arXiv subjects

James Lloyd-Hughes

Publications and source records attributed to James Lloyd-Hughes.

6 recordsLinked to original sources

arXiv2025

A tutorial on THz pulse analysis: accurate retrieval of pulse arrival times, spectral energy density and absolute spectral phase

Electro-optic sampling allows the electric field of THz, mid-infrared and visible light pulses to be measured directly as a function of time, with data analysis often performed in the frequency domain after fast Fourier transform. Here we review aspects of Fourier theory relevant to the frequency-domain analysis of light pulses recorded in the time-domain. We describe a ``best practise'' approach to using the discrete Fourier transform that ensures consistency with analytical results from the continuous Fourier transform. We summarise a phenomenological time-domain model of THz pulses, based on carrier and envelope waves, and show that it can reproduce a wide variety of experimental single- to multi-cycle THz pulses, with exemplary data from lab-based sources (photoconductive antennae, optical rectification, spintronic emitters) and a THz free electron laser. A quantitative comparison of the spectral energy density of these distinct sources is enabled by the amplitude-accuate discrete Fourier transform. We describe a method that ensures the accurate calculation of the absolute spectral phase (valid for arbitrary sampling windows in the time-domain) and summarise how the carrier-envelope phase, pulse arrival time and chirp can be obtained from the phase. Our aim with this overview of THz pulse analysis is to highlight algorithms and concepts that are useful to newcomers to time-domain spectroscopy and experts, alike.

physics.optics↗

arXiv2024

Distinguishing Carrier Transport and Interfacial Recombination at Perovskite-Transport Layer Interfaces Using Ultrafast Spectroscopy and Numerical Simulation

In perovskite solar cells, photovoltaic action is created by charge transport layers (CTLs) either side of the light-absorbing metal halide perovskite semiconductor. Hence, the rates for desirable charge extraction and unwanted interfacial recombination at the perovskite-CTL interfaces play a critical role for device efficiency. Here, the electrical properties of perovskite-CTL bilayer heterostructures are obtained using ultrafast THz and optical studies of the charge carrier dynamics after pulsed photoexcitation, combined with a physical model of charge carrier transport that includes the prominent Coulombic forces that arise after selective charge extraction into a CTL, and cross-interfacial recombination. The charge extraction velocity at the interface and the ambipolar diffusion coefficient within the perovskite are determined from the experimental decay profiles for heterostructures with three of the highest performing CTLs, namely C$_{60}$, PCBM and Spiro-OMeTAD. Definitive targets for the further improvement of devices are deduced: fullerenes deliver fast electron extraction, but suffer from a large rate constant for cross-interface recombination or hole extraction. Conversely, Spiro-OMeTAD exhibits slow hole extraction but does not increase the perovskite's surface recombination rate, likely contributing to its success in solar cell devices.

cond-mat.mtrl-sci↗

arXiv2023

Optimum optical designs for diffraction-limited terahertz spectroscopy and imaging systems using off-axis parabolic mirrors

Off-axis parabolic mirrors (OAPMs) are widely used in the THz and mm-wave communities for spectroscopy and imaging applications, as a result of their broadband, low-loss operation and high numerical apertures. However, the aspherical shape of an OAPM creates significant geometric aberrations that make achieving diffraction-limited performance a challenge, and which lowers the peak electric field strength in the focal plane. Here we quantify the impact of geometric aberrations on the performance of the most widely-used spectrometer designs, by using ray tracing and physical optics calculations to investigate whether diffraction-limited performance can be achieved in both the sample and the detector plane. We identify simple rules, based on marginal ray propagation, that allow spectrometers to be designed that are more robust to misalignment errors, and which have minimal aberrations for THz beams. For a given source this allows the design of optical paths that give the smallest THz beam focal spot, with the highest THz electric field strength possible. This is desirable for improved THz imaging, for better signal-to-noise ratios in linear THz spectroscopy and optical-pump THz-probe spectroscopy, and to achieve higher electric field strengths in non-linear THz spectroscopy

physics.optics↗

arXiv2021

Hot electron cooling in InSb probed by ultrafast time-resolved terahertz cyclotron resonance

Measuring terahertz (THz) conductivity on an ultrafast time scale is an excellent way to observe charge-carrier dynamics in semiconductors as a function of time after photoexcitation. However, a conductivity measurement alone cannot separate the effects of charge-carrier recombination from effective mass changes as charges cool and experience different regions of the electronic band structure. Here we present a form of time-resolved magneto-THz spectroscopy which allows us to measure cyclotron effective mass on a picosecond time scale. We demonstrate this technique by observing electron cooling in the technologically-significant narrow-bandgap semiconductor indium antimonide (InSb). A significant reduction of electron effective mass from 0.032$m_\mathrm{e}$ to 0.017$m_\mathrm{e}$ is observed in the first 200ps after injecting hot electrons. Measurement of electron effective mass in InSb as a function of photo-injected electron density agrees well with conduction band non-parabolicity predictions from ab initio calculations of the quasiparticle band structure.

cond-mat.mtrl-sci↗

arXiv2019

Landau polaritons in highly non-parabolic 2D gases in the ultra-strong coupling regime

We probe ultra-strong light matter coupling between metallic terahertz metasurfaces and Landau-level transitions in high mobility 2D electron and hole gases. We utilize heavy-hole cyclotron resonances in strained Ge and electron cyclotron resonances in InSb quantum wells, both within highly non-parabolic bands, and compare our results to well known parabolic AlGaAs/GaAs quantum well (QW) systems. Tuning the coupling strength of the system by two methods, lithographically and by optical pumping, we observe a novel behavior clearly deviating from the standard Hopfield model previously verified in cavity quantum electrodynamics: an opening of a lower polaritonic gap.

cond-mat.mes-hall↗

arXiv2010

Observation of Zone-Folded Acoustic Phonons in Terahertz Quantum Cascade Lasers using Picosecond Ultrasonics

We have investigated the time-resolved vibrational properties of terahertz quantum cascade lasers by means of ultra-fast laser spectroscopy. By the observation of the acoustic folded branches, and by analyzing the involved phonon modes it is possible to extract accurate structural information of these devices, which are essential for their design and performance.

cond-mat.mes-hall↗