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For directed development of solar cells using nanomaterials such as quantum dots, there is a need to understand the device function in detail. Understanding where photovoltage is generated in a device and where energy losses occur is a key aspect of this, and development of methods which can provide this information is needed. We have previously shown that time-resolved photoelectron spectroscopy of core levels can be used to follow the photovoltage dynamics at a specific interface of a lead sulfide quantum dot solar cell. Here, we use the method's selectivity and sample design to investigate the photovoltage generation in different parts of this solar cell and determine how the different layers (including the absorber layer thickness) contribute to charge separation. We show that all layers contribute to photovoltage generation and that a gold contact deposited on the quantum dots is necessary for full photovoltage generation and slow charge recombination. By combining the information obtained, we are able to experimentally follow the time evolution of the solar cell band structure during the charge separation process. Furthermore, we can identify which specific layers need to be optimized for an overall improvement of quantum dot cells. In the future, this methodology can be applied to other types of devices to provide insights into photovoltage generation mechanisms.

In this work, we study the interface obtained by depositing a monolayer of a Blatter radical derivative on polycrystalline cobalt. By examining the occupied and unoccupied states at the interface, using soft X-ray techniques, combined with electronic structure calculations, we could simultaneously determine the electronic structure of both the molecular and ferromagnetic sides of the interface, thus obtaining a full understanding of the interfacial magnetic properties. We found that the molecule is strongly hybridized with the surface. Changes in the core level spectra reflect the modification of the molecule and the cobalt electronic structures inducing a decrease in the magnetic moment of the cobalt atoms bonded to the molecules which, in turn, lose their radical character. Our method allowed us to screen, beforehand, organic/ferromagnetic interfaces given their potential applications in spintronics., (© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

The study of surface properties at the nanoscale plays a crucial role in material science applications. This paper demonstrates the capabilities of Auger PhotoElectron Coincidence Spectroscopy (APECS) to obtain data with varying surface sensitivities from a single measurement. This makes it possible to extract the spectrum from the outermost surface layer even when faced with strongly overlapping surface and bulk spectral features, which we demonstrate by accurately extracting the surface component in Au 4f photoemission. Leveraging high energy resolution, transmission efficiency, tunable photon energy, and remarkable surface sensitivity of the APECS setup, we propose that optimal experimental conditions can be tailored to determine surface spectra accurately for a diverse range of materials. This opens new avenues for advancing our understanding of nanoscale surface phenomena across various material systems.

The understanding of the interfacial properties in perovskite devices under irradiation is crucial for their engineering. In this study we show how the electronic structure of the interface between CsPbBr 3 perovskite nanocrystals (PNCs) and Au is affected by irradiation of X-rays, near-infrared (NIR), and ultraviolet (UV) light. The effects of X-ray and light exposure could be differentiated by employing low-dose X-ray photoelectron spectroscopy (XPS). Apart from the common degradation product of metallic lead (Pb 0 ), a new intermediate component (Pb int ) was identified in the Pb 4f XPS spectra after exposure to high intensity X-rays or UV light. The Pb int component is determined to be monolayer metallic Pb on-top of the Au substrate from underpotential deposition (UPD) of Pb induced from the breaking of the perovskite structure allowing for migration of Pb 2+ .

A limiting factor for solid polymer electrolyte (SPE)-based Li-batteries is the functionality of the electrolyte decomposition layer that is spontaneously formed at the Li metal anode. A deeper understanding of this layer will facilitate its improvement. This study investigates three SPEs - polyethylene oxide:lithium tetrafluoroborate (PEO:LiBF 4 ), polyethylene oxide:lithium bis(oxalate)borate (PEO:LiBOB), and polyethylene oxide:lithium difluoro(oxalato)borate (PEO:LiDFOB) - using a combination of electrochemical impedance spectroscopy (EIS), galvanostatic cycling, in situ Li deposition photoelectron spectroscopy (PES), and ab initio molecular dynamics (AIMD) simulations. Through this combination, the cell performance of PEO:LiDFOB can be connected to the initial SPE decomposition at the anode interface. It is found that PEO:LiDFOB had the highest capacity retention, which is correlated to having the least decomposition at the interface. This indicates that the lower SPE decomposition at the interface still creates a more effective decomposition layer, which is capable of preventing further electrolyte decomposition. Moreover, the PES results indicate formation of polyethylene in the SEI in cells based on PEO electrolytes. This is supported by AIMD that shows a polyethylene formation pathway through free-radical polymerization of ethylene., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Fermi surfaces are essential for predicting, characterizing and controlling the properties of crystalline metals and semiconductors. Angle-resolved photoemission spectroscopy (ARPES) is the only technique directly probing the Fermi surface by measuring the Fermi momenta (k F ) from energy- and angular distribution of photoelectrons dislodged by monochromatic light. Existing apparatus is able to determine a number of k F -vectors simultaneously, but direct high-resolution 3D Fermi surface mapping remains problematic. As a result, no such datasets exist, strongly limiting our knowledge about the Fermi surfaces. Here we show that using a simpler instrumentation it is possible to perform 3D-mapping within a very short time interval and with very high resolution. We present the first detailed experimental 3D Fermi surface as well as other experimental results featuring advantages of our technique. In combination with various light sources our methodology and instrumentation offer new opportunities for high-resolution ARPES in the physical and life sciences., (© 2022. The Author(s).)

Blatter radical derivatives are very attractive due to their potential applications, ranging from batteries to quantum technologies. In this work, we focus on the latest insights regarding the fundamental mechanisms of radical thin film (long-term) degradation, by comparing two Blatter radical derivatives. We find that the interaction with different contaminants (such as atomic H, Ar, N, and O and molecular H 2 , N 2 , O 2 , H 2 O, and NH 2 ) affects the chemical and magnetic properties of the thin films upon air exposure. Also, the radical-specific site, where the contaminant interaction takes place, plays a role. Atomic H and NH 2 are detrimental to the magnetic properties of Blatter radicals, while the presence of molecular water influences more specifically the magnetic properties of the diradical thin films, and it is believed to be the major cause of the shorter diradical thin film lifetime in air.

Electron spectroscopy with the unprecedented transmission of angle-resolved time-of-flight detection, in combination with pulsed X-ray sources, brings new impetus to functional materials science. We showcase recent developments towards chemical sensitivity from electron spectroscopy for chemical analysis and structural information from photoelectron diffraction using the phase transition properties of 1T-TaS 2 . Our development platform is the SurfaceDynamics instrument located at the Femtoslicing facility at BESSY II, where femtosecond and picosecond X-ray pulses can be generated and extracted. The scientific potential is put into perspective to the current rapidly developing pulsed X-ray source capabilities from Lasers and Free-Electron Lasers.

Hexacene, composed of six linearly fused benzene rings, is an organic semiconductor material with superior electronic properties. The fundamental understanding of the electronic and chemical properties is prerequisite to any possible application in devices. We investigate the orientation and interface properties of highly ordered hexacene monolayers on Ag(110) and Cu(110) with X-ray photoemission spectroscopy (XPS), photoemission orbital tomography (POT), X-ray absorption spectroscopy (XAS), low-energy electron diffraction (LEED), scanning tunneling microscopy (STM), and density functional theory (DFT). We find pronounced differences in the structural arrangement of the molecules and the electronic properties at the metal/organic interfaces for the two substrates. While on Cu(110) the molecules adsorb with their long molecular axis parallel to the high symmetry substrate direction, on Ag(110), hexacene adsorbs in an azimuthally slightly rotated geometry with respect to the metal rows of the substrate. In both cases, molecular planes are oriented parallel to the substrate. A pronounced charge transfer from both substrates to different molecular states affects the effective charge of different C atoms of the molecule. Through analysis of experimental and theoretical data, we found out that on Ag(110) the LUMO of the molecule is occupied through charge transfer from the metal, whereas on Cu(110) even the LUMO+1 receives a charge. Interface dipoles are determined to a large extent by the push-back effect, which are also found to differ significantly between 6A /Ag(110) and 6A /Cu(110)., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Organic bilayer systems and heterostructures are of enormous importance for optoelectronic devices. We study interface properties and the structural ordering of cobalt phthalocyanine (CoPc) on a highly ordered monolayer hexa-peri-hexabenzocoronene (HBC), grown on Au(111), using photoemission, X-ray absorption, scanning tunneling microscopy, and low-energy electron diffraction. A charge transfer between CoPc and the gold substrate is almost completely prevented by the HBC intermediate layer. We show that HBC acts as a template for the initial growth of CoPc molecules. After annealing to 630 K, a molecular exchange takes place, resulting in a coexistence of domains of both CoPc and HBC molecules on the surface.