Ultrafast two-dimensional field spectroscopy of terahertz intersubband saturable absorbers.

Intersubband (ISB) transitions in semiconductor multi-quantum well (MQW) structures are promising candidates for the development of saturable absorbers at terahertz (THz) frequencies. Here, we exploit amplitude and phase-resolved two-dimensional (2D) THz spectroscopy on the sub-cycle time scale to observe directly the saturation dynamics and coherent control of ISB transitions in a metal-insulator MQW structure. Clear signatures of incoherent pump-probe and coherent four-wave mixing signals are recorded as a function of the peak electric field of the single-cycle THz pulses. All nonlinear signals reach a pronounced maximum for a THz electric field amplitude of 11 kV/cm and decrease for higher fields. We demonstrate that this behavior is a fingerprint of THz-driven carrier-wave Rabi flopping. A numerical solution of the Maxwell-Bloch equations reproduces our experimental findings quantitatively and traces the trajectory of the Bloch vector. This microscopic model allows us to design tailored MQW structures with optimized dynamical properties for saturable absorbers that could be used in future compact semiconductor-based single-cycle THz sources.

High Electron Mobility and Insights into Temperature-Dependent Scattering Mechanisms in InAsSb Nanowires.

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 cm2 V-1 s-1 at 10 K.

Nanoscale Near-Field Tomography of Surface States on (Bi0.5Sb0.5)2Te3.

Three-dimensional topological insulators (TIs) have attracted tremendous interest for their possibility to host massless Dirac Fermions in topologically protected surface states (TSSs), which may enable new kinds of high-speed electronics. However, recent reports have outlined the importance of band bending effects within these materials, which results in an additional two-dimensional electron gas (2DEG) with finite mass at the surface. TI surfaces are also known to be highly inhomogeneous on the nanoscale, which is masked in conventional far-field studies. Here, we use near-field microscopy in the mid-infrared spectral range to probe the local surface properties of custom-tailored (Bi0.5Sb0.5)2Te3 structures with nanometer precision in all three spatial dimensions. Applying nanotomography and nanospectroscopy, we reveal a few-nanometer-thick layer of high surface conductivity and retrieve its local dielectric function without assuming any model for the spectral response. This allows us to directly distinguish between different types of surface states. An intersubband transition within the massive 2DEG formed by quantum confinement in the bent conduction band manifests itself as a sharp, surface-bound, Lorentzian-shaped resonance. An additional broadband background in the imaginary part of the dielectric function may be caused by the TSS. Tracing the intersubband resonance with nanometer spatial precision, we observe changes of its frequency, likely originating from local variations of doping or/and the mixing ratio between Bi and Sb. Our results highlight the importance of studying the surfaces of these novel materials on the nanoscale to directly access the local optical and electronic properties via the dielectric function.

An Ultrafast Switchable Terahertz Polarization Modulator Based on III-V Semiconductor Nanowires.

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.

Single n+-i-n+ InP nanowires for highly sensitive terahertz detection.

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 single-nanowire 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-to-noise 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.

Broadband Phase-Sensitive Single InP Nanowire Photoconductive Terahertz Detectors.

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 (∼1260 cm(2) V(-1) s(-1)) and low dark current (∼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.

Single nanowire photoconductive terahertz detectors.

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.

Modulation doping of GaAs/AlGaAs core-shell nanowires with effective defect passivation and high electron mobility.

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 × 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.

In(x)Ga(1-x)As nanowires with uniform composition, pure wurtzite crystal phase and taper-free morphology.

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 µm photoluminescence, close to the technologically important optical fibre telecommunication wavelength, which is promising for application in photodetectors and nanoscale lasers.

Narrowband, Angle-Tunable, Helicity-Dependent Terahertz Emission from Nanowires of the Topological Dirac Semimetal Cd3As2.

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, polarization control remains difficult. Here, we demonstrate that by exploiting band structure 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 polarization. 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 to 45°. We therefore present Cd3As2 nanowires as a promising novel material platform for controllable terahertz emission.

Showcasing the optical properties of monocrystalline zinc phosphide thin films as an earth-abundant photovoltaic absorber.

Zinc phosphide, Zn3P2, is a semiconductor with a high absorption coefficient in the spectral range relevant for single junction photovoltaic applications. It is made of elements abundant in the Earth's crust, opening up a pathway for large deployment of solar cell alternatives to the silicon market. Here we provide a thorough study of the optical properties of single crystalline Zn3P2 thin films grown on (100) InP by molecular beam epitaxy. The films are slightly phosphorus-rich as determined by Rutherford backscattering. We elucidate two main radiative recombination pathways: one transition at approximately 1.52 eV attributed to zone-center band-to-band electronic transitions; and a lower-energy transition observed at 1.3 eV to 1.4 eV attributed to a defect band or band tail related recombination mechanisms. We believe phosphorus interstitials are likely at the origin of this band.

Towards higher electron mobility in modulation doped GaAs/AlGaAs core shell nanowires.

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 cm2 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 cm2 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.

Increased Photoconductivity Lifetime in GaAs Nanowires by Controlled n-Type and p-Type Doping.

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.

Low ensemble disorder in quantum well tube nanowires.

We have observed very low disorder in high quality quantum well tubes (QWT) in GaAs-Al(0.4)Ga(0.6)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.

Charge-Carrier Dynamics and Mobilities in Formamidinium Lead Mixed-Halide Perovskites.

The mixed-halide perovskite FAPb(Bry I1-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 cm(2) V(-1) s(-1) and diffusion lengths exceeding 1 µm, while mobilities across the mixed Br/I system depend on crystalline phase disorder.