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We use transient Rayleigh scattering to study the thermalization of hot photoexcited carriers in single GaAs0.7Sb0.3/InP nanowire heterostructures. By comparing the energy loss rate in single core-only GaAs0.7Sb0.3 nanowires which do not show substantial hot carrier effects with the core-shell nanowires, we show that the presence of an InP shell substantially suppresses the longitudinal optical phonon emission rate at low temperatures which then leads to strong hot carrier effects.

We report an analysis method that combines microphotoluminescence mapping and lifetime mapping data of single semiconductor nanowires to extract the doping concentration, nonradiative lifetime, and internal quantum efficiency along the length of the nanowires. Using this method, the doping concentration of single Si-doped wurtzite InP nanowires are mapped out and confirmed by the electrical measurements of single nanowire devices. Our method has important implication for single nanowire detectors and LEDs and nanowire solar cells applications.

The development of earth abundant materials for optoelectronics and photovoltaics promises improvements in sustainability and scalability. Recent studies have further demonstrated enhanced material efficiency through the superior light management of novel nanoscale geometries such as the nanowire. Here we show that an industry standard epitaxy technique can be used to fabricate high quality II-V nanowires (1D) and nanoplatelets (2D) of the earth abundant semiconductor Zn3As2. We go on to establish the optoelectronic potential of this material by demonstrating efficient photoemission and detection at 1.0 eV, an energy which is significant to the fields of both photovoltaics and optical telecommunications. Through dynamical spectroscopy this superior performance is found to arise from a low rate of surface recombination combined with a high rate of radiative recombination. These results introduce nanostructured Zn3As2 as a high quality optoelectronic material ready for device exploration.

We use polarized photoluminescence excitation spectroscopy to observe the energy and symmetry of the predicted second conduction band in 130 nm diameter wurtzite InP nanowires. We find direct spectroscopic signatures for optical transitions among the A, B, and C hole bands and both the first and the second conduction bands. We determine that the splitting between the first and second conduction bands is 228 ± 7 meV in excellent agreement with theory. From these energies we show that the spin-orbit energy changes substantially between zinc blende and wurtzite InP. We discuss the two quite different solutions within the quasi-cubic approximation and the implications for these measurements. Finally, the observation of well-defined optical transitions between the B- and C-hole bands and the second conduction band suggests that either the theoretical description of the second conduction band as possessing Γ8 symmetry is incomplete, or other interactions are enabling these forbidden transitions.

We use temperature-dependent photoluminescence (PL), photoluminescence imaging, and time-resolved photoluminescence measurements to gain insights into the localization of excitons in single 2 nm GaAs/AlGaAs quantum well tube nanowires. PL spectra reveal the coexistence of localized and delocalized states at low temperatures, with narrow quantum dot-like emission lines on the high energy side of a broad emission band, and delocalized states on the low energy side. We find that the high energy QD-like emissions are metastable, disappearing at higher temperatures with only delocalized states (quantum well tube ground states) surviving. By comparing temperature- and time-dependent PL, we develop a theoretical model which provides insights into the confinement potentials and relaxation dynamics which localize the excitons in these quantum well tube nanowires.

Using a new technique, transient Rayleigh scattering, we show that measurements from a single GaAs/AlGaAs core-shell semiconductor nanowire provide sensitive and detailed information on the time evolution of the density and temperature of the electrons and holes after photoexcitation by an intense laser pulse. Through band filling, band gap renormalization, and plasma screening, the presence of a dense and hot electron-hole plasma directly influences the real and imaginary parts of the complex index of refraction that in turn affects the spectral dependence of the Rayleigh scattering cross-section in well-defined ways. By measuring this spectral dependence as a function of time, we directly determine the thermodynamically independent density and temperature of the electrons and holes as a function of time after pulsed excitation as the carriers thermalize to the lattice temperature. We successfully model the results by including ambipolar transport, recombination, and cooling through optic and acoustic phonon emission that quantify the hole mobility at ∼68,000 cm(2)/V·s, linear decay constant at 380 ps, bimolecular recombination rate at 4.8 × 10(-9) cm(3)/s and the energy-loss rate of plasma due to optical and acoustic phonon emission.

In this Letter, we explore the nature of exciton localization in single GaAs/AlGaAs nanowire quantum well tube (QWT) devices using photocurrent (PC) spectroscopy combined with simultaneous photoluminescence (PL) and photoluminescence excitation (PLE) measurements. Excitons confined to GaAs quantum well tubes of 8 and 4 nm widths embedded into an AlGaAs barrier are seen to ionize at high bias levels. Spectroscopic signatures of the ground and excited states confined to the QWT seen in PL, PLE, and PC data are consistent with simple numerical calculations. The demonstration of good electrical contact with the QWTs enables the study of Stark effect shifts in the sharp emission lines of excitons localized to quantum dot-like states within the QWT. Atomic resolution cross-sectional TEM measurements and an analysis of the quantum confined Stark effect of these dots provide insights into the nature of the exciton localization in these nanostructures.

We investigate the absorption properties of ensembles of wurtzite (WZ) InP nanowires (NWs) by high-resolution polarization-resolved photoluminescence excitation (PLE) spectroscopy at T = 10 K. The degree of linear polarization of absorbed light, ρ(abs), resulting from the PLE spectra is governed by a competition between the dielectric mismatch effect and the WZ selection rules acting differently on different optical transitions. These two contributions are deconvoluted with the help of finite-difference time-domain simulations, thus providing information about the symmetry of the three highest valence bands (A, B, and C) of WZ InP and the extent of the spin-orbit interaction on these states. Moreover, ρ(abs) shows two characteristic dips corresponding to the two sharp A and B exciton resonances in the PLE spectra. A model developed for the dip in A provides the first experimental evidence of an enhancement in the dielectric mismatch effect originating from the Coulomb interaction between electron and hole.

The electronic properties of thin, nanometer scale GaAs quantum well tubes embedded inside the AlGaAs shell of a GaAs core–multishell nanowire are investigated using optical spectroscopies. Using numerical simulations to model cylindrically and hexagonally symmetric systems, we correlate these electronic properties with structural characterization by aberration-corrected scanning transmission electron microscopy of nanowire cross sections. These tubular quantum wells exhibit extremely high quantum efficiency and intense emission for extremely low submicrowatt excitation powers in both photoluminescence and photoluminescence excitation measurements. Numerical calculations of the confined eigenstates suggest that the electrons and holes in their ground states are confined to extremely localized one-dimensional filaments at the corners of the hexagonal structure which extend along the length of the nanowire.

The internal electronic structures of single semiconductor nanowires can be resolved using photomodulated Rayleigh scattering spectroscopy. The Rayleigh scattering from semiconductor nanowires is strongly polarization sensitive which allows a nearly background-free method for detecting only the light that is scattered from a single nanowire. While the Rayleigh scattering efficiency from a semiconductor nanowire depends on the dielectric contrast, it is relatively featureless as a function of energy. However, if the nanowire is photomodulated using a second pump laser beam, the internal electronic structure can be resolved with extremely high signal-to-noise and spectral resolution. The photomodulated Rayleigh scattering spectra can be understood theoretically as a first derivative of the scattering efficiency that results from a modulation of the band gap and depends sensitively on the nanowire diameter. Fits to spectral lineshapes provide both the band structure and the diameter of individual GaAs and InP nanowires under investigation.

Highly strained GaAs/GaP nanowires of excellent optical quality were grown with 50 nm diameter GaAs cores and 25 nm GaP shells. Photoluminescence from these nanowires is observed at energies dramatically shifted from the unstrained GaAs free exciton emission energy by 260 meV. Using Raman scattering, we show that it is possible to separately measure the degree of compressive and shear strain of the GaAs core and show that the Raman response of the GaP shell is consistent with tensile strain. The Raman and photoluminescence measurement are both on good agreement with 8 band k.p calculations. This result opens up new possibilities for engineering the electronic properties of the nanowires for optimal design of one-dimensional nanodevices by controlling the strain of the core and shell by varying the nanowire geometry.

We use time-resolved photoluminescence from single InP nanowires containing both wurtzite (WZ) and zincblende (ZB) crystalline phases to measure the carrier dynamics of quantum confined excitons in a type-II homostructure. The observed recombination lifetime increases by nearly 2 orders of magnitude from 170 ps for excitons above the conduction and valence band barriers to more than 8400 ps for electrons and holes that are strongly confined in quantum wells defined by monolayer-scale ZB sections in a predominantly WZ nanowire. A simple computational model, guided by detailed high-resolution transmission electron microscopy measurements from a single nanowire, demonstrates that the dynamics are consistent with the calculated distribution of confined states for the electrons and holes.

Low-temperature time-resolved photoluminescence spectroscopy is used to probe the dynamics of photoexcited carriers in single InP nanowires. At early times after pulsed excitation, the photoluminescence line shape displays a characteristic broadening, consistent with emission from a degenerate, high-density electron-hole plasma. As the electron-hole plasma cools and the carrier density decreases, the emission rapidly converges toward a relatively narrow band consistent with free exciton emission from the InP nanowire. The free excitons in these single InP nanowires exhibit recombination lifetimes closely approaching that measured in a high-quality epilayer, suggesting that in these InP nanowires, electrons and holes are relatively insensitive to surface states. This results in higher quantum efficiencies than other single-nanowire systems as well as significant state-filling and band gap renormalization, which is observed at high electron-hole carrier densities.

Nonequilibrium spin distributions in single GaAs/AlGaAs core-shell nanowires are excited using resonant polarized excitation at 10 K. At all excitation energies, we observe strong photoluminescence polarization due to suppressed radiative recombination of excitons with dipoles aligned perpendicular to the nanowire. Excitation resonances are observed at 1- or 2-LO phonon energies above the exciton ground states. Using rate equation modeling, we show that, at the lowest energies, strongly nonequilibrium spin distributions are present and we estimate their spin relaxation rate.