Ultrafast & Terahertz Photonics Group

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-accurate 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.

A dual-beam THz spectrometer is reported that substantially reduces the influence of systematic errors in THz time-domain spectroscopy such as those caused by variations in femtosecond laser power or the environmental temperature and humidity. Dual THz beams with single-cycle waveforms were generated simultaneously using a dual-pixel interdigitated photoconductive antenna, allowing the simultaneous acquisition of sample and reference data in the spectrometer using the same optical components. A low-aberration optical geometry ensured diffraction-limited spatial profiles for both beams despite their off-axis propagation and was validated experimentally by measuring frequency-dependent beam profiles and theoretically via physical optics calculations. Although the experimental amplitudes and absolute phase spectra of both beams were very similar, we further provided a correction procedure to eliminate these small differences. The robustness of the dual-beam spectrometer design was evaluated by measuring the complex transmission of a thin plastic sheet after intentionally introducing a change in the relative humidity of the THz beam path. The dual-beam THz spectrometer was effective at removing systematic errors in the amplitude and phase by simultaneously measuring the two THz beams under the same conditions.

Improved knowledge of the influence of temperature upon layered perovskites is essential to enable perovskite-based devices to operate over a broad temperature range and to elucidate the impact of structural changes upon the optoelectronic properties. We examined the Ruddlesden–Popper layered perovskite 2-thiophenemethylammonium lead iodide (ThMA2PbI4) and observed a structural phase transition between a high- and a low-temperature phase at 220 K using temperature-dependent X-ray diffraction, UV–visible absorption, and photoluminescence (PL) spectroscopy. The structural phase transition altered the tilt pattern of the inorganic octahedra layer, modifying the absorption and PL spectra. Further, we found a narrow and intense additional PL peak in the low-temperature phase, which we assigned to radiative emission from a defect-bound exciton state. In both phases we determined the thermal expansion coefficient and found values similar to those of cubic 3D perovskites, i.e., larger than those of typical substrates such as glass. These results demonstrate that the organic spacer plays a critical role in controlling the temperature-dependent structural and optoelectronic properties of layered perovskites and suggests more widely that strain management strategies may be needed to fully utilize layered perovskites in device applications.

Transdermal drug delivery patches are a good alternative to hypodermic drug injection. The drug delivery efficiency depends strongly on the hydration of the skin under treatment, and therefore, it is essential to study the effects on the skin induced by the application of these medical-grade patches. Terahertz (THz) spectroscopy shows great promise for non-invasive skin evaluation due to its high sensitivity to subtle changes in water content, low power and non-ionizing properties. In this work, we study the effects of transdermal drug delivery patches (three fully occlusive and three partially occlusive) applied on the upper arms of ten volunteers for a maximum period of 28 h. Three different levels of propylene glycol (0 %, 3 % and 6 %) are added to the patches as excipient. By performing multilayer analysis, we successfully retrieve the water content of the stratum corneum (SC) which is the outermost layer of skin, as well as its thickness at different times before and after applying the patches. This study demonstrates the potential of using THz sensing for non invasive skin monitoring and has wide applications for skin evaluation as well as the development of skin products.