Revue des recherches récentes dans le domaine des propriétés optiques des nanofils à base de GaN: luminescence continue et résolue en temps, excitons, propriétés liées aux phénomènes de surface.

We report on the direct observation of biexcitons in a III-nitride based multiple quantum well microcavity operating in the strong light-matter coupling regime by means of nonresonant continuous wave and time-resolved photoluminescence at low temperature. First, the biexciton dynamics is investigated for the bare active medium (multiple quantum wells alone) evidencing localization on potential fluctuations due to alloy disorder and thermalization between both localized and free excitonic and biexcitonic populations. Then, the role of biexcitons is considered for the full microcavity: in particular, we observe that for specific detunings the bottom of the lower polariton branch is directly fed by the radiative dissociation of either cavity biexcitons or excitons mediated by one LO-phonon. Accordingly, minimum polariton lasing thresholds are observed, when the bottom of the lower polariton branch corresponds in energy to the exciton or cavity biexciton first LO-phonon replica. This singular observation highlights the role of excitonic molecules in the polariton condensate formation process as being a more efficient relaxation channel when compared to the usually assumed acoustical phonon emission one.

GaN and InGaN nanocolumns of various compositions are studied by room-temperature photoluminescence (PL) under different ambient conditions. GaN nanocolumns exhibit a reversible quenching upon exposure to air under constant UV excitation, following a t (power) - 1/2 time dependence and resulting in a total reduction of intensity by 85-90%, as compared to PL measured in vacuum, with no spectral change. This effect is not observed when exposing the samples to pure nitrogen. We attribute this effect to photoabsorption and photodesorption of oxygen that modifies the surface potential bending. InGaN nanocolumns, under the same experimental conditions do not show the same quenching features: The high-energy part of the broad PL line is not modified by exposure to air, whereas a lower-energy part, which does quench by 80-90%, can now be distinguished. We discuss the different behaviors in terms of carrier localization and possible composition or strain gradients in the InGaN nanocolumns.

This work reports on the morphology control of the selective area growth of GaN-based nanostructures on c-plane GaN templates. By decreasing the substrate temperature, the nanostructures morphology changes from pyramidal islands (no vertical m-planes), to GaN nanocolumns with top semipolar r-planes, and further to GaN nanocolumns with top polar c-planes. When growing InGaN nano-disks embedded into the GaN nanocolumns, the different morphologies mentioned lead to different optical properties, due to the semi-polar and polar nature of the r-planes and c-planes involved. These differences are assessed by photoluminescence measurements at low temperature and correlated to the specific nano-disk geometry.

Picosecond and femtosecond spectroscopy allow for a detailed study of carrier dynamics in nanosctructured materials [1]. In such experiments, a laser pulse usually excites several nanostructures at once. However, spectroscopic information may also be acquired using pulses from an electron beam in a modern scanning electron microscope (SEM), exploiting cathodoluminescence (CL) where electrons are promoted from the conduction band to the valence band upon impingement of the high energy electron beam onto a semiconductor. This approach offers several advantages over the usual optical spectroscopy . The multimode imaging capabilities of the SEM enable the correlation of optical properties (via CL) with surface morphology (secondary electron mode) at the nanometer scale [2] and the large energy of the electrons allows the excitation of wide -bandgap materials. Here, we present results obtained with an original time-resolved cathodoluminescence (TRCL) setup [3]. This setup uses ultrafast UV laser pulses to create short photoelectron pulses. The light pulses from an ultrafast UV laser illuminate a metal photocathode from which the electrons are extracted and accelerated inside the high voltage column of the microscope and focused on the sample surface. The collected CL signal is dispersed in a spectrometer and analyzed with an ultrafast STREAK camera to obtain high time resolution. Our current setup reaches combined space and time resolutions of 50 nm and 10 ps, respectively. Measurements can be carried out at temperatures between 25 K and 300 K. We will describe the TRCL setup in detail and will also present results obtained on a-plane GaN and a-plane (Al,Ga)N/GaN quantum wells (QW) [4]. We first study an epitaxial lateral overgrown (ELO) a-plane GaN grown by hydride vapor phase epitaxy on r-plane sapphire that has been studied at 27 K. Large densities of basal stacking faults (BSFs) are usually observed in a-plane GaN. These extended defects can be seen as a type-II QWs and give rise to a broad and intense emission at 3.42 eV (50 meV below the emission energy of the D°X of wurtzite GaN [6]). We evidence that exciton localization and recombination processes are strongly dependent on the local BSF density. In low-BSF-density zones, we show that the diffusion of free excitons towards BSFs is donor assisted. On the other hand, zones with BSF bundles present a totally inhibited D°X emission. The change in BSF-bound exciton luminescence decay time is explained through direct relation to the local BSF density.As a next step, we proceeded to grow a (Al,Ga)N/GaN single QW by molecular beam epitaxy on the GaN sample studied above. Interest has been very high in a-plane GaN since Waltereit et al. demonstrated ten years ago the realization of polarization free (Al,Ga)N/GaN quantum wells (QWs) [5]. Built-in electric fields are indeed absent in a-plane GaN (non-polar GaN), which allows for the growth of wide QWs without decreasing the radiative recombination probability of electrons and holes. However, even when processing techniques such as epitaxial lateral overgrowth (ELO) are used, non-polar GaN grown on sapphire presents high densities of extended defects. While dislocations are considered as non-radiative recombination centers, basal plane stacking faults (BSFs) are optically active and give rise to an emission centered 50 meV below the excitonic bandgap of GaN [7]. We present a low-temperature TRCL study of exciton dynamics as a function of the local BSF density in a-plane (Al,Ga)N/GaN single QWs grown by molecular beam epitaxy on an ELO-GaN template. First, CL experiments demonstrate the existence of nearly BSF-free regions as well as the existence of regions with BSF bundles. This indicates that the BSF distribution of the underlying a-plane GaN template [8] is reproduced in the QW. We confirm the results obtained by Badcock et al., who demonstrated that the intersection of BSFs with the QW leads to the formation of quantum wires (QWR) [9]. We then study the local relaxation-recombination dynamics of excitons in both QW and QWRs. In particular, we show that the dynamics of QW excitons is dominated by their capture by the BSFs. The QW CL decay time therefore exhibits a strong spatial dependency, explaining the large range of values reported so far for exciton radiative lifetimes in non-polar (Al,Ga)N/GaN QWs [4]. We finally demonstrate that below 60 K, QWR excitons exhibit a zero-dimensional behavior, which we relate to their binding on localization centers such as QWR-width fluctuations. [1] Shah, J. Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures, Ch. 8 (Springer, Berlin, 1999).[2] Reimer, L. Scanning Electron Microscopy, Ch. 1 (Springer, Berlin, 1998).[3] M. Merano et al. , Nature 438, 479 (2005).[4] P. Corfdir et al., J. Appl. Phys. 107, 043524 (2010). [5] P. Waltereit et al., Nature 406, 865 (2000).[6] P. Corfdir et al., J. Appl. Phys. 105,043102(2009). [7] G. Salviati et al., Phys. Stat. Sol. (a) 171, 325 (1999). [8] P. Corfdir et al.,Appl. Phys. Lett. 94, 201115 (2009). [9] T. J. Badcock et al., Appl. Phys. Lett. 93, 101901 (2008).

Microcavity polaritons attract nowadays a lot of interest from the scientific community as they allow for the realization of low-threshold coherent light emitters that operate up to 300 K. It is usually admitted that, at low-temperature and negative cavity detunings, the mechanism limiting the polariton lasing threshold is the relaxation of polaritons towards the bottom of the lower-polariton branch, which is mediated by scattering with acoustic phonons. However, it has been theoretically predicted that in multi quantum well (QW) microcavities, dark exciton and biexciton states should play an important role in the overall relaxation mechanisms of cavity polaritons. Here, we address this issue through a time-resolved photoluminescence (TR-PL) study of the relaxation dynamics at 10 K of microcavity polaritons in a 3!-cavity containing 67 Al0.2Ga0.8N/GaN QWs. The vacuum Rabi splitting of our microcavity is 60 meV and cavity detunings (!) ranging between -100 and 0 meV are investigated. At 10 K, the microcavity PL at small angle is dominated by a transition at 3.63 eV attributed to lower polaritons with a small in-plane wave vector. Two additional non-dispersive lines at 3.673 and 3.693 eV are also observed. From excitation/power-dependent experiments, we attribute them to the recombination of cavity biexcitons and localized dark excitons, respectively. We show by TR-PL that the lower polariton PL at zero-angle exhibits at all times the same PL decay as biexcitons. From this dynamical behavior, together with the !-dependence of the biexciton emission energy, we can describe the interplay between polaritons and biexcitons. In particular, we demonstrate that in nitride-based multi QW microcavities, the mechanism limiting the relaxation of polaritons towards the center of the Brillouin zone is the radiative dissociation of cavity biexcitons into lower polaritons with high in-plane wave vector.