arXiv subjects

Bradley J. Siwick

Publications and source records attributed to Bradley J. Siwick.

15 recordsLinked to original sources

arXiv2026

Prospects for Direct Electron Detectors in Ultrafast Electron Diffraction and Scattering Experiments

Ultrafast electron diffraction and phonon-diffuse scattering [UED(S)] experiments make use of photo-induced changes to electron scattering intensity across 2D detectors to report on a very wide range of dynamic structural phenomena in molecules and materials. Hybrid pixel counting detectors (HPCDs) are a promising technology for improved sensitivity and signal-to-noise in UED(S) experiments, as they offer near-zero readout noise and dark counts with the possibility of new acquisition modalities (e.g., shot-to-shot normalization) due to their high frame rates. However, it is well known that HPCDs suffer from count losses at high electron fluxes even in CW beam applications. How this translates to ultrashort electron pulse exposures has yet to be determined and is critical to understanding the application of this technology to ultrafast electron scattering experiments. Here we show that count losses are significantly exacerbated in ultrafast (pulsed) experiments and that HPCDs require unconventional data handling and saturate above $\approx\!2$ electrons per pixel per pulse. This count-rate limitation presents a severe constraint on electron bunch charge when interrogating single crystal samples. Normalization strategies to optimize signal-to-noise in UED(S) and a complete model for measurement uncertainties using HPCDs are developed and tested using a large dataset. Finally, we suggest ways HPCDs could be better adapted to ultrashort pulsed beam experiments.

physics.ins-det↗

arXiv2026

Transition from population- to coherence-dominated nondiffusive thermal transport

Deviations from diffusive heat transport in high thermal conductivity crystalline insulators are generally understood within the framework of the phonon Boltzmann Transport Equation. However, for low thermal conductivity materials with large primitive cells or strong anharmonicity, the recently developed Wigner Transport Equation is more appropriate as it includes tunnelling between overlapping phonon bands. In this work, via solutions to the Wigner Transport Equation, we develop a scheme to obtain the dynamics of the phonon populations and coherences as a function of an arbitrary heat source. The approach is applied to predict size effects and dynamical thermal conductivities in CsPbBr$_\text{3}$ and La$_\text{2}$Zr$_\text{2}$O$_\text{7}$ using first-principles data as input. We predict significant deviations from the bulk thermal conductivity in these materials at length scales on the order of hundreds of nanometers to a few microns at room temperature, well within the reach of direct observation using current experimental techniques.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Electron Diffuse Scattering as a Tool for Studying Phonon Transport: Phonon Hydrodynamics and Second Sound Oscillations

Hydrodynamic phonon transport phenomena, like second sound, have been observed in liquid Helium more than 50 years ago. More recently second sound has been observed in graphite at over 200 K using transient thermal grating techniques. In this work we explore the signatures of second sound in ultrafast electron diffuse scattering (UEDS) patterns. We use density functional theory and solve the Boltzmann transport equation to determine time-resolved non-equilibrium phonon populations and subsequently calculate one-phonon structure factors and diffuse scattering patterns to simulate experimental data covering the regimes of ballistic, diffusive, and hydrodynamic phonon transport. For systems like graphite, UEDS is capable of extracting time-dependent phonon occupancies across the entire Brillouin zone and ultimately lead to a more fundamental understanding of the hydrodynamic phonon transport regime.

cond-mat.mes-hall↗

arXiv2023

Ultrafast Phonon-Diffuse Scattering as a Tool for Observing Chiral Phonons in Monolayer Hexagonal Lattices

At the 2D limit, hexagonal systems such as monolayer transition metal dichalcogenides (TMDs) and graphene exhibit unique coupled spin and momentum-valley physics (valley pseudospin) owing to broken spatial inversion symmetry and strong spin-orbit coupling. Circularly polarized light provides the means for pseudospin-selective excitation of excitons (or electrons and holes) and can yield momentum-valley polarized populations of carriers that are the subject of proposed valleytronic applications. The chirality of these excited carriers have important consequences for the available relaxation/scattering pathways, which must conserve (pseudo)angular momentum as well as energy. One available relaxation channel that satisfies these constraints is coupling to chiral phonons. Here we show that chiral carrier-phonon coupling following valley-polarized photoexcitation is expected to leads to a strongly valley-polarized chiral phonon distribution that is directly measurable using ultrafast phonon-diffuse scattering techniques. Using ab-initio calculations we show how the dynamic phonon occupations and valley anisotropy determined by nonequilibrium observations can provide a new window on the physical processes that drive carrier valley-depolarization in monolayer TMDs.

cond-mat.mtrl-sci↗

arXiv2022

Direct view of phonon dynamics in atomically thin MoS$_{2}$

Transition metal dichalcogenide monolayers and heterostructures are highly tunable material systems that provide excellent models for physical phenomena at the two-dimensional (2D) limit. While most studies to date have focused on electrons and electron-hole pairs, phonons also play essential roles. Here, we apply ultrafast electron diffraction and diffuse scattering to directly quantify, with time and momentum resolution, electron-phonon coupling (EPC) in monolayer molybdenum disulfide (MoS$_{2}$) and phonon transport from the monolayer to a silicon nitride (Si$_3$N$_4$) substrate. Optically generated hot carriers result in a profoundly anisotropic distribution of phonons in the monolayer on the $\sim$ 5 ps time scale. A quantitative comparison with ab-initio ultrafast dynamics simulations reveals the essential role of dielectric screening in weakening EPC. Thermal transport from the monolayer to the substrate occurs with the phonon system far from equilibrium. While screening in 2D is known to strongly affect equilibrium properties, our findings extend this understanding to the dynamic regime.

cond-mat.mtrl-sci↗

arXiv2021

Direct visualization of polaron formation in the thermoelectric SnSe

SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of the carrier system in SnSe is also determined by strong coupling to phonons by directly visualizing polaron formation in the material. We employ ultrafast electron diffraction and diffuse scattering to track the response of phonons in both momentum and time to the photodoping of free carriers across the bandgap, observing the bimodal and anisotropic lattice distortions that drive carrier localization. Relatively large (\SI{18.7}{\angstrom}), quasi-1D polarons are formed on the \SI{300}{\femto\second} timescale with smaller (\SI{4.2}{\angstrom}) 3D polarons taking an order of magnitude longer (\SI{4}{\pico\second}) to form. This difference appears to be a consequence of the profoundly anisotropic electron-phonon coupling in SnSe, with strong Fröhlich coupling only to zone center polar optical phonons. These results demonstrate that carriers in SnSe at optimal doping levels results in a high polaron density and that strong electron-phonon coupling is also critical to the thermoelectric performance of this benchmark material and potentially high-performance thermoelectrics more generally.

cond-mat.mtrl-sci↗

arXiv2020

Mechanisms of electron-phonon coupling unraveled in momentum and time: The case of soft-phonons in TiSe$_2$

The complex coupling between charge carriers and phonons is responsible for diverse phenomena in condensed matter. We apply ultrafast electron diffuse scattering to unravel electron-phonon coupling phenomena in 1T-TiSe$_2$ in both momentum and time. We are able to distinguish effects due to the real part of the many-body bare electronic susceptibility, $\Re\left[χ_0(\mathbf{q})\right]$, from those due to the electron-phonon coupling vertex, $g_{\mathbf{q}}$, by following the response of semi-metallic (normal phase) 1T-TiSe$_2$ to the selective photo-doping of carriers into the electron pocket at the Fermi level. Quasi-impulsive and wavevector-specific renormalization of soft zone-boundary phonon frequencies (stiffening) is observed, followed by wavevector-independent electron-phonon equilibration. These results unravel the underlying mechanisms driving the phonon softening that is associated with the charge density wave transition at lower temperatures.

cond-mat.str-el↗

arXiv2020

Extreme Lightwave Electron Field Emission from a Nanotip

We report on sub-cycle terahertz light-field emission of electrons from tungsten nanotips under extreme conditions corresponding to a Keldysh parameter $γ_K\approx10^{-4}$. Local peak THz fields up to 40~GV/m are achieved at the apex of an illuminated nanotip, causing sub-cycle cold-field electron emission and acceleration in the quasi-static field. By simultaneous measurement of the electron bunch charge and energy distribution, we perform a quantitative test of quasi-static Fowler-Nordheim tunnelling theory under field conditions that completely suppress the tunnel barrier. Very high bunch charges of $\sim10^6$ electrons/pulse are observed, reaching maximum energies of 3.5~keV after acceleration in the local field. The energy distribution and emission current show good agreement with Fowler-Nordheim theory even in this extreme field regime. Extending this model to the single-shot regime under these conditions predicts peak electron distributions with a spectral purity of $10^{-4}$. THz field-induced reshaping and sharpening of the nanotip is observed, reducing the tip radius from 120~nm to 35~nm over roughly $10^9$ THz shots. These results indicate THz-driven nanotips in the extreme field limit are promising electron sources for ultrafast electron diffraction and microscopy.

physics.optics↗

arXiv2020

Tracking ultrafast solid-state dynamics using high harmonic spectroscopy

We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency characteristic of a coherent phonon in the equilibrium monoclinic phase over a wide range of excitation fluences. These results demonstrate that tr-HHG is capable of tracking complex dynamics in solids through its sensitivity to the band structure.

physics.optics↗

arXiv2019

Time- and momentum-resolved phonon population dynamics with ultrafast electron diffuse scattering

Interactions between the lattice and charge carriers can drive the formation of phases and ordering phenomena that give rise to conventional superconductivity, insulator-to-metal transitions, and charge-density waves. These couplings also play a determining role in properties that include electric and thermal conductivity. Ultrafast electron diffuse scattering (UEDS) has recently become a viable laboratory-scale tool to track energy flow into and within the lattice system across the entire Brillouin zone, and deconvolves interactions in the time domain. Here, we present a detailed quantitative framework for the interpretation of UEDS signals, ultimately extracting the phonon mode occupancies across the entire Brillouin zone. These transient populations are then used to extract momentum- and mode-dependent electron-phonon and phonon-phonon coupling constants. Results of this analysis are presented for graphite, which provides complete information on the phonon-branch occupations and a determination of the $A_1'$ phonon mode-projected electron-phonon coupling strength $\langle g_{e,A_1'}^2 \rangle = 0.035 \pm 0.001$ eV$^2$ that is in agreement with other measurement techniques and simulations.

cond-mat.mtrl-sci↗

arXiv2018

How optical excitation controls the structure and properties of vanadium dioxide

We combine ultrafast electron diffraction and time-resolved terahertz spectroscopy measurements to unravel the connection between structure and electronic transport properties during the photoinduced insulator-metal transitions in vanadium dioxide. We determine the structure of the metastable monoclinic metal phase, which exhibits anti-ferroelectric charge order arising from a thermally activated, orbital-selective phase transition in the electron system. The relative contribution of this photoinduced monoclinic metal (which has no equilibrium analog) and the photoinduced rutile metal (known from the equilibrium phase diagram) to the time and pump-fluence dependent multi-phase character of the film is established, as is the respective impact of these two distinct phase transitions on the observed changes in terahertz conductivity. Our results represent an important new example of how light can control the properties of strongly correlated materials and elucidate that multi-modal experiements are essential when seeking a detailed connection between ultrafast changes in optical-electronic properties and lattice structure in complex materials.

cond-mat.str-el↗

arXiv2017

Mapping momentum-dependent electron-phonon coupling and non-equilibrium phonon dynamics with ultrafast electron diffuse scattering

Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone (BZ) has proved difficult to obtain. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time-resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the $K$-point transverse optical phonon of $A_1'$ symmetry ($K-A_1'$) and along the entire longitudinal optical branch between $Γ-K$, not only to the $Γ-E_{2g}$ phonon as previously emphasized. We also determine that the subsequent phonon relaxation pathway involves three stages; decay via several identifiable channels to transverse acoustic (TA) and longitudinal acoustic (LA) phonons (1-2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30-40 ps) and interband relaxation of the LA/TA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems have a strong influence on emergent properties.

cond-mat.mtrl-sci↗

arXiv2017

Solving the Jitter Problem in Microwave Compressed Ultrafast Electron Diffraction Instruments: Robust Sub-50 fs Cavity-Laser Phase Stabilization

We demonstrate the compression of electron pulses in a high-brightness ultrafast electron diffraction (UED) instrument using phase-locked microwave signals directly generated from a mode-locked femtosecond oscillator. Additionally, a continuous-wave phase stabilization system that accurately corrects for phase fluctuations arising in the compression cavity from both power amplification and thermal drift induced detuning was designed and implemented. An improvement in the microwave timing stability from 100 fs to 5 fs RMS is measured electronically and the long-term arrival time stability ($>$10 hours) of the electron pulses improves to below our measurement resolution of 50 fs. These results demonstrate sub-relativistic ultrafast electron diffraction with compressed pulses that is no longer limited by laser-microwave synchronization.

physics.plasm-ph↗

arXiv2014

Coherent and incoherent electron-phonon coupling in graphite observed with radio-frequency compressed ultrafast electron diffraction

Radio-frequency compressed ultrafast electron diffraction has been used to probe the coherent and incoherent coupling of impulsive electronic excitation at 1.55 eV (800 nm) to optical and acoustic phonon modes directly from the perspective of the lattice degrees of freedom. A bi-exponential suppression of diffracted intensity due to relaxation of the electronic system into incoherent phonons is observed, with the 250 fs fast contribution dominated by coupling to the $E_{2g2}$ optical phonon mode at the $Γ$-point ($Γ-E_{2g2}$) and $A_1^{'}$ optical phonon mode at the $K$-point ($K-A_1^{'}$). Both modes have Kohn anomalies at these points in the Brillouin zone. The result is a unique non-equilibrium state with the electron subsystem in thermal equilibrium with only a very small subset of the lattice degrees of freedom within 500 fs following photoexcitation. This state relaxes through further electron-phonon and phonon-phonon pathways on the 6 ps timescale. In addition, electronic excitation leads to both in-plane and out-of-plane coherent lattice responses in graphite whose character we are able to fully determine based on spot positions and intensity modulations in the femtosecond electron diffraction data. The in-plane motion is specifically a $Γ$-point shearing mode of the graphene planes with an amplitude of approximately 0.06 pm and the out-of-plane motion an acoustic breathing mode response of the film.

cond-mat.mtrl-sci↗

arXiv2014

A photoinduced metallic phase of monoclinic vanadium dioxide

The complex interplay between several active degrees of freedom (charge, lattice, orbtial and spin order) is thought to determine the electronic properties of many oxides, but the respective role of the various contributions is often extremely difficult to determine. Vanadium dioxide (VO$_2$) is a particularly notorious example. Here we report on combined ultrafast electron diffraction (UED) and infrared transmissivity experiments in which we directly watch and separate the lattice and charge density reorganizations that are associated with the optically-induced semiconductor-metal transition (SMT) in VO$_2$. These studies have uncovered a previously unreported photoinduced transition to a metastable state with the periodic lattice distortion (PLD) characteristic of the insulator intact, but differing by a 1D rearrangement of charge density along the octahedrally coordinated vanadium dimer chains and a transition to metal-like mid IR optical properties. The results demonstrate that UED is capable of following details of both lattice and electronic structural dynamics on the ultrafast timescale.

cond-mat.str-el↗