arXiv subjects

Yana Vaynzof

Publications and source records attributed to Yana Vaynzof.

At least 19 recordsLinked to original sources

arXiv2026

Operando Charge Carrier Dynamics by Intensity-Modulated Photoluminescence: From Perovskite Thin Films to Solar Cells

The charge-carrier lifetime in halide perovskites often varies by orders of magnitude with the injection level, complicating the analysis of conventional time-resolved photoluminescence and comparisons of reported lifetimes. We use intensity-modulated photoluminescence spectroscopy (IMPLS) as a frequency-domain alternative. Carried out under operating conditions, it yields the lifetime at a specific injection level, e.g., one-sun-equivalent illumination. On thin films, IMPLS and steady-state photoluminescence yield comparable lifetimes. For perovskite/transport-layer stacks, the IMPLS response becomes more complex. A dedicated transfer function disentangles charge transfer from interface recombination and predicts an upper limit on the charge-carrier lifetime in the solar cell. In devices, electrical methods such as intensity-modulated photovoltage spectroscopy (IMVS) often fail to measure the lifetime due to capacitive effects. IMPLS shows not only the same two characteristic frequencies as IMVS, but also a third one, thereby resolving the lifetime itself.

cond-mat.mtrl-sci↗

arXiv2026

Mobility-lifetime relation links photodegradation in spin-coated and gravure-printed organic solar cells

The degradation mechanisms of organic solar cells (OSCs) have been studied primarily in spin-coated, laboratory-scale devices, whereas scalable processing modifies the device architecture, active-layer morphology, and underlying charge-transport and recombination properties. Whether these changes also alter how solar cells degrade remains unclear. Here, we compare spin-coated and fully roll-to-roll-compatible gravure-printed PM6:Y12 solar cells during $\sim$1000 h of continuous illumination. Despite distinct initial properties and degradation signatures, the loss of power-conversion efficiency systematically follows the mobility-lifetime product $μτ$. Remarkably, ageing of the printed devices increases the recombination lifetime while strongly reducing charge-carrier mobility, showing that a longer lifetime alone does not imply improved device performance. The mobility reduction is accompanied by decreased PM6 lamellar order, whereas the additional open-circuit voltage loss originates predominantly from increased non-radiative recombination. Dark recovery further reveals a metastable contribution specific to the printed architecture. These results identify the mobility-lifetime product as a unifying physical descriptor for photodegradation, linking ageing-induced microscopic changes to macroscopic performance loss across spin-coated and scalable printed OSCs.

cond-mat.mtrl-sci↗

arXiv2026

Pulse-Burst Excitation Reveals Time-Dose Reciprocity Breakdown in Mixed-Halide Perovskites

Time-dose reciprocity, commonly associated with the Bunsen-Roscoe law, states that the response of a photosensitive system depends only on the total exposure dose, regardless of how that energy is delivered over time. Light-sensitive processes in mixed-halide perovskites, such as photoinduced halide segregation, often exhibit threshold-like behavior that may violate this principle and enable material-state control by photon timing. We test this using pulse-burst excitation, which introduces an additional temporal control dimension beyond conventional parameters such as pulse fluence, repetition rate, and average power. By redistributing the same photon dose over microsecond-to-millisecond timescales, we create distinct nonequilibrium excitation conditions and show that mixed-halide perovskites can evolve into different metastable states, revealing a breakdown of time-dose reciprocity in the combined processes of halide segregation and remixing. This additional temporal degree of freedom not only enables control of the material state but also provides a new experimental framework for disentangling the competing processes underlying photoinduced halide redistribution. Our findings establish photon timing as a control parameter for perovskite photochemistry and open additional opportunities for optical memory and neuromorphic photonic applications.

cond-mat.mtrl-sci↗

arXiv2026

Unraveling the Roles of Shallow, Deep and Auger Trapping in Charge Carrier Recombination in Triple-Cation Perovskites

Understanding charge-carrier recombination in metal halide perovskites is essential for accurately identifying the factors limiting solar cell efficiency, yet it remains challenging due to the interplay of multiple competing processes. Here, we combine time-resolved photoluminescence and excitation dependent photoluminescence quantum yield measurements over a wide range of fluences and repetition rates to investigate recombination dynamics in triple-cation perovskite thin films. By jointly analyzing these multidimensional datasets, we develop a unified model that quantitatively reproduces both photoluminescence decays and absolute quantum yields across all excitation conditions. Our results reveal the coexistence of deep and shallow traps, as well as a second-order nonradiative recombination pathway attributed to Auger-assisted trapping. Importantly, this mechanism dominates under one-sun illumination, making it a critical limiting factor for photovoltaic performance. These findings provide a comprehensive framework for understanding recombination in perovskites and highlight the importance of higher-order defect-mediated processes in determining their efficiency.

cond-mat.mtrl-sci↗

arXiv2026

Additive-Induced Stabilization of the Energetic Landscape of PM6:Y12 Organic Solar Cells

Solvent additive engineering is a common strategy in organic photovoltaic (OPV) fabrication to improve film morphology and enhance device performance by controlling phase-separation kinetics and crystallinity. However, its effect on photostability, particularly with respect to the evolution of the energetic landscape under operational stress, remains unclear. This study investigates the impact of the additive 1-chloronaphthalene (1-CN) on the evolution of the device's energetic landscape in PM6:Y12 bulk heterojunction organic solar cells upon photoaging. Ultraviolet photoemission spectroscopy combined with argon gas cluster ion beam depth profiling is employed to probe the depth-resolved evolution of donor (PM6) and acceptor (Y12) energy levels before and after photodegradation. Our findings show that in additive-free devices, photodegradation leads to a significant 200 meV downward shift in the PM6 highest occupied molecular orbital (HOMO) level, reducing the donor-acceptor HOMO offset and impairing the driving force for hole transfer. As a consequence, the device experiences substantial efficiency loss. On the other hand, the incorporation of 1-CN effectively stabilizes the PM6 HOMO level, preserving adequate driving force for efficient exciton dissociation. Advanced X-ray diffraction characterization reveals more pronounced nanostructural degradation in blends without 1-CN than those with 1-CN upon photoaging. Collectively, these findings identify PM6 as the primary degradation pathway in PM6:Y12 blends and demonstrate that 1-CN enhances device stability by stabilizing PM6 energetics and preserving the nanostructural integrity upon photoaging.

cond-mat.mtrl-sci↗

arXiv2026

Rethinking Charge Transport and Recombination in Donor-diluted Organic Solar Cells

We systematically investigate PM6:Y12 bulk-heterojunction solar cells with donor fractions ranging from 1% to 45%, linking morphology, charge transport, and recombination to device performance. Complementary structural and spectroscopic methods reveal that a percolating PM6 network forms even at below 5% donor content, with lamellar stacking and vertical composition gradients that do not hinder the charge extraction. The reduction of the effective active layer conductivity towards low donor fractions obeys a three-dimensional percolation model, indicating that charge transport is governed by network topology rather without a pronounced percolation threshold. A transition from nongeminate Langevin recombination to a dispersive Smoluchowski-type loss occurs below 5% donor fraction. The latter regime is also nongeminate, i.e., pertains to recombination of the total charge carrier density. Correspondingly, we observe that the Langevin reduction in the higher donor fractions - mostly dominated by redissociation of electron-hole pairs after encounter - changes towards low donor fractions: in these cases, the nongeminate loss rate exceeds the prediction of the Langevin model. This regime coincides with increasing transport resistance due to topology-limited hole conduction, leading to reduced fill factors despite a high retained charge-generation efficiency. Our results demonstrate that strong donor dilution preserves photogeneration if a continuous donor network is maintained, and unveil how topology-controlled transport and non-Langevin recombination jointly define the performance limits of donor-diluted organic solar blends.

cond-mat.mtrl-sci↗

arXiv2026

Wide-angle emission in cylindrical moiré lattices enabled by rolling origami

Twisted photonic lattices that form moiré superlattices have attracted significant attention owing to their unique properties, such as strong field confinement and high-quality factors, in which the localized optical modes can serve as efficient light sources. However, in conventional moiré lattices, the emission direction of confined modes is typically fixed, and achieving a broad range of emission angles through simple modulation remains a significant challenge. Here, we design and fabricate single-layer moiré photonic lattices into cylindrical geometries using a nanomembrane origami technique. This approach enables wide-angle localized-mode emission while maintaining stable single-mode operation and excellent spectral uniformity. The moiré supercells support localized flat-band modes under various effective twist angles, resulting in the observation of periodic localized-mode emission over a wide range of azimuthal angles. Our research provides an approach for developing moiré light sources on curved surfaces, offering significant potential in applications that demand spatial light control, including three dimensional imaging, light detection and ranging, and topological states manipulation.

physics.optics↗

arXiv2025

Molecular Cross-linking of MXenes: Tunable Interfaces and Chemiresistive Sensing

MXenes, a family of 2D transition metal compounds, have emerged as promising materials due to their unique electronic properties and tunable surface chemistry. However, the translation of these nanoscale properties into macroscopic devices is constrained by suitable cross-linking strategies that enable both processability and controlled inter-flake charge transport. Herein, we demonstrate the tunability of interfaces and the inter-layer spacing between Ti$_3$C$_2$T$_x$ MXene flakes through molecular cross-linking with homologous diamines. Oleylamine was first used to stabilize MXenes in chloroform, followed by diamine-mediated cross-linking to tune precisely the interlayer spacing. Grazing incidence X-ray scattering (GIXRD/GIWAXS) confirmed the correlation between ligand chain length and inter-layer spacing, which was further supported by Density Functional Theory (DFT) calculations. Furthermore, we investigated the charge transport properties of thin films consisting of these diamine-crosslinked Ti$_3$C$_2$T$_x$ MXenes and observed a strong dependence of the conductivity on the interlayer spacing. The dominating charge transport mechanism is variable range hopping (VRH) in accordance with the structure analysis of the films. Finally, we probed chemiresistive vapor sensing in MXene composites, observing pronounced water sensitivity and selectivity, highlighting their potential for use in humidity sensors. Insights into molecular cross-linking and its impact on charge transport open avenues for next-generation MXene-based electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Exciton diffusion in two-dimensional chiral perovskites

Two-dimensional (2D) organic-inorganic hybrid perovskites emerged as a versatile platform for light-emitting and photovol-taic applications due to their unique structural design and chemical flexibility. Their properties depend heavily on both the choice of the inorganic lead halide framework and the surrounding organic layers. Recently, the introduction of chiral cations into 2D perovskites has attracted major interest due to their potential for introducing chirality and tuning the chiro-optical response. Importantly, the optical properties in these materials are dominated by tightly bound excitons that also serve as primary carriers for the energy transport. The mobility of photoinjected excitons is thus important from the perspectives of fundamental material properties and optoelectronic applications, yet remains an open question. Here, we demonstrate exciton propagation in a 2D chiral perovskite methylbenzylammonium lead iodide (MBA2PbI4) using transient photoluminescence microscopy and reveal density-dependent transport over more than 100 nanometers at room temperature with diffusion coeffi-cients as high as 2 cm2/s. We observe two distinct regimes of initially rapid diffusive propagation and subsequent localiza-tion. Moreover, perovskites with enantiomer pure cations are found to exhibit faster exciton diffusion compared to the race-mic mixture, correlated with the impact of the material composition on disorder. Altogether, the observations of efficient exciton diffusion at room temperature highlight the potential of 2D chiral perovskites to merge chiro-optical properties with strong light-matter interaction and efficient energy transport.

cond-mat.mtrl-sci↗

arXiv2024

Hidden photoexcitations probed by multi-pulse photoluminescence

Time-resolved photoluminescence is a validated method for tracking the photoexcited carrier dynamics in luminescent materials. This technique probes the photoluminescence decays upon a periodic excitation by short laser pulses. Herein, we demonstrate that this approach cannot directly detect hidden photoexcitations with much slower dynamics than the photoluminescence decay. We demonstrate a new method based on a multi-pulse excitation scheme that enables an unambiguous detection and an easily interpreted tracking of these hidden species. The multi-pulse excitation consists of a single pulse (Read) followed by a burst of many closely separated pulses (Write) and finally another single pulse (Read). To illustrate the efficacy of the Read-Write-Read excitation scheme, we apply it to metal halide perovskites to directly visualize carrier trapping, extract the concentration of trapped charges and determine the rate constant of trap depopulation. The developed approach allows studying performance-limiting processes in energy devices using a versatile, highly applicable all-optical method.

physics.optics↗

arXiv2024

Structural colors with embedded anti-counterfeit features fabricated by laser-based methods

Structural colors can be induced on metals not only to fabricate logos or decorative motives but also to embed anti-counterfeit features for product protection. In this study, stainless steel (EN 1.4301) plates are colorized by growing a thin oxide layer using direct laser writing (DLW) and hidden anti-counterfeit measures are included on their surfaces by direct laser interference patterning (DLIP) processing. The periodic microstructures resulting from the DLIP treatment have a spatial period of 1 um and act as relief diffraction gratings, featuring a characteristic diffraction pattern. These microstructures are not visible to the human eye but are easily detectable upon shining a coherent beam on the surface. Furthermore, the reflectance over the visible spectrum of the colorized surfaces with and without the DLIP microtexture is measured, giving low differences in the color perception following the so-called "CIE L*a*b*" color space. Finally, a demonstrator is fabricated, in which colorized fields with and without the security features are shown.

physics.optics↗

arXiv2024

Photophysics of defect-passivated quasi-2D (PEA)2PbBr4 perovskite using an organic small-molecule

2D Ruddlesden - Popper perovskites are promising candidates for energy harvesting applications due to their tunable optical properties and excellent ambient stability. Moreover, they are solution-processable and compatible with upscalable manufacturing via various printing techniques. Unfortunately, such methods often induce large degrees of heterogeneity due to poorly controlled crystallization. Here, we address this issue by blending the well-known 2D perovskite (PEA)2PbBr4 with an organic small-molecule, namely C8-BTBT, employed as an additive with different blending ratios. Using terahertz (THz) absorption and temperature-dependent photoluminescence (PL) spectroscopy techniques we observe that with the C8-BTBT additive the photophysical properties are altered while the perovskite structure in the film remains unaffected. More precisely, the inclusion of trace amounts of C8-BTBT in the hybrid films results in defect passivation at perovskite platelet boundaries and at the surfaces, as indicated by increased carrier lifetimes and substantially increased photoluminescence quantum yields (PLQY). This in turn improves the responsivity of photodetectors using the 2D perovskite as active layer. Our study highlights a straightforward strategy for fabricating high-quality 2D perovskites via large-area processing techniques.

cond-mat.mtrl-sci↗

arXiv2024

Intermolecular charge transfer enhances the performance of molecular rectifiers

Molecular-scale diodes made from self-assembled monolayers (SAMs) could complement silicon-based technologies with smaller, cheaper, and more versatile devices. However, advancement of this emerging technology is limited by insufficient electronic performance exhibited by the molecular current rectifiers. We overcome this barrier by exploiting the charge-transfer state that results from co-assembling SAMs of molecules with strong electron donor and acceptor termini. We obtain a substantial enhancement in current rectification, which correlates with the degree of charge transfer, as confirmed by several complementary techniques. These findings provide a previously unexplored method for manipulating the properties of molecular electronic devices by exploiting donor/acceptor interactions. They also serve as a model test platform for the study of doping mechanisms in organic systems. Our devices have the potential for fast widespread adoption due to their low-cost processing and self-assembly onto silicon substrates, which could allow seamless integration with current technologies.

cond-mat.mtrl-sci↗

arXiv2024

Perovskite Phase Heterojunction Solar Cells

Modern photovoltaic devices are often based on a heterojunction structure where two components with different optoelectronic properties are interfaced. The properties of each side of the junction can be tuned by either utilizing different materials (e.g. donor/acceptor) or doping (e.g. PN Si junction) or even varying their dimensionality (e.g. 3D/2D). In this work we demonstrate the concept of phase heterojunction (PHJ) solar cells by utilizing two polymorphs of the same material. We demonstrate the approach by forming $γ$-CsPbI3/$β$-CsPbI3 perovskite PHJ solar cells. We find that all of the photovoltaic parameters of the PHJ device significantly surpass those of each of the single-phase devices, resulting in a maximum power conversion efficiency of 20.1%. These improvements originate from the efficient passivation of the $β$-CsPbI3 by the larger bandgap $γ$-CsPbI3, the increase in the built-in potential of the PHJ devices enabled by the energetic alignment between the two phases and the enhanced absorption of light by the PHJ structure. The approach demonstrated here offers new possibilities for the development of photovoltaic devices based on polymorphic materials.

cond-mat.mtrl-sci↗

arXiv2024

Bis(stearoyl) Sulfide: A Stable, Odor-free Sulfur Precursor for High-Efficiency Metal Sulfide Quantum Dot Photovoltaics

The synthesis of metal sulfide nanocrystals is a crucial step in the fabrication of quantum dot (QD) photovoltaics. Control over the quantum dot size during synthesis allows for precise tuning of their optical and electronic properties, making them an appealing choice for electronic applications. This flexibility has led to the implementation of quantum dots in both highly-efficient single junction solar cells and other optoelectronic devices including photodetectors and transistors. Most commonly, metal sulfide quantum dots are synthesized using the hot-injection method utilizing toxic, and air- and moisture sensitive sulfur source: bis(trimethylsilyl) sulfide (TMS)2S. Here, we present bis(stearoyl) sulfide (St2S) as a new type of air-stable sulfur precursor for the synthesis of sulfide-based QDs, which yields uniform, pure, and stable nanocrystals. Photovoltaic devices based on these QDs are equally efficient as those fabricated by (TMS)2S but exhibit an enhanced operational stability. These results highlight that St2S can be widely adopted for the synthesis of metal sulfide quantum dots for a range of optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Remarkable performance recovery in highly defective perovskite solar cells by photo-oxidation

Exposure to environmental factors is generally expected to cause degradation in perovskite films and solar cells. Herein, we show that films with certain defect profiles can display the opposite effect, healing upon exposure to oxygen under illumination. We tune the iodine content of methylammonium lead triiodide perovskite from understoichiometric to overstoichiometric and expose them to oxygen and light prior to the addition of the top layers of the device, thereby examining the defect dependence of their photooxidative response in the absence of storage-related chemical processes. The contrast between the photovoltaic properties of the cells with different defects is stark. Understoichiometric samples indeed degrade, demonstrating performance at 33% of their untreated counterparts, while stoichiometric samples maintain their performance levels. Surprisingly, overstoichiometric samples, which show low current density and strong reverse hysteresis when untreated, heal to maximum performance levels (the same as untreated, stoichiometric samples) upon the photooxidative treatment. A similar, albeit smaller-scale, effect is observed for triple cation and methylammonium-free compositions, demonstrating the general application of this treatment to state-of-the-art compositions. We examine the reasons behind this response by a suite of characterization techniques, finding that the performance changes coincide with microstructural decay at the crystal surface, reorientation of the bulk crystal structure for the understoichiometric cells, and a decrease in the iodine-to-lead ratio of all films. These results indicate that defect engineering is a powerful tool to manipulate the stability of perovskite solar cells.

cond-mat.mtrl-sci↗

arXiv2024

Towards low-temperature processing of efficient $γ$-CsPbI$_3$ perovskite solar cells

Inorganic cesium lead iodide (CsPbI$_3$) perovskite solar cells (PSCs) have attracted enormous attention due to their excellent thermal stability and optical bandgap (~1.73 eV), well-suited for tandem device applications. However, achieving high-performing photovoltaic devices processed at low temperatures is still challenging. Here we reported a new method to fabricate high-efficiency and stable $γ$-CsPbI$_3$ PSCs at lower temperatures than was previously possible by introducing the long-chain organic cation salt ethane-1,2-diammonium iodide (EDAI2) and regulating the content of lead acetate (Pb(OAc)2) in the perovskite precursor solution. We find that EDAI2 acts as an intermediate that can promote the formation of $γ$-CsPbI$_3$, while excess Pb(OAc)2 can further stabilize the $γ$-phase of CsPbI$_3$ perovskite. Consequently, improved crystallinity and morphology and reduced carrier recombination are observed in the CsPbI$_3$ films fabricated by the new method. By optimizing the hole transport layer of CsPbI$_3$ inverted architecture solar cells, we demonstrate up to 16.6% efficiencies, surpassing previous reports examining $γ$-CsPbI$_3$ in inverted PSCs. Notably, the encapsulated solar cells maintain 97% of their initial efficiency at room temperature and dim light for 25 days, demonstrating the synergistic effect of EDAI2 and Pb(OAc)2 on stabilizing $γ$-CsPbI$_3$ PSCs.

cond-mat.mtrl-sci↗

arXiv2024

Solvent-antisolvent interactions in metal halide perovskites

The fabrication of metal halide perovskite films using the solvent-engineering method is increasingly common. In this method, the crystallisation of the perovskite layer is triggered by the application of an antisolvent during the spin-coating of a perovskite precursor solution. Herein, we introduce the current state of understanding of the processes involved in the crystallisation of perovskite layers formed by solvent engineering, focusing in particular on the role of antisolvent properties and solvent-antisolvent interactions. By considering the impact of the Hansen solubility parameters, we propose guidelines for selecting the appropriate antisolvent and outline open questions and future research directions for the fabrication of perovskite films by this method.

cond-mat.mtrl-sci↗