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De Wolf, Stefaan

Publications and source records attributed to De Wolf, Stefaan.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Single-source pulsed laser-deposited perovskite solar cells with enhanced performance via bulk and 2D passivation

Single-source vapor deposition of halide perovskites has, to date, remained challenging due to the dissimilar volatilities of the precursors, limiting the controlled transfer of multiple elements at once. Here, we demonstrate that pulsed laser deposition (PLD) addresses the rate-control challenges of single-source evaporation, enabling perovskite solar cells with power conversion efficiencies above 19% after passivation. Combining dry mechanochemical synthesis and PLD, we fabricated (Cl-passivated) MA1−xFAxPbI3 films from a single-source target. These films grow on hole-selective self-assembled monolayers, initially forming a thin PbI2-rich layer, which fully converts to perovskite. An oleylammonium iodide (OAmI) post-treatment is then applied to passivate the perovskite’s top surface by forming a 2D perovskite film. Incorporating PbCl2 in the target and applying OAmI-based 2D passivation results in a remarkable 19.7% efficiency for p-i-n perovskite solar cells with enhanced device stability. This highlights the appeal of PLD to fully unlock the potential of single-source vapor-deposited perovskites.

Soto-Montero, Tatiana↗
DOE OSTI2024

Reverse-Bias Resilience of Monolithic Perovskite/Silicon Tandem Solar Cells

Metal halide perovskites have rapidly enabled a range of high-performance photovoltaic technologies. However, catastrophic failure under reverse voltage bias hinders their commercialization. In this work, we demonstrate that by employing a monolithic perovskite/silicon tandem structure, the perovskite subcell can be effectively protected by the silicon subcell under reverse bias, owing to the low reverse-bias diode current of the silicon subcell. As a result, the tested perovskite/silicon tandem devices show superior reverse-bias resilience compared to perovskite single-junction devices in both long-term reverse voltage biasing tests at the single-cell level and partial shading tests at the module level. These results highlight that, compared to other perovskite technologies, monolithic perovskite/silicon tandems are at a higher technology readiness level in terms of tackling the reverse-bias and partial shading challenge, which is a considerable advantage towards commercialization.

commercialization↗
DOE OSTI2024

Diamine chelates for increased stability in mixed Sn–Pb and all-perovskite tandem solar cells

Perovskite tandem solar cells show promising performance but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here, in this study, we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface – and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. As a result, encapsulated tandems retain 90% of initial efficiency following 1000 hours of operating at the maximum power point under simulated one-sun illumination in air without cooling.

14 SOLAR ENERGY↗
DOE OSTI2023

Photovoltaics at multi-terawatt scale: Waiting is not an option

We report a major renewable-energy milestone occurred in 2022: Photovoltaics (PV) exceeded a global installed capacity of 1 TW dc . But despite considerable growth and cost reduction over time, PV is still a small part of global electricity generation (4 to 5% for 2022), and the window is increasingly closing to take action at scale to cut greenhouse gas (GHG) emissions while meeting global energy needs for the future. PV is one of very few options that can be dispatched relatively quickly, but discussions of TW-scale growth at the global level may not be clearly communicating the needed size and speed for renewable-energy installation. A major global risk would be to make poor assumptions or mistakes in modeling and promoting the required PV deployment and industry growth and then realize by 2035 that we were profoundly wrong on the low side and need to ramp up manufacturing and deployment to unrealistic or unsustainable levels.

14 SOLAR ENERGY↗
DOE OSTI2023

Suppressed phase segregation for triple-junction perovskite solar cells

The tunable band gaps and facile fabrication of perovskites make them attractive for multi-junction photovoltaics. However, light-induced phase segregation limits their efficiency and stability: this occurs in wide band gap (> 1.65 eV) I/Br mixed perovskite absorbers, and becomes even more acute in the top cells of triple-junction solar photovoltaics that requires a fully 2.0 eV band gap absorber. We report herein that lattice distortion in I/Br mixed perovskites is correlated with the suppression of phase segregation, generating an increased ion migration energy barrier arising from the decreased average interatomic distance between A-site cation and iodide. Using a ~2.0 eV Rb/Cs mixed-cation inorganic perovskite with large lattice distortion in the top subcell, we fabricated all-perovskite triple-junction solar cells and achieved an efficiency of 24.3% (23.3% certified quasi-steady-state efficiency) with an open-circuit voltage of 3.21 V. This is, to our knowledge, the first reported certified efficiency for perovskite-based triple-junction solar cells. The triple-junction devices retain 80% of their initial efficiency following 420 hours of operation at the maximum power point.

14 SOLAR ENERGY↗
DOE OSTI2022

Regulating surface potential maximizes voltage in all-perovskite tandems

The open circuit voltage (V OC ) deficit in perovskite solar cells (PSCs) is greater in wide bandgap (>1.7 eV) cells than in ~1.5 eV perovskites. Quasi-Fermi level splitting (QFLS) measurements reveal V OC -limiting recombination at the electron transport layer (ETL) contact. This, we find, stems from inhomogeneous surface potential and poor perovskite-ETL energetic alignment. Common monoammonium surface treatments fail to address this; instead we introduce diammonium molecules to modify the perovskite surface states and achieve a more uniform spatial distribution of surface potential. Using 1,3-propane diammonium (PDA), QFLS increases by 90 meV, enabling 1.79 eV PSCs with a certified 1.33 V V OC , and > 19% power conversion efficiency (PCE). Incorporating this layer into a monolithic all-perovskite tandem, we report a record V OC of 2.19 V (89% of the Detailed Balance V OC limit) and > 27% PCE (26.3% certified quasi-steady-state). Furthermore, these tandems retain more than 86% of their initial PCE after 500 hrs operation.

14 SOLAR ENERGY↗
DOE OSTI2022

Photoactivated p-Doping of Organic Interlayer Enables Efficient Perovskite/Silicon Tandem Solar Cells

Solution-processed organic semiconductor layers on rough surfaces tend to vary widely in thickness, significantly hindering charge extraction in relevant optoelectronic devices. Herein, we report the photoactivated p-doping of hole-transporting material (HTM) to enhance hole extraction for (textured) perovskite/silicon tandem solar cells, making the device performance less sensitive to the variation of hole transport layer thickness. We used the ionic compound 4-isopropyl-4'-methyldiphenyliodonium tetrakis(penta-fluorophenyl-borate) (DPI-TPFB) as a p-type dopant in poly(triaryl amine) (PTAA), which we used as the HTM. We observed that light soaking DPI-TPFB-doped PTAA shows approximately 22 times higher conductivity compared with an undoped PTAA film, which translated into an improved fill factor (FF) for tandem solar cells. Our tandem solar cells achieved an ~80% FF and 27.8% efficiency and operated at their maximum power point for 200 h without loss of performance, in addition to retaining ~83% of initial performance over a month of operation in an outdoor environment.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,S↗
DOE OSTI2020

Polymeric Electron-Selective Contact for Crystalline Silicon Solar Cells with an Efficiency Exceeding 19%

Carrier-selective contacts have become a prominent path forward toward efficient crystalline silicon (c-Si) photovoltaics. Among the proposed contacting materials, organic materials may offer simplified and low-cost processing compared with typical vacuum deposition techniques. In this paper, branched polyethylenimine (b-PEI) is presented as an electron-transport layer (ETL) for c-Si solar cells. The incorporation of a b-PEI interlayer between c-Si(n) and Al leads to a low contact resistivity of 24 mΩ cm 2 . A silicon heterojunction solar cell integrated with b-PEI is demonstrated achieving a power conversion efficiency of 19.4%, which improves the benchmark efficiency of a c-Si solar cell with an organic ETL. This electron selectivity of b-PEI is attributed to its Lewis basicity, i.e., electron-donating ability, promoting favorable band bending at the c-Si surface for electron transport. Moreover, several other Lewis base polymers perform as efficient ETLs in organic/c-Si hybrid devices, indicating Lewis basicity could be a guideline for future organic ETL design.

14 SOLAR ENERGY↗
DOE OSTI2019

Passivating contacts for crystalline silicon solar cells

The global photovoltaic (PV) market is dominated by crystalline silicon (c-Si) based technologies with heavily doped, directly metallized contacts. Recombination of photo-generated electrons and holes at the contact regions is increasingly constraining the power conversion efficiencies of these devices as other performance-limiting energy losses are overcome. To move forward, c-Si PV technologies must implement alternative contacting approaches. Passivating contacts, which incorporate thin films within the contact structure that simultaneously supress recombination and promote charge-carrier selectivity, are a promising next step for the mainstream c-Si PV industry. Here, we review the fundamental physical processes governing contact formation in c-Si. In doing so we identify the role passivating contacts play in increasing c-Si solar cell efficiencies beyond the limitations imposed by heavy doping and direct metallization. Strategies towards the implementation of passivating contacts in industrial environments are discussed.

14 SOLAR ENERGY↗
DOE OSTI2019

Terawatt-scale photovoltaics: Transform global energy

Solar energy has the potential to play a central role in the future global energy system because of the scale of the solar resource, its predictability, and its ubiquitous nature. Global installed solar photovoltaic (PV) capacity exceeded 500 GW at the end of 2018, and an estimated additional 500 GW of PV capacity is projected to be installed by 2022-2023, bringing us into the era of TW-scale PV. Given the speed of change in the PV industry, both in terms of continued dramatic cost decreases and manufacturing-scale increases, the growth toward TW-scale PV has caught many observers, including many of us (1), by surprise. Two years ago, we focused on the challenges of achieving 3 to 10 TW of PV by 2030. Here, we envision a future with ~10 TW of PV by 2030 and 30 to 70 TW by 2050, providing a majority of global energy. PV would be not just a key contributor to electricity generation but also a central contributor to all segments of the global energy system. We discuss ramifications and challenges for complementary technologies (e.g., energy storage, power to gas/liquid fuels/chemicals, grid integration, and multiple sector electrification) and summarize what is needed in research in PV performance, reliability, manufacturing, and recycling.

14 SOLAR ENERGY↗
DOE OSTI2019

Dip Coating Passivation of Crystalline Silicon by Lewis Acids

The reduction of carrier recombination processes by surface passivation is vital for highly efficient crystalline silicon (c-Si) solar cells and bulk wafer metrological characterization. In this paper, we report a dip coating passivation of silicon surfaces in ambient air and temperature with Nafion, achieving a champion effective carrier lifetime of 12 ms on high resistivity n-type c-Si, which is comparable to state-of-the-art passivation methods. Nafion is a nonreactive polymer with strong Lewis acidity, thus leading to the formation of a large density of fixed charges at silicon surface, 1-2 orders of magnitude higher than what is achievable with conventional thin-film passivation layers. Notably, Nafion passivates the c-Si surface only by the fixed charges without chemical modification of dangling bonds, which is fundamentally different from the common practice of combining chemical with field-effect passivation. This dip coating process is simple and robust, without the need for complex equipment or parameter optimization as there is no chemical reaction involved.

14 SOLAR ENERGY↗
DOE OSTI2018

Device physics underlying silicon heterojunction and passivating‐contact solar cells: A topical review

Abstract The device physics of commercially dominant diffused‐junction silicon solar cells is well understood, allowing sophisticated optimization of this class of devices. Recently, so‐called passivating‐contact solar cell technologies have become prominent, with Kaneka setting the world's silicon solar cell efficiency record of 26.63% using silicon heterojunction contacts in an interdigitated configuration. Although passivating‐contact solar cells are remarkably efficient, their underlying device physics is not yet completely understood, not in the least because they are constructed from diverse materials that may introduce electronic barriers in the current flow. To bridge this gap in understanding, we explore the device physics of passivating contact silicon heterojunction (SHJ) solar cells. Here, we identify the key properties of heterojunctions that affect cell efficiency, analyze the dependence of key heterojunction properties on carrier transport under light and dark conditions, provide a self‐consistent multiprobe approach to extract heterojunction parameters using several characterization techniques (including dark J‐V, light J‐V, C‐V, admittance spectroscopy, and Suns‐V oc ), propose design guidelines to address bottlenecks in energy production in SHJ cells, and develop a process‐to‐module modeling framework to establish the module's performance limits. We expect that our proposed guidelines resulting from this multiscale and self‐consistent framework will improve the performance of future SHJ cells as well as other passivating contact‐based solar cells.

Chavali, Raghu V. K.↗
DOE OSTI2017

Transparent Electrodes for Efficient Optoelectronics

With the development of new generations of optoelectronic devices that combine high performance and novel functionalities (e.g., flexibility/bendability, adaptability, semi or full transparency), several classes of transparent electrodes have been developed in recent years. These range from optimized transparent conductive oxides (TCOs), which are historically the most commonly used transparent electrodes, to new electrodes made from nano‐ and 2D materials (e.g., metal nanowire networks and graphene), and to hybrid electrodes that integrate TCOs or dielectrics with nanowires, metal grids, or ultrathin metal films. Here, the most relevant transparent electrodes developed to date are introduced, their fundamental properties are described, and their materials are classified according to specific application requirements in high efficiency solar cells and flexible organic light‐emitting diodes (OLEDs). This information serves as a guideline for selecting and developing appropriate transparent electrodes according to intended application requirements and functionality.

Morales‐Masis, Monica↗
DOE OSTI2016

Asymmetric band offsets in silicon heterojunction solar cells: Impact on device performance

Amorphous/crystalline silicon interfaces feature considerably larger valence than conduction band offsets. In this article, we analyze the impact of such band offset asymmetry on the performance of silicon heterojunction solar cells. To this end, we use silicon suboxides as passivation layers—inserted between substrate and (front or rear) contacts—since such layers enable intentionally exacerbated band-offset asymmetry. Investigating all topologically possible passivation layer permutations and focussing on light and dark current-voltage characteristics, we confirm that to avoid fill factor losses, wider-bandgap silicon oxide films (of at least several nanometer thin) should be avoided in hole-collecting contacts. As a consequence, device implementation of such films as window layers—without degraded carrier collection—demands electron collection at the front and hole collection at the rear. Furthermore, at elevated operating temperatures, once possible carrier transport barriers are overcome by thermionic (field) emission, the device performance is mainly dictated by the passivation of its surfaces. In this context, compared to the standard amorphous silicon layers, the wide-bandgap oxide layers applied here passivate remarkably better at these temperatures, which may represent an additional benefit under practical operation conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Environmental stability of high-mobility indium-oxide based transparent electrodes

Large-scale deployment of a wide range of optoelectronic devices, including solar cells, critically depends on the long-term stability of their front electrodes. Here, we investigate the performance of Sn-doped In{sub 2}O{sub 3} (ITO), H-doped In{sub 2}O{sub 3} (IO:H), and Zn-doped In{sub 2}O{sub 3} (IZO) electrodes under damp heat (DH) conditions (85 °C, 85% relative humidity). ITO, IO:H capped with ITO, and IZO show high stability with only 3%, 9%, and 13% sheet resistance (R{sub s}) degradation after 1000 h of DH, respectively. For uncapped IO:H, we find a 75% R{sub s} degradation, due to losses in electron Hall mobility (μ{sub Hall}). We propose that this degradation results from chemisorbed OH- or H{sub 2}O-related species in the film, which is confirmed by thermal desorption spectroscopy and x-ray photoelectron spectroscopy. While μ{sub Hall} strongly degrades during DH, the optical mobility (μ{sub optical}) remains unchanged, indicating that the degradation mainly occurs at grain boundaries.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Transparent electrodes in silicon heterojunction solar cells: Influence on contact passivation

Charge carrier collection in silicon heterojunction solar cells occurs via intrinsic/doped hydrogenated amorphous silicon layer stacks deposited on the crystalline silicon wafer surfaces. Usually, both the electron and hole collecting stacks are externally capped by an n-type transparent conductive oxide, which is primarily needed for carrier extraction. Earlier, it has been demonstrated that the mere presence of such oxides can affect the carrier recombination in the crystalline silicon absorber. Here, we present a detailed investigation of the impact of this phenomenon on both the electron and hole collecting sides, including its consequences for the operating voltages of silicon heterojunction solar cells. As a result, we define guiding principles for improved passivating contact design for high-efficiency silicon solar cells.

14 SOLAR ENERGY↗