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Understanding the origin of hot carrier relaxation in nanowires (NWs) with one-dimensional (1D) geometry is significant for designing efficient hot carrier solar cells with such nanostructures. Here, we study the influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics of catalyst-free InGaAs-InAlAs core-shell NWs. Using steady-state and time-resolved photoluminescence (PL) spectroscopy the dependencies of hot carrier effects on the degree of confinement of photo-generated carriers induced by the nanowire diameter are determined at different lattice temperatures. Analysis of excitation-power dependent data and temperature-dependent PL linewidth broadening reveal that at low temperatures, strong Auger recombination and phonon-bottleneck are responsible for hot carrier effects. Our analysis gives also insights into electron-phonon and ionized impurity scattering, showing opposing trends with NW diameter, and it allows to estimate the Fr\"ohlich coupling constant for the InGaAs NWs. Conversely, with increasing lattice temperature, hot carrier relaxation rates increase due to enhanced Shockley-Read Hall and surface recombination. Time-resolved spectroscopy reveals a fourfold increase in the rate of Shockley-Read-Hall recombination from 6 ns at 10 K to 1.5 ns at 150 K. The findings suggest that minimizing defect densities in the bulk and surfaces of these NWs will be key to enhance hot carrier effects towards higher temperatures., Comment: 15 pages, 5 figures

Under continuous-wave laser excitation in an InGaAs multi-quantum-well (MQW) structure, the carrier temperature extracted from photoluminescence rises faster for 405 nm excitation compared with 980 nm excitation, as the injected carrier density increases. Ensemble Monte Carlo simulation of the carrier dynamics in the MQW system shows that this carrier temperature rise is dominated by nonequilibrium LO phonon effects, with the Pauli exclusion having a significant effect at high carrier densities. Further, we find a significant fraction of carriers reside in the satellite L-valleys for 405 nm excitation due to strong intervalley transfer, leading to a cooler steady-state electron temperature in the central valley compared with the case when intervalley transfer is excluded from the model. Good agreement between experiment and simulation has been shown, and a detailed analysis has been presented. This study expands our knowledge of the dynamics of the hot carrier population in semiconductors, which can be applied to further limit energy loss in solar cells., Comment: 22 pages, 7 figures, submitted for publication

Carrier thermalization in a superlattice solar cell made of polar semiconductors is studied theoretically by considering a minimal model where electron-phonon scattering is the principal channel of carrier energy loss. Importantly, the effect of an intrinsic quantum mechanical property; the phonon coherence, on carrier thermalization is investigated, within semiclassical picture in terms of phonon wave packet. It turns out that coherent longitudinal optical (LO) phonons weaken the effective electron-phonon coupling, thus supposedly lowering the carrier energy loss rate in solar cell. The resulting thermalization power is indeed significantly reduced by the coherent phonons, resulting in enhanced hot carrier effect, particularly for thin enough well layer where carrier confinement is also strong. A recent experiment on superlattice solar cell prototype is shown to manifest the coherent phonons-driven phenomenon. Our results demonstrate the practical implications of the fundamental quantum coherence property of phonons in semiconductors for improving superlattice solar cell performance, via hot carrier effect., Comment: Accepted, to appear in Physical Review Applied (2023)

Semiconductor nanowires (NWs) have shown evidence of robust hot carrier effects due to their small dimensions. The relaxation dynamics of hot carriers in these nanostructures, generated by photo-absorption, are of great importance in optoelectronic devices and high efficiency solar cells, such as hot carrier solar cells. Among various III-V semiconductors, indium arsenide (InAs) NWs are promising candidates for their applications in advanced light harvesting devices due to their high photo-absorptivity and high mobility. Here, we investigate the hot carrier dynamics in InAs-AlAsSb core-shell NWs, as well as bare-core InAs NWs, using ultrafast pump-probe spectroscopy with widely tuned pump and probe energies. We have found a lifetime of 2.3 ps for longitudinal optical (LO) phonons and hot electron lifetimes of about 3 ps and 30 ps for carrier-carrier interactions and electron-phonon interactions, respectively. In addition, we have investigated the electronic states in the AlAsSb-shell and found that, despite the large band offset of the core-shell design in the conduction band, excited carriers remain in the shell longer than 100 ps. Our results indicate evidence of plasmon-tailored core-shell NWs for efficient light harvesting devices, which could open potential avenues for improving the efficiency of photovoltaic solar cells.

A theoretical model using electron-phonon scattering rate equations is developed for assessing carrier thermalization under steady-state conditions in two-dimensional systems. The model is applied to investigate the hot carrier effect in III-V hot-carrier solar cells with a quantum well absorber. The question underlying the proposed investigation is: what is the power required to maintain two populations of electron and hole carriers in a quasi-equilibrium state at fixed temperatures and quasi-Fermi level splitting? The obtained answer is that the thermalization power density is reduced in two-dimensional systems compared to their bulk counterpart, which demonstrates a confinement-induced enhancement of the hot carrier effect in quantum wells. This power overall increases with the well thickness, and it is moreover shown that the intra-subband contribution dominates at small thicknesses while the inter-subband contribution increases with thickness and dominates in the bulk limit. Finally, the effects of the thermodynamic state of phonons and screening are clarified. In particular, the two-dimensional thermalization power density exhibits a non-monotonic dependence on the thickness of the quantum well layer, when both out-of-equilibrium longitudinal optical phonons and screening effects are taken into account. Our theoretical and numerical results provide tracks to interpret intriguing experimental observations in quantum well physics. They will also offer guidelines to increase the yield of photovoltaic effect based on the hot carrier effect using quantum well heterostructures, a result critical to the research toward high-efficiency solar cell devices.

Hot carrier solar cells aim to overcome the theoretical limit of single-junction photovoltaic devices by suppressing the thermalization of hot carriers and extracting them through energy selective contacts. Designing efficient hot carrier absorbers requires further investigation on hot carrier properties in materials. Although the thermalization of hot carriers is responsible for a large portion of energy loss in solar cells, it is still one of the least understood phenomena in semiconductors. Here, the impact of excitation energy on the properties of photo-generated hot carriers in an InGaAs multi-quantum well (MQW) structure at various lattice temperatures and excitation powers is studied. Photoluminescence (PL) emission of the sample is detected by a hyperspectral luminescence imager, which creates spectrally and spatially resolved PL maps. The thermodynamic properties of hot carriers, such as temperature and quasi-Fermi level splitting, are carefully determined via applying full PL spectrum fitting, which solves the Fermi-Dirac integral and considers the band-filling effect in the nanostructured material. In addition, the impact of thermalized power density and carrier scattering with longitudinal optical phonons on the spectral linewidth broadening under two excitation energies is studied., Comment: 20 pages, 14 figures

A type-II InAs/AlAs$_{0.16}$Sb$_{0.84}$ multiple-quantum well sample is investigated for the photoexcited carrier dynamics as a function of excitation photon energy and lattice temperature. Time-resolved measurements are performed using a near-infrared pump pulse, with photon energies near to and above the band gap, probed with a terahertz probe pulse. The transient terahertz absorption is characterized by a multi-rise, multi-decay function that captures long-lived decay times and a metastable state of for an excess-photon energy of $>100$ meV. For sufficient excess-photon energy, excitation of the metastable state is followed by a transition to the long-lived states. Excitation dependence of the long-lived states map onto a near-direct band gap ($E{_g}$) density of states with an Urbach tail below $E{_g}$. As temperature increases, the long-lived decay times increase $E{_g}$. Additionally, Auger (and/or trap-assisted Auger) scattering above the onset of the plateau may also contribute to longer hot-carrier lifetimes. Meanwhile, the initial decay component shows strong dependence on excitation energy and temperature, reflecting the complicated initial transfer of energy between valence-band and defect states, indicating methods to further prolong hot carriers for technological applications.