N. Chopra and J. Lloyd-Hughes J Infrared Milli Terahz Waves 44, 981 (Nov 2023)
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: these make achieving diffraction-limited performance a challenge, and lower 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.
Nathaniel P. Gallop, Dumitru Sirbu, David Walker, James Lloyd-Hughes, Pablo Docampo and Rebecca L. Milot ACS Photonics 104022(October 2023)
We report on the emission of high-intensity pulsed terahertz radiation from the metal-free halide perovskite single crystal methyl-DABCO ammonium iodide (MDNI) under femtosecond illumination. The power and angular dependence of the THz output implicate optical rectification of the 800 nm pump as the mechanism of THz generation. Further characterization finds that, for certain crystal orientations, the angular dependence of THz emission is modulated by phonon resonances attributable to the motion of the methyl-DABCO moiety. At maximum, the THz emission spectrum of MDNI is free from significant phonon resonances, resulting in THz pulses with a temporal width of <900 fs and a peak-to-peak electric field strength of approximately 0.8 kV cm–1─2 orders of magnitude higher than any other reported halide perovskite emitters. Our results point toward metal-free perovskites as a promising new class of THz emitters that brings to bear many of the advantages enjoyed by other halide perovskite materials. In particular, the broad tunability of optoelectronic properties and ease of fabrication of perovskite materials opens up the possibility of further optimizing the THz emission properties within this material class.
A. Ren, H. Wang, L. Dai, J. Xia, E. Butler-Caddle, J.A. Smith, ... S.A. Hindmarsh, A.M. Sanchez, J. Lloyd-Hughes, S. J Sweeney, ... and Wei Zhang Nature Photonics17, 798–805 (July 2023)
Light-emitting diodes (LEDs) are ubiquitous in modern society, with applications spanning from lighting and displays to medical diagnostics and data communications. Metal-halide perovskites are promising materials for LEDs because of their excellent optoelectronic properties and solution processability. Although research has progressed substantially in optimizing their external quantum efficiency, the modulation characteristics of perovskite LEDs remain unclear. Here we report a holistic approach for realizing fast perovskite photonic sources on silicon based on tailoring alkylammonium cations in perovskite systems. We reveal the recombination behaviour of charged species at various carrier density regimes relevant for their modulation performance. By integrating a Fabry–Pérot microcavity on silicon, we demonstrate perovskite devices with efficient light outcoupling. We achieve device modulation bandwidths of up to 42.6 MHz and data rates above 50 Mbps, with further analysis suggesting that the bandwidth may exceed gigahertz levels. The principles developed here will support the development of perovskite light sources for next-generation data-communication architectures. The demonstration of solution-processed perovskite emitters on silicon substrates also opens up the possibility of integration with micro-electronics platforms.
Jake D. Hutchinson, Edoardo Ruggeri, Jack M. Woolley, Géraud Delport, Samuel D. Stranks, Rebecca L. Milot Advanced Functional Materials2305736, (August 2023)
Mixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light- emitting diode (LED) communities due to their impressive opto-electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead-tin perovskite containing distinct, self-assembled domains of either 3D structures or highly phase-pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump-terahertz probe spectroscopy, the effective charge-carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long-range charge-transport should not be impeded by the heterogeneous structure of the material.
A. Whittock, X. Ding, X. Ramirez Barker, N. Auckloo, R. Sellers, J.M. Woolley V. Krishnan, C. Marine, C. Corre, E. Pickwell-MacPherson and V.G. Stavros Chem. Sci. 14, 6763 (June 2023)
Biomimicry has become a key player in researching new materials for a whole range of applications. In this study, we have taken a crude extract from the red algae Palmaria palmata containing mycosporine-like amino acids – a photoprotective family of molecules. We have applied the crude extract onto a surface to assess if photoprotection, and more broadly, light-to-heat conversion, is retained; we found it is. Considering sunscreens as a specific application, we have performed transmission and reflection terahertz spectroscopy of the extract and glycerol to demonstrate how one can monitor stability in real-world applications.
M.G. Burdanova, A.P. Tsapenko, S. Ahmad, E.I. Kauppinen and J. Lloyd-Hughes Nanotechnology 34405203, (June 2023)
Mixed-nanomaterial composites can combine the excellent properties of well-known low-dimensional nanomaterials. Here we highlight the potential of one-dimensional single-walled carbon nanotubes interfaced with two-dimensional graphene by exploring the composite's ac conductivity and photoconductivity, and the influence of HAuCl4 doping. In the composite, the equilibrium terahertz conductivity from free carrier motion was boosted, while the localised plasmon peak shifted towards higher frequencies, which we attribute to shorter conductivity pathways in the composite. A negative terahertz photoconductivity was observed for all samples under 410nm optical excitation and was reproduced by a simple model, where the Drude spectral weight and the momentum scattering rate were both lowered under photoexcitation. The composite had an enhanced modulation depth in comparison to reference carbon nanotube films, while retaining their characteristically fast (picosecond) response time. The results show that CNT-graphene composites offer new opportunities in devices by controlling charge carrier transport and tuning their optoelectronic properties.
A. Leitenstorfer, ..., E. Pickwell-MacPherson, ... and J. Cunningham J. Phys. D: Appl. Phys. 56, 223001 (April 2023)
Terahertz (THz) radiation encompasses a wide spectral range within the electromagnetic spectrum that extends from microwaves to the far infrared (100 GHz–∼30 THz). Within its frequency boundaries exist a broad variety of scientific disciplines that have presented, and continue to present, technical challenges to researchers. During the past 50 years, for instance, the demands of the scientific community have substantially evolved and with a need for advanced instrumentation to support radio astronomy, Earth observation, weather forecasting, security imaging, telecommunications, non-destructive device testing and much more. Furthermore, applications have required an emergence of technology from the laboratory environment to production-scale supply and in-the-field deployments ranging from harsh ground-based locations to deep space. In addressing these requirements, the research and development community has advanced related technology and bridged the transition between electronics and photonics that high frequency operation demands. The multidisciplinary nature of THz work was our stimulus for creating the 2017 THz Science and Technology Roadmap (Dhillon et al 2017 J. Phys. D: Appl. Phys. 50 043001). As one might envisage, though, there remains much to explore both scientifically and technically and the field has continued to develop and expand rapidly. It is timely, therefore, to revise our previous roadmap and in this 2023 version we both provide an update on key developments in established technical areas that have important scientific and public benefit, and highlight new and emerging areas that show particular promise. The developments that we describe thus span from fundamental scientific research, such as THz astronomy and the emergent area of THz quantum optics, to highly applied and commercially and societally impactful subjects that include 6G THz communications, medical imaging, and climate monitoring and prediction. Our Roadmap vision draws upon the expertise and perspective of multiple international specialists that together provide an overview of past developments and the likely challenges facing the field of THz science and technology in future decades. The document is written in a form that is accessible to policy makers who wish to gain an overview of the current state of the THz art, and for the non-specialist and curious who wish to understand available technology and challenges. A such, our experts deliver a 'snapshot' introduction to the current status of the field and provide suggestions for exciting future technical development directions. Ultimately, we intend the Roadmap to portray the advantages and benefits of the THz domain and to stimulate further exploration of the field in support of scientific research and commercial realisation.
X. Ding, G. Costa, A. I. Hernandez-Serrano, R.I. Stantchev, G. Nurumbetov, D.M. Haddleton, and E. Pickwell-MacPherson Bio. Opt. Express 14, 1146 (Feb 2023)
Transdermal drug delivery (TDD) has been widely used in medical treatments due to various advantages, including delivering drugs at a consistent rate. However, variations in skin hydration can have a significant effect on the permeability of chemicals. Therefore, it is essential to study the changes in skin hydration induced by TDD patches for better control of the delivery rate. In this work, in vivo terahertz (THz) spectroscopy is conducted to quantitatively monitor human skin after the application of patches with different backing materials and propylene glycol concentrations. Changes in skin hydration and skin response to occlusion induced by other patches are investigated and compared. Our work demonstrates the potential application of in vivo THz measurements in label-free, non-invasive evaluation of transdermal patches on human skin and further reveals the mechanism behind the effect.
Z. Hu, B. Breeze, M. Walker, E. Faulques, J. Sloan and J. Lloyd-Hughes ACS Appl. Nano Mater. 6, 2883 (Feb 2023)
Studying the optical performance of carbon nanotubes (CNTs) filled with guest materials can reveal the fundamental photochemical nature of ultrathin one-dimensional (1D) nanosystems, which are attractive for applications including photocatalysis. Here, we report comprehensive spectroscopic studies of how infiltrated HgTe nanowires (NWs) alter the optical properties of small-diameter (dt < 1 nm) single-walled carbon nanotubes (SWCNTs) in different environments: isolated in solution, suspended in a gelatin matrix, and heavily bundled in network-like thin films. Temperature-dependent Raman and photoluminescence measurements revealed that the HgTe NW filling can alter the stiffness of SWCNTs and therefore modify their vibrational and optical modes. Results from optical absorption and X-ray photoelectron spectroscopy demonstrated that the semiconducting HgTe NWs did not provide substantial charge transfer to or from the SWCNTs. Transient absorption spectroscopy further highlighted that the filling-induced nanotube distortion can alter the temporal evolution of excitons and their transient spectra. In contrast to previous studies on functionalized CNTs, where electronic or chemical doping often drove changes to the optical spectra, we highlight structural distortion as playing an important role.
N. Chopra,J. Deveikis and J. Lloyd-Hughes Appl. Phys. Lett. 122061102 (Feb 2023)
The spatial profile of a beam of pulsed terahertz (THz) radiation is controlled electrically using a multi-pixel photoconductive emitter, which consists of an array of interdigitated electrodes fabricated on semi-insulating GaAs. Activating individual pixels allows the transverse position of the THz beam's focus to be varied off-axis, as verified by spatial beam profiles. Enabling multiple pixels simultaneously permits non-Gaussian beam shapes to be created. The diffraction-limited performance of the system is established by comparison with the Abbé and Sparrow criteria, and a condition for effective beam steering using this design is derived. The spatial resolution of the approach is linked to the frequency of the THz radiation and the f-number of the collection optic.
G.M. Katyba, N.I. Raginov, E.M. Khabushev, V.A. Zhelnov, A. Gorodetsky, D.A. Ghazaryan, M.S. Mironov, D.V. Krasnikov, Y.G. Gladush, J. Lloyd-Hughes, A.G. Nasibulin, A.V. Arsenin, V.S. Volkov, K.I. Zaytsev, and M.G. Burdanova Optica 10, 53 (Jan 2023)
Tunable optoelectronics have attracted a lot of attention in recent years because of their variety of applications in next-generation devices. Among the potential uses for tuning optical elements, those allowing consistent parameter control stand out. We present an approach for the creation of mechanically tunable zone plate lenses in the THz range. Our devices comprise single-walled carbon nanotube (SWCNT) thin films of predetermined design integrated with stretchable polymer films. These offer high-performance and in situ tunability of focal length up to 50%. We studied the focusing properties of our lenses using the backward-wave oscillator THz imaging technique, supported by numerical simulations based on the finite element frequency domain method. Our approach may further enable the integration of SWCNT films into photonic and optoelectronic applications and could be of use for the creation of a variety of flexible and stretchable THz optical elements.
E. Butler-Caddle, N.E. Grant, S.L. Pain, J.D. Murphy, K.D.G.I. Jayawardena and J. Lloyd-Hughes Appl. Phys. Lett. 122012101 (Jan 2023)
Optical pump terahertz probe spectroscopy (OPTP) is a versatile non-contact technique that measures transient photoconductance decays with femtosecond temporal resolution. However, its maximum temporal range is limited to only a few nanoseconds by the mechanical delay lines used. We extended the temporal range of OPTP to milliseconds and longer while retaining sub-nanosecond resolution. A separate pump laser was electrically synchronized to the probe pulses, allowing the pump–probe delay to be controlled with an electronic delay generator. We demonstrated the capabilities of this technique by examining the photoconductance decays of semiconductors with lifetimes ranging over six orders of magnitude: III-Vs, metal halide perovskites, germanium, and silicon. A direct comparison of results on silicon from OPTP and inductively coupled photoconductance decay highlighted the higher spatial and temporal resolution of OPTP, which allowed in-plane and out-of-plane carrier diffusion to be studied.