arXiv subjects

David G. Cooke

Publications and source records attributed to David G. Cooke.

13 recordsLinked to original sources

arXiv2026

Coexisting Large and Small Polarons in Photoexcited CeO$_2$

Time-resolved terahertz (THz) spectroscopy is used to probe polaron formation in CeO$_2$. The ultrafast THz photoconductivity is dominated by contributions from large hole and small electron polarons. Delocalized large hole polarons are formed on a $820 \pm 50$ fs time scale and are of Fröhlich type, with optical conductivity well described by a simple Drude model and a transient hole mobility of $100$ cm$^2$/Vs. Small electron polarons form via localized coupling to Ce lattice sites, revealed by reduction in the lattice Born effective charge causing a transient phonon softening. These results establish the dual polaron nature of CeO$_2$ and provide a basis for understanding charge transfer dynamics in metal oxide photocatalysts.

cond-mat.mtrl-sci↗

arXiv2026

Photoinduced phase heterogeneity and charge localization in SnSe

Time-resolved multi-terahertz (THz) spectroscopy is used to observe pump fluence-dependent dynamics in the optical conductivity of photoexcited tin selenide (SnSe) over an ultrabroadband spectral range of 0.5 - 11 THz at fluences from 0.1 - 7.5 mJ/cm$^2$. A free carrier Drude spectrum is observed at pump fluences below 3 mJ/cm$^2$, with optical phonons well described by the equilibrium Pnma structural phase. With increasing fluence, a suppression of the DC photoconductivity is observed, indicating an interruption of long range transport due to phase disorder. Concomitantly, the optical phonons exhibit features that can no longer be explained by a pure Pnma phase, with a frequency shift and narrowing of the $B^2_{1u}$ mode and a new mode appearing at $\sim$3.0 THz consistent with a transition to a higher-symmetry structure. At an intermediate fluence of 3.1 mJ/cm$^2$, a high frequency Lorentzian component consistent with phase heterogeneity appears that rapidly redshifts after 2 ps and whose amplitude exponentially decays on a 90 ps time scale. Our experimental measurements and theoretical calculations provide evidence for a non-thermal, photo-induced nucleation of higher symmetry, semi-metallic phase domains in SnSe appearing within 200 fs.

cond-mat.mtrl-sci↗

arXiv2025

Intrinsic temporal and spectral mixing in time-resolved terahertz spectroscopy

In an ultrafast optical-pump terahertz-probe measurement, the photoinduced material response can be modulated on a timescale shorter than the extent of the THz pulse. In this situation, the measured time-frequency response deviates from a simple time-dependent linear response. When full two-dimensional time-frequency maps are measured, this yields complex features that can be incorrectly assigned to a photoexcited coherent response. We investigate this experimentally via the measured response of photoexcited SnSe, whereby photoinduced phase change dynamics lead to ultrafast changes of the charge carrier and lattice optical conductivity response. Two-dimensional time-frequency THz transmission maps subsequently show unexpected time-frequency features at early pump-probe delay times. These features are reproduced in both finite-difference time-domain simulations of the THz experiment and in an extension of non-equilibrium response function theory, demonstrating their systematic origin. This work improves the understanding of systematic effects in high time resolution optical-pump THz-probe spectroscopy, and explores the conditions in which they are likely to appear.

physics.optics↗

arXiv2025

Sub-cycle Nanotip Field Emission of Electrons Driven by Air Plasma Generated THz Pulses

Terahertz pulses generated by two-color laser plasmas have reported peak field strengths exceeding MV/cm, and when illuminating metal nanotips the near-field enhancement at the tip apex should result in extremely high bunch charges and electron energies via sub-cycle cold field emission. Here, electron emission from tungsten nanotips driven by THz pulses generated by a long filament air-plasma are reported. Electron energies up to 1.1 keV and bunch charges up to 2x$10^5$ electrons per pulse were detected, well below values expected for peak field calculated via the time averaged Poynting vector. Investigations revealed a failure in the use of the time-averaged Poynting vector when applied to long filament THz pulses, due to spatio-temporal restructuring of the THz pulse in the focus. Accounting for this restructuring significantly reduces the field strength to approximately 160 ~kV/cm, consistent with the observed electron bunch charges, peak energies and their dependence on the tip position in the THz focus. Despite these findings, our results surpass previous THz plasma-driven electron generation by an order of magnitude in both electron energy and bunch charge and a path to increasing these by an additional order of magnitude by modification of the THz optics is proposed.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Photo-induced Phase Change in SnSe

Time-resolved multi-terahertz (THz) spectroscopy is used to observe an ultrafast, non-thermal electronic phase change in SnSe driven by interband photoexcitation with 1.55 eV pump photons. The transient THz photoconductivity spectrum is found to be Lorentzian-like, indicating charge localization and phase segregation. The rise of photoconductivity is bimodal in nature, with both a fast and slow component due to excitation into multiple bands and subsequent intervalley scattering. The THz conductivity magnitude, dynamics, and spectra show a drastic change in character at a critical excitation fluence of approximately 6 mJ/cm^2 due to a photo-induced phase segregation and a macroscopic collapse of the band gap.

cond-mat.mtrl-sci↗

arXiv2021

Front-induced transitions control THz waves

Relativistically moving dielectric perturbations can be used to manipulate light in new and exciting ways beyond the capabilities of traditional nonlinear optics. Adiabatic interaction with the moving front modulates the wave simultaneously in both space and time, and manifests a front-induced transition in both wave vector and frequency yielding exotic effects including non-reciprocity and time-reversal. Here, we introduce a technique called SLIPSTREAM, Spacetime Light-Induced Photonic STRucturEs for Advanced Manipulation. The technique is based on the creation of relativistic fronts in a semiconductor-filled planar waveguide by photoexcitation of mobile charge carriers. Here we demonstrate the capabilities of SLIPSTREAM for novel manipulation of THz light pulses through relativistic front-induced transitions. In the sub-luminal front velocity regime, we generate temporally stretched THz waveforms, with a quasi-static field lasting for several picoseconds tunable with the front interaction distance. In the super-luminal regime, the carrier front outpaces the THz pulse and a time-reversal operation is performed via a front-induced intra-band transition. We anticipate our platform will be a versatile tool for future applications in the THz spectral band requiring direct and advanced control of light at the sub-cycle level.

physics.optics↗

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↗

arXiv2018

Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite

Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties (1-3), believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons (4-7). Few experimental techniques are capable of probing these correlations directly, requiring simultaneous sub-meV energy and femtosecond temporal resolution after absorption of a photon (8). Here we use transient multi-THz spectroscopy, sensitive to the internal motions of charges within the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single crystal CH3NH3PbI3 (MAPI). We observe room temperature quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide unambiguous evidence of the existence of polarons in MAPI.

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↗

arXiv2015

High field response of gated graphene at THz frequencies

We study the Fermi energy level dependence of nonlinear terahertz (THz) transmission of gated multi-layer and single-layer graphene transferred onto sapphire and quartz substrates. The two samples represent two limits of low-field impurity scattering: short-range neutral and long-range charged impurity scattering, respectively. We observe an increase in the transmission as the field amplitude is increased due to intraband absorption bleaching starting at fields above 8 kV/cm. This effect arises from a field-induced reduction in THz conductivity that depends strongly on the Fermi energy. We account for intraband absorption using a free carrier Drude model that includes neutral and charged impurity scattering as well as optical phonon scattering. We find that although the Fermi-level dependence in the monolayer and five-layer samples is quite different, both exhibit a strong dependence on the field amplitude that cannot be explained on the basis of an increase in the lattice temperature alone. Our results provide a deeper understanding of transport in graphene devices operating at THz frequencies and in modest kV/cm field strengths where nonlinearities exist.

cond-mat.mes-hall↗

arXiv2015

Intrinsic femtosecond charge generation dynamics in a single crystal organometal halide perovskite

Hybrid metal-organic perovskite solar cells have astounded the solar cell community with their rapid rise in efficiency over the past three years. Despite this success, the basic processes governing the photogeneration of free charges, particularly their dynamics and efficiency, remain unknown. Here we use ultrabroadband pulses of THz frequency light to see the intrinsic photophysical properties of single crystal lead halide perovskite just femtoseconds after a photon is first absorbed. Our spectra reveal the dynamics and efficiencies of free charge creation, the remarkable ease in which they move through the lattice and the complicated interplay between free and bound charges in these materials.

cond-mat.mtrl-sci↗

arXiv2014

Temporal and Spectral Shaping of Broadband THz Pulses in a Photoexcited Semiconductor

Transmission through photoexcited semiconductors is used to temporally and spectrally shape a Terahertz pulse. By adjusting the optical pump-THz probe delay, we experimentally introduce a polar asymmetry in the pulse profile as high as 92%. To shape the spectrum, we apply the same technique after strongly chirping the Terahertz pulse. This led to significant reshaping of the spectrum with a 52% upshift of spectrum median. Pulse shaping techniques introduced here are of particular importance for temporal and spectral shape-sensitive THz nonlinear experiments.

physics.optics↗

arXiv2013

Picosecond Dynamics of Internal Exciton Transitions in CdSe Nanorods

The picosecond dynamics of excitons in colloidal CdSe nanorods are directly measured via their 1s to 2p-like internal transitions by ultra-broadband terahertz spectroscopy. Broadened absorption peaks from both the longitudinal and transverse states are observed at 8.5 and 11 THz, respectively. The onset of exciton-LO phonon coupling appears as a bleach in the optical conductivity spectra at the LO phonon energy for times > 1 ps after excitation. Simulations show a suppressed exciton temperature due to thermally excited hole states being rapidly captured onto ligands or unpassivated surface states. The relaxation kinetics are manipulated and the longitudinal transition is quenched by surface ligand exchange with hole capturing pyridine.

cond-mat.mes-hall↗