our results are in good agreement with the measured data wherever available.

The Fabrication And Characterization Of Granular Aluminium/Palladium Bilayer Microbolometers, Thomas E. Wilson

Thomas E. Wilson

Superconducting granular aluminium/palladium bilayer microbolometers with subnanosecond response can be easily fabricated using an all lift-off process with image-reversal lithography. The palladium capping layer allows for convenient and reproducible Ohmic contacts to be made to the device. We report their fabrication, resistance–current calibration, responsivity and response time. Finally, a deconvolution algorithm is used to improve the time resolution to approximately 1 ns while obtaining the incident photon and phonon fluxes in both direct photoexcitation and phonon heat pulse experiments.

Progress Towards Terahertz Acoustic Phonon Generation In Doping Superlattices, Thomas E. Wilson

Thomas E. Wilson

Progress is described in experiments to generate coherent terahertz acoustic phonons in silicon doping superlattices by the resonant absorption of nanosecond-pulsed far-infrared laser radiation. Future experiments are proposed that would use the superlattice as a transducer in a terahertz cryogenic acoustic reflection microscope with sub-nanometer resolution.

Phonon Thermal Transport Through Tilt Grain Boundaries In Strontium Titanate, Zexi Zheng, Xiang Chen, Bowen Deng, Aleksandr V. Chernatynskiy, Shengfeng Yang, Jinjun Xiong, Youping Chen

Physics Faculty Research & Creative Works

In this work, we perform nonequilibrium molecular dynamics simulations to study phonon scattering at two tilt grain boundaries (GBs) in SrTiO₃. Mode-wise energy transmission coefficients are obtained based on phonon wave-packet dynamics simulations. The Kapitza conductance is then quantified using a lattice dynamics approach. The obtained results of the Kapitza conductance of both GBs compare well with those obtained by the direct method, except for the temperature dependence. Contrary to common belief, the results of this work show that the optical modes in SrTiO₃ contribute significantly to phonon thermal transport, accounting for over 50% of the Kapitza …

Kapitza Resistance Of Si/Sio₂ Interface, Bowen Deng, Aleksandr V. Chernatynskiy, Marat Khafizov, David H. Hurley, Simon R. Phillpot

Physics Faculty Research & Creative Works

A phonon wave packet dynamics method is used to characterize the Kapitza resistance of a Si/SiO₂ interface in a Si/SiO₂/Si heterostructure. By varying the thickness of SiO₂ layer sandwiched between two Si layers, we determine the Kapitza resistance for the Si/SiO ₂ interface from both wave packet dynamics and a direct, non-equilibrium molecular dynamics approach. The good agreement between the two methods indicates that they have each captured the anharmonic phonon scatterings at the interface. Moreover, detailed analysis provides insights as to how individual phonon mode scatters at the interface and their contribution to the Kapitza …

Temperature-Dependent Photoluminescence Of Ge/Si And Ge 1-Ysn Y/Si, Indicating Possible Indirect-To-Direct Bandgap Transition At Lower Sn Content, Mee-Yi Ryu, Thomas R. Harris, Yung Kee Yeo, Richard T. Beeler, John Kouvetakis

Faculty Publications

Temperature (T)-dependent photoluminescence (PL) has been investigated for both p-Ge and n-Ge_1-ySn_y films grown on Si substrates. For the p-Ge, strong direct bandgap (E_D) along with weak indirect bandgap related (E_ID) PL at low temperatures (LTs) and strong E_D PL at room temperature (RT) were observed. In contrast, for the n-Ge_1-ySn_y, very strong dominant E_ID PL at LT and strong E_D PL were observed at RT. This T-dependent PL study indicates that the indirect-to-direct bandgap transitions of Ge_1-ySn …

Pump Dependence Of The Dynamics Of Quantum Dot Based Waveguide Absorbers, T. Piwonski, Jaroslaw Pulka, Guillaume Huyet, Et. Al.

Physical Sciences Publications

The nonlinear two stage recovery of quantum dot based reverse-biased waveguide absorbers is investigated experimentally and analytically as a function of the initial ground state occupation probability of the dot. The latter is controlled experimentally by the pump pulse power. The slow stage of the recovery is exponential and its basic timescale is independent of pump power. The fast stage of the recovery is a logistic function which we analyze in detail. The relative strength of slow to fast components is highlighted and the importance of higher order absorption processes at the highest pump level is demonstrated.

An Embedded Atom Method Investigation Into The Lattice Dynamics Of Metallic Surfaces, Richard B. Wilson

All Graduate Theses and Dissertations, Spring 1920 to Summer 2023

The explosion in electronic devices over the last half century is a result of the successful development and application of theories that explain the physical properties of solids. For example, the theory of lattice vibrations developed in the first half of the 20^th century has had a huge impact on our ability to understand and design devices. The idea that atoms vibrate together in grouped vibrational modes, called phonons, has enabled scientists to quantify the impact that atomic motion has on mechanical, thermal, electrical, and optical properties. This has aided the creation of all sorts of useful technology ranging …

Observation Of An Oxygen Isotope Effect In Yba2Cu3O7, Kevin Leary, Hans Conrad Zur Loye, Steven Keller, Tanya Faltens, William Ham, James Michaels, Angelica Stacy

Hans Conrad zur Loye

A small decrease in Tc of 0.3 K to 0.5 K is observed when as much as 90% of the 16O in YBa2Cu3O7 is substituted with18O. This result is consistent with our observation that there is an oxygen isotope effect in La1.85Sr0.15CuO4, but in contrast with previous reports that there is no isotope effect for YBa2Cu3O7. This new result suggests that phonons play an important role in the electron-pairing mechanism in YBa2Cu3O7.

Graphitized Carbon On Gaas(100) Substrates, J. Simon, P. J. Simmonds, J. M. Woodall, M. L. Lee

Paul J. Simmonds

We report on the formation of graphitized carbon on GaAs(100) surfaces by molecular beam epitaxy. We grew highly carbon-doped GaAs on AlAs, which was then thermally etched in situ leaving behind carbon atoms on the surface. After thermal etching, Raman spectra revealed characteristic phonon modes for sp²-bonded carbon, consistent with the formation of graphitic crystallites. We estimate that the graphitic crystallites are 1.5–3 nm in size and demonstrate that crystallite domain size can be increased through the use of higher etch temperatures.

Spin-Lattice Coupling In The Iron-Pnictide High-Temperature Superconductors, Daniel E Parshall

Doctoral Dissertations

The recent discovery of the iron-pnictide superconductors has generated tremendous excitement, in part because there are many tantalizing similarities to the cuprate superconductors. As with the cuprates, it is strongly suspected that the spins contribute to superconductivity.

There seems to be a strong relationship between the lattice and magnetism in this system. Several authors have discussed the possibility of spin-phonon coupling, but direct experimental evidence has remained elusive.

This work discusses the relationship between the spins and the lattice in the $BaFe_{2}As_{2}$ family. We demonstrate the presence of negative thermal expansion in these materials, which is a strong indicator of …

Induced Absorption Dynamics In Quantum Dot Based Waveguide Electroabsorbers, T. Piwonski, Jaroslaw Pulka, Guillaume Huyet, Et. Al.

Physical Sciences Publications

Two-color pump-probe measurements are used to study the carrier dynamics of InAs/GaAs quantum dots in a waveguide structure under reverse bias conditions. For the case of initially populating the ground state (GS), we find relaxation dynamics that include both absorptive and bleaching components in the excited state (ES) wavelength range. We reproduce the main features of this induced absorption dynamics using a simple model with an additional term for induced absorption at the ES due to carriers injected at the GS. The induced absorption dynamics includes multiple recovery timescales which can be attributed to phonon-assisted processes of GS/ES interaction.

Structural, Electronic, Vibrational And Thermodynamical Properties Of Surfaces And Nanoparticles, Handan Yildirim

Electronic Theses and Dissertations

The main focus of the thesis is to have better understanding of the atomic and electronic structures, vibrational dynamics and thermodynamics of metallic surfaces and bi-metallic nanoparticles (NPs) via a multi-scale simulational approach. The research presented here involves the study of the physical and chemical properties of metallic surfaces and NPs that are useful to determine their functionality in building novel materials. The study follows the 'bottom-up' approach for which the knowledge gathered at the scale of atoms and NPs serves as a base to build, at the macroscopic scale, materials with desired physical and chemical properties. We use a …

Sum Rules And Universality In Electron-Modulated Acoustic Phonon Interaction In A Free-Standing Semiconductor Plate, Shigeyasu Uno, Darryl H. Yong, Nobuya Mori

All HMC Faculty Publications and Research

Analysis of acoustic phonons modulated due to the surfaces of a free-standing semiconductor plate and their deformation-potential interaction with electrons are presented. The form factor for electron-modulated acoustic phonon interaction is formulated and analyzed in detail. The form factor at zero in-plane phonon wave vector satisfies sum rules regardless of electron wave function. The form factor is larger than that calculated using bulk phonons, leading to a higher scattering rate and lower electron mobility. When properly normalized, the form factors lie on a universal curve regardless of plate thickness and material.

The Fast Recovery Dynamics Of A Quantum Dot Semiconductor Optical Amplifier, T. Piwonski, Guillaume Huyet, Et. Al.

Physical Sciences Publications

We consider a rate equation model of a quantum dot semiconductor optical amplifier that takes into account carrier capture, escape, and Pauli blocking processes. We evaluate possible differences between phonon-assisted or Auger processes being dominant for recovery. An analytical solution which corresponds to phonon-assisted interaction is then used to accurately fit experimental recovery curves and allows an estimation of both the carrier capture and escape rates.

Ferroelectric Phase Transitions In Three-Component Short-Period Superlattices Studied By Ultraviolet Raman Spectroscopy, Dmitri Tenne, H. N. Lee, R. S. Katiyar, X. X. Xi

Physics Faculty Publications and Presentations

Vibrational spectra of three-component BaTiO₃SrTiO₃CaTiO₃ short-period superlattices grown by pulsed laser deposition with atomic-layer control have been investigated by ultraviolet Raman spectroscopy. Monitoring the intensity of the first-order phonon peaks in Raman spectra as a function of temperature allowed determination of the ferroelectric phase transition temperature, T_c. Raman spectra indicate that all superlattices remain in the tetragonal ferroelectric phase with out-of-plane polarization in the entire temperature range below T_c. The dependence of T_c on the relative thicknesses of ferroelectric (BaTiO₃) to non-ferroelectric materials (SrTiO₃ and CaTiO_{3 …}