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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Experimental investigation on structures and velocity of liquid jets in a supersonic crossflow

Particle image velocimetry was applied in the study focusing on the structure and velocity of water jets injected into a Ma = 2.1 crossflow. The instantaneous structures of the jet, including surface waves in the near-injector region and vortices in the far-field, were visualized clearly. Spray velocity increases rapidly to 66% of the mainstream velocity in the region of x/d < 15, owing to the strong gas-liquid interaction near the orifice. By contrast, the velocity grows slowly in the far-field region, where the liquid inside the spray is accelerated mainly by the continuous driven force provided by the mainstream with the gas-liquid shear. The injection and atomization of liquid jet in a supersonic crossflow serves as a foundation of scramjet combustion process, by affecting the combustion efficiency and some other performances. With various forces acting on the liquid jet (Mashayek et al. [AIAA J. 46, 2674–2686 (2008)] and Wang et al. [AIAA J. 50, 1360–1366 (2012)]), the atomization process involves very complex flow physics. These physical processes include strong vortical structures, small-scale wave formation, stripping of small droplets from the jet surface, formations of ligaments, and droplets with a wide range of sizes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Thermodynamically leveraged solventless aerobic deconstruction of polyethylene-terephthalate plastics over a single-site molybdenum-dioxo catalyst

Here, we describe the solventless catalytic deconstruction of polyethylene-terephthalate (PET) under an aerobic atmosphere, mediated by an earth-abundant, low-cost activated carbon (AC)-supported single-site molybdenum-dioxo catalyst (AC/MoO 2 ). Catalytic amounts of AC/MoO 2 selectively convert waste PET into its monomer, terephthalic acid (TPA), within 4 h at 265 °C with yields as high as 94% under 1 atm air. Pure crystalline TPA product sublimes from the reaction hot zone, crystallizing on the reactor cold zone, thus avoiding the need for separation and purification steps. This process does not employ any hazardous/toxic reducing agents or solvents, and the catalyst can be recycled multiple times without loss of activity, rendering this process highly atom-efficient. According to computational and experimental mechanistic studies, the AC/MoO 2 catalyst mediates a thermoneutral metal-catalyzed β-scission step, followed by an exothermic step that converts the vinyl benzoate intermediate to TPA and acetaldehyde using trace amounts of moisture in the air. The formation of gaseous acetaldehyde makes the isolation of TPA from the reaction mixture facile and industrially favorable, especially since solvents are unnecessary. The present methodology is also extended to the deconstruction of other frequently used polyester plastics, polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), and polyethylene furanoate (PEF), and operates equally well with post-consumer waste products. Notably, this process is also compatible with plastic mixtures of polyesters with polyolefins, polyamides, and polycarbonates, leading to the selective conversion of each polyester to the corresponding monomer, leaving the residual polymer unchanged and polyester-free.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage

Crystalline defects are commonly generated in lithium-metal-oxide electrodes during cycling of lithium-ion batteries. Their role in electrochemical reactions is not yet fully understood because, until recently, there has not been an effective operando technique to image dynamic processes at the atomic level. In this study, two types of defects were monitored dynamically during delithiation and concomitant oxidation of oxygen ions by using in situ high-resolution transmission electron microscopy supported by density functional theory calculations. One stacking fault with a fault vector b/6[110] and low mobility contributes minimally to oxygen release from the structure. In contrast, dissociated dislocations with Burgers vector of c/2[001] have high gliding and transverse mobility; they lead to the formation, transport and release subsequently of oxygen related species at the surface of the electrode particles. This work advances the scientific understanding of how oxygen participates and the structural response during the activation process at high potentials.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Perspective: Size selected clusters for catalysis and electrochemistry

We report that size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this Perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition, cluster-support interactions and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modelling based on density functional theory sampling of local minima and energy barriers or ab initio Molecular Dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Lastly, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Molecular dynamics study of silicon atomic layer etching by chlorine gas and argon ions

Classical molecular dynamics (MD) is used to simulate atomic layer etching processes of silicon by alternating exposure to chlorine gas and argon ions. In order to validate our model, a rigorous comparison is done with ion beam experiments found in the literature [Park et al., Jpn. J. Appl. Phys. 44, 389 (2005)]. Here it is shown that the etch per cycle (EPC) as a function of argon ion energy from simulations is in quantitative agreement with experimental results if the correct argon ion fluence is used in the simulations. The EPC as a function of ion irradiation time and amount of chlorine exposure also show good agreement with the experiment. The MD simulations also show the formation of an amorphous silicon region with chlorine atoms mixed uniformly throughout following ion bombardment. Finally, the etch products during the ion irradiation step are analyzed and discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Half-life determination of heavy ions in a storage ring considering feeding and depleting background processes

Heavy-ion storage rings have relatively large momentum acceptance which allows for multiple ion species to circulate at the same time. This needs to be considered in radioactive decay measurements of highly charged ions, where atomic charge exchange reactions can significantly alter the intensities of parent and daughter ions. In this study, we investigate this effect using the decay curves of ion numbers in the recent 205 Tl 81+ bound-state beta decay experiment conducted using the Experimental Storage Ring at GSI Darmstadt. To understand the intricate dynamics of ion numbers, we present a set of differential equations that account for various atomic and nuclear reaction processes—bound state beta decay, atomic electron recombination and capture, and electron ionization. By incorporating appropriate boundary conditions, we develop a set of differential equations that accurately simulate the decay curves of various simultaneously stored ions in the storage ring: 205 Tl 81+ , 205 Pb 81+ , 205 Pb 82+ , 200 Hg 79+ , and 200 Hg 80+ . Through a quantitative comparison between simulations and experimental data, we provide insights into the detailed reaction mechanisms governing stored heavy ions within the storage ring. Our approach effectively models charge-changing processes, reduces the complexity of the experimental setup, and provides a simpler method for measuring the decay half-lives of highly charged ions in storage rings.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Titanium Disulfide Coated Carbon Nanotube Hybrid Electrodes Enable High Energy Density Symmetric Pseudocapacitors

While electrochemical supercapacitors often show high power density and long operation lifetimes, they are plagued by limited energy density. Pseudocapacitive materials, in contrast, operate by fast surface redox reactions and are shown to enhance energy storage of supercapacitors. Furthermore, several reported systems exhibit high capacitance but restricted electrochemical voltage windows, usually no more than 1 V in aqueous electrolytes. Here, it is demonstrated that vertically aligned carbon nanotubes (VACNTs) with uniformly coated, pseudocapacitive titanium disulfide (TiS 2 ) composite electrodes can extend the stable working range to over 3 V to achieve a high capacitance of 195 F g -1 in an Li-rich electrolyte. A symmetric cell demonstrates an energy density of 60.9 Wh kg -1 —the highest among symmetric pseudocapacitors using metal oxides, conducting polymers, 2D transition metal carbides (MXene), and other transition metal dichalcogenides. Nanostructures prepared by an atomic layer deposition/sulfurization process facilitate ion transportation and surface reactions to result in a high power density of 1250 W kg -1 with stable operation over 10 000 cycles. In conclusion, a flexible solid-state supercapacitor prepared by transferring the TiS 2 –VACNT composite film onto Kapton tape is demonstrated to power a 2.2 V light emitting diode (LED) for 1 min.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Dissociation energies of Ag–RG (RG = Ar, Kr, Xe) and AgO molecules from velocity map imaging studies

The near ultraviolet photodissociation dynamics of silver atom—rare gas dimers have been studied by velocity map imaging. Ag–RG (RG = Ar, Kr, Xe) species generated by laser ablation are excited in the region of the C ({sup 2}Σ{sup +})←X ({sup 2}Σ{sup +}) continuum leading to direct, near-threshold dissociation generating Ag* ({sup 2}P{sub 3/2}) + RG ({sup 1}S{sub 0}) products. Images recorded at excitation wavelengths throughout the C ({sup 2}Σ{sup +})←X ({sup 2}Σ{sup +}) continuum, coupled with known atomic energy levels, permit determination of the ground X ({sup 2}Σ{sup +}) state dissociation energies of 85.9 ± 23.4 cm{sup −1} (Ag–Ar), 149.3 ± 22.4 cm{sup −1} (Ag–Kr), and 256.3 ± 16.0 cm{sup −1} (Ag–Xe). Three additional photolysis processes, each yielding Ag atom photoproducts, are observed in the same spectral region. Two of these are markedly enhanced in intensity upon seeding the molecular beam with nitrous oxide, and are assigned to photodissociation of AgO at the two-photon level. These features yield an improved ground state dissociation energy for AgO of 15 965 ± 81 cm{sup −1}, which is in good agreement with high level calculations. The third process results in Ag atom fragments whose kinetic energy shows anomalously weak photon energy dependence and is assigned tentatively to dissociative ionization of the silver dimer Ag{sub 2}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

UPDATED ATOMIC DATA AND CALCULATIONS FOR X-RAY SPECTROSCOPY

We describe the latest release of AtomDB, version 2.0.2, a database of atomic data and a plasma modeling code with a focus on X-ray astronomy. This release includes several major updates to the fundamental atomic structure and process data held within AtomDB, incorporating new ionization balance data, state-selective recombination data, and updated collisional excitation data for many ions, including the iron L-shell ions from Fe{sup +16} to Fe{sup +23} and all of the hydrogen- and helium-like sequences. We also describe some of the effects that these changes have on calculated emission and diagnostic line ratios, such as changes in the temperature implied by the He-like G-ratios of up to a factor of two.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Imaging Valley Excitons in a 2D Semiconductor with Scanning Tunneling Microscope-Induced Luminescence

Valley excitons dominate the optoelectronic response of transition-metal dichalcogenides and are drastically affected by structural and environmental inhomogeneities localized in these materials. Critical to understanding and controlling these nanoscale excitonic changes is the ability to correlate the imaging of excitonic states with crystalline structures on the atomic scale. Here, in this study, we apply scanning tunneling microscope-induced luminescence microscopy to image valley excitons in a semiconducting transition-metal dichalcogenide monolayer decoupled by a 10 nanometer-thick hexagonal-boron-nitride flake incorporated in a lateral homojunction on an Au electrode surface. This design enables the observation of chiral excitonic emission arising from neutral and charged valley excitons of the monolayer semiconductor at ambipolar voltages with a quantum efficiency up to similar to ~10 -5 photon/electron. The measured light helicity demonstrates considerable circular polarization dependent on the sample voltage, reaching as much as 40%. The real-space luminescence imaging maps$-$at subnanometer resolution$-$of the valley excitons reveal striking spatial variations associated with localized inhomogeneities, including surface impurities and possibly nanoscale dielectric and/or potential disorders in the monolayer. Our study introduces a promising format for 2D materials to explore and tailor their optoelectronic processes at the atomic scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

ADVANCING TURBULENT SPRAY AND COMBUSTION MODELS FOR COMPRESSION IGNITION ENGINE SIMULATIONS

This thesis seeks to investigate the turbulent mixing influence on spray atomization and combustion processes encountered in compression ignition diesel engines. Despite greater thermal efficiency of diesel engine than spark ignition engine, the nature of stratified air-fuel mixture and non-premixed flame gives rise to unacceptable levels of nitrogen oxides (NOx) and particulate matter (PM), thus the use of diesel engines has often been limited to heavy-duty vehicle and industrial power sources. However, recent advancement in diesel engine combustion strategies, e.g. low temperature combustion (LTC), has demonstrated promising pathways towards improvement in the engine-out pollutants. Therefore, particularly in the effort of computer-aided engine design tasks, such a new engine design concept requires more accurate modeling techniques applicable over a broader range of engine operating conditions than those of conventional engine strategies. In the notion of challenges in new engine operating conditions, this thesis aims to present successful implementation of improvement in numerical modeling techniques in high-pressure spray atomization and resulting turbulent spray flame of interest. Three-dimensional Computational Fluid Dynamics (CFD) in in-cylinder turbulent combustion is considered an integral part of engine design progress, but rather a cost-prohibitive to apply over a broad range of engine relevant conditions. In spite of successful use of existing spray atomization modeling, prior researchers have pointed out some degree of failure in LTC targeted injection strategies. Furthermore, finite rate and strong nonlinearity of chemistry influenced by local turbulent mixing still remain in challenges to account for in cost-efficient CFD analysis. In this context, a new attempt of hybrid spray primary breakup modeling is presented and demonstrated in successful application aimed at LTC technique. In addition, the Representative Interactive Flamelets (RIF) model with aid of multi-flamelets approach is extensively assessed in terms of predictive capability against classical combustion model. The combustion model employed in this study are fully examined in the general diesel combustion metric, e.g., ignition delay and flame lift-off length as well as newly suggested test metric, combustion recession. The combustion recession has been recently idenfied, but still remain largely unknown. Since the governing physics of this phenomenon is characterized by turbulent mixing coupled with finite rate chemistry, this can be considered as a relevant test metric for turbulent combustion models. In addition, very recent experimental studies have introduced a new non-sooting diesel combustion technique by manipulating direct injection method. The ducted fuel injection (DFI) has thus been demonstrated with its potential of low soot emissions. Knowing that the duct equipped ahead of injector nozzle was identifed to enhance turbulent mixing, investigations of DFI combustion may prove the effectiveness of turbulece-chemistry interaction modeling. This thesis presents comprehensive understandings of aformentioned diesel combustion techniques in terms of several important physics keywords, e.g., turbulent mixing and detailed chemistry.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2019

Advancing Turbulent Spray and Combustion Models for Compression Ignition Engine Simulations

This thesis seeks to investigate the turbulent mixing influence on spray atomization and combustion processes encountered in compression ignition diesel engines. Despite greater thermal efficiency of diesel engine than spark ignition engine, the nature of stratified air-fuel mixture and non-premixed flame gives rise to unacceptable levels of nitrogen oxides (NOx) and particulate matter (PM), thus the use of diesel engines has often been limited to heavy-duty vehicle and industrial power sources. However, recent advancement in diesel engine combustion strategies, e.g. low temperature com-bustion (LTC), has demonstrated promising pathways towards improvement in the engine-out pollutants. Therefore, particularly in the effort of computer-aided en-gine design tasks, such a new engine design concept requires more accurate modeling techniques applicable over a broader range of engine operating conditions than those of conventional engine strategies. In the notion of challenges in new engine operat-ing conditions, this thesis aims to present successful implementation of improvement in numerical modeling techniques in high-pressure spray atomization and resulting turbulent spray flame of interest. Three-dimensional Computational Fluid Dynamics (CFD) in in-cylinder turbu-lent combustion is considered an integral part of engine design progress, but rather a cost-prohibitive to apply over a broad range of engine relevant conditions. In spite of successful use of existing spray atomization modeling, prior researchers have pointed out some degree of failure in LTC targeted injection strategies. Furthermore, finite rate and strong nonlinearity of chemistry influenced by local turbulent mixing still re-main in challenges to account for in cost-efficient CFD analysis. In this context, a new attempt of hybrid spray primary breakup modeling is presented and demonstrated in successful application aimed at LTC technique. In addition, the Representative Interactive Flamelets (RIF) model with aid of multi-flamelets approach is extensively assessed in terms of predictive capability against classical combustion model. The combustion model employed in this study are fully examined in the general diesel combustion metric, e.g., ignition delay and flame lift-off length as well as newly sug-gested test metric, combustion recession. The combustion recession has been recently idenfied, but still remain largely unknown. Since the governing physics of this phe-nomenon is characterized by turbulent mixing coupled with finite rate chemistry, this can be considered as a relevant test metric for turbulent combustion models. In ad-dition, very recent experimental studies have introduced a new non-sooting diesel combustion technique by manipulating direct injection method. The ducted fuel in-jection (DFI) has thus been demonstrated with its potential of low soot emissions. Knowing that the duct equipped ahead of injector nozzle was identifed to enhance turbulent mixing, investigations of DFI combustion may prove the effectiveness of turbulece-chemistry interaction modeling. This thesis presents comprehensive under-standings of aformentioned diesel combustion techniques in terms of several important physics keywords, e.g., turbulent mixing and detailed chemistry

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2015

Theoretical modeling of the plasma-assisted catalytic growth and field emission properties of graphene sheet

A theoretical modeling for the catalyst-assisted growth of graphene sheet in the presence of plasma has been investigated. It is observed that the plasma parameters can strongly affect the growth and field emission properties of graphene sheet. The model developed accounts for the charging rate of the graphene sheet; number density of electrons, ions, and neutral atoms; various elementary processes on the surface of the catalyst nanoparticle; surface diffusion and accretion of ions; and formation of carbon-clusters and large graphene islands. In our investigation, it is found that the thickness of the graphene sheet decreases with the plasma parameters, number density of hydrogen ions and RF power, and consequently, the field emission of electrons from the graphene sheet surface increases. The time evolution of the height of graphene sheet with ion density and sticking coefficient of carbon species has also been examined. Some of our theoretical results are in compliance with the experimental observations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

On the radiolysis of ethylene ices by energetic electrons and implications to the extraterrestrial hydrocarbon chemistry

The chemical processing of ethylene ices (C{sub 2}H{sub 4}) by energetic electrons was investigated at 11 K to simulate the energy transfer processes and synthesis of new molecules induced by secondary electrons generated in the track of galactic cosmic ray particles. A combination of Fourier transform infrared spectrometry (solid state) and quadrupole mass spectrometry (gas phase) resulted in the identification of six hydrocarbon molecules: methane (CH{sub 4}), the C2 species acetylene (C{sub 2}H{sub 2}), ethane (C{sub 2}H{sub 6}), the ethyl radical (C{sub 2}H{sub 5}), and—for the very first time in ethylene irradiation experiments—the C4 hydrocarbons 1-butene (C{sub 4}H{sub 8}) and n-butane (C{sub 4}H{sub 10}). By tracing the temporal evolution of the newly formed molecules spectroscopically online and in situ, we were also able to fit the kinetic profiles with a system of coupled differential equations, eventually providing mechanistic information, reaction pathways, and rate constants on the radiolysis of ethylene ices and the inherent formation of smaller (C1) and more complex (C2, C4) hydrocarbons involving carbon-hydrogen bond ruptures, atomic hydrogen addition processes, and radical-radical recombination pathways. We also discuss the implications of these results on the hydrocarbon chemistry on Titan's surface and on ice-coated, methane-bearing interstellar grains as present in cold molecular clouds such as TMC-1.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2012

COLLISIONLESS SHOCKS IN A PARTIALLY IONIZED MEDIUM. I. NEUTRAL RETURN FLUX AND ITS EFFECTS ON ACCELERATION OF TEST PARTICLES

A collisionless shock may be strongly modified by the presence of neutral atoms through the processes of charge exchange between ions and neutrals and ionization of the latter. These two processes lead to exchange of energy and momentum between charged and neutral particles both upstream and downstream of the shock. In particular, neutrals that suffer a charge exchange downstream with shock-heated ions generate high-velocity neutrals that have a finite probability of returning upstream. These neutrals might then deposit heat in the upstream plasma through ionization and charge exchange, thereby reducing the fluid Mach number. A consequence of this phenomenon, which we refer to as the neutral return flux, is a reduction of the shock compression factor and the formation of a shock precursor upstream. The scale length of the precursor is determined by the ionization and charge-exchange interaction lengths of fast neutrals moving toward upstream infinity. In the case of a shock propagating in the interstellar medium, the effects of ion-neutral interactions are especially important for shock velocities <3000 km s{sup -1}. Such propagation velocities are common among shocks associated with supernova remnants, the primary candidate sources for the acceleration of Galactic cosmic rays. We then investigate the effects of the return flux of neutrals on the spectrum of test particles accelerated at the shock. We find that, for shocks slower than {approx}3000 km s{sup -1}, the particle energy spectrum steepens appreciably with respect to the naive expectation for a strong shock, namely, {proportional_to}E{sup -2}.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Spectral diagnostics based on Doppler-broadened H{sub α} line shape in a single element of a matrix source

The study is on optical emission spectroscopy diagnostics of a single element of a matrix source of negative hydrogen ions. The method developed for description of the hydrogen atoms behaviour is based on analysis of the Balmer H{sub α} line profile, and it can be readily applied to various low pressure hydrogen discharges. The present observations reveal the existence of thermal as well as of non-thermal fast hydrogen atoms in the discharge. For processing of the experimental data a line shape model, which accounts for details of the plasma kinetics and the fine structure of the Balmer lines is developed. The fit of this model to the recorded at different experimental conditions line shapes results in the temperature of the thermal atoms, the mean energy of the fast atoms, the ratio between the densities of these two group of atoms and the relative populations of the fine structure components of the n = 3 hydrogen state. The present study indicates that the reactions leading to production of fast atoms and the process of energy exchange between thermal and fast atoms may be important for the correct modeling of the plasma kinetics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Kinetically Controlled Fabrication of Single‐Crystalline TiO 2 Nanobrush Architectures with High Energy {001} Facets

This study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single‐crystalline anatase TiO 2 nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface‐smoothing processes. High‐resolution scanning transmission electron microscopy data reveal that defect‐mediated aggregation is the key to TiO 2 nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growth of the single‐crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials

Application of zinc‐blende‐related chalcogenide absorbers such as CdTe and Cu(In,Ga)Se 2 (CIGSe) has enabled remarkable advancement in laboratory‐ and commercial‐scale thin‐film photovoltaic performance; however concerns remain regarding the toxicity (CdTe) and scarcity (CIGSe/CdTe) of the constituent elements. Recently, kesterite‐based Cu 2 ZnSn(S,Se) 4 (CZTSSe) materials have emerged as attractive non‐toxic and earth‐abundant absorber candidates. Despite the similarities between CZTSSe and CIGSe/CdTe, the record power conversion efficiency of CZTSSe solar cells (12.6%) remains significantly lower than that of CIGSe (22.6%) and CdTe (22.1%) devices, with the performance gap primarily being attributed to cationic disordering and associated band tailing. To capture the promise of kesterite‐like materials as prospective “drop‐in” earth‐abundant replacements for closely‐related CIGSe, current research has focused on several key directions to control disorder, including: (i) examination of the interaction between processing conditions and atomic site disorder, (ii) isoelectronic cation substitution to introduce ionic size mismatch, and (iii) structural diversification beyond the zinc‐blende‐type coordination environment. In this review, recent efforts targeting accurate identification and engineering of anti‐site disorder in kesterite‐based CZTSSe are considered. Lessons learned from CZTSSe are applied to other complex chalcogenide semiconductors, in an effort to develop promising pathways to avoid anti‐site disordering and associated band tailing in future high‐performance earth‐abundant photovoltaic technologies.

Shin, Donghyeop↗