Moritz Riede

Abstract:

<jats:title>Abstract</jats:title> <jats:p>Photovoltaics (PVs) are a critical technology for curbing growing levels of anthropogenic greenhouse gas emissions, and meeting increases in future demand for low-carbon electricity. In order to fulfil ambitions for net-zero carbon dioxide equivalent (CO<jats:sub>2</jats:sub>eq) emissions worldwide, the global cumulative capacity of solar PVs must increase by an order of magnitude from 0.9 TW<jats:sub>p</jats:sub> in 2021 to 8.5 TW<jats:sub>p</jats:sub> by 2050 according to the International Renewable Energy Agency, which is considered to be a highly conservative estimate. In 2020, the Henry Royce Institute brought together the UK PV community to discuss the critical technological and infrastructure challenges that need to be overcome to address the vast challenges in accelerating PV deployment. Herein, we examine the key developments in the global community, especially the progress made in the field since this earlier roadmap, bringing together experts primarily from the UK across the breadth of the photovoltaics community. The focus is both on the challenges in improving the efficiency, stability and levelized cost of electricity of current technologies for utility-scale PVs, as well as the fundamental questions in novel technologies that can have a significant impact on emerging markets, such as indoor PVs, space PVs, and agrivoltaics. We discuss challenges in advanced metrology and computational tools, as well as the growing synergies between PVs and solar fuels, and offer a perspective on the environmental sustainability of the PV industry. Through this roadmap, we emphasize promising pathways forward in both the short- and long-term, and for communities working on technologies across a range of maturity levels to learn from each other.</jats:p>

Abstract:

<jats:title>Abstract</jats:title><jats:p>Organic semiconductors still lag behind their inorganic counterparts in terms of mobility due to their lower structural order, in particular in thin films. Here, the highly ordered phase of triclinic rubrene – characterized by high vertical hole mobility – grown from a vacuum‐deposited thin film is used by post‐annealing and implemented into organic photodetectors. Since the triclinic rubrene exhibits a high roughness with a peak‐to‐valley value of 250 nm, which is detrimental to the dark current, strategies to control the crystal growth are developed. These investigations show that a suppression layer of 20 nm C<jats:sub>60</jats:sub> is the most promising approach to successfully reduce the surface roughness while maintaining the triclinic phase, proven by grazing‐incidence wide‐angle X‐ray scattering (GIWAXS). With the smoothened active layer, the dark current density is reduced by three orders of magnitude compared to the neat rubrene layer. It is as low as 2.5 × 10<jats:sup>−10 </jats:sup>A cm<jats:sup>−2</jats:sup> at −0.1 V bias, reflected in an overall specific detectivity of 6 × 10<jats:sup>11</jats:sup> Jones at zero bias (based on noise measurements) and a high linear dynamic range of 170 dB. This strategy using a suppression layer thus proves successful and is very promising to be applied to other crystalline materials.</jats:p>

Abstract:

Free charge generation after photoexcitation of donor or acceptor molecules in organic solar cells generally proceeds via (1) formation of charge transfer states and (2) their dissociation into charge separated states. Research often either focuses on the first component or the combined effect of both processes. Here, we provide evidence that charge transfer state dissociation rather than formation presents a major bottleneck for free charge generation in fullerene-based blends with low energetic offsets between singlet and charge transfer states. We investigate devices based on dilute donor content blends of (fluorinated) ZnPc:C60 and perform density functional theory calculations, device characterization, transient absorption spectroscopy and time-resolved electron paramagnetic resonance measurements. We draw a comprehensive picture of how energies and transitions between singlet, charge transfer, and charge separated states change upon ZnPc fluorination. We find that a significant reduction in photocurrent can be attributed to increasingly inefficient charge transfer state dissociation. With this, our work highlights potential reasons why low offset fullerene systems do not show the high performance of non-fullerene acceptors.

Abstract:

Carbon nanomaterials are expected to be bright and efficient emitters, but structural disorder, intermolecular interactions and the intrinsic presence of dark states suppress their photoluminescence. Here, we study synthetically-made graphene nanoribbons with atomically precise edges and which are designed to suppress intermolecular interactions to demonstrate strong photoluminescence in both solutions and thin films. The resulting high spectral resolution reveals strong vibron-electron coupling from the radial-breathing-like mode of the ribbons. In addition, their cove-edge structure produces inter-valley mixing, which brightens conventionally-dark states to generate hitherto-unrecognised twilight states as predicted by theory. The coupling of these states to the nanoribbon phonon modes affects absorption and emission differently, suggesting a complex interaction with both Herzberg–Teller and Franck– Condon coupling present. Detailed understanding of the fundamental electronic processes governing the optical response will help the tailored chemical design of nanocarbon optical devices, via gap tuning and side-chain functionalisation.

Abstract:

The ability to characterise perovskite phases non-destructively is key on the route to ensuring their long-term stability in operando. Raman spectroscopy holds the promise to play an important role in this task. Among all perovskites, formamidinium lead iodide (FAPbI3) has emerged as one of the most promising candidates for single-junction photovoltaic cells. However, Raman spectroscopy of FAPbI3 remains challenging as is evidenced by conflicting reports in the literature. Here, we demonstrate that due to the vulnerability of FAPbI3 to laser-induced degradation, the detected Raman spectrum depends strongly on the experimental conditions. This can lead to conflicting results and is revealed as the origin of discrepancies in the literature. We overcome this issue by deploying defocused Raman spectroscopy, preventing laser-induced damage to the sample and simultaneously improving the signal-to-noise ratio, allowing us to furthermore resolve much weaker Raman modes than was previously possible. We offer step-by-step instructions on how to apply this technique to a given spectrometer. Non-destructive characterisation of the FAPbI3 phases further enables us to quantify the phase stability of pristine FAPbI3 crystals and FAPbI3 grown with the high-performance additive methylenediammonium chloride (MDACl2). This shows that the neat crystals fully degrade within two weeks, whereas in samples grown with the additive only about 2% of the crystal bulk is in the δ-phase after 400 days. This establishes defocused Raman spectroscopy as a powerful tool for the characterisation of FAPbI3 and other perovskite materials.