Rokas Jasiunas

Layered semiconductors are promising for new optoelectronic applications due to their unique optical and electronic properties. This study focuses on the synthesis of thin germanium monosulfide (GeS) films and the characterization of their structural and optoelectrical properties. We show that rapid thermal evaporation (RTE) enables effective synthesis of large-area polycrystalline GeS thin films on glass, fluorine-doped tin oxide and interdigitated array (IDA) electrode substrates. However, the one-step deposition process leads to uncontrolled, randomly oriented crystal growth. We have developed a two-step process that involves the initial deposition of an amorphous film at a temperature below 350 °C and subsequent annealing at 370 °C, ensuring complete GeS crystallization and the formation of high-quality polycrystalline GeS films with controlled thickness and layer orientation. Photoelectric characterization using current-voltage (JV) characteristics, transient photocurrent and time-delayed collection field (TDCF) measurements revealed that polycrystalline GeS is a photosensitive material with long carrier lifetimes but with rapidly decreasing mobility. GeS is potentially promising for optoelectrical applications. • A rapid thermal evaporation (RTE) method allows synthesizing large-area polycrystalline GeS films. • The two-step deposition process enhances GeS film crystallinity and orientation controll. • Light sensitivity and long carrier lifetimes show the potential of polycrystalline GeS films for optoelectronic applications.

Abstract In recent years, organic solar cells (OSCs) have shown high power efficiencies approaching 20%. However, the fundamental mechanisms of charge separation in these highly efficient devices have been a subject of intensive debates. Here, the charge separation efficiency (CSE) is extensively investigated across a wide range of blend systems with different energetic offsets. The findings unveil the temperature‐dependent nature of charge separation in low‐offset systems, emphasizing its significant contribution to the overall CSE. An intriguing inverse correlation between CSE and charge separation activation energy in relation to the offset is also observed. These results shed new light on the factors underlying the high CSE observed in the state‐of‐the‐art devices.

Transient absorption and time‐resolved fluorescence measurements in a wide temperature range are used to investigate the mechanism of charge carrier generation in efficient organic solar cells based on a PM6:Y6 donor–acceptor blend. The generation mechanisms differ significantly under excitation of a donor or acceptor. The investigations reveal a temperature‐dependent interplay between the formation of interfacial charge transfer (CT) states and intra‐moiety CT states of the acceptor, their separation into free charge carriers and carrier recombination. The efficient charge carrier generation is ensured by the carrier separation over a small energy barrier, which is easily surmountable at room temperature. However, the overall yield of charge carrier generation at room temperature is reduced by the recombination of charge carriers due to the thermally activated back transfer of electrons from the acceptor to the donor via the highest occupied molecular orbit (HOMO) levels, which is enabled by the small energy offset between HOMO levels of the donor and the acceptor.

Although organic photovoltaics has made significant progress since its appearance decades ago, the underlying physics of charge transport in working cells is still under debate. Carrier mobility, determining the carrier extraction and recombination, is one of the most important but complex and still poorly understood parameters. Low-energy charge carrier states acting as traps play a particularly important role in carrier transport. Occupation of these states under real operation conditions of solar cells induces additional complexity. In this study, we use several transient methods and numerical modeling to address carrier transport under actual working conditions of bulk heterojunction organic solar cells based on fullerene and nonfullerene acceptors. We show that occupation of low-energy states strongly depends on the blend materials and the effective electric field. We define conditions when such occupation increases carrier mobility, making it less time-dependent on the microsecond time scale, and when its influence is only marginal. We also show that the initial mobility, determined by carrier relaxation within the high-energy part of the distributed density of states, strongly decreases with time independently of the low-energy state population.

Abstract Understanding of charge trapping processes in halide perovskites is vital to further improve performance of perovskite optoelectronic devices such as solar cells, photodetectors, and LEDs. In this work, transient photocurrent, time‐delayed collection field and transient fluorescence techniques along with numerical simulations are combined to address charge carrier trapping processes during their lateral motion in prototypical methylammonium lead iodide perovskite films formed on interdigitated electrodes. Carrier mobility decreases on hundreds of ns timescale, and its rate depends on the motion character—it is faster when charge carriers drift in the electric field and slower when the motion is caused by diffusion only. This difference becomes particularly evident at low temperatures. Based on the time‐delayed collection field data and carrier motion modelling results, it is demonstrated that the rapid mobility decay at low temperatures is mainly caused by the energy barriers, most likely formed at crystallite boundaries. Even though these barriers are surmountable at room temperature, they still play a major role in determining carrier mobility and diffusion rates. Suggested concept of the potential barriers moves beyond the conventional understanding of carrier mobility, diffusion, and recombination processes in hybrid perovskites.

Non-fullerene organic solar cells (NFOSCs) demonstrate record efficiencies exceeding 16%. In comparison with cells with the fullerene-based acceptor, the NFOSCs benefit from a longer wavelength absorption, which leads to a small highest occupied molecular orbital (HOMO) level offset. Here, we use several advanced transient investigation techniques, covering timescale from sub-ps to μs, to address all sequence of processes starting from photoexcitation of donors or acceptors to carrier extraction in several NFOSCs and cells with phenyl-C71-butyric acid methyl ester (PCBM). Though small offsets result in higher open-circuit voltage, we show that at the same time, it limits cell performance because of inefficient hole transfer from excited acceptors to donors and enhanced geminate recombination. We demonstrate that 100 meV HOMO level offset and proper acceptor molecule structures are sufficient for efficient hole transfer (>70%) and for reduction of the geminate recombination losses down to about 20%. Subsequent extraction of unbound charge carriers in all NFOSCs is slightly faster than in cells with PCBM, while non-geminate carrier recombination causing additional losses is slightly slower in the best performing NFOSCs than in cells with PCBM.

Perovskite‐based solar cells currently are one of the most rapidly developing fields in solar photovoltaics. Chemical doping of perovskites with foreign atoms is a promising way to tailor material properties toward improving the performance and stability of solar cells. Herein, efficiency enhancement of planar MAPbI 3 perovskite solar cells by doping them with 0.1–5% Sr 2+ is discussed. A small amount (<1%) of Sr 2+ added to the perovskite improves the V oc by ≈80 mV and consequently increases the power conversion efficiency (PCE) from 16.8% to 17.8%. Using transient photoluminescence, transient photocurrent, and time‐delayed collection field measurements, it is demonstrated that Sr 2+ additives reduce the trap density and increase the perovskite photoluminescence lifetime. However, reaching ≈1% concentration, Sr 2+ additives create additional carrier traps, which cause fast photoluminescence quenching and slow carrier recombination.

Non-fullerene organic solar cells (NFOSCs) demonstrate record efficiencies exceeding 16%. In comparison with cells with the fullerene-based acceptor, the NFOSCs benefit from a longer wavelength absorption, which leads to a small highest occupied molecular orbital (HOMO) level offset. Here, we use several advanced transient investigation techniques, covering timescale from sub-ps to μs, to address all sequence of processes starting from photoexcitation of donors or acceptors to carrier extraction in several NFOSCs and cells with phenyl-C71-butyric acid methyl ester (PCBM). Though small offsets result in higher open-circuit voltage, we show that at the same time, it limits cell performance because of inefficient hole transfer from excited acceptors to donors and enhanced geminate recombination. We demonstrate that 100 meV HOMO level offset and proper acceptor molecule structures are sufficient for efficient hole transfer (>70%) and for reduction of the geminate recombination losses down to about 20%. Subsequent extraction of unbound charge carriers in all NFOSCs is slightly faster than in cells with PCBM, while non-geminate carrier recombination causing additional losses is slightly slower in the best performing NFOSCs than in cells with PCBM.

Abstract Recent years have witnessed considerable progress in the development of solar cells based on lead halide perovskite materials. However, their intrinsic instability remains a limitation. In this context, the interplay between the thermal degradation and the hydrophobicity of perovskite materials is investigated. To this end, the salt 1‐(4‐ethenylbenzyl)‐3‐(3,3,4,4,5,5,6,6,7,7,8,8,8‐tridecafluorooctylimidazolium iodide (ETI), is employed as an additive in hybrid perovskites, endowing the photoactive materials with high thermal stability and hydrophobicity. The ETI additive inhibits methylammonium (MA) permeation in methylammonium lead triiodide (MAPbI 3 ) occurring due to intrinsic thermal degradation, by inhibiting out‐diffusion of the MA + cation, preserving the pristine material and preventing decomposition. With this simple approach, high efficiency solar cells based on the unstable MAPbI 3 perovskite are markedly stabilized under maximum power point tracking, leading to greater than twice the preserved efficiency after 700 h of continuous light illumination and heating (60 °C). These results suggest a strategy to tackle the intrinsic thermal decomposition of MAI, an essential component in all state‐of‐the‐art perovskite compositions.

Abstract Extraction of photocreated charge carriers from a prototypical all‐polymer organic solar cell is investigated by combining transient photocurrent and time‐delayed collection field experiments with numerical simulations. It is found that extraction is significantly hampered by charges getting trapped in spatial traps that are tentatively attributed to dead ends in the intermixed polymer network—in photovoltaic devices based on the same donor polymer and a fullerene acceptor this effect is much weaker. The slow‐down in charge extraction leads to enhanced recombination and associated performance losses. These effects are observed in addition to the dispersive behavior that is characteristic of charge motion in energetically disordered media. Upon annealing the effects of spatial traps diminish, rationalizing the doubling in device power conversion efficiency after annealing.