arXiv subjects

Caterina Ducati

Publications and source records attributed to Caterina Ducati.

11 recordsLinked to original sources

arXiv2026

Rapid Atmospheric Vapor Deposition of H:In2O3 Transparent Conducting Oxide Thin Films

Transparent conducting oxides (TCOs) are essential for the optoelectronics industry, but there is a critical gap in cost-effective methods to rapidly deposit low sheet resistance, high transmittance films without damaging delicate materials, including emerging soft semiconductors like metal-halide perovskites. In this work, atmospheric pressure chemical vapor deposition (AP-CVD) is used to synthesise H:In2O3 films with 7.20+/-0.01 Ohm/sq sheet resistance (0.50+/-0.06 mOhm.cm resistivity) and transmittance up to 89% in the near-infrared (NIR), surpassing commercial sputter-deposited indium tin oxide. The growth rate is 40x higher than atomic layer deposition (ALD), and the AP-CVD films are fully processed under atmospheric conditions at only 140 C. Comparison of secondary ion mass spectrometry and time-of-flight elastic recoil detection analysis with changes in carrier concentration indicate that H dopants are introduced from the water oxidant. There is an increase in mobility form 40+/-10 cm2/Vs to 160+/-30 cm2/Vs when changing from O2 to H2O as the oxidant, which is attributed to H dopants passivating oxygen vacancies that act as carrier scattering centers. This work establishes AP-CVD as a promising method for manufacturing high figure-of-merit TCOs in a rapid, scalable and cost-effective manner, using mild growth conditions compatible with thermally-sensitive materials.

cond-mat.mtrl-sci↗

arXiv2026

Controlling the growth of 2D conjugated coordination polymers to induce metallic and spin-dependent transport signatures

Understanding growth evolution and thereby implementing precise microstructural tuning of two-dimensional (2D) conjugated coordination polymers (cCPs) is crucial to achieve efficient electronic conduction towards their full potential and to observe materials' intrinsic properties. However, fundamental understanding of how 2D cCPs films grow remains very limited. Here, we use copper-benzenehexathiol (Cu-BHT) cCP as a model system to unravel the growth evolution of layered films in liquid-liquid interfacial synthesis in order to identify strategies to achieve tuning of structure-property relationships. We find that thin films formed at the early stage of growth in 20 minutes facilitate smoother, denser, and horizontally oriented films, and thereby achieve higher electrical conductivity of > 3000 S/cm with a metallic temperature dependence down to 20 K. They also reveal signatures of quantum interference mediated weak antilocalisation and Kondo-like effect in magnetotransport at low temperatures. These phenomena are not observed when long reaction time was employed. Our findings offer a new perspective for the growth of dynamically reversible self-assemblies, that is different from the traditional paradigm of longer reaction time being associated with higher ordering and performance, and offer a platform to study spin-related transport properties of these materials with higher performance for advanced electronic, thermoelectric, and potential spintronic applications.

cond-mat.mtrl-sci↗

arXiv2026

Boosting high-current alkaline water electrolysis and carbon dioxide reduction with novel CuNiFe-based anodes

The transition to a green hydrogen economy demands robust, scalable, and sustainable anodes for alkaline water electrolysis operating at industrial current densities (>1 A/cm2). However, achieving high activity and long-term stability under such conditions remains a formidable challenge with conventional catalysts. Here, we report a novel trimetallic CuNiFe anode fabricated through a rapid, single-step electrodeposition process at room temperature without organic additives. The catalyst exhibits an exceptionally low overpotential of <270 mV at 100 mA cm(-2) and operates stably for over 500 hours at 1 A cm(-2) in 30 wt% KOH. In a practical anion exchange membrane water electrolyzer (AEM-WE), the CuNiFe anode enables a current density of 2.5 A cm(-2) at only 2.5 V, with a voltage efficiency of 66.8%. Beyond water splitting, this anode also significantly enhances CO2 electrolysis, tripling the CO2 reduction current density and steering selectivity toward valuable multi-carbon products when paired with commercial copper cathodes. A cradle-to-gate life cycle assessment confirms that the CuNiFe anode reduces the carbon footprint by an order of magnitude and decreases environmental impacts by 40-60% across multiple categories compared to benchmark IrRuO2. Our work establishes a scalable, high-performance, and environmentally benign anode technology, paving the way for cost-effective electrochemical production of green hydrogen and carbon-neutral chemicals.

cond-mat.mtrl-sci↗

arXiv2024

Efficient short-wave infrared upconversion by self-sensitized holmium-doped nanoparticles

Photon upconversion, combining several low-energy photons to generate one high-energy photon is of wide interest for biomedical, catalytic and photonic applications. Lanthanide-doped nanoparticles (LnNP) are a unique type of upconversion nanoconverter, which can realize ultralarge anti-Stokes shift (>1000 nm) and high photostability, without photo-bleaching and photo-blinking. The excitation wavelength of LnNPs has been limited to the second near-infrared window (1000-1700 nm), mainly sensitized by erbium ions with absorption centered around 1.5 $μ$m. Here, we demonstrate novel self-sensitized holmium (Ho)-doped nanoconverters to further expand the sensitization range to the short-wave infrared at 2 $μ$m and achieve efficient upconversion to 640 nm. We show that this upconversion is a 4-photon conversion process with an underlying energy transfer upconversion mechanism. Via careful control of dopant concentration and shelling we achieve a relative upconversion-to-downconversion efficiency up to 15.2%, more than half the theoretical maximum. The placement of the Ho doped LnNPs into a plasmonic nanocavity device enables large gains in emission intensity (up to 32-fold), due to the dramatic shortening of the emission lifetime of Ho from 29 $μ$s to <1 ns, indicating a high Purcell-enhancement factor of 3x10$^4$. These results open new possibilities at the frontier of short-wave infrared upconversion and the nanoplasmonic enhancement of LnNP emission, with potential applications in detection, theranostics, photonics and optoelectronics.

physics.optics↗

arXiv2022

Reduced Recombination via Tunable Surface Fields in Perovskite Solar Cells

The ability to reduce energy loss at semiconductor surfaces through passivation or surface field engineering has become an essential step in the manufacturing of efficient photovoltaic (PV) and optoelectronic devices. Similarly, surface modification of emerging halide perovskites with quasi-2D heterostructures is now ubiquitous to achieve PV power conversion efficiencies (PCEs) > 22% and has enabled single-junction PV devices to reach 25.7%, yet a fundamental understanding to how these treatments function is still generally lacking. This has established a bottleneck for maximizing beneficial improvements as no concrete selection and design rules currently exist. Here we uncover a new type of tunable passivation strategy and mechanism found in perovskite PV devices that were the first to reach the > 25% PCE milestone, which is enabled by surface treating a bulk perovskite layer with hexylammonium bromide (HABr). We uncover the simultaneous formation of an iodide-rich 2D layer along with a Br halide gradient achieved through partial halide exchange that extends from defective surfaces and grain boundaries into the bulk layer. We demonstrate and directly visualize the tunability of both the 2D layer thickness, halide gradient, and band structure using a unique combination of depth-sensitive nanoscale characterization techniques. We show that the optimization of this interface can extend the charge carrier lifetime to values > 30 μs, which is the longest value reported for a direct bandgap semiconductor (GaAs, InP, CdTe) over the past 50 years. Importantly, this work reveals an entirely new strategy and knob for optimizing and tuning recombination and charge transport at semiconductor interfaces and will likely establish new frontiers in achieving the next set of perovskite device performance records.

physics.app-ph↗

arXiv2022

Unveiling the interaction mechanisms of electron and X-ray radiation with halide perovskite semiconductors using scanning nano-probe diffraction

The interaction of high-energy electrons and X-ray photons with soft semiconductors such as halide perovskites is essential for the characterisation and understanding of these optoelectronic materials. Using nano-probe diffraction techniques, which can investigate physical properties on the nanoscale, we perform studies of the interaction of electron and X-ray radiation with state-of-the-art (FA$_{0.79}$MA$_{0.16}$Cs$_{0.05}$)Pb(I$_{0.83}$Br$_{0.17}$)$_3$ hybrid halide perovskite films (FA, formamidinium; MA, methylammonium). We track the changes in the local crystal structure as a function of fluence using scanning electron diffraction and synchrotron nano X-ray diffraction techniques. We identify perovskite grains from which additional reflections, corresponding to PbBr$_2$, appear as a crystalline degradation phase after fluences of ~200 e$^-$Å$^{-2}$. These changes are concomitant with the formation of small PbI$_2$ crystallites at the adjacent high-angle grain boundaries, with the formation of pinholes, and with a phase transition from tetragonal to cubic. A similar degradation pathway is caused by photon irradiation in nano-X-ray diffraction, suggesting common underlying mechanisms. Our approach explores the radiation limits of these materials and provides a description of the degradation pathways on the nanoscale. Addressing high-angle grain boundaries will be critical for the further improvement of halide polycrystalline film stability, especially for applications vulnerable to high-energy radiation such as space photovoltaics.

cond-mat.mtrl-sci↗

arXiv2020

Sequentially Deposited versus Conventional Nonfullerene Organic Solar Cells: Interfacial Trap States, Vertical Stratification, and Exciton Dissociation

Bulk-heterojunction (BHJ) non-fullerene organic solar cells prepared from sequentially deposited donor and acceptor layers (sq-BHJ) have recently been promising to be highly efficient, environmentally friendly, and compatible with large area and roll-to-toll fabrication. However, the related photophysics at donor-acceptor interface and the vertical heterogeneity of donor-acceptor distribution, critical for exciton dissociation and device performance, are largely unexplored. Herein, steady-state and time-resolved optical and electrical techniques are employed to characterize the interfacial trap states. Correlation with the luminescent efficiency of interfacial states and its non-radiative recombination, interfacial trap states are characterized to be about 50% more populated in the sq-BHJ than as-cast BHJ (c-BHJ), which probably limits the device voltage output. Cross-sectional energy-dispersive X-ray spectroscopy and ultraviolet photoemission spectroscopy depth profiling directly vizualize the donor-acceptor vertical stratification with a precision of 1-2 nm. From the proposed "needle" model, the high exciton dissociation efficiency is rationalized. Our study highlights the promise of sequential deposition to fabricate efficient solar cells, and points towards improving the voltage output and overall device performance via eliminating interfacial trap states.

physics.app-ph↗

arXiv2018

Inducing transparency in the films of highly scattering particles

Today colloids are employed in various products from creams and coatings to electronics. The ability to control their chemical, optical, or electronic features by controlling their size and shape explains why these materials are so widely employed. Nevertheless, altering some of these properties may also lead to some undesired side effects, one of which is an increase in optical scattering upon concentration. Here, we address this strong scattering issue in films made of colloids with high surface roughness. We focus on raspberry type polymeric particles made of a spherical polystyrene core decorated by small hemispherical domains of acrylate. Owing to their surface charge and model roughness, aqueous dispersions of these particles display an unusual stability against aggregation. Under certain angles, their solid films display a brilliant red color due to Bragg scattering but otherwise appear completely white on account of`strong scattering. To suppress the scattering and induce transparency, we prepared films by hybridizing them either with oppositely-charged PS-particles that fit the length-scale of the raspberry roughness or with quantum dots. We report that the smaller PS-particles prevent raspberry particle aggregation in solid films and suppress scattering by decreasing the spatial variation of the refractive index. We believe that the results presented here provide a simple strategy to suppress strong scattering of rough particles and allow for their utilization in optical coatings, cosmetics, or photonics.

physics.app-ph↗

arXiv2017

Maximising and Stabilising Luminescence in Metal Halide Perovskite Device Structures

Metal halide perovskites are attracting tremendous interest for a variety of optoelectronic applications. The ability to tune the perovskite bandgap by tweaking the chemical compositions opens up new applications as coloured emitters and as components of tandem photovoltaics. Nevertheless, non-radiative losses are still limiting performance, with luminescence yields in state-of-the-art perovskite solar cells still far from 100% under solar illumination conditions. Furthermore, in mixed halide perovskite systems designed for continuous bandgap tunability (bandgaps ~1.7-1.9 eV), photo-induced ion segregation leads to bandgap instabilities. Here, we substantially mitigate both non-radiative losses and photo-induced ion migration in perovskite structures by decorating the surfaces and grain boundaries with passivating potassium-halide interlayers. We demonstrate external photo-luminescence quantum yields of 66%, translating to internal yields exceeding 95%. The high luminescence yields are achieved while maintaining high mobilities over 40 cm2V-1s-1, giving the elusive combination of both high luminescence and excellent charge transport. We find that the external luminescence yield when interfaced with electrodes in a solar cell device stack, a quantity that must be maximized to approach the efficiency limits, remains as high as 15%, indicating very clean interfaces. We also demonstrate the inhibition of photo-induced ion migration processes across a wide range of mixed halide perovskite bandgaps that otherwise show bandgap instabilities. We validate these results in full operating solar cells, highlighting the importance of stabilising luminescence in device structures. Our work represents a critical breakthrough in the construction of tunable halide perovskite films and interfaces that can approach the efficiency limits in tandem solar cells and coloured LEDs.

cond-mat.mtrl-sci↗

arXiv2016

Signature of magnetic-dependent gapless odd frequency states at superconductor/ferromagnet interfaces

The theory of superconductivity developed by Bardeen, Cooper and Schrieffer (BCS) explains the stabilization of electron pairs into a spin-singlet, even frequency, state by the formation of an energy gap within which the density of states is zero. At a superconductor interface with an inhomogeneous ferromagnet, a gapless odd frequency superconducting state is predicted, in which the Cooper pairs are in a spin-triplet state. Although indirect evidence for such a state has been obtained, the gap structure and pairing symmetry have not so far been determined. Here we report scanning tunnelling spectroscopy of Nb superconducting films proximity coupled to epitaxial Ho. These measurements reveal pronounced changes to the Nb subgap superconducting density of states on driving the Ho through a metamagnetic transition from a helical antiferromagnetic to a homogeneous ferromagnetic state for which a BCS-like gap is recovered. The results prove odd frequency spin-triplet superconductivity at superconductor/inhomogeneous magnet interfaces.

cond-mat.supr-con↗

arXiv2015

Controlling Multipolar Surface Plasmon Excitation through the Azimuthal Phase Structure of Electron Vortex Beams

We have theoretically studied how the azimuthal phase structure of an electron vortex beam excites surface plasmons on metal particles of different geometries as observed in electron energy loss spectroscopy. To do so, we have developed a semi-classical approximation combining an azimuthal phase factor and the dielectric formalism. Our results indicate that the vortex beam order may be used to modify and control surface plasmon multipole excitation in nanoparticles. In favorable cases, specific plasmon modes can even attain enhancement factor of several orders of magnitude. Since, electron vortex beams interact with particles mostly through interference effects due to azimuthal symmetries, i.e. in the plane perpendicular to the electron beam, anisotropy information (longitudinal and transversal) of the sample can be derived in EELS studies by comparing non-vortex and vortex beam measurements.

cond-mat.mtrl-sci↗