arXiv subjects

Daniel B. Durham

Publications and source records attributed to Daniel B. Durham.

5 recordsLinked to original sources

arXiv2025

Nanoscale and Element-Specific Lattice Temperature Measurements using Core-Loss Electron Energy-Loss Spectroscopy

Measuring nanoscale local temperatures, particularly in vertically integrated and multi-component systems, remains challenging. Spectroscopic techniques like X-ray absorption and core-loss electron energy-loss spectroscopy (EELS) are sensitive to lattice temperature, but understanding thermal effects is nontrivial. This work explores the potential for nanoscale and element-specific core-loss thermometry by comparing the Si L2,3 edge's temperature-dependent redshift against plasmon energy expansion thermometry (PEET) in a scanning TEM. Using density functional theory (DFT), time-dependent DFT, and the Bethe-Salpeter equation, we ab initio model both the Si L2,3 and plasmon redshift. We find that the core-loss redshift occurs due to bandgap reduction from electron-phonon renormalization. Our results indicate that despite lower core-loss signal intensity compared to plasmon features, core-loss thermometry has key advantages and can be more accurate through standard spectral denoising. Specifically, we show that the Varshni equation easily interprets the core-loss redshift for semiconductors, which avoids plasmon spectral convolution for PEET in complex junctions and interfaces. We also find that core-loss thermometry is more accurate than PEET at modeling thermal lattice expansion in semiconductors, unless the specimen's temperature-dependent dielectric properties are fully characterized. Furthermore, core-loss thermometry has the potential to measure nanoscale heating in multi-component materials and stacked interfaces with elemental specificity at length scales smaller than the plasmon's wavefunction.

cond-mat.mtrl-sci↗

arXiv2023

Experimental characterization of photoemission from plasmonic nanogroove arrays

Metal photocathodes are an important source of high-brightness electron beams, ubiquitous in the operation of both large-scale accelerators and table-top microscopes. When the surface of a metal is nano-engineered with patterns on the order of the optical wavelength, it can lead to the excitation and confinement of surface plasmon polariton waves which drive nonlinear photoemission. In this work, we aim to evaluate gold plasmonic nanogrooves as a concept for producing bright electron beams for accelerators via nonlinear photoemission. We do this by first comparing their optical properties to numerical calculations from first principles to confirm our ability to fabricate these nanoscale structures. Their nonlinear photoemission yield is found by measuring emitted photocurrent as the intensity of their driving laser is varied. Finally, the mean transverse energy of this electron source is found using the solenoid scan technique. Our data demonstrate the ability of these cathodes to provide a tenfold enhancement in the efficiency of photoemission over flat metals driven with a linear process. We find that these cathodes are robust and capable of reaching sustained average currents over 100 nA at optical intensities larger than 2 GW/cm$^2$ with no degradation of performance. The emittance of the generated beam is found to be highly asymmetric, a fact we can explain with calculations involving the also asymmetric roughness of the patterned surface. These results demonstrate the use of nano-engineered surfaces as enhanced photocathodes, providing a robust, air-stable source of high average current electron beams with great potential for industrial and scientific applications.

physics.acc-ph↗

arXiv2023

Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, we examine ultrafast laser heating of single-crystal gold films. Comparison of kinematical and dynamical models reveals the strong effects of dynamical scattering within nm-scale films and their dependence on sample topography and probe kinetic energy. Applying to UED experiments on an 11 nm thick film using 750 keV electron probe pulses, the dynamical models provide a tenfold improvement over a comparable kinematical model in matching the measured UED patterns. Also, the retrieved lattice temperature rise is in very good agreement with predictions based on previously measured optical constants of gold, whereas fitting the Debye-Waller factor retrieves values that are more than three times lower. Altogether, these results show the importance of dynamical scattering theory for quantitative analysis of UED and demonstrate models that can be practically applied to single-crystal materials and heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast optical melting of trimer superstructure in layered 1T'-TaTe2

Quasi-two-dimensional transition-metal dichalcogenides are a key platform for exploring emergent nanoscale phenomena arising from complex interactions. Access to the underlying degrees-of-freedom on their natural time scales motivates the use of advanced ultrafast probes sensitive to self-organised atomic-scale patterns. Here, we report the first ultrafast investigation of TaTe2, which exhibits unique charge and lattice trimer order characterised by a transition upon cooling from stripe-like chains into a $(3 \times 3)$ superstructure of trimer clusters. Utilising MeV-scale ultrafast electron diffraction, we capture the photo-induced TaTe2 structural dynamics -- exposing a rapid $\approx\!1.4$ ps melting of its low-temperature ordered state followed by recovery via thermalisation into a hot cluster superstructure. Density-functional calculations indicate that the initial quench is triggered by intra-trimer Ta charge transfer which destabilises the clusters, unlike melting of charge density waves in other TaX2 compounds. Our work paves the way for further exploration and ultimately rapid optical and electronic manipulation of trimer superstructures.

cond-mat.mtrl-sci↗

arXiv2019

Plasmonic lenses for tunable ultrafast electron emitters at the nanoscale

Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential impact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source brightness and size. We present the design, fabrication, and optical characterization of bullseye plasmonic lenses for next-generation ultrafast electron sources. Using electromagnetic simulations, we examine how the interplay between light-plasmon coupling, plasmon propagation, dispersion, and resonance governs the properties of the photoemitted electron pulse. We also illustrate how the pulse duration and strength can be tuned by geometric design, and predict sub-10 fs pulses with nanoscale diameter can be achieved. We then fabricated lenses in gold films and characterized their plasmonic properties with cathodoluminescence spectromicroscopy, demonstrating suitable plasmonic behavior for ultrafast, nanoscale photoemission.

physics.app-ph↗