arXiv subjects

Aldo Di Carlo

Publications and source records attributed to Aldo Di Carlo.

At least 19 recordsLinked to original sources

arXiv2026

Analysis of degradation in perovskite solar cells through physics-based machine learning

Degradation in lead halide perovskite solar cells is analysed by inverse modelling of published measurements of characteristics of a single solar cell at ages 0, 90, 280, 480 minutes. We employ machine learning to deduce distributions of material parameter values and hence the physics linked to measured changes. Bayesian parameter estimation is coupled with drift diffusion simulations using the IonMonger code combined with an optical model. We accurately replicated measured changes in device performance with age through variations in model input parameters. Our key result is that degradation is influenced by correlated changes in the concentrations and diffusion coefficients of mobile ions and by interface recombination at large mobile ion concentrations. This study demonstrates the power of machine learning combined with simulations to reliably interpret experimental results, a task which is problematic if using simulation models with only manual exploration of the input parameter space.

physics.comp-ph↗

arXiv2026

Quantifying Perovskite Solar Cell Degradation via Machine Learning from Spatially Resolved Multimodal Luminescence Time Series

Perovskite solar cells achieve remarkable power conversion efficiencies, yet operational stability remains a major barrier to large-scale deployment. Reliable and rapid assessment of device state of health is therefore essential. Conventional electrical diagnostics, such as illuminated current-voltage (J--V) sweeps, provide accurate performance metrics but are time-consuming and do not resolve spatially localized degradation, motivating non-invasive imaging-based alternatives. A deep-learning framework is introduced to estimate PSC efficiency retention, $R_\mathrm{PCE}=\mathrm{PCE}_t/\mathrm{PCE}_0$, directly from multimodal luminescence imaging acquired during device aging. Each sample combines electroluminescence (EL), open-circuit photoluminescence (PLoc), and short-circuit photoluminescence (PLsc) at an aged state with device-specific reference images at $t=0$, enabling learning of degradation-relevant spatial changes. LumPerNet, a compact convolutional neural network, is benchmarked against a spatially homogenized control in which each luminescence channel is replaced by its spatial average while retaining the same learning framework and leakage-aware protocol. The comparison indicates that global luminescence evolution contains most of the predictive signal, while spatial information provides a secondary contribution to robustness. These results establish spatially resolved luminescence imaging as a practical route for accelerated stability testing and non-invasive degradation monitoring in perovskite photovoltaics.

cond-mat.mtrl-sci↗

arXiv2026

A green solvent screening tool for emerging materials via uncertainty aware, transformer enhanced transfer learning

Accurate prediction of solubility remains a central challenge across materials science and sustainable chemistry. In particular due to emerging technologies like organic and hybrid photovoltaics, batteries, and catalysis, solvent usage is expected to increase significantly within the coming years. Therefore, substituting solvents with greener alternatives is vital. This is where machine learning can have substantial impact. However, the limited data on critical parameters of solubility significantly constraints machine learning efficacy. In this work, we transfer a pre-trained foundational model on QM9 targets to our application with minimal data requirements. Additionally, the pipeline integrates uncertainty quantification, allowing the user to gauge the confidence of the predictions. As baseline, we succeed in predicting the Hansen solubility parameters and Dielectric Constant for which extensive databases exist. Importantly, we achieve high model performance on additional targets, such as Gutmann Donor and Acceptor numbers, where the available data is extremely limited. Overall, we augment data on solubility descriptors by orders of magnitude with high quality predictions. For effective dissemination, we deploy easy-to-use, easily integrateable with high throughput labs, customizable tool for ranking and screening possible solvent substitutes. Finally, we rediscovered known green solvent alternatives and proposed new candidates proving its relevance for finding eco-friendly solvents.

cs.LG↗

arXiv2025

Cracking in polymer substrates for flexible devices and its mitigation

Mechanical reliability plays an outsized role in determining the durability of flexible electronic devices because of the significant mechanical stresses they can experience during manufacturing and operation. These devices are typically built on sheets comprising stiff thin-film electrodes on compliant polymer substrates, and it is generally assumed that the high-toughness substrates do not crack easily. Contrary to this widespread assumption, here we reveal severe, pervasive, and extensive cracking in the polymer substrates during bending of electrode/substrate sheets, which compromises the overall mechanical integrity of the entire device. The substrate-cracking phenomenon appears to be general, and it is driven by the amplified stress intensity factor caused by the elastic mismatch at the film/substrate interface. To mitigate this substrate cracking, an interlayer-engineering approach is designed and experimentally demonstrated. This approach is generic, and it is potentially applicable to myriad flexible electronic devices that utilize stiff films on compliant substrates, for improving their durability and reliability.

cond-mat.mtrl-sci↗

arXiv2024

Breaking 1.7V open circuit voltage in large area transparent perovskite solar cells using bulk and interfaces passivation

Efficient semi-transparent solar cells can trigger the adoption of building integrated photovoltaics. Halide perovskites are particularly suitable in this respect owing to their tunable bandgap. Main drawbacks in the development of transparent perovskite solar cells are the high Voc deficit and the difficulties in depositing thin films over large area substrates, given the low solubility of bromide and chloride precursors. In this work, we develop a 2D and passivation strategies for the high band-gap Br perovskite able to reduce charge recombination and consequently improving the open-circuit voltage. We demonstrate 1cm 2 perovskite solar cells with Voc up to 1.73 V (1.83 eV QFLS) and a PCE of 8.2%. The AVT exceeds 70% by means of a bifacial light management and a record light utilization efficiency of 5.72 is achieved, setting a new standard for transparent photovoltaics. Moreover, we show the high ceiling of our technology towards IoT application due to a bifaciality factor of 87% along with 17% PCE under indoor lighting. Finally, the up-scaling has been demonstrated fabricating 20cm 2 -active area modules with PCE of 7.3% and Voc per cell up to 1.65V.

physics.app-ph↗

arXiv2023

Single-step Chemical Vapor Deposition of Methyl Ammonium Lead Halide Perovskite for p-i-n Solar Cells

Metal halide perovskite solar cells being one of the fastest emerging technologies for renewable energy still has to become more industry friendly in a way that will allow using it for thin film modules or tandems with conventional silicon devices. The simplest way to achieve this is to use chemical vapor deposition (CVD) technique for tandem production. In this work, we show a method for a single step production of MAPbI3 films in a simple two-zone CVD reactor from lead diacetate and methyl-ammonium iodide powders. Obtained films show highly ordered cubic MAPbI3 phase with a thickness of 400-500 um, good photoluminescence response and absorption band edge similar to spin-coated film. We used those films to produce p-i-n solar cells with ITO/NiO/MAPbI3/C60/Cu structure. The best cell showed negligible 0.23 % PCE right after the manufacturing but significantly improved to 5.5 % PCE after 8 hours of storage in the dark. The main limiting factor affecting the efficiency is low current density, which we attribute to non-optimized growth conditions; however, our approach is a first step to a single step CVD deposition of MAPbI3 on any type of substrates including texturized silicon subcells for better overall efficiency.

cond-mat.mtrl-sci↗

arXiv2023

Photo Stabilization of p-i-n Perovskite Solar Cells with Bathocuproine: MXene

Interface engineering is one of the promising strategies for the long-term stabilization of perovskite solar cells, preventing chemical decomposition induced by external agents and promoting fast charge transfer. Recently, MXenes-2D structured transition metal carbides and nitrides with various functionalization (=O,-F,-OH) demonstrated high potential for mastering the work function in halide perovskite absorbers and significantly improved the n-type charge collection in solar cells. This work demonstrates that MXenes allow for efficient stabilization of perovskite solar cells besides improving their performances. We introduce a new mixed composite bathocuproine:MXene, i.e., (BCP:MXene) interlayer at the interface between an electron-transport layer (ETL) and a metal cathode in the p-in device structure. Our investigation demonstrates that the use of BCP:MXene interlayer slightly increases the power conversation efficiency (PCE) for PSCs (from 16.5 for reference to 17.5%) but dramatically improves the out of Glove-Box stability. Under ISOS-L-2 light soaking stress at 63$\pm$ 1.5{\textdegree}C, The T80 (time needed to reduce efficiency down to 80% of the initial one) period increased from 460 h to > 2300 h.

cond-mat.mtrl-sci↗

arXiv2023

Practical development of efficient thermoelectric-photovoltaic hybrid systems based on wide-gap solar cells

The decrease of solar cell efficiency with temperature is a known problem for photovoltaics (PV). Temperature sensitivity can lead to a considerable amount of energy losses over the lifetime of solar panels. In this perspective Hybrid Thermoelectric-Photovoltaic (HTEPV) systems, which recover solar cell heat losses to produce an additional power output, can be a suitable option. However only hybridization of wide-gap solar cells is convenient in terms of efficiency gains and deserves investigation to evaluate HTEPV devices effectiveness. In this work we report the modeling and the development of customized bismuth telluride thermoelectric generators, optimized to be hybridized with amorphous silicon (aSi), Gallium Indium Phosphide (GaInP) or Perovskites solar cells. The model results showed in all three cases efficiency gains with a maximum of +3.1% for Perovskites (from 16.4% to 19.5%). These enhancements were then experimentally validated for the case of Perovskites solar cells, for which maximum gains were found to occur at typical operating temperatures of conventional PVs. This experimental evaluation demonstrated in an accurate fashion the real potential of thermoelectric hybridization of solar cells.

physics.app-ph↗

arXiv2023

Phase transition at 350 K in the Ti$_3$C$_2$T$_x$ MXene: possible sliding (moiré) ferroelectricity

A phase transition is found in Ti$_3$C$_2$T$_x$ MXene at 350 K, by measuring the complex Young's modulus of self-standing thick films. A step-like softening and increase of the mechanical losses is found below 350 K, indicative of a phase transition, where the square of the order parameter is coupled to strain. It is argued that it should be a ferroelectric transition, most likely of the sliding (moiré) type, due to charge transfer between facing flakes sliding with respect to each other. If the transition will be confirmed to be ferroelectric, Ti$_3$C$_2$T$_x$ will be added to the class of metallic ferroelectrics and open new perspectives of applications, in addition to the numerous already studied.

cond-mat.mtrl-sci↗

arXiv2023

Matching the photocurrent of perovskite/organic tandem solar modules by varying the cell width

Photocurrent matching in conventional monolithic tandem solar cells is achieved by choosing semiconductors with complementary absorption spectra and by carefully adjusting the optical properties of the complete top and bottom stacks. However, for thin film photovoltaic technologies at the module level, another design variable significantly alleviates the task of photocurrent matching, namely the cell width, whose modification can be readily realized by the adjustment of the module layout. Herein we demonstrate this concept at the experimental level for the first time for a 2T-mechanically stacked perovskite (FAPbBr3)/organic (PM6:Y6:PCBM) tandem mini-module, an unprecedented approach for these emergent photovoltaic technologies fabricated in an independent manner. An excellent Isc matching is achieved by tuning the cell widths of the perovskite and organic modules to 7.22 mm (PCEPVKT-mod= 6.69%) and 3.19 mm (PCEOPV-mod= 12.46%), respectively, leading to a champion efficiency of 14.94% for the tandem module interconnected in series with an aperture area of 20.25 cm2. Rather than demonstrating high efficiencies at the level of small lab cells, our successful experimental proof-of-concept at the module level proves to be particularly useful to couple devices with non-complementary semiconductors, either in series or in parallel electrical connection, hence overcoming the limitations imposed by the monolithic structure.

cond-mat.mtrl-sci↗

arXiv2023

Dielectric properties and plasmon modes of gapped momentum systems of different dimensionality

The concept of the energy gap is a fundamental characteristic of the band structure of a material and it determines its physical properties. Formally the energy gap appears in the dispersion relation $E_k$, where the vector $k$ is determined on the whole momentum space. However, today the {\it gapped momentum materials} are in the focus of research in which the so-called {\it momentum or $k$-gap} can emerge, i.e. some lacunae of momentum space are excluded from the domain of the function $E_k$. One of such examples present the non-Hermitian systems. Within the random phase approximation we study the dielectric properties of the momentum gapped materials in one, two and three dimensions for both cases of zero and finite temperatures. We find the corresponding plasmon modes and determine the unusual behavior of the appropriate dispersion relations for each dimensionality. Based on these findings we evaluate the absorption coefficient of gapped momentum media and provide some numerical estimations of its value for the practical applications.

cond-mat.str-el↗

arXiv2022

Giant and tunable excitonic optical anisotropy in single-crystal CsPbX$_3$ halide perovskites

During the last years, giant optical anisotropy demonstrated its paramount importance for light manipulation which resulted in numerous applications ranging from subdiffraction light guiding to switchable nanolasers. In spite of recent advances in the field, achieving continuous tunability of optical anisotropy remains an outstanding challenge. Here, we present a solution to the problem through chemical alteration of the ratio of halogen atoms (X = Br or Cl) in single-crystal CsPbX$_3$ halide perovskites. It turns out that the anisotropy originates from an excitonic resonance in the perovskite, which spectral position and strength are determined by the halogens composition. As a result, we manage to continually modify the optical anisotropy by 0.14. We also discover that the halide perovskite can demonstrate optical anisotropy up to 0.6 in the visible range -- the largest value among non-van der Waals materials. Moreover, our results reveal that this anisotropy could be in-plane and out-of-plane, depending on perovskite shape -- rectangular and square. Hence, it can serve as an additional degree of freedom for anisotropy manipulation. As a practical demonstration, we created perovskite anisotropic nanowaveguides and show a significant impact of anisotropy on high-order guiding modes. These findings pave the way for halide perovskites as a next-generation platform for tunable anisotropic photonics.

physics.app-ph↗

arXiv2021

Solution-processed two-dimensional materials for next-generation photovoltaics

In the ever-increasing energy demand scenario, the development of novel photovoltaic (PV) technologies is considered to be one of the key solutions to fulfil the energy request. In this context, graphene and related two-dimensional (2D) materials (GRMs), including nonlayered 2D materials and 2D perovskites, as well as their hybrid systems, are emerging as promising candidates to drive innovation in PV technologies. The mechanical, thermal, and optoelectronic properties of GRMs can be exploited in different active components of solar cells to design next-generation devices. These components include front (transparent) and back conductive electrodes, charge transporting layers, and interconnecting-recombination layers, as well as photoactive layers. The production and processing of GRMs in the liquid phase, coupled with the ability to on-demand tune their optoelectronic properties exploiting wet-chemical functionalization, enable their effective integration in advanced PV devices through scalable, reliable, and inexpensive printing-coating processes. Herein, we review the progresses in the use of solution-processed 2D materials in organic solar cells, dye-sensitized solar cells, perovskite solar cells, quantum dot solar cells, and organic-inorganic hybrid solar cells, as well as in tandem systems. We first provide a brief introduction on the properties of 2D materials and their production methods by solution-processing routes. Then, we discuss the functionality of 2D materials for electrodes, photoactive layer components-additives, charge transporting layers, and interconnecting layers through figures of merit, which allow the performance of solar cells to be determined and compared with the state-of-the-art values. We finally outline the roadmap for the further exploitation of solution-processed 2D materials to boost the performance of PV devices.

physics.app-ph↗

arXiv2020

Photoluminescence of MAPbI$_3$: a semiconductor science and technology point of view

In this work, we perform steady-state continuous wave (cw) photoluminescence (PL) measurements on a MAPbI$_3$ thin film in the temperature range of 10-160 K, using excitation densities spanning over almost seven orders of magnitude, in particular investigating very low densities, rarely used in the published literature. The temperature range used in this study is below or at the edge of the orthorhombic-tetragonal phase transition in MAPbI$_3$. In particular, we show that even in high quality MAPbI$_3$, capable of providing high photovoltaic efficiency, the defect density is high enough to give rise to an energy level band. Furthermore, we show that the intensity ratio between the two PL components related to the two crystalline phases, is a function of temperature and excitation. At high excitation intensities, we show that amplified spontaneous emission is attainable even in cw conditions. Time-resolved PL is also performed to justify some assignments of the PL features. Finally, our systematic approach, typical for the characterization of semiconductors, suggests that it should also be applied to hybrid halide perovskites and that, under suitable conditions, the PL characteristics of MAPbI$_3$ can be reconciled with those of conventional inorganic semiconductors.

physics.app-ph↗

arXiv2019

CVD-graphene/graphene flakes dual-films as advanced DSSC counter electrodes

The use of graphene-based electrodes is burgeoning in a wide range of applications, including solar cells, light emitting diodes, touch screens, field-effect transistors, photodetectors, sensors and energy storage systems. The success of such electrodes strongly depends on the implementation of effective production and processing methods for graphene. In this work, we take advantage of two different graphene production methods to design an advanced, conductive oxide- and platinum-free, graphene-based counter electrode for dye-sensitized solar cells (DSSCs). In particular, we exploit the combination of a graphene film, produced by chemical vapor deposition (CVD) (CVD-graphene), with few-layer graphene (FLG) flakes, produced by liquid phase exfoliation. The CVD-graphene is used as charge collector, while the FLG flakes, deposited atop by spray coating, act as catalyst for the reduction of the electrolyte redox couple (i.e., I3-/I-- and Co+2/+3). The as-produced counter electrodes are tested in both I3-/I-- and Co+2/+3-based semitransparent DSSCs, showing power conversion efficiencies of 2.1% and 5.09%, respectively, under 1 SUN illumination. At 0.1 SUN, Co+2/+3-based DSSCs achieve a power conversion efficiency as high as 6.87%. Our results demonstrate that the electrical, optical, chemical and catalytic properties of graphene-based dual films, designed by combining CVD-graphene and FLG flakes, are effective alternatives to FTO/Pt counter electrodes for DSSCs for both outdoor and indoor applications.

physics.app-ph↗

arXiv2019

MoS2 Quantum Dot/Graphene Hybrids for Advanced Interface Engineering of CH3NH3PbI3 Perovskite Solar Cell with Efficiency over 20%

Interface engineering of organic-inorganic halide perovskite solar cells (PSCs) plays a pivotal role in achieving high power conversion efficiency (PCE). Graphene and related two-dimensional materials (GRMs) are promising candidates to tune on demand the interface properties of PSCs. In this work, we fully exploit the potential of GRMs by controlling the optoelectronic properties of hybrids between molybdenum disulfide (MoS2) and reduced graphene oxide (RGO) as hole transport layer (HTL) and active buffer layer (ABL) in mesoscopic methylammonium lead iodide (CH3NH3PbI3) perovskite (MAPbI3)-based PSC. We show that zero-dimensional MoS2 quantum dots (MoS2 QDs), derived by liquid phase exfoliated MoS2 flakes, provide both hole-extraction and electron-blocking properties. In fact, on the one hand, intrinsic n-type doping-induced intra-band gap states effectively extract the holes through an electron injection mechanism. On the other hand, quantum confinement effects increase the optical band gap of MoS2 (from 1.4 eV for the flakes to > 3.2 for QDs), raising the minimum energy of its conduction band (from -4.3 eV for the flakes to -2.2 eV for QDs) above the one of conduction band of MAPbI3 (between -3.7 and -4 eV) and hindering electron collection. The van der Waals hybridization of MoS2 QDs with functionalized reduced graphene oxide (f-RGO), obtained by chemical silanization-induced linkage between RGO and (3-mercaptopropyl)trimethoxysilane, is effective to homogenize the deposition of HTLs or ABLs onto the perovskite film, since the two-dimensional (2D) nature of RGO effectively plug the pinholes of the MoS2 QDs films. Our graphene interface engineering (GIE) strategy based on van der Waals MoS2 QD/graphene hybrids enable MAPbI3-based PSCs to achieve PCE up to 20.12% (average PCE of 18.8%).

physics.app-ph↗

arXiv2016

Large deviation theory to model systems under an external feedback

In this paper we address the problem of systems under an external feedback. This is performed using a large deviation approach and rate distortion from information theory. In particular we define a lower boundary for the maximum entropy reduction that can be obtained using a feedback apparatus with a well defined accuracy in terms of measurement of the state of the system. The large deviation approach allows also to define a new set of potentials, including information, which similarly to more conventional thermodynamic potentials can define the state with optimal use of the information given the accuracy of the feedback apparatus.

cond-mat.stat-mech↗

arXiv2015

Unraveling the "Green Gap" problem: The role of random alloy fluctuations in InGaN/GaN light emitting diodes

White light emitting diodes based on III-nitride InGaN/GaN quantum wells currently offer the highest overall efficiency for solid state lighting applications. Although current phosphor-converted white LEDs have high electricity-to-light conversion efficiencies, it has been recently pointed out that the full potential of solid state lighting could be exploited only by color mixing approaches without employing phosphor-based wavelength conversion. Such an approach requires direct emitting LEDs of different colors, in particular in the green/yellow range ov the visible spectrum. This range, however, suffers from a systematic drop in efficiency, known as the "green gap", whose physical origin has not been understood completely so far. In this work we show by atomistic simulations that a consistent part of the "green gap" in c-plane InGaN/GaN based light emitting diodes may be attributed to a decrease in the radiative recombination coefficient with increasing Indium content due to random fluctuations of the Indium concentration naturally present in any InGaN alloy.

cond-mat.mtrl-sci↗