172 research outputs found
Time-resolved imaging of non-diffusive carrier transport in long-lifetime halide perovskite thin films
Owing to their exceptional semiconducting properties, hybrid
inorganic-organic perovskites show great promise as photovoltaic absorbers. In
these materials, long-range diffusion of charge carriers allows for most of the
photogenerated carriers to contribute to the photovoltaic efficiency. Here,
time-resolved photoluminescence (PL) microscopy is used to directly probe
ambipolar carrier diffusion and recombination kinetics in hybrid perovskites.
This technique is applied to thin films of methylammonium lead tri-iodide
MAPbI obtained with two different fabrication routes, methylammonium lead
tribromide (MAPbBr), and an alloy of formamidinium lead tri-iodide
(FAPbI) and methylammonium lead bromide
FAMAPb(IBr_). Average diffusion
coefficients in the films leading to the highest device efficiencies and
longest lifetimes, i.e., in FAMAPb(IBr)
and acetonitrile-processed MAPbI, are found to be several orders of
magnitude lower than in the other films. Further examination of the
time-dependence shows strong evidence for non-diffusive transport. In
particular, acetonitrile-processed MAPbI shows distinct diffusion regimes
on short and long timescales with an effective diffusion constant varying over
2 orders of magnitude. Our results also highlight the fact that increases in
carrier lifetime in this class of materials are not necessarily concomitant
with increased diffusion lengths and that the PL quantum efficiency under solar
cell operating conditions is a greater indication of material, and ultimately
device, quality
Semitransparent organic photovoltaic cells
We demonstrate semitransparent, small molecular weight organic solar cells employing a thin silver/indium tin oxide compound cathode with a maximum transmission of (60±6)%(60±6)% averaged over the visible spectral range and with a power conversion efficiency, ηp = (0.28±0.03)%ηp=(0.28±0.03)% under simulated, AM1.5G, 1 sun illumination. By increasing the Ag thickness, an average transmission of (26±3)%(26±3)% is achieved with ηp = (0.62±0.06)%ηp=(0.62±0.06)%, a value approximately half of that obtained for the same structure employing a conventional, reflective, and thick Ag cathode. A semitransparent tandem organic solar cell with ηp = (0.48±0.02)%ηp=(0.48±0.02)% and an average transmission of (44±4)%(44±4)% is also demonstrated. Semitransparent organic photovoltaic cells have potential uses as tinted and power-generating thin-film coatings on architectural surfaces, such as windows and walls. The use of a transparent top electrode also significantly simplifies the design of tandem cells, relaxing requirements for the placement of different absorbing materials at the maxima of optical fields introduced by reflective cathodes.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/87783/2/233502_1.pd
LLM-Prop: Predicting Physical And Electronic Properties Of Crystalline Solids From Their Text Descriptions
The prediction of crystal properties plays a crucial role in the crystal
design process. Current methods for predicting crystal properties focus on
modeling crystal structures using graph neural networks (GNNs). Although GNNs
are powerful, accurately modeling the complex interactions between atoms and
molecules within a crystal remains a challenge. Surprisingly, predicting
crystal properties from crystal text descriptions is understudied, despite the
rich information and expressiveness that text data offer. One of the main
reasons is the lack of publicly available data for this task. In this paper, we
develop and make public a benchmark dataset (called TextEdge) that contains
text descriptions of crystal structures with their properties. We then propose
LLM-Prop, a method that leverages the general-purpose learning capabilities of
large language models (LLMs) to predict the physical and electronic properties
of crystals from their text descriptions. LLM-Prop outperforms the current
state-of-the-art GNN-based crystal property predictor by about 4% in predicting
band gap, 3% in classifying whether the band gap is direct or indirect, and 66%
in predicting unit cell volume. LLM-Prop also outperforms a finetuned MatBERT,
a domain-specific pre-trained BERT model, despite having 3 times fewer
parameters. Our empirical results may highlight the current inability of GNNs
to capture information pertaining to space group symmetry and Wyckoff sites for
accurate crystal property prediction.Comment: Code for LLM-Prop can be found at:
https://github.com/vertaix/LLM-Pro
Reactions at Noble Metal Contacts with Methylammonium Lead Triiodide Perovskites: Role of Underpotential Deposition and Electrochemistry
Chemical reactivity of halide perovskites coupled with a low energy of formation makes it a challenge to characterize material properties and achieve long-term device stability. In this study, we elucidate electrochemical reactions occurring at the methylammonium lead triiodide (MAPbI3)/Au interface. X-ray photoemission spectroscopy is used to identify a type of reduction/oxidation reaction termed underpotential deposition (UPD) involving lead, iodine, and hydrogen occurring at interfaces with noble metals. Changes in surface compositions and oxidation states suggest that UPD derived adsorbates at MAPbI3/Au interfaces lower the energy barrier for release of volatile HI and/or I2catalyzing degradation at exposed contacts. Additionally, comparison to PbI2/Au interfaces demonstrates that the presence of methylammonium/methylamine accelerates the formation of a Pb0 adlayer on the Au. Reactions involving UPD Pb0 can transform the typically anodic (hole collecting) Au to a cathode in a photovoltaic measurement. Cyclic voltammetry reveals electrochemical reaction peaks in indium tin oxide (ITO)/MAPbI3/Au devices occurring within voltage ranges commonly used for perovskite characterization. The electrochemical stability window of this device architecture is measured to be betweenâ0.5 V and 0.9 V. Voltage induced interfacial reactions contribute to reversible electrochemical peaks, hysteresis, switchable perovskite diode polarity, and permanent degradation at larger voltages. These types of surface reactions alter the interface/interphase composition beyond ion accumulation, provide a source for the diffusion of defects, and contribute to electrode material dependent current-voltage hysteresis. Moreover, the results imply fundamental limitations to achieving high device stability with noble metals and/or methylammonium containing perovskites
Near-field interactions between metal nanoparticle surface plasmons and molecular excitons in thin-films: part I: absorption
In this and the following paper (parts I and II, respectively), we systematically study the interactions between surface plasmons of metal nanoparticles (NPs) with excitons in thin-films of organic media. In an effort to exclusively probe near-field interactions, we utilize spherical Ag NPs in a size-regime where far-field light scattering is negligibly small compared to absorption. In part I, we discuss the effect of the presence of these Ag NPs on the absorption of the embedding medium by means of experiment, numerical simulations, and analytical calculations, all shown to be in good agreement. We observe absorption enhancement in the embedding medium due to the Ag NPs with a strong dependence on the medium permittivity, the spectral position relative to the surface plasmon resonance frequency, and the thickness of the organic layer. By introducing a low index spacer layer between the NPs and the organic medium, this absorption enhancement is experimentally confirmed to be a near field effect In part II, we probe the impact of the Ag NPs on the emission of organic molecules by time-resolved and steady-state photoluminescence measurements
Best practices for measuring emerging light-emitting diode technologies
The arrival of light-emitting diodes based on new materials is posing challenges for the characterization and comparison of devices in a trusted and consistent manner. Here we provide some advice and guidelines that we hope will benefit the community
Roadmap on perovskite light-emitting diodes
In recent years, the field of metal-halide perovskite emitters has rapidly emerged as a new community in solid-state lighting. Their exceptional optoelectronic properties have contributed to the rapid rise in external quantum efficiencies (EQEs) in perovskite light-emitting diodes (PeLEDs) from <1% (in 2014) to over 30% (in 2023) across a wide range of wavelengths. However, several challenges still hinder their commercialization, including the relatively low EQEs of blue/white devices, limited EQEs in large-area devices, poor device stability, as well as the toxicity of the easily accessible lead components and the solvents used in the synthesis and processing of PeLEDs. This roadmap addresses the current and future challenges in PeLEDs across fundamental and applied research areas, by sharing the communityâs perspectives. This work will provide the field with practical guidelines to advance PeLED development and facilitate more rapid commercialization
Device Performance of Emerging Photovoltaic Materials (Version 3)
Following the 2nd release of the âEmerging PV reports,â the best achievements in the performance of emerging photovoltaic devices in diverse emerging photovoltaic research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2021. Updated graphs, tables, and analyses are provided with several performance parameters, e.g., power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, e.g., the detailed balance efficiency limit. The 3rd installment of the âEmerging PV reportsâ extends the scope toward triple junction solar cells
Device Performance of Emerging Photovoltaic Materials (Version 3)
Following the 2nd release of the âEmerging PV reports,â the best achievements in the performance of emerging photovoltaic devices in diverse emerging photovoltaic research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2021. Updated graphs, tables, and analyses are provided with several performance parameters, e.g., power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, e.g., the detailed balance efficiency limit. The 3rd installment of the âEmerging PV reportsâ extends the scope toward triple junction solar cells
- âŠ