Perspective on the physics of two-dimensional perovskites in high magnetic field

Two-dimensional (2D) metal halide perovskites consist of atomically thin layers composed of low bandgap metal-halide slabs, surrounded by high bandgap organic ligands, which behave as barriers. In this Perspective, we highlight how the use of large magnetic fields has been an extremely insightful tool to unravel some of the fundamental electronic properties of 2D perovskites. We focus on the combination of magnetoabsorption measurements and theoretical modeling to extract the carrier effective mass, on the use of magnetic field to clarify the fine structure of the exciton manifold, and on how magnetic fields can be helpful to correctly assign side peaks in the complex absorption or photoluminescence spectra displayed by 2D perovskites. We finally point out some challenges which might be successfully addressed by magneto-optical experimental techniques

Ultrahigh magnetic field spectroscopy reveals the band structure of the 3D topological insulator Bi2_2Se3_3

We have investigated the band structure at the $\Gamma$ point of the three-dimensional (3D) topological insulator Bi$_2$Se$_3$ using magneto-spectroscopy over a wide range of energies ($0.55-2.2$\,eV) and in ultrahigh magnetic fields up to 150\,T. At such high energies ($E>0.6$\,eV) the parabolic approximation for the massive Dirac fermions breaks down and the Landau level dispersion becomes nonlinear. At even higher energies around 0.99 and 1.6 eV, new additional strong absorptions are observed with a temperature and magnetic-field dependence which suggest that they originate from higher band gaps. Spin orbit splittings for the further lying conduction and valence bands are found to be 0.196 and 0.264 eV

Revealing large-scale homogeneity and trace impurity sensitivity of GaAs nanoscale membranes

III-V nanostructures have the potential to revolutionize optoelectronics and energy harvesting. For this to become a reality, critical issues such as reproducibility and sensitivity to defects should be resolved. By discussing the optical properties of MBE grown GaAs nanomembranes we highlight several features that bring them closer to large scale applications. Uncapped membranes exhibit a very high optical quality, expressed by extremely narrow neutral exciton emission, allowing the resolution of the more complex excitonic structure for the first time. Capping of the membranes with an AlGaAs shell results in a strong increase of emission intensity but also to a shift and broadening of the exciton peak. This is attributed to the existence of impurities in the shell, beyond MBE-grade quality, showing the high sensitivity of these structures to the presence of impurities. Finally, emission properties are identical at the sub-micron and sub-millimeter scale, demonstrating the potential of these structures for large scale applications.Comment: just accepted in Nano Letters, http://pubs.acs.org/doi/abs/10.1021/acs.nanolett.7b0025

Site-selective measurement of coupled spin pairs in an organic semiconductor

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S=0) and dark triplet quintet (S=1,2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems

Non equilibrium anisotropic excitons in atomically thin ReS2_2

We present a systematic investigation of the electronic properties of bulk and few layer ReS$_2$ van der Waals crystals using low temperature optical spectroscopy. Weak photoluminescence emission is observed from two non-degenerate band edge excitonic transitions separated by $\sim$ 20 meV. The comparable emission intensity of both excitonic transitions is incompatible with a fully thermalized (Boltzmann) distribution of excitons, indicating the hot nature of the emission. While DFT calculations predict bilayer ReS$_2$ to have a direct fundamental band gap, our optical data suggests that the fundamental gap is indirect in all cases

Probing the inter-layer exciton physics in a MoS2_2/MoSe2_2/MoS2_2 van der Waals heterostructure

Stacking atomic monolayers of semiconducting transition metal dichalcogenides (TMDs) has emerged as an effective way to engineer their properties. In principle, the staggered band alignment of TMD heterostructures should result in the formation of inter-layer excitons with long lifetimes and robust valley polarization. However, these features have been observed simultaneously only in MoSe$_2$/WSe$_2$ heterostructures. Here we report on the observation of long lived inter-layer exciton emission in a MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructure. The inter-layer nature of the observed transition is confirmed by photoluminescence spectroscopy, as well as by analyzing the temporal, excitation power and temperature dependence of the inter-layer emission peak. The observed complex photoluminescence dynamics suggests the presence of quasi-degenerate momentum-direct and momentum-indirect bandgaps. We show that circularly polarized optical pumping results in long lived valley polarization of inter-layer exciton. Intriguingly, the inter-layer exciton photoluminescence has helicity opposite to the excitation. Our results show that through a careful choice of the TMDs forming the van der Waals heterostructure it is possible to control the circular polarization of the inter-layer exciton emission.Comment: 19 pages, 3 figures. Just accepted for publication in Nano Letters (http://pubs.acs.org/doi/10.1021/acs.nanolett.7b03184

Excitonic Properties of Low-Band-Gap Lead-Tin Halide Perovskites

The MAPb1–xSnxI3 (x = 0–1) (MA = methylammonium) perovskite family comprises a range of ideal absorber band gaps for single- and multijunction perovskite solar cells. Here, we use spectroscopic measurements to reveal a range of hitherto unknown fundamental properties of this materials family. Temperature-dependent transmission results show that the temperature of the tetragonal to orthorhombic structural transition decreases with increasing tin content. Through low-temperature magnetospectroscopy, we show that the exciton binding energy is lower than 16 meV, revealing that the dominant photogenerated species at typical operational conditions of optoelectronic devices are free charges rather than excitons. The reduced mass increases approximately proportionally to the band gap, and the mass values (0.075–0.090me) can be described with a two-band k·p perturbation model extended across the broad band gap range of 1.2–2.4 eV. Our findings can be generalized to predict values for the effective mass and binding energy for other members of this family of materials

Integrated III-V Photonic Crystal - Si waveguide platform with tailored optomechanical coupling

Optomechanical systems, in which the vibrations of a mechanical resonator are coupled to an electromagnetic radiation, have permitted the investigation of a wealth of novel physical effects. To fully exploit these phenomena in realistic circuits and to achieve different functionalities on a single chip, the integration of optomechanical resonators is mandatory. Here, we propose a novel approach to heterogeneously integrate arrays of two-dimensional photonic crystal defect cavities on top of silicon-on-insulator waveguides. The optomechanical response of these devices is investigated and evidences an optomechanical coupling involving both dispersive and dissipative mechanisms. By controlling the optical coupling between the waveguide and the photonic crystal, we were able to vary and understand the relative strength of these couplings. This scalable platform allows for an unprecedented control on the optomechanical coupling mechanisms, with a potential benefit in cooling experiments, and for the development of multi-element optomechanical circuits in the framework of optomechanically-driven signal-processing applications