Cs₂AgBiBr₆ (CABB) has been proposed as a promising nontoxic alternative to lead halide perovskites. However, low charge carrier collection efficiencies remain an obstacle for the incorporation of this material in optoelectronic applications. In this work, we study the optoelectronic properties of CABB thin films using steady state and transient absorption and reflectance spectroscopy. We find that optical measurements on such thin films are distorted as a consequence of multiple reflections within the film. Moreover, we discuss the pathways behind conductivity loss in these thin films, using a combination of microsecond transient absorption spectroscopy and time-resolved microwave conductivity measurements. We demonstrate that a combined effect of carrier loss and localization results in the conductivity loss in CABB thin films. Moreover, we find that the charge carrier diffusion length and grain size are of the same order of magnitude. This suggests that the material's surface is an important contributor to charge-carrier loss.

@en

Accurately controlling light emission using nano- and microstructured lenses and antennas is an active field of research. Dielectrics are especially attractive lens materials due to their low optical losses over a broad bandwidth. In this work we measure highly directional light emission from patterned quantum dots (QDs) aligned underneath all-dielectric nanostructured microlenses. The lenses are designed with an evolutionary algorithm and have a theoretical directivity of 160. The fabricated structures demonstrate an experimental full directivity of 61 ± 3, three times higher than what has been estimated before, with a beaming half-angle of 2.6°. This high value compared to previous works is achieved via three mechanisms. First, direct electron beam patterning of QD emitters and alignment markers allowed for more localized emission and better emitter-lens alignment. Second, the lens fabrication was refined to minimize distortions between the designed shape and the final structure. Finally, a new measurement technique was developed that combines integrating sphere microscopy with Fourier microscopy. This enables complete directivity measurements, contrary to other reported values, which are typically only partial directivities or estimates of the full directivity that rely partly on simulations. The experimentally measured values of the complete directivity were higher than predicted by combining simulations with partial directivity measurements. High directivity was obtained from three different materials (cadmium-selenide-based QDs and two lead halide perovskite materials), emitting at 520, 620, and 700 nm, by scaling the lens size according to the emission wavelength.

@en

Present day nanowire solar cells have reached an efficiency of 17.8%. Nanophotonic engineering by nanowire tapering allows for high solar light absorption. In combination with sufficiently high carrier selectivity at the contacts, the short-circuit current (J_sc) has presently reached 29.3 mA/cm², reasonably close to the 34.6 mA/cm² theoretical limit for InP. Although further optimization of the current is important, an equally challenging condition to approach the Shockley Queisser (S-Q) limit is to increase the open-circuit voltage (V_oc) towards the radiative limit. The key requirement to reach the radiative limit is to increase the external radiative efficiency at open-circuit conditions towards unity. It is the main purpose of this review to highlight recent progress in nanophotonic engineering to further enhance the open circuit voltage of a nanowire solar cell. In addition to material optimization for increasing the internal photoluminescence efficiency, the light extraction efficiency is a major design criterion for enhancing the external radiative efficiency and thus the V_oc. Since the semiconductor substrate is a sink for internally generated photoluminescence, it is equally important to eliminate the loss of emitted light into the substrate. Even at the S-Q limit, the V_oc is still substantially decreased by a photon entropy loss due to the conversion of a parallel beam of photons from the sun into an isotropic emission pattern, in which each individual photon is emitted into a random direction. The 46.7% ultimate solar cell limit for direct solar irradiation can only be approached, once the cell is capable to focus all emitted photoluminescence back to the sun. We will show that nanophotonic engineering provides a pathway to approach the ultimate limit.

@en

The emergence of two-dimensional transition metal dichalcogenide materials has sparked intense activity in valleytronics, as their valley information can be encoded and detected with the spin angular momentum of light. We demonstrate the valley-dependent directional coupling of light using a plasmonic nanowire-tungsten disulfide (WS₂) layers system. We show that the valley pseudospin in WS₂ couples to transverse optical spin of the same handedness with a directional coupling efficiency of 90 ± 1%. Our results provide a platform for controlling, detecting, and processing valley and spin information with precise optical control at the nanoscale.

@en

Charge carrier-selective contacts transform a light-absorbing semiconductor into a photovoltaic device. Current record efficiency solar cells nearly all use advanced heterojunction contacts that simultaneously provide carrier selectivity and contact passivation. One remaining challenge with heterojunction contacts is the tradeoff between better carrier selectivity/contact passivation (thicker layers) and better carrier extraction (thinner layers). Here we demonstrate that the nanowire geometry can remove this tradeoff by utilizing a permanent local gate (molybdenum oxide surface layer) to control the carrier selectivity of an adjacent ohmic metal contact. We show an open-circuit voltage increase for single indium phosphide nanowire solar cells by up to 335 mV, ultimately reaching 835 mV, and a reduction in open-circuit voltage spread from 303 to 105 mV after application of the surface gate. Importantly, reference experiments show that the carriers are not extracted via the molybdenum oxide but the ohmic metal contacts at the wire ends.@en

The chiral interaction between transverse optical spin and circularly polarized emitters provides a novel way to manipulate spin information at the nanoscale. Here, we demonstrate the valley(spin)-dependent directional emission of transition metal chalcogenides (TMDs) into plasmonic eigenstates of a silver nanowire. Due to the spin-path locking of the plasmonic eigenstates, the emission from the two different valleys of TMDs material will couple to the guided modes propagating in opposite directions. The high valley polarization of TMDs and high density of the transverse optical spin of the plasmonic wire together offer a novel platform for a chiral network even at room temperature without any magnetic fields.@en

Monocrystalline materials are essential for optoelectronic devices such as solar cells, LEDs, lasers, and transistors to reach the highest performance. Advances in synthetic chemistry now allow for high quality monocrystalline nanomaterials to be grown at low temperature in solution for many materials; however, the realization of extended structures with control over the final 3D geometry still remains elusive. Here, a new paradigm is presented, which relies on epitaxy between monocrystalline nanocube building blocks. The nanocubes are assembled in a predefined pattern and then epitaxially connected at the atomic level by chemical growth in solution, to form monocrystalline nanopatterns on arbitrary substrates. As a first demonstration, it is shown that monocrystalline silver structures obtained with such a process have optical properties and conductivity comparable to single-crystalline silver. This flexible multiscale process may ultimately enable the implementation of monocrystalline materials in optoelectronic devices, raising performance to the ultimate limit.

@en

Solar-assisted water splitting can potentially provide an efficient route for large-scale renewable energy conversion and storage. It is essential for such a system to provide a sufficiently high photocurrent and photovoltage to drive the water oxidation reaction. Here we demonstrate a photoanode that is capable of achieving a high photovoltage by engineering the interfacial energetics of metal-insulator-semiconductor junctions. We evaluate the importance of using two metals to decouple the functionalities for a Schottky contact and a highly efficient catalyst. We also illustrate the improvement of the photovoltage upon incidental oxidation of the metallic surface layer in KOH solution. Additionally, we analyse the role of the thin insulating layer to the pinning and depinning of Fermi level that is responsible to the resulting photovoltage. Finally, we report the advantage of using dual metal overlayers as a simple protection route for highly efficient metal-insulator-semiconductor photoanodes by showing over 200 h of operational stability.

@en

Approaching the theoretically limiting open circuit voltage (V_oc) of solar cells is crucial to optimize their photovoltaic performance. Here, we demonstrate experimentally that nanostructured layers can achieve a fundamentally larger Fermi level splitting, and thus a larger V_oc, than planar layers. By etching tapered nanowires from planar indium phosphide (InP), we directly compare planar and nanophotonic geometries with the exact same material quality. We show that the external radiative efficiency of the nanostructured layer at 1 sun is increased by a factor 14 compared to the planar layer, leading to a 70 mV enhancement in V_oc. The higher voltage arises from both the enhanced outcoupling of photons, which promotes radiative recombination, and the lower active material volume, which reduces bulk recombination. These effects are generic and promise to enhance the efficiency of current record planar solar cells made from other materials as well.

@en

Nanophotonic engineering shows great potential for photovoltaics: the record conversion efficiencies of nanowire solar cells are increasing rapidly and the record open-circuit voltages are becoming comparable to the records for planar equivalents. Furthermore, it has been suggested that certain nanophotonic effects can reduce costs and increase efficiencies with respect to planar solar cells. These effects are particularly pronounced in single-nanowire devices, where two out of the three dimensions are subwavelength. Single-nanowire devices thus provide an ideal platform to study how nanophotonics affects photovoltaics. However, for these devices the standard definition of power conversion efficiency no longer applies, because the nanowire can absorb light from an area much larger than its own size. Additionally, the thermodynamic limit on the photovoltage is unknown a priori and may be very different from that of a planar solar cell. This complicates the characterization and optimization of these devices. Here, we analyse an InP single-nanowire solar cell using intrinsic metrics to place its performance on an absolute thermodynamic scale and pinpoint performance loss mechanisms. To determine these metrics we have developed an integrating sphere microscopy set-up that enables simultaneous and spatially resolved quantitative absorption, internal quantum efficiency (IQE) and photoluminescence quantum yield (PLQY) measurements. For our record single-nanowire solar cell, we measure a photocurrent collection efficiency of >90% and an open-circuit voltage of 850mV, which is 73% of the thermodynamic limit (1.16V).@en