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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Chemometric modeling of power conversion efficiency of organic dyes in dye sensitized solar cells for the future renewable energy

The present study reports chemometric modeling of power conversion efficiency (PCE) of dye sensitized solar cells (DSSCs) using the biggest available data set till date which comprises around 1200 dyes covering 7 chemical classes. To extract the best structural features required for higher PCE, we have developed multiple partial least squares (PLS) quantitative structure-property relationship (QSPR) models for the Triphenylamine, Phenothiazine, Indoline, Porphyrin, Coumarin, Carbazole and Diphenylamine chemical classes using descriptors derived from the best subset selection method followed by selection of best five models in each dataset based on the Mean Absolute Error (MAE) values. The models were validated both internally and externally followed by the consensus predictions employing “Intelligent Consensus Predictor” tool to examine whether the quality of predictions can be improved with the “intelligent” selection of multiple PLS models. The quality of predictions for the respective external sets showed that the consensus models (CM) are better than the individual models (IM) in most of the cases. From the insights of the developed models, we concluded that attributes like a packed structure toward higher conductivity of electrons, auxiliary donor fragment of aromatic tertiary amines, number of thiophenes inducing the bathochromic shift and augmenting the absorption, presence of additional electron donors, enhancement of electron-donating abilities, number of non-aromatic conjugated C(sp 2 ) which helps as conjugation extension units to broaden the absorption and highly conjugated $π$-systems exert positive contributions to the PCE. On the contrary, features negatively contributing to PCE are the followings: fragments which lower the tendency of localized $π–π*$ transition, fragments related to larger volume and surface area of dyes along with hydrophobicity resulting in poor adhesion, fragment RC = N causing dye hydrolysis, steric hindrance for π electronic mobility, fragments enhancing polarity, etc. Finally, the identified features from the best QSPR model of the coumarin dataset was employed in designing of ten more efficient coumarin dyes (predicted %PCE ranging from 8.93 to 10.62) than the existing ones.

14 SOLAR ENERGY↗
DOE OSTI2020

Crystal Structure and Atomic Vacancy Optimized Thermoelectric Properties in Gadolinium Selenides

Thermoelectric materials enable the energy conversion of waste heat into electricity, helpful to relieve global energy crisis. Here, we report a systematic investigation on high-temperature thermoelectric gadolinium selenides, cubic Gd 3-x Se 4 (x = 0.16, 0.21 and 0.25) and orthorhombic Gd 2 Se 3-y (y = 0.02, 0.06 and 0.08). High energy synchrotron x-ray diffraction and total scattering have been used to investigate the crystallographic and local structures. Atomic-scale clusters of Gd vacancy in the cubic phase are observed by employing the reverse Monte Carlo simulation. For cubic Gd 3-x Se 4 , adjusting Gd vacancy triggers the effect of multiple conduction bands, confirmed by the increase in effective masses and theoretical calculations. A reasonable peak zT value of 0.27 is achieved at 850 K for Gd 3-x Se 4 (x = 0.16). On the other hand, tuning Se vacancy enables the optimization of electron concentration for the orthorhombic Gd 2 Se 3-y . More significantly, its low deformation potential (Ξ = 12eV) gives rise to enhanced electron mobility and higher peak zT value of 0.54 at 850 K for Gd 2 Se 3-y (y = 0.02). Intriguingly, a higher zT of 1.2 at 1200 K is reasonably predicted by quality factor analysis. Finally, this work extends the scope of high-temperature thermoelectric materials and facilitates the exploration of novel high-temperature thermoelectric materials

36 MATERIALS SCIENCE↗
DOE OSTI2021

Radically Tunable n-Type Organic Semiconductor via Polymorph Control

Polymorphism has emerged as an important design consideration in organic semiconductors (OSCs). Previously, in many OSCs, even small changes in molecular stacking can cause drastic changes to the optical and electronic properties. However, investigation into n-type semiconductors has significantly lagged behind their p-type counterparts. In this work, we present the prolific polymorphism of 2-dimensional quinoidal terthiophene (2DQTT-o-B) and systematically investigate each of 5 polymorphs, 3 of which have been previously unreported. Grazing incidence X-ray diffraction provided a key method to understanding the structure of each polymorph. Via the polymorphic transitions mapped, we tuned the electron mobility by 5 orders of magnitude, from 5.63 × 10 –5 to 0.22 cm 2 V –1 s –1 . These were accompanied by modifications to the optical properties, namely we observed substantial differences in the refractive index noted by intensity differences under polarized optical microscopy and a large shift in optical band gap from 1.18 eV up to 1.40 eV. Lastly, we suggest that changes to these properties may be related to the unique quinoidal to aromatic transition observed in quinoidal molecules.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Li 2 GeS 3 : Lithium Ionic Conductor with an Unprecedented Structural Type

Lithium-ion batteries (LIBs) are widely used in electric vehicles, mobile electronic devices, and large-scale stationary energy storage systems. However, their liquid electrolytes present significant safety concerns due to their inherent flammability. To address this, the focus has shifted toward all-solid-state batteries (ASSBs) utilizing inorganic solid electrolytes that promise enhanced safety. In this work, we report the discovery of a new crystal structural type of Li-ion conductor, Li 2 GeS 3 , with a unique structure, synthesized by a solid-state reaction from Li 2 S and GeS 2 . It was first reported in 2000 with an orthorhombic unit cell, but its detailed crystal structure remains veiled. Here, we have unveiled its structure for the first time, employing an ab initio structure determination technique from powder X-ray and time-of-flight neutron diffraction data. The compound has an unprecedented crystal structural type with a hexagonal $P6_1$ symmetry and a unit cell of α = 6.79364(4) Å and c = 17.90724(14) Å. Its structure is comprised of a distorted hexagonal close-packed arrangement of sulfur anions with three asymmetric metal atoms: Li1, Li2, and Ge are in tetrahedral cavities surrounded by sulfur atoms. The ionic conductivity of Li 2 GeS 3 was measured to be 1.63 × 10 –8 S cm –1 at 303 K and 2.45 × 10 –7 S cm –1 at 383 K. Bond valence energy landscape calculations revealed three-dimensional lithium diffusion pathways within the structure. This novel crystal structure in Li 2 GeS 3 holds the potential for developing high-performance ionic conductors through suitable chemical substitution and offers valuable insights into designing new ionic conductors for ASSBs.

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

Metal Sulfide Ion Exchangers: High Acid Stability of Na 2 x Mg 2 y – x Sn 4– y S 8 (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character

Metal sulfide ion exchange materials (MSIEs) are of interest for nuclear waste remediation applications. Here, we report the high stability of two structurally related metal sulfide ion exchange materials, Na 2x Mg 2y–x Sn 4–y S 8 (Mg-NMS) and Na 2 SnS 3 (Na-NMS), in strongly acid media, in addition to the preparation of Na 2x Ni 2y–x Sn 4–y S 8 (Ni-NMS). Their formation progress during synthesis is studied with in-situ methods, with the target phases appearing in <15 min, reaction completion in <12 h, and high yields (75–80%). Upon contact with nitric or hydrochloric acid, these materials topotactically exchange Na + for H + , proceeding in a stepwise protonation pathway for Na 5.33 Sn 2.67 S 8 . Na-NMS is stable in 2 M HNO 3 and Mg-NMS is stable in 4 M HNO 3 for up to 4 h, while both NMS materials are stable in 6 M HCl for up to 4 days. However, the treatment of Mg-NMS and Na-NMS with 2–6 M H 2 SO 4 reveals a much slower protonation process since after 4 h of contact both NMS and HMS are present in the solution. The resultant protonated materials, H 2x Mg 2y–x Sn 4–y S 8 and H 4x [(H y Na y–1 ) 1.33x Sn 4––1.33x ]S 8 , are themselves solid acids and readily react with and intercalate a variety of organic amines, where the band gap of the resultant adduct is influenced by amine choice and can be tuned within the range of 1.88(5)–2.27(5) eV. The work function energy values for all materials were extracted from photoemission yield spectroscopy in air (PYSA) measurements and range from 5.47 (2) to 5.76 (2) eV, and the relative band alignments of the materials are discussed. DFT calculations suggest that the electronic structure of Na 2 MgSn 3 S 8 and H 2 MgSn 3 S 8 makes them indirect gap semiconductors with multi-valley band edges, with carriers confined to the [MgSn 3 S 8 ] 2– layers. Light electron effective masses indicate high electron mobilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Restoring Symmetry and Enhancing Exchange via Chiral Molecular-Magnetic Hexagons

Modified behaviors of molecules, designed for device or energy applications, can occur due to lattice-molecule incompatibilities in point-group symmetries (PGS), long-range interactions between neighboring molecules, or latticemolecule charge transfer. Such sensitivities are prerequisite for the use of quantum molecules as devices, but removing certain broken symmetries is desirable from the standpoint of simplifying their behaviors. Here, we demonstrate symmetry restoration to molecular-magnetic lattices and show that it leads to strengthened exchange-coupling due to dipolar electrostatic interactions between neighboring molecules and due to manifestations of an earlier identification of a spin-sensitive slightly mobile electron by Hooshmand et al. Starting with a broken symmetry molecular magnet of current interest, we demonstrate a more robust structure composed of six molecular magnets on a h-BN-like surface. The broken point-group symmetry is healed by constructing interpenetrating equilateral triangular structures that are appropriately ratcheted to preserve three-fold rotational symmetry and inversion symmetry.

Pederson, Mark R.↗
DOE OSTI2020

Observation of [VCu1–Ini2+VCu1–] Defect Triplets in Cu-Deficient CuInS2

Copper indium disulfide (CuInS2) is a semiconductor with a direct energy band gap of 1.53 eV, an optimal value for highly efficient thin-film solar cells. But it has reached only ~ 11 % power conversion efficiency, far less than the theoretically achievable value of ~ 30 %. The cause of this low performance is not understood. A single crystal grown from 1 mol% Cu-deficient melt was studied, using atomic resolution high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) and electron dispersive spectroscopy (EDS). While the bulk crystal is exactly stoichiometric CuInS2, it contains nanometer-thick, structurally coherent, Cu-deficient interphases that form along rotational twin boundaries in the {112} plane. Transition zones from bulk crystal to interphase are observed, where In is seen to move from its normal site InIn in the chalcopyrite structure to a tetrahedral interstitial site Ini, while Cu remains in its normal CuCu position. Two InIn rows of the bulk crystal merge into one row of Ini, causing excess Ini in the interphase. The concentrations of CuCu and Ini reflect a ratio of Cu vacancies, VCu, to excess Ini of ~ 2. Their relative lattice positions, and the high electrical resistivity of the crystal, suggests that VCu and excess Ini ‘precipitate’ as self-compensating, electrically neutral, [VCu1- Ini2+ VCu1-] defect triplets. This is the first atomic-level observation of the ordered defect that has been invoked as the basic structural modifier in chalcopyrite compound homologs. The interphases introduce an optical gap of 1.47 eV. Electron trapping in band tail states, evident from a photoconductivity exponent of 0.54, is the likely cause of an unusually low electron mobility of 0.1 cm2V-1s-1. The overall result is that making CuInS2 slightly copper-poor inserts nanometer-thick layers of the interphase into the bulk crystal. This study shows that apparently conflicting results of the effect of Cu deficiency on CuInS2 thin-film solar cells may be resolved by analyzing structure and composition at nanometer spatial resolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Highly Responsive Near-Infrared Photodetector Based on Contactless PdSe 2 Integration with a Few-Layered MoSe 2 Field-Effect Transistor

Two-dimensional (2D) semiconductors with narrow bandgaps are promising candidates for near- and far-infrared (IR) photodetection, particularly in the telecommunication spectral window. However, current low-bandgap IR photodetectors face significant challenges due to their high dark current, increased carrier recombination, and thermally generated noise. Here, in this work, a hybrid phototransistor is demonstrated by integrating direct, contact-free palladium diselenide (PdSe 2 ) as a highly responsive IR detection layer with a non-IR-absorbing molybdenum diselenide (MoSe 2 ) field-effect transistor (FET), using a near-IR source at a wavelength of λ = 1650 nm. Exfoliated PdSe 2 flakes integrated into a back-gated FET architecture exhibit ambipolar transport behavior, with extracted hole and electron mobilities of 24.8 cm 2 V –1 s –1 and 58.4 cm 2 V –1 s –1 , respectively. The devices show a clear photocurrent generation under the illumination of a λ = 1650 nm laser source, achieving a notable responsivity of ∼300 mA W -1 at an applied gate voltage of 15 V, which highlights the suitability of PdSe 2 as a narrow-bandgap material for photodetection. Photoresponsivity saturates and does not have any effect above an applied gate voltage of 15 V. To further tune the photoresponsivity performance continuously with the applied gate voltage, we construct a van der Waals heterostructure phototransistor, where few layers of PdSe 2 are directly transferred onto the 2D channel region of a MoSe 2 FET, while avoiding any contact with the metal electrodes. In this heterostructure, PdSe 2 works as the primary active IR-absorbing layer, while MoSe 2 provides high-performance FET characteristics. This spatial separation of absorption and transport facilitates efficient interlayer charge transfer and charge separation, resulting in high responsivities of up to 972 mA W –1 at near-IR wavelengths and a low power density of 1.5 mW/mm 2 . The responsivity of our photodetector is comparable to that of some state-of-the-art commercially available NIR photodetectors, highlighting the potential of PdSe 2 -based heterostructures as scalable, CMOS-compatible platforms for high-performance near-IR detection.

Infrared (IR) photodetectors↗
DOE OSTI2026

Dithieno[3,2-c:3′,2′‑ h ][2,6]naphthyridine-4,9(5H,10H)-dione-Based Conjugated Polymers for High Stable n‑Type Organic Electrochemical Transistors

Amide/imide-based conjugated polymers have been utilized as n-type OECT materials and have demonstrated promising device performance. However, their performance remains insufficient in terms of both efficiency and stability, which limits their practical applications. The development of conjugated polymers based on amide and imide groups represents a promising approach to address this issue. Here, in this study, we introduced dithieno­[3,2-c:3′,2′-h]­[2,6]­naphthyridine-4,9­(5H,10H)-dione (TVTDA) into the design of the OECT materials for the first time. By copolymerizing it with (E)-2,2′-(ethene-1,2-diyl)­bis­(thiophene-3-carbonitrile), we prepared two polymers, TVTDA-2CNTVT-ST and TVTDA-2CNTVT-BR, which contain linear or branched ethylene glycol side chains, respectively. OECT devices based on these polymers demonstrate n-type charge transport characteristics, achieving promising μC* values of 7.17 and 26.5 F cm –1 V –1 s –1 for TVTDA-2CNTVT-ST and TVTDA-2CNTVT-BR, respectively. The higher electron mobility and μC* of TVTDA-2CNTVT-BR can be attributed to its mixed edge-on and face-on stacking mode, larger crystalline coherence length, and larger domain size in the thin film. To our delight, the OECT devices based on both polymers exhibit good operational stability after operating in an aqueous solution for 2000 s, with current retention rates exceeding 93%, representing the high level among the OECT devices based on amide/imide-conjugated polymers. Our study demonstrates that the TVTDA unit holds great potential for constructing high-performance n-type OECT materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The Subchalcogenides Ir 2 In 8 Q (Q = S, Se, Te): Dirac Semimetal Candidates with Re-entrant Structural Modulation

Subchalcogenides are uncommon compounds where the metal atoms are in unusually low formal oxidation states. They bridge the gap between intermetallics and semiconductors and can have unexpected structures and properties because of the exotic nature of their chemical bonding as they contain both metal–metal and metal–main group (e.g., halide, chalcogenide) interactions. Finding new members of this class of materials presents synthetic challenges as attempts to make them often result in phase separation into binary compounds. We overcome this difficulty by utilizing indium as a metal flux to synthesize large (millimeter scale) single crystals of novel subchalcogenide materials. Herein, we report two new compounds Ir 2 In 8 Q (Q = Se, Te) and compare their structural and electrical properties to the previously reported Ir 2 In 8 S analogue. Ir 2 In 8 Se and Ir 2 In 8 Te crystallize in the $P_{4_2}$/mnm space group and are isostructural to Ir2In8S, but also have commensurately modulated (with q vectors q = 1/6a* + 1/6b* and q = 1/10a* + 1/10b* for Ir 2 In 8 Se and Ir 2 In 8 Te, respectively) low-temperature phase transitions, where the chalcogenide anions in the channels experience a distortion in the form of In–Q bond alternation along the ab plane. Both compounds display re-entrant structural behavior, where the supercells appear on cooling but revert to the original subcell below 100 K, suggesting competing structural and electronic interactions dictate the overall structure. Notably, these materials are topological semimetal candidates with symmetry-protected Dirac crossings near the Fermi level and exhibit high electron mobilities (~1500 cm 2 V –1 s –1 at 1.8 K) and moderate carrier concentrations (~10 20 cm –3 ) from charge transport measurements. This work highlights metal flux as a synthetic route to high quality single crystals of novel intermetallic subchalcogenides with Dirac semimetal behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Revealing the Full Potential of Glycolated Mixed Ionic-Electronic Semiconductors – Symmetric Monomer Polymerization to Boost Electrochemical Transistor Performance

Organic electrochemical transistors (OECTs) enable the transduction of ionic signals into electronic outputs, positioning them as ideal candidates for next-generation sensing and (bio)signal processing applications. Recent years have witnessed the development of various OECT channel materials, affording insights into structural fine-tuning to achieve optimal performance and/or stability. However, homocouplings, commonly present in alternating conjugated polymers, have largely been overlooked. This study investigates the effect of homocoupling on OECT materials by employing two synthesis methods – standard Stille polymerization and an alternative symmetric approach – to create the p-type enhancement-mode benchmark polymer pgBTTT. The impact of homocoupling, and its absence, is studied by comparing the bulk properties of the two polymers and evaluating their respective OECT metrics. The new, homocoupling-free polymer exhibits a notably improved OECT performance ( μC *), mainly due to an average 3-fold increase in electronic mobility (μ).

defects↗
DOE OSTI2020

Ab initio electron-two-phonon scattering in GaAs from next-to-leading order perturbation theory

Electron-phonon (e–ph) interactions are usually treated in the lowest order of perturbation theory. Here we derive next-to-leading order e–ph interactions, and compute from first principles the associated electron-two-phonon (2ph) scattering rates. The derivations involve Matsubara sums of two-loop Feynman diagrams, and the numerical calculations are challenging as they involve Brillouin zone integrals over two crystal momenta and depend critically on the intermediate state lifetimes. Using Monte Carlo integration together with a self-consistent update of the intermediate state lifetimes, we compute and converge the 2ph scattering rates, and analyze their energy and temperature dependence. We apply our method to GaAs, a weakly polar semiconductor with dominant optical-mode long-range e–ph interactions. We find that the 2ph scattering rates are as large as nearly half the value of the one-phonon rates, and that including the 2ph processes is necessary to accurately predict the electron mobility in GaAs from first principles.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Precise synthesis and photovoltaic properties of giant molecule acceptors

Series of giant molecule acceptors DY, TY and QY with two, three and four small molecule acceptor subunits are synthesized by a stepwise synthetic method and used for systematically investigating the influence of subunit numbers on the structure-property relationship from small molecule acceptor YDT to giant molecule acceptors and to polymerized small molecule acceptor PY-IT. Among these acceptors-based devices, the TY-based film shows proper donor/acceptor phase separation, higher charge transfer state yield and longer charge transfer state lifetime. Combining with the highest electron mobility, more efficient exciton dissociation and lower charge carrier recombination properties, the TY-based device exhibits the highest power conversion efficiency of 16.32%. These results indicate that the subunit number in these acceptors has significant influence on their photovoltaic properties. This stepwise synthetic method of giant molecule acceptors will be beneficial to diversify their structures and promote their applications in high-efficiency and stable organic solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Symmetry-engineered chiral magnetotransport in the correlated oxide SrNbO 3

Chiral transport in topological materials, arising from the interplay between topology and chirality, holds significant potential for energy-efficient spintronics and quantum information technologies through dissipationless, coherent charge flow. However, the emergence of chiral transport by tuning the electronic states of novel chiral materials is largely unexplored. Here, we report chiral transport driven by correlated Dirac fermions in SrNbO 3 epitaxial thin films, where strain-induced nonsymmorphic symmetry of oxygen octahedra tunes the material from metallic to Dirac states. Such symmetry-driven Dirac fermions feature a remarkable enhancement of electron mobility and magnetoresistance. Signatures of chiral transport induced by the chiral anomaly, including negative longitudinal magnetoresistance and twofold planar Hall oscillation, are observed in the Dirac semimetallic state, whereas they are absent in the metallic state of SrNbO 3 thin films. This work highlights a crucial role of symmetry engineering in generating chiral charge transport in oxide Dirac semimetals, opening an avenue to novel oxide-based topological and quantum devices.

Materials science↗
DOE OSTI2020

Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis

The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. In this work, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co 2 P (Pt–Co 2 P) to introduce a stronger dopant–host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H–H bond formation. As a proof-of-concept, the interior-modified Pt–Co 2 P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm –2 , and excellent durability for long-term utilization. The interior-modified Pt–Co 2 P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design.

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

Effect of the chlorine substitution position of the end-group on intermolecular interactions and photovoltaic performance of small molecule acceptors

The structure–property relationships of small molecular acceptors (SMAs) are a key issue in the molecular design of new-generation acceptor materials for further improving the device efficiencies of polymer solar cells (PSCs). Herein, three couples of SMA isomers were synthesized, based on three central fused ring units and two 1,1-dicyanomethylene-3-indanone (IC) isomer electron-withdrawing terminal units with chlorine substitutions in different positions of its benzene ring: Cl-1 with chlorine on the same side as a C=O group of IC and Cl-2 with chlorine on the same side as the CN groups of IC. Through systematical investigation, we found that the chlorine substitution position of the terminal groups has a regular and significant influence on the molecular packing and photovoltaic performance of the SMAs. The molecular packing behavior of the SMAs is closely related to and determined by the configuration of their terminal groups, no matter which central fused ring of the SMAs is used. In particular, the Cl-1-based SMAs possess a stronger crystallinity with long range ordering packing in their molecular plane direction, while the more abundant and stereoscopic π–π intermolecular interaction in the Cl-2-based SMAs promotes the molecules to form three-dimensional charge transporting channels and leads to their red-shifted absorption and higher electron mobilities. Therefore, the Cl-2-based PSCs exhibit a higher power conversion efficiency (PCE) compared to that of the Cl-1-based devices, and the best PCE of a Cl-2 SMA-based PSC reached 16.42%. These results highlight the importance of the investigation of intermolecular interactions, packing and the arrangement of the SMAs in the solid-state, which may provide direct insights for exploring the relationship between the molecular structure and property of the photovoltaic materials. Moreover, we envision that if fragments such as end groups or side chains with more diverse molecular interactions are added into the design and the subsequent synthesis of the SMAs, this may be beneficial to promoting molecular π–π accumulation and further improving the molecular order, forming suitable molecular packing and morphology in the resulting blend films, and finally affecting the efficiency of the PSCs.

14 SOLAR ENERGY↗
DOE OSTI2022

Sequentially regular polymer acceptors featuring flexible spacers for high-performance and mechanically robust all-polymer solar cells

Developing high-performance and mechanically robust polymer solar cells (PSCs) is crucial for realizing wearable power sources. While efficient all-polymer solar cells (all-PSCs) can be fabricated from polymerized small-molecule acceptors (PSMAs) with high optical absorption and electron mobilities, they still show limited mechanical robustness. Here, we achieve highly efficient and mechanically robust all-PSCs by designing a PSMA (PYFS-Reg) containing sequence-regular flexible spacers (FSs). The regular incorporation of the FS units into PSMAs is essential in simultaneously improving the electrical and mechanical properties of blend films. As a result, all-PSCs featuring PYFS-Reg achieve a high power conversion efficiency (PCE = 16.1%) and stretchability (crack onset strain (COS) = 22.4%), outperforming PSMAs without FSs (i.e., PYBDT, PCE = 12.6% and COS = 11.7%) or with randomly distributed FSs (i.e., PYFS-Ran, PCE = 12.2% and COS = 18.1%). Importantly, these all-PSCs are fabricated by an environmentally benign, non-halogenated solvent process. To further demonstrate their feasible applications in wearable devices, we construct intrinsically stretchable (IS) all-PSCs by using PYFS-Reg-based active layers, which exhibit a high PCE (10.6%) and excellent device stretchability (strain at PCE 80% = 36.7%).

14 SOLAR ENERGY↗