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DOE OSTI2020

Optoelectronic and material properties of solution-processed Earth-abundant Cu 2 BaSn(S, Se) 4 films for solar cell applications

Copper barium thioselenostannate, Cu 2 BaSnS 4-x Se x (CBTSSe), absorbers employ low-toxicity and abundant metals while offering low-cost manufacturing options, controllable stoichiometry and band gap tunability (from 2 eV at x = 0 to 1.55 eV at x = 3). CBTSSe can therefore be considered a prospective candidate for maintaining or improving upon the advantages of already commercialized Cu(In,Ga)(S,Se) 2 (CIGSSe) and CdTe absorbers. Here, we focus on solution-deposited stoichiometric CBTSSe films with band gap of 1.59 eV (x ≈ 3) and explore the fundamental film properties. Temperature- and excitation-dependent photoluminescence studies reveal a dominant defect emission at ~1.5 eV and a second deep defect feature at 1.15 eV. From time-resolved terahertz measurements, we find a charge carrier (electron and hole sum) mobility of ~140 cm 2 /Vs—i.e., comparable to values in CIGSSe or Cu 2 ZnSnS 4-x Se x (CZTSSe)—as well as a two-component minority carrier lifetime. A longer-lived lifetime component (~2 ns) arises from bulk recombination. However, strong recombination at the (bare) surface leads to a ~50 ps lifetime, inferior to state-of-the-art CIGSSe or CZTSSe absorbers. This recombination issue may worsen for CBTSSe/CdS interfaces, due to a cliff-like band alignment with 0.6 eV band offset, as revealed by ultraviolet photoemission spectroscopy. A low number of charge carriers within the absorber further contributes to a high series resistance. Employing these films, we also report the highest performance achieved from solution-processed trigonal CBTSSe thin-film photovoltaic devices, with open circuit voltage, short-circuit current density, fill factor and efficiency of 470 mV, 14.3 mA/cm 2 , 43.6% and 2.9%, respectively. The physical measurements provided on the stoichiometric solution-processed CBTSSe absorber further point to critical areas for future improvement of CBTSSe and related photovoltaic cells in the quest for higher efficiency devices based on earth abundant metals.

14 SOLAR ENERGY↗

DOE OSTI2020

A Comparison of the Optoelectronic Properties of High-Efficiency Polycrystalline and Epitaxial Cu(In,Ga)Se2 Photovoltaic Films

Over the last several decades, champion photovoltaic (PV) devices using CuInGaSe2 (CIGS) as the absorber material have been achieved using polycrystalline films exclusively. This has led to the assumption that polycrystalline CIGS generally outperform single-crystal CIGS in PV devices. However, recently, very high-quality epitaxial CIGS has been grown on GaAs substrates producing PV device efficiencies of 20.0%. These results have revived the debate on what effects grain boundaries have on PV device efficiencies. In this contribution, we compare the optoelectronic properties of polycrystalline CIGS films with those of high-efficiency epitaxial CIGS films. This comparison reveals that grain boundaries are associated with properties that negatively impact PV device efficiency. Additionally, we find that the grain interiors in polycrystalline films exhibit properties that are similar to the high-performance epitaxial films. Our results suggest that it may be possible to achieve higher device efficiencies with epitaxial CIGS than with polycrystalline films.

41 EE - Solar Energy Technologies Office (EE-4S)↗

DOE OSTI2022

Overcoming Shockley-Queisser limit using halide perovskite platform?

The Intergovernmental Panel on Climate Change (IPCC) reveals that the global temperature has reached its highest level in the last 2,000 years. Development of emissions-free electrification technologies such as photovoltaics (PV) can be a great paramountcy to balance the climate pressure and the growing demand on energy. Although many PV technologies have been demonstrated so far, all the single-junction PVs are still subjected to the well-known efficiency cap of the Shockley-Queisser limit (33.7%), with most of the absorbed solar energy lost into heat. In parallel to delicate system-level designs, such as tandem, multi-junction, photothermal, or up-/down-conversion, we ask the question about the feasibility of overcoming the SQ limit at material level. In this study, we first dissect the origin of the limit, and then, by using the emerging perovskite as the platform, we list several potential pathways (i.e., hot carrier, multi-exciton generation, intermediate band gap, and ferroelectricity that have been newly discovered or can be introduced in the perovskite) to the roadmap of exceeding the SQ limit.

14 SOLAR ENERGY↗

DOE OSTI2024

Complex dislocation loop networks as natural extensions of the sink efficiency of saturated grain boundaries in irradiated metals

The development of radiation-tolerant structural materials is an essential element for the success of advanced nuclear energy concepts. A proven strategy to increase radiation resistance is to create microstructures with a high density of internal defect sinks, such as grain boundaries (GBs). However, as GBs absorb defects, they undergo internal transformations that limit their ability to capture defects indefinitely. Here, we show that, as the sink efficiency of GBs becomes exhausted with increasing irradiation dose, networks of irradiation loops form in the vicinity of saturated or near-saturated GB, maintaining and even increasing their capacity to continue absorbing defects. The formation of these networks fundamentally changes the driving force for defect absorption at GB, from “chemical” to “elastic.” Using thermally-activated dislocation dynamics simulations, we show that these networks are consistent with experimental measurements of defect densities near GB. Our results point to these networks as a natural continuation of the GB once they exhaust their internal defect absorption capacity.

36 MATERIALS SCIENCE↗

NASA NTRS1977

Thermal performance evaluation of Solar Energy Products Company (SEPCO) 'Soloron' collector tested outdoors

The test article, Model EF-212, Serial Nr. 002, is a single glazed collector with a nonselective absorber plate, using flowing air as the heat transfer medium. The absorber plate and box frame are aluminum and the insulation is one inch isocyanurate foam board with thermal conductivity of 0.11 (BTU/sq ft Hr0/ft.) The tests included the following. (1) time constant test, (2) collector efficiency test, (3) collector stagnation test, (4) incident angle modifier test, (5) load test, (6) weathering test, and (7) absorber plate optical properties test. The results of these tests are tabulated, graphed, or otherwise recorded.

Chiou, J., Sr.↗

NASA NTRS1994

Resonant infrared detector with substantially unit quantum efficiency

A resonant infrared detector includes an infrared-active layer which has first and second parallel faces and which absorbs radiation of a given wavelength. The detector also includes a first tuned reflective layer, disposed opposite the first face of the infrared-active layer, which reflects a specific portion of the radiation incident thereon and allows a specific portion of the incident radiation at the given wavelength to reach the infrared-active layer. A second reflective layer, disposed opposite the second face of the infrared-active layer, reflects back into the infrared-active layer substantially all of the radiation at the given wavelength which passes through the infrared-active layer. The reflective layers have the effect of increasing the quantum efficiency of the infrared detector relative to the quantum efficiency of the infrared-active layer alone.

Farhoomand, Jam↗

DOE OSTI2025

Experiments on a vapor compression air conditioner with liquid desiccants for efficient dehumidification

Buildings require air conditioning systems that not only cool and dehumidify supply air but also provide sufficient ventilation to ensure indoor air quality and occupant comfort. However, standard recirculation systems-which introduce about a 10 % to 20 % fraction of outdoor air-often fail to deliver air that is precisely cooled and dry, particularly because 80-90 % of the ventilation cooling load is latent. Mixing humid ventilation air with recirculated indoor air increases the energy and costs required to condition the air to comfortable levels. Dedicated outdoor air systems (DOASs) are designed to handle this latent dominated ventilation load and thus need to have efficient humidity removal. Many cooling cycles can perform this task. Here we describe a liquid desiccant DOAS, which combines a vapor compression cycle and a liquid desiccant absorber and desorber pair. We present its performance at 26 operating conditions and a thermodynamic model which can accurately predict the moisture removal efficiency. The model's performance predictions have a mean percentage error of 2.5 % and a coefficient of variation of the root mean square error of 7.5 %. We also compare the performance of this vapor-compression-coupled liquid desiccant system with a standard vapor compression system with the same components but no liquid desiccant. For the 26 conditions tested in this study, this comparison shows that adding liquid desiccants lowers the required evaporator cooling load by 21 %, allows for 25 % lower compressor volumetric capacity, and 25 % lower electricity use. Future work will leverage this model to quantify the reduction in annual electricity use across different climates, including the need for a standard vapor compression system to reheat the air during some of the year.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2021

Design of High-Performance Lead-Free Quaternary Antiperovskites for Photovoltaics via Ion Type Inversion and Anion Ordering

The emergence of halide double perovskites significantly increases the compositional space for lead-free and air-stable photovoltaic absorbers compared to halide perovskites. Nevertheless, most halide double perovskites exhibit oversized band gaps (>1.9 eV) or dipole-forbidden optical transition, which are unfavorable for efficient single-junction solar cell applications. The current device performance of halide double perovskite is still inferior to that of lead-based halide perovskites, such as CH 3 NH 3 PbI 3 (MAPbI 3 ). Here, by ion type inversion and anion ordering on perovskite lattice sites, two new classes of pnictogen-based quaternary antiperovskites with the formula of X 6 B 2 AA' and X 6 BB'A 2 are designed. Phase stability and tunable band gaps in these quaternary antiperovskites are demonstrated based on first-principles calculations. Further photovoltaic-functionality-directed screening of these materials leads to the discovery of 5 stable compounds (Ca 6 N 2 AsSb, Ca 6 N 2 PSb, Sr 6 N 2 AsSb, Sr 6 N 2 PSb, and Ca 6 NPSb 2 ) with suitable direct band gaps, small carrier effective masses and low exciton binding energies, and dipole-allowed strong optical absorption, which are favorable properties for a photovoltaic absorber material. The calculated theoretical maximum solar cell efficiencies based on these five compounds are all larger than 29%, comparable to or even higher than that of the MAPbI 3 based solar cell. Finally, our work reveals the huge potential of quaternary antiperovskites in the optoelectronic field and provides a new strategy to design lead-free and air-stable perovskite-based photovoltaic absorber materials.

three-dimensional electronic transport↗

DOE OSTI2023

Quantum efficiency enhancement in simulated nanostructured negative electron affinity GaAs photocathodes

We report nanostructured negative electron affinity GaAs photocathodes for a polarized electron source are studied using finite difference time domain optical simulation. The structures studied are nanosquare columns, truncated nanocones, and truncated nanopyramids. Mie-type resonances in the 700–800 nm waveband, suitable for generation of polarized electrons, are identified. At resonance wavelengths, the nanostructures can absorb up to 99% of the incident light. For nanosquare columns and truncated nanocones, the maximum quantum efficiency (QE) at 780 nm obtained from simulation is 27%, whereas for simulated nanopyramids, the QE is ~21%. The high photocathode quantum efficiency is due to the shift of Mie resonance toward the longer wavelength, leading to increased light absorption. The field profile distribution shows the excitation of dipole and quadrupole modes within the nanostructures at resonant frequencies. This leads to enhanced photoabsorption and photoelectron generation closer to emission surfaces than for a flat photocathode. The enhanced photoabsorption and reduced electron transport distance for the nanostructured photocathode enhance its QE compared to that for the flat surface wafer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2007

Design and Fabrication of High-Efficiency CMOS/CCD Imagers

An architecture for back-illuminated complementary metal oxide/semiconductor (CMOS) and charge-coupled-device (CCD) ultraviolet/visible/near infrared- light image sensors, and a method of fabrication to implement the architecture, are undergoing development. The architecture and method are expected to enable realization of the full potential of back-illuminated CMOS/CCD imagers to perform with high efficiency, high sensitivity, excellent angular response, and in-pixel signal processing. The architecture and method are compatible with next-generation CMOS dielectric-forming and metallization techniques, and the process flow of the method is compatible with process flows typical of the manufacture of very-large-scale integrated (VLSI) circuits. The architecture and method overcome all obstacles that have hitherto prevented high-yield, low-cost fabrication of back-illuminated CMOS/CCD imagers by use of standard VLSI fabrication tools and techniques. It is not possible to discuss the obstacles in detail within the space available for this article. Briefly, the obstacles are posed by the problems of generating light-absorbing layers having desired uniform and accurate thicknesses, passivation of surfaces, forming structures for efficient collection of charge carriers, and wafer-scale thinning (in contradistinction to diescale thinning). A basic element of the present architecture and method - the element that, more than any other, makes it possible to overcome the obstacles - is the use of an alternative starting material: Instead of starting with a conventional bulk-CMOS wafer that consists of a p-doped epitaxial silicon layer grown on a heavily-p-doped silicon substrate, one starts with a special silicon-on-insulator (SOI) wafer that consists of a thermal oxide buried between a lightly p- or n-doped, thick silicon layer and a device silicon layer of appropriate thickness and doping. The thick silicon layer is used as a handle: that is, as a mechanical support for the device silicon layer during micro-fabrication.

Pain, Bedabrata↗

DOE OSTI2023

CdTe-based thin film photovoltaics: Recent advances, current challenges and future prospects

Cadmium telluride (CdTe)-based cells have emerged as the leading commercialized thin film photovoltaic technology and has intrinsically better temperature coefficients, energy yield, and degradation rates than Si technologies. More than 30 GW peak (GWp) of CdTe-based modules are installed worldwide, multiple companies are in production, modules are shipping at up to 18.6% efficiency, and lab cell efficiency is above 22%. We review developments in the science and technology that have occurred over approximately the past decade. These achievements were enabled by manufacturing innovations and scaling module production, as well as maximizing photocurrent through window layer optimization and alloyed CdSe x Te 1-x (CST) absorbers. Improved chlorine passivation processes, film microstructure, and serendipitous Se defect passivation significantly increased minority carrier lifetime. Efficiencies >22% have been realized for both Cu and As doped CST-based cells. The path to further efficiency gains hinges primarily on increasing open circuit voltage (V oc ) and fill factor (FF) through innovations in materials, fabrication methods, and device stacks. Replacing the longstanding Cu doping with As doping is resulting in better module stability and is being translated to large-scale production. To realize 25% efficiency and >1 V V oc , research and development is needed to increase the minority carrier lifetime beyond 100 ns, reduce grain boundary and interface recombination, and tailor band diagrams at the front and back interfaces. Many of these goals have been realized separately however combining them together using scalable manufacturing approaches has been elusive to date. We review these achievements and outstanding opportunities for this remarkable photovoltaic technology.

14 SOLAR ENERGY↗

DOE OSTI2020

Visible-Light-Driven Triplet Sensitization of Polycyclic Aromatic Hydrocarbons Using Thionated Perinones

Metal-free chromophores that efficiently generate triplet excited states represent enticing alternatives with respect to transition metal-containing photosensitizers, such as those featuring metal-to-ligand charge transfer excited states. Yet, such molecular constructs have remained underexplored due to the unclear relationship(s) between molecular structure and efficient/rapid intersystem crossing. In this regard, we present a series of three thionated perinone chromophores serving as a newly conceived class of heavy metal-free triplet photosensitizers. We demonstrate that thionation of the lone C=O substituent in each highly fluorescent perinone imparts red-shifted absorbance bands that maintain intense extinction coefficients across the visible spectrum, as well as unusually efficient triplet excited state formation as inferred from the measured singlet O 2 quantum yields at 1270 nm (Φ Δ = 0.78–1.0). Electronic structure calculations revealed the emergence of a low energy S 1 (n → π*) excited state in the proximity of a slightly higher energy S 2 (π → π*) excited state. The distinct character in each of the two lowest-lying singlet state manifolds resulted in the energetic inversion of the corresponding triplet excited states due to differences in electron exchange interactions. Rapid S 1 → T 1 intersystem crossing was thereby facilitated in this manner through spin–orbit coupling as predicted by the El Sayed rules. The lifetimes of the resultant triplet excited states persisted into the microsecond time regime, as measured by transient absorbance spectroscopy, enabling effective bimolecular triplet sensitization of some common polycyclic aromatic hydrocarbons. The synthetically facile interchange of a single O atom to an S atom in the investigated perinones resulted in marked changes to their photophysical properties, namely, conversion of dominant singlet state fluorescence in the former to long-lived triplet excited states in the latter. The combined results suggest a general strategy for accessing long-lived triplet excited states in organic chromophores featuring a lone C=O moiety residing within its structure, valuable for the design of metal-free triplet photosensitizers.

14 SOLAR ENERGY↗

DOE OSTI2022

Mix and match light absorbers

Here, perovskite and organic semiconductors can be combined to make tandem solar cells but, to date, their efficiency has hovered around 20%. Now, researchers demonstrate a 23.6% tandem by reducing interfacial defects to improve the perovskite cell's voltage and developing an ultrathin interconnection layer.

14 SOLAR ENERGY↗

DOE OSTI2026

Understanding Defect Activation and Kinetics in Next Generation CdTe Absorbers

This project investigated the role of defects and dopants in cadmium telluride (CdTe) solar cells to improve efficiency and long-term stability. Advanced X-ray microscopy and spectroscopy techniques were used to map composition, identify defect structures, and measure charge collection at the nanoscale. These experimental results were combined with computational modeling to understand how dopants such as copper and arsenic interact with other elements during processing. The study found that many dopants become electrically inactive due to the formation of complexes with chlorine and oxygen, limiting carrier concentration and device performance. It also showed that selenium, used to enhance efficiency, can migrate within the material during both manufacturing and operation, altering local structure and potentially affecting stability. The project developed new diagnostic and analysis tools for studying photovoltaic materials and provided a mechanistic understanding of key performance limitations. These insights support the development of more efficient, stable, and cost-effective CdTe solar technologies for large-scale energy deployment.

14 SOLAR ENERGY↗

DOE OSTI2023

Tracking Photochemical and Photophysical Processes for Solar Energy Conversion Via Multidimensional Visible and Vibrational Spectroscopic Methods

This project was motivated by an overarching goal to elucidate the mechanism of energy and electron transfer that governs the efficient charge separation in photosystem I (PSI) complexes. PSI is a natural light harvesting complex that drives oxygenic photosynthesis in plants, algae, and cyanobacteria. It uses ~300 tightly packed chlorophylls (Chls) to absorb photons, transfer the excitation energy to the reaction center (RC), and generate a charge separated state with near unity quantum efficiency (QE). A better understanding of the mechanism of energy transfer and charge separation in PSI is required for understanding the high QE of natural light harvesting complexes, and it could lead to the further development of artificial photosynthetic systems for solar energy conversion. We applied two-dimensional electronic spectroscopy (2DES) to different cyanobacterial photosystem I complexes to map energy transfer pathways to gain insight into the efficient light harvesting of PSI. We interpreted the 2DES spectra through a global analysis procedure, finding two ultrafast equilibration processes involving red-shifted Chl states. The analysis procedure is general and can be readily applied to other natural and artificial light harvesting systems. In addition to investigating PSI complexes, we also performed measurements on model systems to establish general data analysis procedures for interpreting 2D spectra.

14 SOLAR ENERGY↗

DOE OSTI2024

Elucidating Photoinduced Processes of Photosystem I Via Multidimensional Electronic and Vibrational Spectroscopies

This project was motivated by an overarching goal to elucidate the mechanism of energy and electron transfer that governs the efficient charge separation in photosystem I (PSI) complexes. PSI is a natural light harvesting complex that drives oxygenic photosynthesis in plants, algae, and cyanobacteria. It uses ~300 tightly packed chlorophylls (Chls) to absorb photons, transfer the excitation energy to the reaction center (RC), and generate a charge separated state with near unity quantum efficiency (QE). A better understanding of the mechanism of energy transfer and charge separation in PSI is required for understanding the high QE of natural light harvesting complexes, and it could lead to the further development of artificial photosynthetic systems for solar energy conversion and modification of light harvesting complexes to improve crop yields. We applied two-dimensional optical spectroscopies to different cyanobacterial photosystem I complexes, including PSI complexes that contain Chl f molecules, to map energy transfer pathways and gain insight into the efficient light harvesting of PSI. We used two-dimensional electronic spectroscopies (2DES) to map energy transfer in Chl a and Chl f containing PSI complexes. To investigate the Chl f PSI complexes, we modified our spectrometer to probe the lower energy states associated with Chl f molecules. We interpreted the 2DES spectra through global analysis procedures to generate maps of energy transfer. We also constructed a two-dimensional electronic vibrational (2DEV) spectrometer that will be used to investigate charge transfer transitions and dynamics within PSI complexes. Measurements were performed on model systems to establish general data analysis procedures for interpreting 2D spectra and gain insight into protein cofactor interactions.

14 SOLAR ENERGY↗

NASA NTRS1989

Roughening Surfaces Of Solar Cells

Proposed treatment involving bombardment by ions gives silicon solar cells rough surfaces and increases amount of light absorbed by cells. First step of treatment, wafer of single-crystal silicon held at temperature of 70 degree C or higher while bombarded with argon or hydrogen ions at kinetic energies between 100 and 2,000 eV. This high dose produces damaged layer on surface, consisting of outer polycrystalline sublayer and underlying sublayer containing extended defects. Bombarded wafer then etched chemically. Photovoltaic conversion efficiency increases with number of reflections at surface of silicon cell because large part of light absorbed at each reflection. Deeply textured surface provides opportunities for multiple reflections.

Singh, Ranbir↗

DOE OSTI2022

Grain boundary strain as a determinant of localized sink efficiency

The opportunity to achieve radiation tolerance in crystalline materials hinges on understanding the structure and response of grain boundary sinks to irradiation. A common descriptor of grain boundary efficiency as a defect sink is the denuded zone, which is a defect free zone adjacent to the grain boundary dictated by its ability to absorb radiation induced defects. This descriptor is often used at the mesoscale, which requires an averaging of absorption events. In this paper, we resolve the defect sink efficiency as a function of interfacial strain with respect to grain boundary character, and correlate high levels of grain boundary strain to an enhanced absorption efficiency. Here, we also introduce a key relationship between localized strain in proximity with the grain boundary sink and the variation absorption efficiency associated with these regions, revealing the pitfalls of averaging absorption events along a grain boundary, and presenting a path forward toward improved models for denuded zones and localized grain boundary absorption phenomena.

36 MATERIALS SCIENCE↗