Oxford Terahertz Photonics Group

Measuring terahertz (THz) conductivity on an ultrafast timescale 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 that allows us to measure cyclotron effective mass on a picosecond timescale. We demonstrate this technique by observing electron cooling in the technologically significant narrow-bandgap semiconductor indium antimonide. A significant reduction of electron effective mass from 0.032 to 0.017 m(e) is observed in the first 200 ps after injecting hot electrons. The measured electron effective mass in InSb as a function of photoinjected electron density agrees well with conduction band nonparabolicity predictions from ab initio calculations of the quasiparticle band structure.

InAsSb nanowires are promising elements for thermoelectric devices, infrared photodetectors, high-speed transistors, as well as thermophotovoltaic cells. By changing the Sb alloy fraction the mid-infrared bandgap energy and thermal conductivity may be tuned for specific device applications. Using both terahertz and Raman noncontact probes, we show that Sb alloying increases the electron mobility in the nanowires by over a factor of 3 from InAs to InAs0.65Sb0.35. We also extract the temperature-dependent electron mobility via both terahertz and Raman spectroscopy, and we report the highest electron mobilities for InAs0.65Sb0.35 nanowires to date, exceeding 16,000 cm(2) V-1 s(-1) at 10 K.

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-terahertzprobe 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 x 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.

Precise control over the electrical conductivity of semiconductor nanowires is a crucial prerequisite for implementation of these nanostructures into novel electronic and optoelectronic devices. Advances in our understanding of doping mechanisms in nanowires and their influence on electron mobility and radiative efficiency are urgently required. Here, we investigate the electronic properties of n-type modulation doped GaAs/AlGaAs nanowires via optical pump terahertz (THz) probe spectroscopy and photoluminescence spectroscopy over the temperature range 5 K-300 K. We directly determine an ionization energy of 6.7 +/- 0.5 meV (T = 52 K) for the Si donors within the AlGaAs shell that create the modulation doping structure. We further elucidate the temperature dependence of the electron mobility, photoconductivity lifetime and radiative efficiency, and determine the charge-carrier scattering mechanisms that limit electron mobility. We show that below the donor ionization temperature, charge scattering is limited by interactions with interfaces, leading to an excellent electron mobility of 4360 +/- 380 cm(2) V-1 s(-1) at 5 K. Above the ionization temperature, polar scattering via longitudinal optical (LO) phonons dominates, leading to a room temperature mobility of 2220 +/- 130 cm(2) V-1 s(-1). In addition, we show that the Si donors effectively passivate interfacial trap states in the nanowires, leading to prolonged photoconductivity lifetimes with increasing temperature, accompanied by an enhanced radiative efficiency that exceeds 10% at room temperature.

Progress in the terahertz (THz) region of the electromagnetic spectrum is undergoing major advances, with advanced THz sources and detectors being developed at a rapid pace. Yet, ultrafast THz communication is still to be realized, owing to the lack of practical and effective THz modulators. Here, we present a novel ultrafast active THz polarization modulator based on GaAs semiconductor nanowires arranged in a wire-grid configuration. We utilize an optical pump-terahertz probe spectroscopy system and vary the polarization of the optical pump beam to demonstrate ultrafast THz modulation with a switching time of less than 5 ps and a modulation depth of -8 dB. We achieve an extinction of over 13% and a dynamic range of -9 dB, comparable to microsecond-switchable graphene- and metamaterial-based THz modulators, and surpassing the performance of optically switchable carbon nanotube THz polarizers. We show a broad bandwidth for THz modulation between 0.1 and 4 THz. Thus, this work presents the first THz modulator which combines not only a large modulation depth but also a broad bandwidth and picosecond time resolution for THz intensity and phase modulation, making it an ideal candidate for ultrafast THz communication.

Developing single-nanowire terahertz (THz) electronics and employing them as sub-wavelength components for highly-integrated THz time-domain spectroscopy (THz-TDS) applications is a promising approach to achieve future low-cost, highly integrable and high-resolution THz tools, which are desirable in many areas spanning from security, industry, environmental monitoring and medical diagnostics to fundamental science. In this work, we present the design and growth of n(+)-i-n(+) InP nanowires. The axial doping profile of the n+-i-n+ InP nanowires has been calibrated and characterized using combined optical and electrical approaches to achieve nanowire devices with low contact resistances, on which the highly-sensitive InP singlenanowire photoconductive THz detectors have been demonstrated. While the n+-i-n+ InP nanowire detector has a only pA-level response current, it has a 2.5 times improved signal-tonoise ratio compared with the undoped InP nanowire detector and is comparable to traditional bulk THz detectors. This performance indicates a promising path to nanowire-based THz electronics for future commercial applications.

Accurately measuring and controlling the electrical properties of semiconductor nanowires is of paramount importance in the development of novel nanowire-based devices. In light of this, terahertz. (THz) conductivity spectroscopy has emerged as an ideal non-contact technique for probing nanowire electrical conductivity and is showing tremendous value in the targeted development of nanowire devices. THz spectroscopic measurements of nanowires enable charge carrier lifetimes, mobilities, dopant concentrations and surface recombination velocities to be measured with high accuracy and high throughput in a contact-free fashion. This review spans seminal and recent studies of the electronic properties of nanowires using THz spectroscopy. A didactic description of THz time-domain spectroscopy, optical pump-THz probe spectroscopy, and their application to nanowires is included. We review a variety of technologically important nanowire materials, including GaAs, InAs, InP, GaN and InN nanowires, Si and Ge nanowires, ZnO nanowires, nanowire heterostructures, doped nanowires and modulation-doped nanowires. Finally, we discuss how THz measurements are guiding the development of nanowire-based devices, with the example of single-nanowire photoconductive THz receivers.

Terahertz time-domain spectroscopy (THz-TDS) has emerged as a powerful tool for materials characterization and imaging. A trend toward size reduction, higher component integration, and performance improvement for advanced THz-TDS systems is of increasing interest. The use of single semiconducting nanowires for terahertz (THz) detection is a nascent field that has great potential to realize future highly integrated THz systems. In order to develop such components, optimized material optoelectronic properties and careful device design are necessary. Here, we present antenna-optimized photoconductive detectors based on single InP nanowires with superior properties of high carrier mobility (similar to 1260 cm(2) V-1 s(-1)) and low dark current (similar to 10 pA), which exhibit excellent sensitivity and broadband performance. We demonstrate that these nanowire THz detectors can provide high quality time-domain spectra for materials characterization in a THz-TDS system, a critical step toward future application in advanced THz-TDS system with high spectral and spatial resolution.

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 1018 cmâ€“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.

The mixed-halide perovskite FAPb(BryI1–y)3 is attractive for color-tunable and tandem solar cells. Bimolecular and Auger charge-carrier recombination rate constants strongly correlate with the Br content, y, suggesting a link with electronic structure. FAPbBr3 and FAPbI3 exhibit charge-carrier mobilities of 14 and 27 cm2 V−1 s−1 and diffusion lengths exceeding 1 μm, while mobilities across the mixed Br/I system depend on crystalline phase disorder.

We have observed very low disorder in high quality quantum well tubes (QWT) in GaAs-Al$_{0.44}$Ga$_{0.56}$As core-multishell nanowires. Room-temperature photoluminescence spectra were measured from 150 single nanowires enabling a full statistical analysis of both intra- and inter-nanowire disorder. By modelling individual nanowire spectra{,} we assigned a quantum well tube thickness{,} a core disorder parameter and a QWT disorder parameter to each nanowire. A strong correlation was observed between disorder in the GaAs cores and disorder in the GaAs QWTs{,} which indicates that variations in core morphology effectively propagate to the shell layers. This highlights the importance of high quality core growth prior to shell deposition. Furthermore{,} variations in QWT thicknesses for different facet directions was found to be a likely cause of intra-wire disorder{,} highlighting the need for accurate shell growth

Photoconductive terahertz detectors based on single GaAs/AlGaAs nanowire were designed, fabricated and incorporated into the pulsed time-domain technique, showing a promise for nanowires in terahertz applications such as near-field terahertz sensors or on-chip terahertz micro-spectrometers.

Obtaining compositional homogeneity without compromising morphological or structural quality is one of the biggest challenges in growing ternary alloy compound semiconductor nanowires. Here we report growth of Au-seeded InxGa1-xAs nanowires via metal-organic vapour phase epitaxy with uniform composition, morphology and pure wurtzite (WZ) crystal phase by carefully optimizing growth temperature and V/III ratio. We find that high growth temperatures allow the InxGa1-xAs composition to be more uniform by suppressing the formation of typically observed spontaneous In-rich shells. A low V/III ratio results in the growth of pure WZ phase InxGa1-xAs nanowires with uniform composition and morphology while a high V/III ratio allows pure zinc-blende (ZB) phase to form. Ga incorporation is found to be dependent on the crystal phase favouring higher Ga concentration in ZB phase compared to the WZ phase. Tapering is also found to be more prominent in defective nanowires hence it is critical to maintain the highest crystal structure purity in order to minimize tapering and inhomogeneity. The InP capped pure WZ In0.65Ga0.35As core-shell nanowire heterostructures show 1.54 mu m photoluminescence, close to the technologically important optical fibre telecommunication wavelength, which is promising for application in photodetectors and nanoscale lasers.

Spectroscopy and imaging in the terahertz (THz) region of the electromagnetic spectrum has proven to provide important insights in fields as diverse as chemical analysis, materials characterization, security screening, and nondestructive testing. However, compact optoelectronics suited to the most powerful terahertz technique, time-domain spectroscopy, are lacking. Here, we implement single GaAs nanowires as microscopic coherent THz sensors and for the first time incorporated them into the pulsed time-domain technique. We also demonstrate the functionality of the single nanowire THz detector as a spectrometer by using it to measure the transmission spectrum of a 290 GHz low pass filter. Thus, nanowires are shown to be well suited for THz device applications and hold particular promise as near-field THz sensors.

Reliable doping is required to realize many devices based on semiconductor nanowires. Group III–V 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 × 1016 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 cm2 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.

Photoconductive terahertz detectors based on single GaAs/AlGaAs core-shell nanowire have been designed and fabricated. The devices were characterised in a terahertz time-domain spectroscopy system, showing excellent sensitivity comparable to the standard bulk ion-implanted InP receiver, with a detection bandwidth of 0.1 ~ 0.6 THz. Finite-difference time-domain simulations were performed to understand the origin of the narrow bandwidth of current detectors as well as optimize antenna designs to improve detector performance.

The photograph shows a polymer reflector that mimics the colour and underlying molecular structure of a golden beetle. It is formed from self-organizing layers of photopolymerised liquid crystal. These require an aligning layer, but we show that a layer of the material can be used as to self-align subsequent coatings, enabling the construction of complex structures by sequential coating of engineered materials.

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Jessica Boland

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