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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Room temperature slot-die coated perovskite layer modified with sulfonyl-γ-AApeptide for high performance perovskite solar devices

Perovskite solar cells (PSCs) exhibited remarkable progress for small aperture area cells, however, the performance of its counterpart, large aperture area cells, lags due to non-uniform and defective perovskite layers. Here, we fabricate reproducible large area homogeneous perovskite films at room temperature and without controlling humidity (up to 40 % RH) with a slot die coater on a c-TiO 2 layer deposited using a large area chemical bath. A new artificial peptide – sulfonyl-γ-AApeptide (F-GLU-S) was employed to modify the slot-die coated perovskite surface, grain boundaries and electronic defects. The multi-functional F-GLU-S with carbonyl, carboxyl, sulfonyl, benzene, and chloro groups was capable of strongly interacting with the perovskite layer and repairing the uncoordinated Pb 2+ ions and halide vacancies. As a result, both the electron and hole densities of defects were significantly suppressed; consequently, the non-radiative recombination was effectively suppressed for the modified device which can be explicitly seen in the device performance where both V oc and FF of the modified device improved considerably. Therefore, F-GLU-S modified slot-die coated MAPbI 3 – based devices demonstrated outstanding performance of 21.44 % PCE with a V oc of 1.13 V, J sc of 24.64 cm –2 , and FF 76.99 %. Furthermore, F-GLU-S passivation impeded the infiltration of moisture and oxygen due to its hydrophobic nature and defect repair potential. As a result, the modified device retained above 92 % of its original PCE after 720 h in air (room temperature and 40–60 % RH).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Improving Efficiency and Stability of Perovskite Solar Cells Enabled by A Near-Infrared-Absorbing Moisture Barrier

Simultaneously improving device efficiency and stability is the most important issue in perovskite solar cell (PSC) research. Here, we strategically introduce a multi-functional interface layer (MFIL) with integrated roles of: (1) electron transport, (2) moisture barrier, (3) near-infrared photocurrent enhancement, (4) trap passivation, and (5) ion migration suppression to enhance the device performance. The narrow-band-gap non-fullerene acceptor, Y6, was screened out to replace the most commonly used PCBM in the inverted PSCs. A significantly improved power conversion efficiency of 21.0% was achieved, along with a remarkable stability (up to 1,700 h) without encapsulation under various external stimuli (light, heat, and moisture). Furthermore, systematic studies of the molecular orientation or passivation and the charge carrier dynamics at the interface between perovskite and MFIL were presented. These results offer deep insights for designing advanced interlayers and establish the correlations between molecular orientation, interface molecular bonding, trap state density, non-radiation recombination, and the device performance.

14 SOLAR ENERGY↗
DOE OSTI2024

Supramolecular design principles in pseudohalides for high-performance perovskite solar mini modules

In this work, we reveal the role of non-covalent interactions, which are known to play important roles in supramolecular phenomena, in achieving efficient perovskite surface and grain boundary passivation. By using a series of pseudohalides, we find that trifluoroacetate (TFA - ) provides the strongest binding to iodide vacancies by means of non-covalent hydrogen bonding and dispersion interactions. By exploiting additional non-covalent dispersion and hydrophobic interactions in aromatic 3,3-diphenylpropylammonium (DPA + ), we present a dual-ion passivation strategy that not only minimizes the non-radiative recombination center and local chemical inhomogeneities but also induces preferentially oriented growth of α-FAPbI 3 lattice. Further, this leads to an outstanding power conversion efficiency (PCE) of 25.63% with an exceptional open-circuit voltage of 1.191 V in a perovskite solar cell with a small area, while perovskite solar mini modules with aperture areas of 25 and 64cm 2 achieved PCE of 22.47% (quasi-steady-state [QSS]-certified 20.50%) and 20.88%, respectively, with outstanding stability under high-humidity conditions.

14 SOLAR ENERGY↗
DOE OSTI2022

Concentric core-shell tracks and spectroscopic properties of SrTiO 3 under intense electronic excitation

A deeper understanding of the intrinsic link between the irradiation-induced microstructures and the corresponding spectroscopic properties is becoming increasingly attractive for the research fields of materials science, physics, and information technology. In this work, the structural damage response, spectroscopic features, and associated physical mechanisms of SrTiO 3 single crystals under swift heavy ion irradiation were comparatively analyzed using a combination of experimental and theoretical approaches. Corresponding to 0.11–5.00 MeV/u ion irradiation with electronic energy loss ranging from 4.0 to 29.3 keV/nm, the inelastic thermal spike calculations combined with molecular dynamics simulations are compared with the experimental observations, revealing the track fine structures (individual spherical defects with a disordered region, and discontinuous and continuous tracks consisting of an amorphous core and a disordered outer shell) and demonstrating the dominant effects of the deposition energy and lattice temperature on track damage formation and evolution; thus, two essential thresholds for defect formation of ~0.60 eV/atom and amorphous region formation of ~1.81 eV/atom were identified to better describe the concentric core-shell track structure. The enhanced nanohillock formation in the surface region is attributed to the combined action of kinetic and potential energy depositions, and the fluence dependence in regulating the hillock dimensions is also presented. The measured refractive index profiles along different crystal axes further indicate the anisotropy of irradiation-induced lattice expansion. With increasing ion fluence and damage level, the intrinsic bandgap gradually decreased, and the concentration of additional radiative recombination centers (1.81 eV, 2.31 eV, and 2.42 eV) accordingly increased in the SrTiO 3 crystal, providing the possibility of regulating related defects to achieve tunable/selective photon emission for more critical technological applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Efficient and stable perovskite solar cells based on blade-coated CH 3 NH 3 PbI 3 thin films fabricated using “green” solvents under ambient conditions

Metal halide perovskites are considered the most promising candidates for solar cells of the decade due to their exceptional optical and electronic properties. The power conversion efficiency of metal halide perovskites, when incorporated as the active layer of solar cells, has become comparable to that observed for conventional silicon solar cells. However, the stability, scaleup, green solvent usage, and fabrication in ambient conditions of metal halide perovskites need to be solved for commercial applications. Here, in this work, we report the fabrication of blade-coated methylammonium lead iodide (MAPbI 3 ) perovskite thin films using methylamine and acetonitrile as “green” solvents under ambient conditions. Our perovskite films are initially prepared from low purity PbI2 (99%) and are blade-coated in dry air at relative humidity (RH) levels above 30%. A significant advantage of fabricating our perovskite thin films via blade-coating protocols is that there is a minimal amount of precursors (5 μL) used compared to spin-coating methods (50μL–60μL) for a 4 cm 2 substrate. With the addition of a small amount of an organic halide salt, namely, phenethylammonium chloride, the film crystallinity is improved and non-radiative recombination is suppressed, resulting in power conversion efficiencies over 20%. In addition, the device maintains more than 95% of its initial efficiency after 500 h under continuous light illumination of 1-sun at open circuit conditions, 50 °C and 60% RH. The above method leads a path towards the commercial fabrication of perovskite solar cells.

14 SOLAR ENERGY↗
DOE OSTI2023

A comprehensive material study of CdSeTe films deposited with differing selenium compositions

The addition of selenium into CdTe to create the ternary alloy CdSeTe has been one of the most impactful advancements to CdTe-based photovoltaics in the last decade. CdSeTe/CdTe bilayer device structures have enabled a gain in short-circuit current due to the narrower bandgap of the alloy, with minimal to no loss in voltage. Intensity of photoluminescence and time-resolved photoluminescence measurements suggest this is due to an increase in carrier lifetime and concomitant greater fraction of radiative vs non-radiative recombination events which allows for a reduction in the voltage deficit. Here, in this work, we study the properties of as-deposited and CdCl 2 -treated CdSeTe films deposited by close-space sublimation under varying conditions from CdSeTe source charges with both 20 and 40 mol% CdSe. We find that the selenium content in the deposited films are substantially reduced from that of the source material. Additionally, deposition temperature, particularly that of the substrate, considerably affects the grain size, crystallinity, and photoluminescence of the material, illustrating the importance of source material selection and process optimization. Finally, we present evidence that the source material, and therefore the properties of the deposited films, change over time as the source material is used.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Excitonic Dynamics in Janus MoSSe and WSSe Monolayers

We report here details of steady-state and time-resolved spectroscopy of excitonic dynamics for Janus transition metal dichalcogenide monolayers, including MoSSe and WSSe, which were synthesized by low-energy implantation of Se into transition metal disulfides. Absorbance and photoluminescence spectroscopic measurements determined the room-temperature exciton resonances for MoSSe and WSSe monolayers. Transient absorption measurements revealed that the excitons in Janus structures form faster than those in pristine transition metal dichalcogenides by about 30% due to their enhanced electron–phonon interaction by the built-in dipole moment. Here, by combining steady-state photoluminescence quantum yield and time-resolved transient absorption measurements, we find that the exciton radiative recombination lifetime in Janus structures is significantly longer than in their pristine samples, supporting the predicted spatial separation of the electron and hole wave functions due to the built-in dipole moment. These results provide fundamental insight in the optical properties of Janus transition metal dichalcogenides.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Transient X-ray Diffraction Reveals Nonequilibrium Phase Transition in Thin Films of CH 3 NH 3 PbI 3 Perovskite

Advantageous optoelectronic properties of methylammonium lead triiodide likely arise from coupling between photogenerated charge-carriers and the soft, deformable lattice. We investigate structural dynamics of MAPbI 3 films using time-resolved X-ray diffraction versus pump-probe time delay and pump intensity. During the first nanosecond, the lattice anisotropically distorts from tetragonal to cubic at excitation intensities that are insufficient to thermally induce the first-order thermodynamic phase transition at 330K. Further, the high-symmetry structure then relaxes back to the starting phase with 11 and 236-ns time constants via a different transition pathway than observed either in the first nanosecond or in previous reports for MAPbI 3 . Early-time dynamics are consistent with polaron formation and lattice strain stabilization while the slower recovery dynamics outlive radiative recombination and relates metastability. Fluence-independence of these lattice deformations in the low-power regime conveys relevance to optoelectronics including photovoltaics and highlights sustained involvement of non-equilibrium, photoinduced lattice reorganization in MAPbI 3 under functional conditions.

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

Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/Cd x Zn 1– x Se Quantum Dots

Colloidal CdSe quantum dots (QDs) designed with a high degree of asymmetric internal strain have recently been shown to host a number of desirable optical properties including subthermal room-temperature line widths, suppressed spectral diffusion, and high photoluminescence (PL) quantum yields. It remains an open question, however, whether they are well-suited for applications requiring emission of identical single photons. Here we measure the low-temperature PL dynamics and the polarization-resolved fluorescence line narrowing spectra from ensembles of these strained QDs. Our spectroscopy reveals the radiative recombination rates of bright and dark excitons, the relaxation rate between the two, and the energy spectra of the quantized acoustic phonons in the QDs that can contribute to relaxation processes. In comparison to conventional colloidal CdSe/ZnS core/shell QDs, we find that in asymmetrically strained CdSe QDs over six times more light is emitted directly by the bright exciton. Furthermore, these results are therefore encouraging for the prospects of chemically synthesized colloidal QDs as emitters of single indistinguishable photons.

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

Synthetic Ligand Selection Affects Stoichiometry, Carrier Dynamics, and Trapping in CuInSe 2 Nanocrystals

CuInSe 2 nanocrystals exhibit tunable near-infrared bandgaps that bolster utility in photovoltaic applications as well as offer potential as substitutes for more-toxic Cd- and Pb-based semiconductor compositions. However, they can present a variety of defect states as well as unusual photophysics. In this work, we examine the effects of ligand composition (oleylamine, diphenylphosphine, and tributylphosphine) on carrier dynamics in these materials. Via spectroscopic measurements such as photoluminescence and transient absorption, we find that ligands present during the synthesis of CuInSe 2 nanocrystals impart non-radiative electronic states which compete with radiative recombination and give rise to low photoluminescence quantum yields. We characterize the nature of these defect states (hole vs. electron traps) and investigate whether they exist at the surface or interior of the nanocrystals. Carrier lifetimes are highly dependent on ligand identity where oleylamine-capped nanocrystals exhibit rapid trapping (< 20 ps) followed by diphenylphosphine (< 500 ps) and finally tributylphosphine (> 2 ns). A majority of carrier population localizes at indium copper antisites (electrons), copper vacancies (holes), or surface traps (electrons and/or holes), all of which are non-emissive.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Lateral Integration of SnS and GeSe van der Waals Semiconductors: Interface Formation, Electronic Structure, and Nanoscale Optoelectronics

The emergence of atomically thin crystals has allowed extending materials integration to lateral heterostructures where different 2D materials are covalently connected in the plane. The concept of lateral heterostructures can be generalized to thicker layered crystals, provided that a suitably faceted seed crystal presents edges to which a compatible second van der Waals material can be attached layer by layer. Here, we examine the possibility of integrating multilayer crystals of the group IV monochalcogenides SnS and GeSe, which have the same crystal structure, small lattice mismatch, and similar bandgaps. In a two-step growth process, lateral epitaxy of GeSe on the sidewalls of multilayer SnS flakes (obtained by vapor transport of a SnS 2 precursor on graphite) yields heterostructures of laterally stitched crystalline GeSe and SnS without any detectable vertical overgrowth of the SnS seeds and with sharp lateral interfaces. Combined cathodoluminescence spectroscopy and ab initio calculations show the effects of small band offsets on carrier transport and radiative recombination near the interface. Further, the results demonstrate the possibility of forming atomically connected lateral interfaces across many van der Waals layers, which is promising for manipulating optoelectronics, photonics, and for managing charge- and thermal transport.

2D layered crystals↗
DOE OSTI2025

Nanoscale Strain and Octahedral Tilting Removes Structural and Nonradiative Defects in 2D-Templated FAPbI 3

The halide perovskite formamidinium lead iodide (FAPbI 3 ) is a prime candidate for photovoltaics due to its excellent optoelectronic properties, but its application has been limited due to its structural instability. The large size of the FA cation results in metastability of the photoactive cubic phase and a facile degradation into thermodynamically stable hexagonal phases at room temperature. Recently, the incorporation of two-dimensional (2D) Ruddlesden-Popper halide perovskite seeds into a FAPbI 3 precursor solution was shown to template the growth of and stabilize cubic FAPbI 3 . Here, in this study, we investigate the nanoscale structural and optoelectronic mechanisms behind the observed bulk stabilization using synchrotron-based X-ray microscopies. Nanoprobe X-ray diffraction reveals 2D-templated FAPbI 3 films exhibit an average compressive strain normal to the substrate of -3.3%, 2-fold larger than that of MACl-stabilized FAPbI 3 . This compression creates locally templated regions composed of tetragonal-phase FAPbI 3 distributed nonuniformly throughout the film with fewer crystalline defects than purely cubic regions. Scanning X-ray excited optical luminescence (X-ray analog of photoluminescence) reveals that this local templating results in increased radiative recombination and red-shifted band edge and emission. Our results provide insight into the microscopic mechanism for the phase stabilization of FAPbI 3 using 2D perovskites as templates.

X-ray diffraction↗
DOE OSTI2023

Origins of Photoluminescence Instabilities at Halide Perovskite/Organic Hole Transport Layer Interfaces

Metal halide perovskites are promising for optoelectronic device applications; however, their poor stability under solar illumination remains a primary concern. While the intrinsic photostability of isolated neat perovskite samples has been widely discussed, it is important to explore how charge transport layers—employed in most devices—impact photostability. Here, in this paper, we study the effect of organic hole transport layers (HTLs) on light-induced halide segregation and photoluminescence (PL) quenching at perovskite/organic HTL interfaces. By employing a series of organic HTLs, we demonstrate that the HTL’s highest occupied molecular orbital energy dictates behavior; furthermore, we reveal the key role of halogen loss from the perovskite and subsequent permeation into organic HTLs, where it acts as a PL quencher at the interface and introduces additional mass transport pathways to facilitate halide phase separation. In doing so, we both reveal the microscopic mechanism of non-radiative recombination at perovskite/organic HTL interfaces and detail the chemical rationale for closely matching the perovskite/organic HTL energetics to maximize solar cell efficiency and stability.

14 SOLAR ENERGY↗
DOE OSTI2024

Ag Intercalation in Layered Cs 3 Bi 2 Br 9 Perovskite for Enhanced Light Emission with Bound Interlayer Excitons

Cesium bismuth bromide (CBB) has garnered considerable attention as a vacancy-ordered layered perovskite with notable optoelectronic applications. However, its use as a light source has been limited due to its weak photoluminescence (PL). Here, we demonstrate metal intercalation as a novel approach to engineer the room-temperature PL of CBB using experimental and computational methods. Ag, when introduced into CBB, occupies vacant sites in the spacer region, forming octahedral coordination with surrounding Br anions. First-principles density functional theory calculations reveal that intercalated Ag represents the most energetically stable Ag species compared to other potential forms, such as Ag substituting Bi. The intercalated Ag forms a strong polaronic trap state close to the conduction band minimum and quickly captures photoexcited electrons with holes remaining in CBB layers, leading to the formation of a bound interlayer exciton, or BIE. The radiative recombination of this BIE exhibits bright room-temperature PL at 600 nm and a decay time of 38.6 ns, 35 times greater than that of free excitons, originating from the spatial separation of photocarriers by half a unit cell separation distance. The BIE as a new form of interlayer exciton is expected to inspire new research directions for vacancy-ordered perovskites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Unraveling the influence of non-fullerene acceptor molecular packing on photovoltaic performance of organic solar cells

In non-fullerene organic solar cells, the long-range structure ordering induced by end-group π–π stacking of fused-ring non-fullerene acceptors is considered as the critical factor in realizing efficient charge transport and high power conversion efficiency. Here, we demonstrate that side-chain engineering of non-fullerene acceptors could drive the fused-ring backbone assembly from a π–π stacking mode to an intermixed packing mode, and to a non-stacking mode to refine its solid-state properties. Different from the above-mentioned understanding, we find that close atom contacts in a non-stacking mode can form efficient charge transport pathway through close side atom interactions. The intermixed solid-state packing motif in active layers could enable organic solar cells with superior efficiency and reduced non-radiative recombination loss compared with devices based on molecules with the classic end-group π–π stacking mode. Our observations open a new avenue in material design that endows better photovoltaic performance.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Single-layered organic photovoltaics with double cascading charge transport pathways: 18% efficiencies

The chemical structure of donors and acceptors limit the power conversion efficiencies achievable with active layers of binary donor-acceptor mixtures. Here, using quaternary blends, double cascading energy level alignment in bulk heterojunction organic photovoltaic active layers are realized, enabling efficient carrier splitting and transport. Numerous avenues to optimize light absorption, carrier transport, and charge-transfer state energy levels are opened by the chemical constitution of the components. Record-breaking PCEs of 18.07% are achieved where, by electronic structure and morphology optimization, simultaneous improvements of the open-circuit voltage, short-circuit current and fill factor occur. The donor and acceptor chemical structures afford control over electronic structure and charge-transfer state energy levels, enabling manipulation of hole-transfer rates, carrier transport, and non-radiative recombination losses.

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

Layer number dependent ferroelasticity in 2D Ruddlesden–Popper organic-inorganic hybrid perovskites

Ferroelasticity represents material domains possessing spontaneous strain that can be switched by external stress. Three-dimensional perovskites like methylammonium lead iodide are determined to be ferroelastic. Layered perovskites have been applied in optoelectronic devices with outstanding performance. However, the understanding of lattice strain and ferroelasticity in layered perovskites is still lacking. Here, using the in-situ observation of switching domains in layered perovskite single crystals under external strain, we discover the evidence of ferroelasticity in layered perovskites with layer number more than one, while the perovskites with single octahedra layer do not show ferroelasticity. Density functional theory calculation shows that ferroelasticity in layered perovskites originates from the distortion of inorganic octahedra resulting from the rotation of aspherical methylammonium cations. The absence of methylammonium cations in single layer perovskite accounts for the lack of ferroelasticity. These ferroelastic domains do not induce non-radiative recombination or reduce the photoluminescence quantum yield.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Traps and transport resistance are the next frontiers for stable non-fullerene acceptor solar cells

Stability is one of the most important challenges facing material research for organic solar cells (OSC) on their path to further commercialization. In the high-performance material system PM6:Y6 studied here, we investigate degradation mechanisms of inverted photovoltaic devices. We have identified two distinct degradation pathways: one requires the presence of both illumination and oxygen and features a short-circuit current reduction, the other one is induced thermally and marked by severe losses of open-circuit voltage and fill factor. We focus our investigation on the thermally accelerated degradation. Our findings show that bulk material properties and interfaces remain remarkably stable, however, aging-induced defect state formation in the active layer remains the primary cause of thermal degradation. The increased trap density leads to higher non-radiative recombination, which limits the open-circuit voltage and lowers the charge carrier mobility in the photoactive layer. Furthermore, we find the trap-induced transport resistance to be the major reason for the drop in fill factor. Our results suggest that device lifetimes could be significantly increased by marginally suppressing trap formation, leading to a bright future for OSC.

14 SOLAR ENERGY↗