Hole and electron effective masses in single InP nanowires with a Wurtzite-Zincblende homojunction

The formation of wurtzite (WZ) phase in III–V nanowires (NWs) such as GaAs and InP is a complication hindering the growth of pure-phase NWs, but it can also be exploited to form NW homostructures consisting of alternate zincblende (ZB) and WZ segments. This leads to different forms of nanostructures, such as crystal-phase superlattices and quantum dots. Here, we investigate the electronic properties of the simplest, yet challenging, of such homostructures: InP NWs with a single homojunction between pure ZB and WZ segments. Polarization-resolved microphotoluminescence (μ-PL) measurements on single NWs provide a tool to gain insights into the interplay between NW geometry and crystal phase. We also exploit this homostructure to simultaneously measure effective masses of charge carriers and excitons in ZB and WZ InP NWs, reliably. Magneto-μ-PL measurements carried out on individual NWs up to 29 T at 77 K allow us to determine the free exciton reduced masses of the ZB and WZ crystal phases, showing the heavier character of the WZ phase, and to deduce the effective mass of electrons in ZB InP NWs (me= 0.080 m0). Finally, we obtain the reduced mass of light-hole excitons in WZ InP by probing the second optically permitted transition Γ7C ↔ Γ7uV with magneto-μ-PL measurements carried out at room temperature. This information is used to extract the experimental light-hole effective mass in WZ InP, which is found to be mlh = 0.26 m0, a value much smaller than the one of the heavy hole mass. Besides being a valuable test for band structure calculations, the knowledge of carrier masses in WZ and ZB InP is important in view of the optimization of the efficiency of solar cells, which is one of the main applications of InP NWs

Ground/space, passive/active remote sensing observations coupled with particle dispersion modelling to understand the inter-continental transport of wildfire smoke plumes

During the 2017 record-breaking burning season in Canada/United States, intense wild fires raged during the first week of September in the Pacific northwestern region (British Columbia, Alberta, Washington, Oregon, Idaho, Montana and northern California) burning mostly temperate coniferous forests. The heavy loads of smoke particles emitted in the atmosphere reached the Iberian Peninsula (IP) a few days later on 7 and 8 September. Satellite imagery allows to identify two main smoke clouds emitted during two different periods that were injected and transported in the atmosphere at several altitude levels. Columnar properties on 7 and 8 September at two Aerosol Robotic Network (AERONET) mid-altitude, background sites in northern and southern Spain are: aerosol optical depth (AOD) at 440 nm up to 0.62, Ångström exponent of 1.6–1.7, large dominance of small particles (fine mode fraction >0.88), low absorption AOD at 440 nm (0.98). Profiles from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) show the presence of smoke particles in the stratosphere during the transport, whereas the smoke is only observed in the troposphere at its arrival over the IP. Portuguese and Spanish ground lidar stations from the European Aerosol Research Lidar Network/Aerosols, Clouds, and Trace gases Research InfraStructure Network (EARLINET/ACTRIS) and the Micro-Pulse Lidar NETwork (MPLNET) reveal smoke plumes with different properties: particle depolarization ratio and color ratio, respectively, of 0.05 and 2.5 in the mid troposphere (5–9 km) and of 0.10 and 3.0 in the upper troposphere (10–13 km). In the mid troposphere the particle depolarization ratio does not seem time-dependent during the transport whereas the color ratio seems to increase (larger particles sediment first). To analyze the horizontal and vertical transport of the smoke from its origin to the IP, particle dispersion modelling is performed with the Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) parameterized with satellite-derived biomass burning emission estimates from the Global Fire Assimilation System (GFAS) of the Copernicus Atmosphere Monitoring Service (CAMS). Three compounds are simulated: carbon monoxide, black carbon and organic carbon. The results show that the first smoke plume which travels slowly reaches rapidly (~1 day) the upper troposphere and lower stratosphere (UTLS) but also shows evidence of large scale horizontal dispersion, while the second plume, entrained by strong subtropical jets, reaches the upper troposphere much slower (~2.5 days). Observations and dispersion modelling all together suggest that particle depolarization properties are enhanced during their vertical transport from the mid to the upper troposphere.Spanish groups acknowledge the Spanish Ministry of Economy and Competitivity (MINECO) (ref. CGL2013-45410-R, CGL2014-52877-R, CGL2014-55230-R, TEC2015-63832-P, CGL2015-73250-JIN, CGL2016-81092-R and CGL2017-85344-R)European Union through H2020 programme ACTRIS-2, grant 654109European Union through H2020 programme EUNADICS-AV, grant 723986European Union through H2020 programme GRASP-ACE, grant 77834

Effect of Electron-Hole Overlap and Exchange Interaction on Excitation Radiative Lifetimes of CdTe/CdSe Heteronanocrystals

Wave function engineering has become a powerful tool to tailor the optical properties of semiconductor colloidal nanocrystals. Core–shell systems allow to design the spatial extent of the electron (e) and hole (h) wave functions in the conduction- and valence bands, respectively. However, tuning the overlap between the e- and h-wave functions not only affects the oscillator strength of the coupled e–h pairs (excitons) that are responsible for the light emission, but also modifies the e–h exchange interaction, leading to an altered excitonic energy spectrum. Here, we present exciton lifetime measurements in a strong magnetic field to determine the strength of the e–h exchange interaction, independently of the e–h overlap that is deduced from lifetime measurements at room temperature. We use a set of CdTe/CdSe core/shell heteronanocrystals in which the electron–hole separation is systematically varied. We are able to unravel the separate effects of e–h overlap and e–h exchange on the exciton lifetimes, and we present a simple model that fully describes the recombination lifetimes of heteronanostructures (HNCs) as a function of core volume, shell volume, temperature, and magnetic fields

Direct and indirect exciton transitions in two-dimensional lead halide perovskite semiconductors

Atomically thin layers of two-dimensional lead halide perovskite semiconductors exhibit prominent light emission due to the inherently strong quantum and dielectric confinement. Electronic band structures and coupled electron-hole pairs (excitons), which govern the optical properties, are not well understood in these emergent two-dimensional materials. Here, we have performed both the steady-state and time-resolved photoluminescence spectroscopies with varying temperature to study the optical responses of a high-quality (PEA)2PbI4 single crystal. We observe a multitude of exciton transitions with different responses to temperature that suggests their different origins. Furthermore, our results suggest that the photoluminescence of layered perovskites is dominated by direct exciton transitions at low temperatures, while by an indirect exciton at high temperatures that can be explained by our proposed exciton band structure incorporating the interplay of Coulomb and Rashba effects. Our study sheds light on the intrinsic optical properties of two-dimensional perovskites that may be beneficial for the novel applications of perovskite-based devices.Ministry of Education (MOE)National Research Foundation (NRF)Published versionQ.X. acknowledges the support from the Singapore National Research Foundation through the NRF Investigatorship Award (Grant No. NRF-NRFI2015-03) and the Singapore Ministry of Education via the AcRF Tier 3 Programme “Geometrical Quantum Materials” (Grant No. MOE2018-T3-1-002), Tier 2 (Grant No. MOE2018-T2-2-068), and Tier 1 (Grant Nos. RG103/15 and RG113/16). A.G.d.A. gratefully acknowledges the financial support from the Presidential Postdoctoral Fellowship program of Nanyang Technological University

Efficient up-conversion photoluminescence in all-inorganic lead halide perovskite nanocrystals

Up-conversion photoluminescence (UCPL) refers to the elementary process where low-energy photons are converted into high-energy ones via consecutive interactions inside a medium. When additional energy is provided by internal thermal energy in the form of lattice vibrations (phonons), the process is called phonon-assisted UCPL. Here, we report the exceptionally large phonon-assisted energy gain of up to ~ 8kBT (kB is Boltzmann constant, T is temperature) on all-inorganic lead halide perovskite semiconductor colloidal nanocrystals that goes beyond the maximum capability of only harvesting optical phonon modes. By systematic optical study in combination with a statistical probability model, we explained the nontrivial phonon-assisted UCPL process in perovskites nanocrystals, where in addition to the strong electron-phonon (light-matter) coupling, other nonlinear processes such as phonon-phonon (matter-matter) interaction also effectively boost the up-conversion efficiency.Ministry of Education (MOE)National Research Foundation (NRF)Accepted versionQ. X. gratefully acknowledges financial support from the Singapore National Research Foundation through the NRF Investigatorship Award (No. NRF-NRFI2015-03) and the Singapore Ministry of Education via AcRF Tier 3 Programme (No. MOE2018-T3-1-002), Tier 2 grant (No. MOE2018-T2-2-068)and Tier 1 grants (Nos. RG103/15 and RG113/16). A. G. D. A. gratefully acknowledges the financial support of the Presidential Postdoctoral Fellowship program of the Nanyang Technological University. We acknowledge Dr. Lulu Zhang for his help on the TEM characterization

Observation of the full exciton and phonon fine structure in CdSe/CdS dot-in-rod heteronanocrystals

Light emission of semiconductor nanocrystals is a complex process, depending on many factors, among which are the quantum mechanical size confinement of excitons (coupled electron-hole pairs) and the influence of confined phonon modes and the nanocrystal surface. Despite years of research, the nature of nanocrystal emission at low temperatures is still under debate. Here we unravel the different optical recombination pathways of CdSe/CdS dot-in-rod systems that show an unprecedented number of narrow emission lines upon resonant laser excitation. By using self-assembled, vertically aligned rods and application of crystallographically oriented high magnetic fields, the origin of all these peaks is established. We observe a clear signature of an acoustic-phonon assisted transition, separated from the zero-phonon emission and optical-phonon replica, proving that nanocrystal light emission results from an intricate interplay between bright (optically allowed) and dark (optically forbidden) exciton states, coupled to both acoustic and optical phonon modes

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide

Monolayer transition-metal dichalcogenides have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. The optical properties of these two-dimensional crystals are dominated by tightly bound electron-hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions). Here we investigate monolayer WS2 samples via photoluminescence and time-resolved Kerr rotation. In photoluminescence and in energy-dependent Kerr rotation measurements, we are able to resolve two different trion states, which we interpret as intravalley and intervalley trions. Using time-resolved Kerr rotation, we observe a rapid initial valley polarization decay for the A exciton and the trion states. Subsequently, we observe a crossover towards exciton-exciton interaction-related dynamics, consistent with the formation and decay of optically dark A excitons. By contrast, resonant excitation of the B exciton transition leads to a very slow decay of the Kerr signal

Two-dimensional and emission-tunable : an unusual perovskite constructed from lindqvist-type [Pb6Br19]7- nanoclusters

Preparing low-dimensional perovskite materials with novel building units is highly desirable because such materials have already been demonstrated to show unusual physical properties. In this report, we first reported a new and unusual two-dimensional perovskite framework, [B(HIm)4]4Pb13Br38 (1), constructed from novel Lindqvist-type [Pb6Br19]7- nanoclusters. The as-prepared material shows good water resistance and chemical/heat stability. More importantly, 1 has been proven to exhibit temperature/excitation-wavelength-dependent emission. A possible mechanism has been provided.MOE (Min. of Education, S’pore