Controlling the helicity of light by electrical magnetization switching.

Controlling the intensity of emitted light and charge current is the basis of transferring and processing information1. By contrast, robust information storage and magnetic random-access memories are implemented using the spin of the carrier and the associated magnetization in ferromagnets2. The missing link between the respective disciplines of photonics, electronics and spintronics is to modulate the circular polarization of the emitted light, rather than its intensity, by electrically controlled magnetization. Here we demonstrate that this missing link is established at room temperature and zero applied magnetic field in light-emitting diodes2-7, through the transfer of angular momentum between photons, electrons and ferromagnets. With spin-orbit torque8-11, a charge current generates also a spin current to electrically switch the magnetization. This switching determines the spin orientation of injected carriers into semiconductors, in which the transfer of angular momentum from the electron spin to photon controls the circular polarization of the emitted light2. The spin-photon conversion with the nonvolatile control of magnetization opens paths to seamlessly integrate information transfer, processing and storage. Our results provide substantial advances towards electrically controlled ultrafast modulation of circular polarization and spin injection with magnetization dynamics for the next-generation information and communication technology12, including space-light data transfer. The same operating principle in scaled-down structures or using two-dimensional materials will enable transformative opportunities for quantum information processing with spin-controlled single-photon sources, as well as for implementing spin-dependent time-resolved spectroscopies.

Kapitza-resistance-like exciton dynamics in atomically flat MoSe2-WSe2 lateral heterojunction.

Being able to control the neutral excitonic flux is a mandatory step for the development of future room-temperature two-dimensional excitonic devices. Semiconducting Monolayer Transition Metal Dichalcogenides (TMD-ML) with extremely robust and mobile excitons are highly attractive in this regard. However, generating an efficient and controlled exciton transport over long distances is a very challenging task. Here we demonstrate that an atomically sharp TMD-ML lateral heterostructure (MoSe2-WSe2) transforms the isotropic exciton diffusion into a unidirectional excitonic flow through the junction. Using tip-enhanced photoluminescence spectroscopy (TEPL) and a modified exciton transfer model, we show a discontinuity of the exciton density distribution on each side of the interface. We introduce the concept of exciton Kapitza resistance, by analogy with the interfacial thermal resistance referred to as Kapitza resistance. By comparing different heterostructures with or without top hexagonal boron nitride (hBN) layer, we deduce that the transport properties can be controlled, over distances far greater than the junction width, by the exciton density through near-field engineering and/or laser power density. This work provides a new approach for controlling the neutral exciton flow, which is key toward the conception of excitonic devices.

Interface engineering of charge-transfer excitons in 2D lateral heterostructures.

The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe2-WSe2 heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. We show that for hBN-encapsulated heterostructures, CT excitons exhibit small binding energies of just a few tens meV and at the same time large dipole moments, making them promising materials for optoelectronic applications (benefiting from an efficient exciton dissociation and fast dipole-driven exciton propagation). Our joint theory-experiment study presents a significant step towards a microscopic understanding of optical properties of technologically promising 2D lateral heterostructures.

Interlayer exciton mediated second harmonic generation in bilayer MoS2.

Second-harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also interlayer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations. Since interlayer exciton transitions are highly tunable also by choosing twist angle and material combination our results open up new approaches for designing the SHG response of layered materials.

Spin/valley pumping of resident electrons in WSe2 and WS2 monolayers.

Monolayers of transition metal dichalcogenides are ideal materials to control both spin and valley degrees of freedom either electrically or optically. Nevertheless, optical excitation mostly generates excitons species with inherently short lifetime and spin/valley relaxation time. Here we demonstrate a very efficient spin/valley optical pumping of resident electrons in n-doped WSe2 and WS2 monolayers. We observe that, using a continuous wave laser and appropriate doping and excitation densities, negative trion doublet lines exhibit circular polarization of opposite sign and the photoluminescence intensity of the triplet trion is more than four times larger with circular excitation than with linear excitation. We interpret our results as a consequence of a large dynamic polarization of resident electrons using circular light.

Light-Induced Passivation in Triple Cation Mixed Halide Perovskites: Interplay between Transport Properties and Surface Chemistry.

Mixed halide perovskites have attracted a strong interest in the photovoltaic community as a result of their high power conversion efficiency and the solid opportunity to realize low-cost and industry-scalable technology. Light soaking represents one of the most promising approaches to reduce non-radiative recombination processes and thus to optimize device performances. Here, we investigate the effects of 1 sun illumination on state-of-the-art triple cation halide perovskite thin films Cs0.05(MA0.14, FA0.86)0.95 Pb (I0.84, Br0.16)3 by a combined optical and chemical characterization. Competitive passivation and degradation effects on perovskite transport properties have been analyzed by spectrally and time-resolved quantitative imaging luminescence analysis and by X-ray photoemission spectroscopy (XPS). We notice a clear improvement of the optoelectronic properties of the material, with a increase of the quasi fermi level splitting and a corresponding decrease of methylammonium MA+ for short (up to 1 h) light soaking time. However, after 5 h of light soaking, phase segregation and in-depth oxygen penetration lead to a decrease of the charge mobility.

Quantitative optical assessment of photonic and electronic properties in halide perovskite.

The development of high efficiency solar cells relies on the management of electronic and optical properties that need to be accurately measured. As the conversion efficiencies increase, there is a concomitant electronic and photonic contribution that affects the overall performances. Here we show an optical method to quantify several transport properties of semiconducting materials and the use of multidimensional imaging techniques allows decoupling and quantifying the electronic and photonic contributions. Example of application is shown on halide perovskite thin film for which a large range of transport properties is given in the literature. We therefore optically measure pure carrier diffusion properties and evidence the contribution of optical effects such as the photon recycling as well as the photon propagation where emitted light is laterally transported without being reabsorbed. This latter effect has to be considered to avoid overestimated transport properties such as carrier mobility, diffusion length or diffusion coefficient.

Highly efficient MoOx-free semitransparent perovskite cell for 4 T tandem application improving the efficiency of commercially-available Al-BSF silicon.

In this work, the fabrication of MoOx-free semitransparent perovskite solar cells (PSC) with Power Conversion Efficiencies (PCE) up to 15.7% is reported. Firstly, opaque PSCs up to 19.7% were fabricated. Then, the rear metal contact was replaced by a highly transparent and conductive indium tin oxide (ITO) film, directly sputtered onto the hole selective layer, without any protective layer between Spiro-OMeTAD and rear ITO. To the best of our knowledge, this corresponds to the most efficient buffer layer-free semitransparent PSC ever reported. Using time-resolved photoluminescence (TRPL) technique on both sides of the semitransparent PSC, Spiro-OMeTAD/perovskite and perovskite/TiO2 interfaces were compared, confirming the great quality of Spiro-OMeTAD/perovskite interface, even after damage-less ITO sputtering, where degradation phenomena result less important than for perovskite/TiO2 one. Finally, a 4-terminal tandem was built combining semitransparent PSC with a commercially-available Aluminium Back Surface Field (Al-BSF) silicon wafer. That silicon wafer presents PCE = 19.52% (18.53% after being reduced to cell size), and 5.75% once filtered, to generate an overall 4 T tandem efficiency of 21.18% in combination with our champion large semitransparent PSC of 15.43%. It means an absolute increase of 1.66% over the original silicon wafer efficiency and a 2.65% over the cut Si cell.

Material challenges for solar cells in the twenty-first century: directions in emerging technologies.

Photovoltaic generation has stepped up within the last decade from outsider status to one of the important contributors of the ongoing energy transition, with about 1.7% of world electricity provided by solar cells. Progress in materials and production processes has played an important part in this development. Yet, there are many challenges before photovoltaics could provide clean, abundant, and cheap energy. Here, we review this research direction, with a focus on the results obtained within a Japan-French cooperation program, NextPV, working on promising solar cell technologies. The cooperation was focused on efficient photovoltaic devices, such as multijunction, ultrathin, intermediate band, and hot-carrier solar cells, and on printable solar cell materials such as colloidal quantum dots.

Determination of n-Type Doping Level in Single GaAs Nanowires by Cathodoluminescence.

We present an effective method of determining the doping level in n-type III-V semiconductors at the nanoscale. Low-temperature and room-temperature cathodoluminescence (CL) measurements are carried out on single Si-doped GaAs nanowires. The spectral shift to higher energy (Burstein-Moss shift) and the broadening of luminescence spectra are signatures of increased electron densities. They are compared to the CL spectra of calibrated Si-doped GaAs layers, whose doping levels are determined by Hall measurements. We apply the generalized Planck's law to fit the whole spectra, taking into account the electron occupation in the conduction band, the bandgap narrowing, and band tails. The electron Fermi levels are used to determine the free electron concentrations, and we infer nanowire doping of 6 × 1017 to 1 × 1018 cm-3. These results show that cathodoluminescence provides a robust way to probe carrier concentrations in semiconductors with the possibility of mapping spatial inhomogeneities at the nanoscale.

Accurate radiation temperature and chemical potential from quantitative photoluminescence analysis of hot carrier populations.

In order to characterize hot carrier populations in semiconductors, photoluminescence measurement is a convenient tool, enabling us to probe the carrier thermodynamical properties in a contactless way. However, the analysis of the photoluminescence spectra is based on some assumptions which will be discussed in this work. We especially emphasize the importance of the variation of the material absorptivity that should be considered to access accurate thermodynamical properties of the carriers, especially by varying the excitation power. The proposed method enables us to obtain more accurate results of thermodynamical properties by taking into account a rigorous physical description and finds direct application in investigating hot carrier solar cells, which are an adequate concept for achieving high conversion efficiencies with a relatively simple device architecture.

Electrodeposition of ZnO window layer for an all-atmospheric fabrication process of chalcogenide solar cell.

This paper presents the low cost electrodeposition of a transparent and conductive chlorine doped ZnO layer with performances comparable to that produced by standard vacuum processes. First, an in-depth study of the defect physics by ab-initio calculation shows that chlorine is one of the best candidates to dope the ZnO. This result is experimentally confirmed by a complete optical analysis of the ZnO layer deposited in a chloride rich solution. We demonstrate that high doping levels (>10(20) cm(-3)) and mobilities (up to 20 cm(2) V(-1) s(-1)) can be reached by insertion of chlorine in the lattice. The process developed in this study has been applied on a CdS/Cu(In,Ga)(Se,S)2 p-n junction produced in a pilot line by a non vacuum process, to be tested as solar cell front contact deposition method. As a result efficiency of 14.3% has been reached opening the way of atmospheric production of Cu(In,Ga)(Se,S)2 solar cell.