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All-optical control of terahertz pulses is essential for the development of optoelectronic devices for next-generation quantum technologies. Despite substantial research in THz generation methods, polarisation control remains difficult. Here, we demonstrate that by exploiting bandstructure topology, both helicity-dependent and helicity-independent THz emission can be generated from nanowires of the topological Dirac semimetal Cd3As2. We show that narrowband THz pulses can be generated at oblique incidence by driving the system with optical (1.55 eV) pulses with circular polarisation. Varying the incident angle also provides control of the peak emission frequency, with peak frequencies spanning 0.21 – 1.40 THz as the angle is tuned from 15° - 45°. We therefore present Cd3As2 nanowires as a promising novel material platform for controllable terahertz emission.

Sierra Leone has one of the highest levels of malnutrition and child mortality worldwide due, in part, to the micronutrient deficiencies that result from a lack of diet diversity and food accessibility. To address these challenges, nutrient-dense, affordable snack foods are being developed for children in Sierra Leone. The products in development are similar to foods that are currently eaten in the region, such that they could easily be integrated into children’s diets. The two lead products are a groundnut butter pudding for children six months to two years of age and a sweet potato based muffin for children two to five years of age. The objectives of this study are (1) to determine the dietary habits of children in Sierra Leone between six months and five years of age, and (2) to perform acceptability testing with the pudding and the muffins. In total, 428 mother-child pairs participated in the study, which was performed in 2019 in multiple locations in the vicinity of Makeni, Sierra Leone. The mothers reported that the most common snacks for children six months to two years of age were porridge and rice, while the most common snacks for two to five year olds were rice and biscuits. These findings confirmed that the pudding and muffins would be familiar and appealing to young children. Moreover, the test results demonstrated that both the pudding and the muffins were acceptable in terms of taste and texture. Based upon these findings, the best formulations were selected, then further modified to reach the target levels of each micronutrient (vitamin A, iron, and zinc) in a single serving size. The estimated cost of each product is 1500 leones ($0.15 USD), making it affordable for Sierra Leoneans. Future steps are to collaborate with local entrepreneurs to sell these products in the markets where people normally shop. This study was approved by the District Medical Officer of Health in Sierra Leone and performed in collaboration with World Hope International, an NGO with a facility in Makeni, Sierra Leone.

An understanding of the factors driving halide segregation in lead mixed-halide perovskites is required for their implementation in tandem solar cells with existing silicon technology. Here we report that the halide segregation dynamics observed in the photoluminescence from CH3NH3Pb(Br0.5I0.5)3 is strongly influenced by the atmospheric environment, and that encapsulation of films with a layer of poly(methyl methacrylate) allows for halide segregation dynamics to be fully reversible and repeatable. We further establish an empirical model directly linking the amount of halide segregation observed in the photoluminescence to the fraction of charge carriers recombining through trap-mediated channels, and the photon flux absorbed. From such quantitative analysis we show that under pulsed illumination, the frequency of the modulation alone has no influence on the segregation dynamics. Additionally, we extrapolate that working CH3NH3Pb(Br0.5I0.5)3 perovskite cells would require a reduction of the trap-related charge carrier recombination rate to ≲105s–1 in order for halide segregation to be sufficiently suppressed.

Intrinsic and extrinsic optoelectronic properties are unraveled for formamidinium tin triiodide (FASnI3) thin films, whose background hole doping density was varied through SnF2 addition during film fabrication. Monomolecular charge-carrier recombination exhibits both a dopant-mediated part that grows linearly with hole doping density and remnant contributions that remain under tin-enriched processing conditions. At hole densities near 1020 cm-3, a strong Burstein-Moss effect increases absorption onset energies by ~300meV beyond the band gap energy of undoped FASnI3 (shown to be 1.2 eV at 5 K and 1.35 eV at room temperature). At very high doping densities (1020 cm-3), temperature-dependent measurements indicate that the effective charge-carrier mobility is suppressed through scattering with ionized dopants. Once the background hole concentration is nearer 1019 cm-3 and below, the charge-carrier mobility increases with decreasing temperature according to ~T-1.2, suggesting it is limited mostly by intrinsic interactions with lattice vibrations. For the lowest doping concentration of 7.2´1018 cm^-3, charge-carrier mobilities reach a value of 67 cm2V-1s-1at room temperature and 470 cm2V-1s-1 at 50 K. Intra-excitonic transitions observed in the THz-frequency photoconductivity spectra at 5K reveal an exciton binding energy of only 3.1 meV for FASnI3, in agreement with the low bandgap energy exhibited by this perovskite.

Bare unpassivated GaAs nanowires feature relatively high electron mobilities (400–2100 cm$^{2}$ V$^{-1}$ s$^{-1}$) and ultrashort charge carrier lifetimes (1–5 ps) at room temperature. These two properties are highly desirable for high speed optoelectronic devices, including photoreceivers, modulators and switches operating at microwave and terahertz frequencies. When engineering these GaAs nanowire-based devices, it is important to have a quantitative understanding of how the charge carrier mobility and lifetime can be tuned. Here we use optical-pump–terahertz-probe spectroscopy to quantify how mobility and lifetime depend on the nanowire surfaces and on carrier density in unpassivated GaAs nanowires. We also present two alternative frameworks for the analysis of nanowire photoconductivity: one based on plasmon resonance and the other based on Maxwell–Garnett effective medium theory with the nanowires modelled as prolate ellipsoids. We find the electron mobility decreases significantly with decreasing nanowire diameter, as charge carriers experience increased scattering at nanowire surfaces. Reducing the diameter from 50 nm to 30 nm degrades the electron mobility by up to 47%. Photoconductivity dynamics were dominated by trapping at saturable states existing at the nanowire surface, and the trapping rate was highest for the nanowires of narrowest diameter. The maximum surface recombination velocity, which occurs in the limit of all traps being empty, was calculated as 1.3 × 10$^{6}$ cm s$^{-1}$. We note that when selecting the optimum nanowire diameter for an ultrafast device, there is a trade-off between achieving a short lifetime and a high carrier mobility. To achieve high speed GaAs nanowire devices featuring the highest charge carrier mobilities and shortest lifetimes, we recommend operating the devices at low charge carrier densities.

Optical pump-terahertz probe spectroscopy was used to study the key electronic properties of GaAs, InAs and InP nanowires at room temperature. Of all nanowires studied, InAs nanowires exhibited the highest mobilities of 6000 cm2V-1s-1. InP nanowires featured the longest photoconductivity lifetimes and an exceptionally low surface recombination velocity of 170 cm/s. © 2013 IEEE.

Terahertz photonics is a rapidly growing field. The ultra-fast dynamics of charge carriers in semiconductors is closely linked to the performance of THz photonic devices. We study a range of ion-implanted and nano-scale semiconductors for application in novel terahertz devices.

We studied charge transport in anodized TiO2 nanotubes in the context of their application in dye-sensitized solar cells. Optical-pump-THz- probe spectroscopy revealed short free carrier lifetimes of about 15-30 ps, which we attribute to shallow trapping. © 2013 IEEE.

Solid-state dye-sensitized solar cells rely on effective infiltration of a solid-state hole-transporting material into the pores of a nanoporous TiO 2 network to allow for dye regeneration and hole extraction. Using microsecond transient absorption spectroscopy and femtosecond photoluminescence upconversion spectroscopy, the hole-transfer yield from the dye to the hole-transporting material 2,2′,7,7′-tetrakis(N,N-di-p- methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD) is shown to rise rapidly with higher pore-filling fractions as the dye-coated pore surface is increasingly covered with hole-transporting material. Once a pore-filling fraction of ≈30% is reached, further increases do not significantly change the hole-transfer yield. Using simple models of infiltration of spiro-OMeTAD into the TiO2 porous network, it is shown that this pore-filling fraction is less than the amount required to cover the dye surface with at least a single layer of hole-transporting material, suggesting that charge diffusion through the dye monolayer network precedes transfer to the hole-transporting material. Comparison of these results with device parameters shows that improvements of the power-conversion efficiency beyond ≈30% pore filling are not caused by a higher hole-transfer yield, but by a higher charge-collection efficiency, which is found to occur in steps. The observed sharp onsets in photocurrent and power-conversion efficiencies with increasing pore-filling fraction correlate well with percolation theory, predicting the points of cohesive pathway formation in successive spiro-OMeTAD layers adhered to the pore walls. From percolation theory it is predicted that, for standard mesoporous TiO2 with 20 nm pore size, the photocurrent should show no further improvement beyond an ≈83% pore-filling fraction. Solid-state dye-sensitized solar cells capable of complete hole transfer with pore-filling fractions as low as ∼30% are demonstrated. Improvements of device efficiencies beyond ∼30% are explained by a stepwise increase in charge-collection efficiency in agreement with percolation theory. Furthermore, it is predicted that, for a 20 nm pore size, the photocurrent reaches a maximum at ∼83% pore-filling fraction. © 2013 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim.

Phonon scattering limits charge-carrier mobilities and governs emission line broadening in hybrid metal halide perovskites. Establishing how charge carriers interact with phonons in these materials is therefore essential for the development of high-efficiency perovskite photovoltaics and low-cost lasers. Here we investigate the temperature dependence of emission line broadening in the four commonly studied formamidinium and methylammonium perovskites, HC(NH2)2 PbI3, HC(NH2)2 PbBr3, CH3NH3PbI3 and CH3 NH3 PbBr3, and discover that scattering from longitudinal optical phonons via the Fröhlich interaction is the dominant source of electron-phonon coupling near room temperature, with scattering off acoustic phonons negligible. We determine energies for the interacting longitudinal optical phonon modes to be 11.5 and 15.3 meV, and Fröhlich coupling constants of ∼40 and 60 meV for the lead iodide and bromide perovskites, respectively. Our findings correlate well with first-principles calculations based on many-body perturbation theory, which underlines the suitability of an electronic band-structure picture for describing charge carriers in hybrid perovskites.

Controlled doping of GaAs nanowires is crucial for the development of nanowire-based electronic and optoelectronic devices. Here, we present a noncontact method based on time resolved terahertz photoconductivity for assessing n- and p-type doping efficiency in nanowires. Using this technique, we measure extrinsic electron and hole concentrations in excess of 10(18) cm(-3) for GaAs nanowires with n-type and p-type doped shells. Furthermore, we show that controlled doping can significantly increase the photoconductivity lifetime of GaAs nanowires by over an order of magnitude: from 0.13 ns in undoped nanowires to 3.8 and 2.5 ns in n-doped and p-doped nanowires, respectively. Thus, controlled doping can be used to reduce the effects of parasitic surface recombination in optoelectronic nanowire devices, which is promising for nanowire devices, such as solar cells and nanowire lasers.

Hybrid metal-halide perovskites have emerged as a leading class of semiconductors for optoelectronic devices because of their desirable material properties and versatile fabrication methods. However, little is known about the chemical transformations that occur in the initial stages of perovskite crystal formation. Here we follow the real-time formation dynamics of MAPbI3 from a bilayer of lead iodide (PbI2) and methylammonium iodide (MAI) deposited through a two-step thermal evaporation process. By lowering the substrate temperature during deposition, we are able to initially inhibit intermixing of the two layers. We subsequently use infrared and visible light transmission, X-ray diffraction, and photoluminescence lifetime measurements to reveal the room-temperature transformations that occur in vacuum and ambient air, as MAI diffuses into the PbI2 lattice to form MAPbI3. In vacuum, the transformation to MAPbI3 is incomplete as unreacted MAI is retained in the film. However, exposure to moist air allows for conversion of the unreacted MAI to MAPbI3, demonstrating that moisture is essential in making MAI more mobile and thus aiding perovskite crystallization. These dynamic processes are reflected in the observed charge-carrier lifetimes, which strongly fluctuate during periods of large ion migration but steadily increase with improving crystallinity.

Reliable doping is required to realize many devices based on semiconductor nanowires. Group IIIV nanowires show great promise as elements of high-speed optoelectronic devices, but for such applications it is important that the electron mobility is not compromised by the inclusion of dopants. Here we show that GaAs nanowires can be n-type doped with negligible loss of electron mobility. Molecular beam epitaxy was used to fabricate modulation-doped GaAs nanowires with Al0.33Ga0.67As shells that contained a layer of Si dopants. We identify the presence of the doped layer from a high-angle annular dark field scanning electron microscopy cross-section image. The doping density, carrier mobility, and charge carrier lifetimes of these n-type nanowires and nominally undoped reference samples were determined using the noncontact method of optical pump terahertz probe spectroscopy. An n-type extrinsic carrier concentration of 1.10 +/- 0.06 x 10(16) cm(3) was extracted, demonstrating the effectiveness of modulation doping in GaAs nanowires. The room-temperature electron mobility was also found to be high at 2200 +/- 300 cm(2) V-1 s(-1) and importantly minimal degradation was observed compared with undoped reference nanowires at similar electron densities. In addition, modulation doping significantly enhanced the room-temperature photoconductivity and photoluminescence lifetimes to 3.9 +/- 0.3 and 2.4 +/- 0.1 ns respectively, revealing that modulation doping can passivate interfacial trap states.

Organic-inorganic lead-halide perovskites have recently drawn great attention as novel absorbers and charge transporters in low-cost solar cells. It is still largely unknown what makes these materials so phenomenally well-suited for charge generation and conduction. Here we show that both CH3NH3PbI3 and CH3NH3PbI3−xClx exhibit exceptionally low mono-molecular and bi-molecular charge-carrier decay rates, defying the Langevin limit by at least 4 orders of magnitude. Using transient THz spectroscopy, we establish lower bounds for the high-frequency charge mobility of 11.6 cm 2/Vs for CH3NH3PbI3−xClx and 8cm2/Vs for CH3NH3PbI3, which are remarkably high for solution-processed materials. We deduce charge-carrier diffusion lengths as a function of charge density and find values exceeding a few microns for CH3NH3PbI3−xClx, under typical device operating conditions. For CH3NH3PbI3, diffusion lengths are a factor∼4 lower because of higher mono- and bi-molecular recombination rates. These findings underline the suitability of this material class for planarheterojunction device structures and highlight the potential for performance tuning through manipulation of the polar metal-halide bond.

The organic-inorganic hybrid perovskites methylammonium lead iodide (CH3NH3PbI3) and the partially chlorine-substituted mixed halide CH3NH3PbI3-xClx emit strong and broad photoluminescence (PL) around their band gap energy of ∼1.6 eV. However, the nature of the radiative decay channels behind the observed emission and, in particular, the spectral broadening mechanisms are still unclear. Here we investigate these processes for high-quality vapor-deposited films of CH3NH3PbI3-xClx using time- and excitation-energy dependent photoluminescence spectroscopy. We show that the PL spectrum is homogenously broadened with a line width of 103 meV most likely as a consequence of phonon coupling effects. Further analysis reveals that defects or trap states play a minor role in radiative decay channels. In terms of possible lasing applications, the emission spectrum of the perovskite is sufficiently broad to have potential for amplification of light pulses below 100 fs pulse duration.

An understanding of aggregation effects in organic semiconductors is essential for their effective use in optoelectronic devices. Typically, the electronic dynamics in such systems are heavily dependant upon the aggregation state, and dynamics often occur on sub-nanosecond timescales. © 2010 IEEE.