We have performed a comparative study of ultrafast charge carrier dynamics in a range of III-V nanowires using optical pump-terahertz probe spectroscopy. This versatile technique allows measurement ...of important parameters for device applications, including carrier lifetimes, surface recombination velocities, carrier mobilities and donor doping levels. GaAs, InAs and InP nanowires of varying diameters were measured. For all samples, the electronic response was dominated by a pronounced surface plasmon mode. Of the three nanowire materials, InAs nanowires exhibited the highest electron mobilities of 6000 cm² V⁻¹ s⁻¹, which highlights their potential for high mobility applications, such as field effect transistors. InP nanowires exhibited the longest carrier lifetimes and the lowest surface recombination velocity of 170 cm s⁻¹. This very low surface recombination velocity makes InP nanowires suitable for applications where carrier lifetime is crucial, such as in photovoltaics. In contrast, the carrier lifetimes in GaAs nanowires were extremely short, of the order of picoseconds, due to the high surface recombination velocity, which was measured as 5.4 × 10⁵ cm s⁻¹. These findings will assist in the choice of nanowires for different applications, and identify the challenges in producing nanowires suitable for future electronic and optoelectronic devices.
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.
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.
Highest reported efficiency cesium lead halide perovskite solar cells are realized by tuning the bandgap and stabilizing the black perovskite phase at lower temperatures. CsPbI2Br is employed in a ...planar architecture device resulting in 9.8% power conversion efficiency and over 5% stabilized power output. Offering substantially enhanced thermal stability over their organic based counterparts, these results show that all‐inorganic perovskites can represent a promising next step for photovoltaic materials.
Solution‐deposited‐converted perovskite solar cells are studied by converting PbI2 planar films into the phase pure, mixed‐halide perovskite (H3CNH3)PbI3‐xClx. These solar cells exhibit very high ...photovoltaic performance and close to unity internal incident photon‐to‐electron conversion.
The addition of large hydrophobic cations to lead halide perovskites has significantly enhanced the environmental stability of photovoltaic cells based on these materials. However, the associated ...formation of two-dimensional structures inside the material can lead to dielectric confinement, higher exciton binding energies, wider bandgaps and limited charge-carrier mobilities. Here we show that such effects are not detrimental to the charge transport for carefully processed films comprising a self-assembled thin layer of quasi-two-dimensional (2D) perovskite interfaced with a 3D MAPbI3 perovskite layer. We apply a combination of time-resolved photoluminescence and photoconductivity spectroscopy to reveal the charge-carrier recombination and transport through the film profile, when either the quasi-2D or the 3D layers are selectively excited. Through modeling of the recorded dynamics, we demonstrate that while the charge-carrier mobility is lower within the quasi-2D region, charge-carrier diffusion to the 3D phase leads to a rapid recovery in photoconductivity even when the quasi-2D region is initially photoexcited. In addition, the blue-shifted emission originating from quasi-2D regions overlaps significantly with the absorption spectrum of the 3D perovskite, allowing for highly effective “heterogeneous photon recycling”. We show that this combination fully compensates for the adverse effects of electronic confinement, yielding quasi-2D perovskites with highly efficient charge transporting properties.
In this work, we couple theoretical and experimental approaches to understand and reduce the losses of wide bandgap Br-rich perovskite pin devices at open-circuit voltage (V
) and short-circuit ...current (J
) conditions. A mismatch between the internal quasi-Fermi level splitting (QFLS) and the external V
is detrimental for these devices. We demonstrate that modifying the perovskite top-surface with guanidinium-Br and imidazolium-Br forms a low-dimensional perovskite phase at the n-interface, suppressing the QFLS-V
mismatch, and boosting the V
. Concurrently, the use of an ionic interlayer or a self-assembled monolayer at the p-interface reduces the inferred field screening induced by mobile ions at J
, promoting charge extraction and raising the J
. The combination of the n- and p-type optimizations allows us to approach the thermodynamic potential of the perovskite absorber layer, resulting in 1 cm
devices with performance parameters of V
s up to 1.29 V, fill factors above 80% and J
s up to 17 mA/cm
, in addition to a thermal stability T
lifetime of more than 3500 h at 85 °C.
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