Individual electron and hole localization in submonolayer InN quantum sheets embedded in GaN

We investigate sub-monolayer InN quantum sheets embedded in GaN(0001) by temperature-dependent photoluminescence spectroscopy under both continuous-wave and pulsed excitation. Both the peak energy and the linewidth of the emission band associated with the quantum sheets exhibit an anomalous dependence on temperature indicative of carrier localization. Photoluminescence transients reveal a power law decay at low temperatures reflecting that the recombining electrons and holes occupy spatially separate, individual potential minima reminiscent of conventional (In,Ga)N(0001) quantum wells exhibiting the characteristic disorder of a random alloy. At elevated temperatures, carrier delocalization sets in and is accompanied by a thermally activated quenching of the emission. We ascribe the strong nonradiative recombination to extended states in the GaN barriers and confirm our assumption by a simple rate-equation model.Comment: 10 pages, 3 figure

Exciton dynamics in GaAs/(Al,Ga)As core-shell nanowires with shell quantum dots

We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in the dynamics of charge carriers in the shell with increasing temperature, with particular emphasis on the transfer of carriers from the shell to the core of the nanowires. We finally discuss the implications of carrier localization in the (Al,Ga)As shell for fundamental studies and optoelectronic applications based on core-shell III-As nanowires

Quenching of the luminescence intensity of GaN nanowires under electron beam exposure: Impact of C adsorption on the exciton lifetime

Electron irradiation of GaN nanowires in a scanning electron microscope strongly reduces their luminous efficiency as shown by cathodoluminescence imaging and spectroscopy. We demonstrate that this luminescence quenching originates from a combination of charge trapping at already existing surface states and the formation of new surface states induced by the adsorption of C on the nanowire sidewalls. The interplay of these effects leads to a complex temporal evolution of the quenching, which strongly depends on the incident electron dose per area. Time-resolved photoluminescence measurements on electron-irradiated samples reveal that the carbonaceous adlayer affects both the nonradiative and the radiative recombination dynamics.Comment: This is an author-created, un-copyedited version of an article accepted for publication/published in Nanotechnology. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at http://dx.doi.org/10.1088/0957-4484/27/45/45570

Coupling of exciton states as the origin of their biexponential decay dynamics in GaN nanowires

Using time-resolved photoluminescence spectroscopy, we explore the transient behavior of bound and free excitons in GaN nanowire ensembles. We investigate samples with distinct diameter distributions and show that the pronounced biexponential decay of the donor-bound exciton observed in each case is not caused by the nanowire surface. At long times, the individual exciton transitions decay with a common lifetime, which suggests a strong coupling between the corresponding exciton states. A system of non-linear rate-equations taking into account this coupling directly reproduces the experimentally observed biexponential decay.Comment: 5 pages, 4 figure

Ga-polar (In,Ga)N/GaN quantum wells vs. N-polar (In,Ga)N quantum disks in GaN nanowires: Comparative analysis of carrier recombination, diffusion, and radiative efficiency

We investigate the radiative and nonradiative recombination processes in planar (In,Ga)N/GaN(0001) quantum wells and (In,Ga)N quantum disks embedded in GaN$(000\bar{1})$ nanowires using photoluminescence spectroscopy under both continuous-wave and pulsed excitation. The photoluminescence intensities of these two samples quench only slightly between 10 and 300 K, which is commonly taken as evidence for high internal quantum efficiencies. However, a side-by-side comparison shows that the absolute intensity of the Ga-polar quantum wells is two orders of magnitude higher than that of the N-polar quantum disks. A similar difference is observed for the initial decay time of photoluminescence transients obtained by time-resolved measurements, indicating the presence of a highly efficient nonradiative decay channel for the quantum disks. In apparent contradiction to this conjecture, the decay of both samples is observed to slow down dramatically after the initial rapid decay. Independent of temperature, the transients approach a power law for longer decay times, reflecting that recombination occurs between individual electrons and holes with varying spatial separation. Employing a coupled system of stochastic integro-differential equations taking into account both radiative and nonradiative Shockley-Read-Hall recombination of spatially separate electrons and holes as well as their diffusion, we obtain simulated transients matching the experimentally obtained ones. The results reveal that even dominant nonradiative recombination conserves the power law decay for (In,Ga)N/GaN{0001} quantum wells and disks

Stacking faults as quantum wells in nanowires: Density of states, oscillator strength and radiative efficiency

We investigate the nature of excitons bound to I1 basal-plane stacking faults [(I1;X)] in GaN nanowire ensembles by continuous-wave and time-resolved photoluminescence spectroscopy. Based on the linear increase of the radiative lifetime of these excitons with temperature, they are demonstrated to exhibit a two-dimensional density of states, i. e., a basal-plane stacking fault acts as a quantum well. From the slope of the linear increase, we determine the oscillator strength of the (I1;X) and show that the value obtained reflects the presence of large internal electrostatic fields across the stacking fault. While the recombination of donor-bound and free excitons in the GaN nanowire ensemble is dominated by nonradiative phenonema already at 10 K, we observe that the (I1;X) recombines purely radiatively up to 60 K. This finding provides important insight into the nonradiative recombination processes in GaN nanowires. First, the radiative lifetime of about 6 ns measured at 60 K sets an upper limit for the surface recombination velocity of 450 cm/s considering the nanowires mean diameter of 105 nm. Second, the density of nonradiative centers responsible for the fast decay of donor-bound and free excitons cannot be higher than 2x10^16 cm^-3. As a consequence, the nonradiative decay of donor-bound excitons in these GaN nanowire ensembles has to occur indirectly via the free exciton state

Coexistence of quantum-confined Stark effect and localized states in an (In,Ga)N/GaN nanowire heterostructure

We analyze the emission of single GaN nanowires with (In,Ga)N insertions using both micro-photoluminescence and cathodoluminescence spectroscopy. The emission spectra are dominated by a green luminescence band that is strongly blueshifted with increasing excitation density. In conjunction with finite-element simulations of the structure to obtain the piezoelectric polarization, these results demonstrate that our (In,Ga)N/GaN nanowire heterostructures are subject to the quantum-confined Stark effect. Additional sharp peaks in the spectra, which do not shift with excitation density, are attributed to emission from localized states created by compositional fluctuations in the ternary (In,Ga)N alloy.Comment: 6 pages, 8 figures; accepted for publication in Phys. Rev.

Radial Stark effect in (In,Ga)N nanowires

We study the luminescence of unintentionally doped and Si-doped In$_x$Ga$_{1-x}$N nanowires with a low In content (x<0.2) grown by molecular beam epitaxy on Si substrates. The emission band observed at 300 K from the unintentionally doped samples is centered at much lower energies (800 meV) than expected from the In content measured by x-ray diffractometry and energy dispersive x-ray spectroscopy. This discrepancy arises from the pinning of the Fermi level at the sidewalls of the nanowires, which gives rise to strong radial built-in electric fields. The combination of the built-in electric fields with the compositional fluctuations inherent to (In,Ga)N alloys induces a competition between spatially direct and indirect recombination channels. At elevated temperatures, electrons at the core of the nanowire recombine with holes close to the surface, and the emission from unintentionally doped nanowires exhibits a Stark shift of several hundreds of meV. The competition between spatially direct and indirect transitions is analyzed as a function of temperature for samples with various Si concentrations. We propose that the radial Stark effect is responsible for the broadband absorption of (In,Ga)N nanowires across the entire visible range, which makes these nanostructures a promising platform for solar energy applications.Comment: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Nano Letters (2016), copyright (C) American Chemical Society after peer review. To access the final edited and published work see http://dx.doi.org/10.1021/acs.nanolett.5b0374

Crystal-phase quantum dots in GaN quantum wires

We study the nature of excitons bound to I1 basal plane stacking faults in ensembles of ultrathin GaN nanowires by continuous-wave and time-resolved photoluminescence spectroscopy. These ultrathin nanowires, obtained by the thermal decomposition of spontaneously formed GaN nanowire ensembles, are tapered and have tip diameters down to 6 nm. With decreasing nanowire diameter, we observe a strong blue shift of the transition originating from the radiative decay of stacking fault-bound excitons. Moreover, the radiative lifetime of this transition in the ultrathin nanowires is independent of temperature up to 60 K and significantly longer than that of the corresponding transition in as-grown nanowires. These findings reveal a zero-dimensional character of the confined exciton state and thus demonstrate that I1 stacking faults in ultrathin nanowires act as genuine quantum dots

Luminescent N-polar (In,Ga)N/GaN quantum wells grown by plasma-assisted molecular beam epitaxy at high temperature

N-polar (In,Ga)N/GaN quantum wells prepared on freestanding GaN substrates by plasma-assisted molecular beam epitaxy at conventional growth temperatures of about 650 {\deg}C do not exhibit any detectable luminescence even at 10 K. In the present work, we investigate (In,Ga)N/GaN quantum wells grown on Ga- and N-polar GaN substrates at a constant temperature of 730 {\deg}C. This exceptionally high temperature results in a vanishing In incorporation for the Ga-polar sample. In contrast, quantum wells with an In content of 20% and abrupt interfaces are formed on N-polar GaN. Moreover, these quantum wells exhibit a spatially homogeneous green luminescence band up to room temperature, but the intensity of this band is observed to strongly quench with temperature. Temperature-dependent photoluminescence transients show that this thermal quenching is related to a high density of nonradiative Shockley-Read-Hall centers with large capture coefficients for electrons and holes.Comment: 10 pages, 2 figures, 1 tabl