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Tsai, Hsinhan

Publications and source records attributed to Tsai, Hsinhan.

33 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Robust Unencapsulated Perovskite Solar Cells Protected by a Fluorinated Fullerene Electron Transporting Layer

The emergent perovskite photovoltaics technology faces challenges like the long-term durability combining moisture, thermal, and photo stresses that prevents them from competing with established technologies. In this work, we introduce a series of new fluorinated fullerenes as an electron-transporting layer (ETL) for robust perovskite photovoltaics that deliver a high power conversion efficiency of 21.27% with substantially improved durability against environmental stressing. The hydrophobic nature of the new fullerene protects the unencapsulated perovskite cell with stability over 1400 h in 85% relative humidity. Notably, the unencapsulated device maintained 80% of their original performance (T-80) after being immersed in water for over 10 min. Detailed characterizations suggest that the fluorinated fullerene can immobilize the cations in perovskites and passivate the surface traps. Therefore, the T-80 lifetime of the devices under constant illumination reached 1920 h. On the basis of the accelerated test, we estimate a lifetime approaching 10 years with encapsulation. The successful demonstration of the new ETL can stimulate further research and momentum for future photovoltaic technology development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Billion-pixel x-ray camera (BiPC-X)

The continuing improvement in quantum efficiency (above 90% for single visible photons), reduction in noise (below 1 electron per pixel), and shrink in pixel pitch (less than 1 μm) enable billion-pixel x-ray cameras (BiPC-X) based on commercial complementary metal–oxide–semiconductor (CMOS) imaging sensors. We describe BiPC-X designs and prototype construction based on flexible tiling of commercial CMOS imaging sensors with millions of pixels. Device models are given for direct detection of low energy x rays (<10 keV) and indirect detection of higher energies using scintillators. Modified Birks’s law is proposed for light yield non-proportionality in scintillators as a function of x-ray energy. Single x-ray sensitivity and spatial resolution have been validated experimentally using a laboratory x-ray source and the Argonne Advanced Photon Source. Possible applications include wide field-of-view or large x-ray aperture measurements in high-temperature plasmas, the state-of-the-art synchrotron, x-ray free electron laser, and pulsed power facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Highly efficient photoelectric effect in halide perovskites for regenerative electron sources

Electron sources are a critical component in a wide range of applications such as electron-beam accelerator facilities, photomultipliers, and image intensifiers for night vision. We report efficient, regenerative and low-cost electron sources based on solution-processed halide perovskites thin films when they are excited with light with energy equal to or above their bandgap. We measure a quantum efficiency up to 2.2% and a lifetime of more than 25 h. Importantly, even after degradation, the electron emission can be completely regenerated to its maximum efficiency by deposition of a monolayer of Cs. The electron emission from halide perovskites can be tuned over the visible and ultraviolet spectrum, and operates at vacuum levels with pressures at least two-orders higher than in state-of-the-art semiconductor electron sources.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Facile Fabrication of Self‐Assembly Functionalized Polythiophene Hole Transporting Layer for High Performance Perovskite Solar Cells

Abstract Crystallinity and crystal orientation have a predominant impact on a materials’ semiconducting properties, thus it is essential to manipulate the microstructure arrangements for desired semiconducting device performance. Here, ultra‐uniform hole‐transporting material (HTM) by self‐assembling COOH‐functionalized P3HT (P3HT‐COOH) is fabricated, on which near single crystal quality perovskite thin film can be grown. In particular, the self‐assembly approach facilitates the P3HT‐COOH molecules to form an ordered and homogeneous monolayer on top of the indium tin oxide (ITO) electrode facilitate the perovskite crystalline film growth with high quality and preferred orientations. After detailed spectroscopy and device characterizations, it is found that the carboxylic acid anchoring groups can down‐shift the work function and passivate the ITO surface, retarding the interface carrier recombination. As a result, the device made with the self‐assembled HTM show high open‐circuit voltage over 1.10 V and extend the lifetime over 4,300 h when storing at 30% relative humidity. Moreover, the cell works efficiently under much reduced light power, making it useful as power source under dim‐light conditions. The demonstration suggests a new facile way of fabricating monolayer HTM for high efficiency perovskite devices, as well as the interconnecting layer needed for tandem cell.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Edge States Drive Exciton Dissociation in Ruddlesden–Popper Lead Halide Perovskite Thin Films

Efficient photovoltaic cells based on thin films of solution-processed 2D Ruddlesden–Popper hybrid perovskites (RPPs) represent an exciting breakthrough due to their enhanced tunability and chemical stability relative to those fabricated from 3D phases. However, reports of efficient charge separation and current collection are in apparent contradiction with the well-known enhancement of the exciton binding energy in multilayered halide perovskites, which should lower the device’s internal quantum efficiency and voltage. This controversy has led to various proposals for the electronic and physical structure of RPP thin films, including phase inhomogeneity as the driving force for exciton dissociation and transport. We address this apparent paradox in high-quality hot-cast RPP films by correlating ultrafast transient absorption spectroscopy with X-ray scattering measurements. We show that a hot-casting fabrication method produces highly phase pure n = 3 (BA) 2 (MA) n-1 Pb n I 3n+1 RPP structures. The high-phase purity and large grain sizes allow us to observe vertical transport of excitons via a diffusive process and allow us to determine that charge separation is primarily driven by dissociation at surface localized subgap electronic states. Furthermore, we analyze the differential absorption kinetics in films of varying thickness to directly determine that the excitonic diffusion constant is ~0.18 cm 2 s –1 . We propose that a surface localized structural distortion, observed using surface selective grazing incidence X-ray scattering measurements, is responsible for the creation of the surface localized defect states. We find that the density and spatial distribution of these defect states is a function of preparation conditions.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

High-efficiency and durable optoelectronic devices using layered 2D perovskites

A thin film for an optoelectronic device includes a layered 2D perovskite material. The thin film including the layered 2D perovskite material forms a substantially or nearly single-crystalline highly uniform thin film with strongly preferential out-of-plane alignment of the inorganic perovskite layers. This single-crystalline, highly uniform, and highly aligned thin film of the layered 2D perovskite material may thereby facilitate efficient charge transport in an optoelectronic device.

14 SOLAR ENERGY↗
DOE OSTI2020

The Role of Metal-Semiconductor Interface in Hybrid Perovskite Devices for High-Performance Radiation Photon Counting

Halide perovskites are promising optoelectronic semiconductors. For applications in solid-state detectors that operate in low photon flux counting mode, blocking interfaces are essential to minimize the dark current noise. Here, we investigate the interface between methylammonium lead tri-iodide (MAPbI 3 ) single crystals and commonly used high and low work function metals to achieve photon counting capabilities in a solid-state detector. Using scanning photocurrent microscopy, we observe a large Schottky barrier at the MAPbI 3 /Pb interface, which efficiently blocks dark current. Moreover, the shape of the photocurrent profile indicates that the MAPbI 3 single-crystal surface has a deep fermi level close to that of Au. Rationalized by first-principle calculations, we attribute this observation to the defects due to excess iodine on the surface underpinning emergence of deep band-edge states. The photocurrent decay profile yields a charge carrier diffusion length of 10–25 μm. Using this knowledge, we demonstrate a single-crystal MAPbI 3 detector that can count single γ-ray photons by producing sharp electrical pulses with a fast rise time of <2 μs. Overall, our study indicates that the interface plays a crucial role in solid-state detectors operating in photon counting mode.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A sensitive and robust thin-film x-ray detector using 2D layered perovskite diodes

Solid-state radiation detectors, using crystalline semiconductors to convert radiation photons to electrical charges, outperform other technologies with high detectivity and sensitivity. Here, we demonstrate a thin-film x-ray detector comprised with highly crystalline two-dimensional Ruddlesden-Popper phase layered perovskites fabricated in a fully depleted p-i-n architecture. It shows high diode resistivity of 10 12 ohm·cm in reverse-bias regime leading to a high x-ray detecting sensitivity up to 0.276 C Gy air –1 cm –3 . Such high signal is collected by the built-in potential underpinning operation of primary photocurrent device with robust operation. The detectors generate substantial x-ray photon–induced open-circuit voltages that offer an alternative detecting mechanism. Furthermore, our findings suggest a new generation of x-ray detectors based on low-cost layered perovskite thin films for future x-ray imaging technologies.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Vacuum-Free, All-Solution, and All-Air Processed Organic Photovoltaics with over 11% Efficiency and Promoted Stability Using Layer-by-Layer Codoped Polymeric Electrodes

Nonfullerene organic photovoltaics (OPVs) have achieved a breakthrough in pushing the efficiency beyond 15%. Although this sheds light on OPV commercialization, the high cost associated with the scalable device fabrications remains a giant challenge. Herein, a vacuum-free, all-solution and all-air processed OPV is reported that yields 11.12% efficiency with a fill factor of 0.725, due to the usages of high-merit polymeric electrodes and modified active blends. The design principle toward the high-merit electrodes is to induce heavy acid doping into the matrices for a raised carrier concentration and mobility, make a large removal of insulating components in the whole matrices rather than surfaces, and restrain the formation of large-domain aggregates. A unique layer-by-layer doping is developed to enable the polymeric electrodes with record-high trade-offs between optical transmittance and electrical conductivity. Moreover, solvent vapor annealing is proposed to boost device efficiency and it has the advantages of finely adjusting the active blend morphology and raising the electron mobility. The resulting devices are highly efficient and most (≈91%) of the initial efficiency are maintained in 30 day storage. Finally, this work indicates bright future for making cost-effective all-solution processed OPVs in air.

14 SOLAR ENERGY↗
DOE OSTI2020

Methylammonium Lead Tribromide Single Crystal Detectors towards Robust Gamma-Ray Photon Sensing

In recent years, hybrid perovskite single crystalline solid-state detectors have shown promise in γ-ray spectroscopy. Here, the γ-ray photon induced electrical pulses are investigated, which are produced by perovskite solid-state detectors made with the commonly used methylammonium lead tribromide crystals with chlorine incorporation. Under low electric field detector operation, slow pulses generated by γ-rays with average rise times of 65 µs are observed, which decreases to 20 µs when a higher electrical field of 500 V cm -1 is applied. However, the baseline becomes noisy quickly, which prevents collection of clean pulses for spectra construction. Further, by systematically measuring the temperature dependence and current–voltage characteristics, such instability is attributed to the local ion migration under electrical field creating a fluctuating dark noise, which presents a major challenge in perovskite γ-ray detector technologies. It is demonstrated that cycling the bias between positive and negative polarity can stabilize the detector, allowing for longer periods of pulse accumulation for generating energy resolved spectra with resolutions of ≈35% at 59.6 keV and ≈25% at 662 keV at room temperature. The study indicates that the main limiting factors of perovskite-based γ-ray detectors are slow rise times and bias instability. Finally, these challenges must be properly addressed to achieve reproducible, high-resolution γ-ray detection.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

The working principle of hybrid perovskite gamma-ray photon counter

Gamma-ray spectroscopy that quantifies the gamma-ray energies is a critical technology widely needed in astrophysics, nuclear material detection and medical treatment. The key is to precisely count gamma-ray photons using sensitive detectors. In this paper, we investigate the operational principles of chlorine-doped methylammonium lead tribromide (MAPbBr 3-x Cl x ) perovskite single crystal detectors that can efficiently count gamma-ray photon events with electrical pulses. Specifically, we find the main dark current originates from the thermally activated electron injection from the impurities, and using high work function contacts can block out the dark noise thus allows for efficient pulse collection at higher electrical fields ~500 V/cm. As a result, we observe strong electrical pulses when exposing the detector under radioactive sources emitting gamma-ray photons at various energies. Our results also reveal the fundamental issues that prevent the reliable observation of photo-electric peak. This work suggest pathway towards energy resolved gamma-ray spectroscopy using perovskite crystal detectors.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic–Inorganic Perovskites on Macro- and Nanoscales

Progress in flexible organic electronics necessitates a full understanding of how local inhomogeneities impact electronic and ionic conduction pathways and underlie macroscopic device characteristics. In this work, we used frequency- and time-resolved macro- and nanoprobe measurements to study spatiotemporal characteristics of multiscale charge transport dynamics in a series of ternary-blended hybrid organic inorganic perovskites (HOIPs) (MA 0.95– x FA x Cs 0.05 PbI 3 ). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10 2 –10 –6 s) and spatial (millimeters–picometers) scales. Ab initio molecular dynamic simulations suggest that insertion of FA results in a dynamic lattice, improved ion transport, and dipole screening. We demonstrate that correlations between macro- and nanoscale measurements provide a pathway for accessing distribution of relaxation in nanoscale polarization and charge transport dynamics of ionically conductive functional perovskites.

36 MATERIALS SCIENCE↗