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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Structural Stability of Tin-Lead Halide Perovskite Solar Cells

One of the key features that makes halide perovskite solar cells such an attractive and intensely researched photovoltaic (PV) technology, is the tunability of the bandgap of these halide perovskite materials [1], [2]. Shortly after it was established that the bandgap could be increased to 1.7-1.8 eV, investigations into the application for silicon based tandem solar cells launched. Within a few years, conversion efficiencies of up to 28 % have been reported [3]. Concurrently, the interest in commercial application of this technology emerged and have rapidly increased. Whereas there are advantages to piggy backing on an established PV technology such as silicon, efforts to develop all-perovskite tandem solar cells are of considerable interest. Partly substituting the metal cation in the ABX3 perovskite enables the low bandgap absorbers required for an all-perovskite tandem solar cell. One common approach is to partially substitute the lead with tin, however these materials often suffered from poor stability. Therefore the development of an efficient, stable mixed tin-lead perovskite is key to enabling all-perovskite tandem solar cells.

degradation↗
DOE OSTI2020

Low-frequency lattice phonons in halide perovskites explain high defect tolerance toward electron-hole recombination

Low-cost solution-based synthesis of metal halide perovskites (MHPs) invariably introduces defects in the system, which could form Shockley-Read-Hall (SRH) electron-hole recombination centers detrimental to solar conversion efficiency. Here, we investigate the nonradiative recombination processes due to native point defects in methylammonium lead halide (MAPbI 3 ) perovskites using ab initio nonadiabatic molecular dynamics within surface-hopping framework. Regardless of whether the defects introduce a shallow or deep band state, we find that charge recombination in MAPbI 3 is not enhanced, contrary to predictions from SRH theory. We demonstrate that this strong tolerance against defects, and hence the breakdown of SRH, arises because the photogenerated carriers are only coupled with low-frequency phonons and electron and hole states overlap weakly. Both factors appreciably decrease the nonadiabatic coupling. We argue that the soft nature of the inorganic lattice with small bulk modulus is key for defect tolerance, and hence, the findings are general to other MHPs.

Science & Technology - Other Topics↗
DOE OSTI2020

Magnetizing lead-free halide double perovskites

Spintronics holds great potential for next-generation high-speed and low–power consumption information technology. Recently, lead halide perovskites (LHPs), which have gained great success in optoelectronics, also show interesting magnetic properties. However, the spin-related properties in LHPs originate from the spin-orbit coupling of Pb, limiting further development of these materials in spintronics. Here, we demonstrate a new generation of halide perovskites, by alloying magnetic elements into optoelectronic double perovskites, which provide rich chemical and structural diversities to host different magnetic elements. In our iron-alloyed double perovskite, Cs 2 Ag(Bi:Fe)Br 6 , Fe 3+ replaces Bi 3+ and forms FeBr 6 clusters that homogenously distribute throughout the double perovskite crystals. Furthermore, we observe a strong temperature-dependent magnetic response at temperatures below 30 K, which is tentatively attributed to a weak ferromagnetic or antiferromagnetic response from localized regions. We anticipate that this work will stimulate future efforts in exploring this simple yet efficient approach to develop new spintronic materials based on lead-free double perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Halide segregation to boost all-solid-state lithium-chalcogen batteries

Mixing electroactive materials, solid-state electrolytes, and conductive carbon to fabricate composite electrodes is the most practiced but least understood process in all-solid-state batteries, which strongly dictates interfacial stability and charge transport. Here, we report on universal halide segregation at interfaces across various halogen-containing solid-state electrolytes and a family of high-energy chalcogen cathodes enabled by mechanochemical reaction during ultrahigh-speed mixing. Bulk and interface characterizations by multimodal synchrotron x-ray probes and cryo–transmission electron microscopy show that the in situ segregated lithium halide interfacial layers substantially boost effective ion transport and suppress the volume change of bulk chalcogen cathodes. Various all-solid-state lithium-chalcogen cells demonstrate utilization close to 100% and extraordinary cycling stability at commercial-level areal capacities.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chapter 1: Halide Organic Photovoltaics for Energy: Hybrid Perovskites for Solar Cells

The following sections are included: Fundamentals of Photovoltaics, What Limits PV Device Efficiencies?, Traditional Photovoltaics, Perovskite Halide-Based Hybrid Semiconductors for Photovoltaics: Novel Materials in a League of Their Own, Solution Processability, Tunability, Perovskite Solar Cell Architectures, Pairing Perovskite Absorbers, Reduction/Oxidation and Electrochemical Reactivity Considerations for High-Performance Halide Perovskite Solar Cells, Metal Electrode Corrosion, Proton-Mediated Reduction of Ni3+ at NiOx Interfaces, Electrochemistry in Solid-State Perovskite Devices, Overview of Stability Considerations for High Performance Perovskite Solar Cells, Moisture-Induced Degradation, Oxygen-Mediated Degradation, Illumination-Dependent Degradation, Bias-Dependent Degradation, Stability Considerations for Charge Selective Contacts, Electrode-Induced Degradation Modes, Conclusion, and References.

absorbers↗
DOE OSTI2021

Cation Dynamics in Hybrid Halide Perovskites

Hybrid halide perovskite semiconductors exhibit complex, dynamical disorder while also harboring properties ideal for optoelectronic applications that include photovoltaics. However, these materials are structurally and compositionally distinct from traditional compound semiconductors composed of tetrahedrally coordinated elements with an average valence electron count of silicon. The additional dynamic degrees of freedom of hybrid halide perovskites underlie many of their potentially transformative physical properties. Neutron scattering and spectroscopy studies of the atomic dynamics of these materials have yielded significant insights into their functional properties. Specifically, inelastic neutron scattering has been used to elucidate the phonon band structure, and quasi-elastic neutron scattering has revealed the nature of the uncorrelated dynamics pertaining to molecular reorientations. Understanding the dynamics of these complex semiconductors has elucidated the temperature-dependent phase stability and origins of defect-tolerant electronic transport from the highly polarizable dielectric response. Furthermore, the dynamic degrees of freedom of the hybrid perovskites provide additional opportunities for application engineering and innovation.

Materials Science↗
DOE OSTI2020

Passivated Interfaces and Surface Recombination Velocities in Halide Perovskites

Surfaces and charge-extracting contacts remain major sources of non-radiative recombination loss; limiting the performance of perovskite PV compared to theoretical limits. We investigate mixed-cation mixed-halide perovskites and demonstrate that, with chemical surface passivation, they can achieve >4 μs minority carrier lifetimes, and >20% external PL quantum yields (PLQY), and nearly single-exponential decay kinetics. This high PLQY observed corresponds to ~97% of the Shockley-Queisser theoretical quasi-fermi level splitting, a first for MA-free mixed-cation mixed-halide compositions. The high PLQY and long PL lifetimes allow us to measure average surface recombination velocities (SRV) <10cm/s, with a champion low of ~1cm/s (a conservative estimate). We show how such improvements in SRV should lead to an absolute improvement in PCE of >4% even with the best of contact alignments. We investigate different MA-free high bandgap compositions, including bandgaps relevant for tandem applications (1.7-1.8eV), and demonstrate performance improvements across all these compositions with our surface passivation strategy. Lastly, using a combination of surface characterization techniques, we show Lewis base interactions of the passivating agent with the perovskite surfaces.

14 SOLAR ENERGY↗
DOE OSTI2021

Vapor-Processing of Metal-Halide Perovskites for Photovoltaics and Optoelectronics

Metal-halide perovskites are an exciting materials platform for next generation optoelectronic devices and solar cells. In this presentation, we review our work in processing metal-halide perovskites via a dry, carrier-gas assisted vapor deposition method, and its ability to be useful for the formation of all-perovskite heterojunctions. We also outline recent work demonstrating the viability of this method for the deposition of lead-based perovskites via co-deposition.

14 SOLAR ENERGY↗
DOE OSTI2021

Vapor-Processing of Metal Halide Perovskite Thin Films and Solar Cells

Metal-halide perovskites are an emerging material for next generation high efficiency solar cells. In this presentation, we review our work in processing metal-halide perovskites via a dry, carrier-gas assisted vapor deposition method, and its ability to be useful for the formation of all-perovskite heterojunctions. We also outline recent work demonstrating the viability of this method for the deposition of lead-based perovskites via co-deposition.

14 SOLAR ENERGY↗
DOE OSTI2020

Passivated Interfaces and Surface Recombination Velocities in Halide Perovskites

Surfaces and charge-extracting contacts remain major sources of non-radiative recombination loss; limiting the performance of perovskite PV compared to theoretical limits. We investigate mixed-cation mixed-halide perovskites and demonstrate that, with chemical surface passivation, they can achieve >4 μs minority carrier lifetimes, and >20% external PL quantum yields (PLQY), and nearly single-exponential decay kinetics. This high PLQY observed corresponds to ~97% of the Shockley-Queisser theoretical quasi-fermi level splitting, a first for MA-free mixed-cation mixed-halide compositions. The high PLQY and long PL lifetimes allow us to measure average surface recombination velocities (SRV) <10cm/s, with a champion low of ~1cm/s (a conservative estimate). We show how such improvements in SRV should lead to an absolute improvement in PCE of >4% even with the best of contact alignments. We investigate different MA-free high bandgap compositions, including bandgaps relevant for tandem applications (1.7-1.8eV), and demonstrate performance improvements across all these compositions with our surface passivation strategy. Lastly, using a combination of surface characterization techniques, we show Lewis base interactions of the passivating agent with the perovskite surfaces.

passivation↗
DOE OSTI2023

Post-growth Recrystallization by Halides for High Throughput CIGS Photovoltaics

The objective of this project in broad terms was to address the capital equipment expense associated with Cu(In,Ga)Se 2 (CIGS) as a material for photovoltaic devices. This project has demonstrated a new method for processing CIGS using metal halides to recrystallize and enhance the quality of the final materials. A wide spectrum of metal halides were examined. Of these Cu and In chlorides and AgBr were found to be most effective; and, of these, AgBr was found to produce exemplary results. Cu and In chlorides were found to produce undesirable changes in film composition. The project demonstrated over 16% efficiency in a CIGS device deposited at 10x the standard rate of ~1 μm/hr and with a >100°C reduction in maximum temperature to 450°C. The entire deposition of the absorber layer including the recrystallization step required only 15 minutes, which is a 4x decrease in processing time.

14 SOLAR ENERGY↗
DOE OSTI2023

Weak Dispersion of Exciton Landé Factor with Band Gap Energy in Lead Halide Perovskites: Approximate Compensation of the Electron and Hole Dependences

The optical properties of lead halide perovskite semiconductors in vicinity of the bandgap are controlled by excitons, so that investigation of their fundamental properties is of critical importance. The exciton Landé or g-factor g X is the key parameter, determining the exciton Zeeman spin splitting in magnetic fields. The exciton, electron, and hole carrier g-factors provide information on the band structure, including its anisotropy, and the parameters contributing to the electron and hole effective masses. Here, g X is measured by reflectivity in magnetic fields up to 60 T for lead halide perovskite crystals. The materials band gap energies at a liquid helium temperature vary widely across the visible spectral range from 1.520 up to 3.213 eV in hybrid organic–inorganic and fully inorganic perovskites with different cations and halogens: FA 0.9 Cs 0.1 PbI 2.8 Br 0.2 , MAPbI 3 , FAPbBr 3 , CsPbBr 3 , and MAPb(Br 0.05 Cl 0.95 ) 3 . The exciton g-factors are found to be nearly constant, ranging from +2.3 to +2.7. Thus, the strong dependences of the electron and hole g-factors on the bandgap roughly compensate each other when combining to the exciton g-factor. The same is true for the anisotropies of the carrier g-factors, resulting in a nearly isotropic exciton g-factor. The experimental data are compared favorably with model calculation results.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Understanding the optoelectronic properties of doped 2D organic-inorganic halide perovskite quantum wells: towards efficient ultrafast quantum well IR photodetectors

This project, titled “Understanding the optoelectronic properties of doped 2D organic-inorganic halide perovskite quantum wells: towards efficient quantum well IR photodetectors”, was funded by the U.S. Department of Energy to explore a new class of materials that could make future light-sensing technologies, such as infrared (IR) cameras and detectors more efficient, affordable, and widely available. The research focused on special layered materials called 2D halide perovskites, which are made up of alternating organic and inorganic layers only a few atoms thick. These materials can be tuned at the atomic level to absorb and emit light in precise ways, making them very attractive for use in optoelectronic devices. The main goal of the project was to understand how these perovskite materials absorb light and move electrical charges at very small scales. However, this is not an easy task. These materials often contain a mixture of different structures in the same film, and traditional tools like regular absorption or photoluminescence spectroscopy are not good at telling those structures apart. To solve this, the research team, led by Professor Luisa Whittaker-Brooks at the University of Utah developed a powerful method called electroabsorption spectroscopy. This technique uses electric fields to highlight the unique “fingerprints” of different excitons, which are tiny packets of energy formed when light hits the material. By using this method, the team could separate overlapping signals and learn exactly how the materials respond to light under different conditions, including changes in temperature, thickness, and chemical makeup.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Measure Effects of Molten Halide Salt on Creep Rupture Lifetime for 316H, 709 and 617

Ongoing commercialization of different molten salt reactor concepts can considerably benefit from quantitative information on the impact of molten halide salts on the engineering properties such as creep and fatigue strength of materials of interest. Limited legacy data from the molten salt reactor experiment (MSRE) program showed a significant reduction in creep rupture strength of a Ni-base alloy in molten fluoride salt. This task evaluated the creep behavior of candidate structural materials 316H, 709 and 617 for advanced nuclear reactors under molten halide salt environments at 650, 700 and 750°C respectively. Creep tests were conducted in air, Ar, fluoride (FLiNaK) and chloride (NaCl-MgCl 2 ) salts. The molten salt environment caused a 50% reduction in creep rupture lifetime for 316H in FLiNaK and an 80% reduction in creep rupture lifetime in NaCl-MgCl 2 compared to air exposures. The molten fluoride salt environment resulted in almost a 90% and 50% reduction in creep rupture time for 709 and 617 irrespective of the cover gas environment (air and Ar). Significant differences in the compositional changes between the salt- and air-facing surfaces were observed in the alloy subsurface which might have potentially lead to formation of phases detrimental to the creep behavior.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2026

Melter Tests to Define LAW Halide Concentrations, Phase 2

The present work represents the second of two phases to address the formation of secondary sulfate phases while processing high waste loading LAW formulations with elevated halide, chromium, and phosphate feed concentrations over a wide range of LAW waste types, including those with high potassium concentrations. The Test Plan for the present work outlines a series of tests designed to assess the formation of secondary phases over a range of sulfur and halide concentrations for two LAW streams and associated glass formulations as well as crucible testing to identify additives that have the potential to suppress the formation of secondary phases for wastes with high chlorine contents. The combined results from both phases of testing and from previous tests with these LAW waste streams will be used as inputs to future work to develop concentration limits for these components in the LAW glass property composition models and to support the modification and updating of the current WTP LAW glass formulation algorithm.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Assessing the Impact of Molten Halide Salts on Creep of Structural Alloys at 650°-750°C

There is a critical lack of data on the mechanical behavior of candidate structural materials for advanced nuclear reactors under molten halide salt environments. Limited legacy data from the molten salt reactor experiment (MSRE) program showed a significant reduction in creep rupture strength of a Ni-base alloy in molten fluoride salt. With ongoing efforts to commercialize different molten salt reactor concepts, the industry can considerably benefit from quantitative information on the impact of molten halide salts on the engineering properties such as creep and fatigue strength of materials of interest. The present work aims to assess the role of molten salt corrosion on the creep behavior of three alloys 316H, 617 and 282 at 650-816 °C. Creep tests were conducted in fluoride (FLiNaK) and chloride (NaCl-MgCl2) salts. Initial results from the ongoing testing will be presented which suggest that the molten salt environment caused a 25-50% reduction in creep rupture lifetime compared to air exposures. Physics-based corrosion and creep models were employed to gain some insights into the potential degradation mechanisms.

Pillai, Rishi↗
DOE OSTI2020

Method to synthesize metal halide perovskite particles with high luminescence and stability

The invention provides a convenient solution-based synthesis for metal halide perovskite particles. This method requires only mild conditions and can be easily scaled up. A ligand of a proper molecule size and an optimized precursor ratio are important to obtain pure phase particles. As an example, lead bromide perovskite particles exhibited a narrow monochromatic band gap, which can be tuned by partial halide substitution, and PLQY up to 75% making this material an excellent candidate for light emission and display applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal Disorder‐Induced Strain and Carrier Localization Activate Reverse Halide Segregation

The reversal of halide ions is studied under various conditions. However, the underlying mechanism of heat-induced reversal remains unclear. This work finds that dynamic disorder-induced localization of self-trapped polarons and thermal disorder-induced strain (TDIS) can be co-acting drivers of reverse segregation. Localization of polarons results in an order of magnitude decrease in excess carrier density (polaron population), causing a reduced impact of the light-induced strain (LIS – responsible for segregation) on the perovskite framework. Meanwhile, exposing the lattice to TDIS exceeding the LIS can eliminate the photoexcitation-induced strain gradient, as thermal fluctuations of the lattice can mask the LIS strain. Under continuous 0.1 W cm -2 illumination (upon segregation), the strain disorder is estimated to be 0.14%, while at 80 °C under dark conditions, the strain is 0.23%. However, in situ heating of the segregated film to 80 °C under continuous illumination (upon reversal) increases the total strain disorder to 0.25%, where TDIS is likely to have a dominant contribution. Therefore, the contribution of entropy to the system's free energy is likely to dominate, respectively. Various temperature-dependent in situ measurements and simulations further support the results. These findings highlight the importance of strain homogenization for designing stable perovskites under real-world operating conditions.

36 MATERIALS SCIENCE↗