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Magnetic order of tetragonal CuO ultrathin films

Here, we present a detailed low-energy muon spin rotation and x-ray magnetic circular dichroism (XMCD) investigation of the magnetic structure in ultrathin tetragonal (T)-CuO films. The measured muon-spin polarization decay indicates an antiferromagnetic (AFM) order with a transition temperature higher than 200 K. The XMCD signal obtained around the CuL 2,3 edges indicates the presence of pinned Cu 2+ moments that are parallel to the sample surface, and additionally, isotropic paramagnetic moments. The pinning of some of the Cu moments is caused by an AFM ordering consisting of moments that lie most likely in plane of the film. Moreover, pinned moments show a larger orbital magnetic moment contribution with an approximate ratio of m orb /m spin =1.5, indicating that these spins are located at sites with reduced symmetry. Some fractions of the pinned moments remain pinned from an AFM background even at 360 K, indicating that T N >360K. We propose a simple model that explains these experimental findings, showing that the magnetic order of the T-CuO ultrathin films differs from the theoretical predictions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Development of Fast, Background-Limited Transition-Edge Sensors for the Background-Limited Infrared/Sub-mm Spectrograph (BLISS) for SPICA

We report experimental progress toward demonstrating background-limited arrays of membrane-isolated transition-edge sensors (TESs) for the Background Limited Infrared/Sub-mm Spectrograph (BLISS). BLISS is a space-borne instrument with grating spectrometers for wavelengths lambda=35-435 micron and with R=lambda/delta lambda approximately equals 500. The goals for BLISS TESs are: noise equivalent power (NEP) = 5x10 (sup -20) W/Hz(exp 1/2) and response time tau <30ms. We expect background-limited performance from bilayers TESs with T(sub c) = 65mK and G=15fW/K. However, such TESs cannot be operated at 50mK unless stray power on the devices, or dark power P(sub D), is less than 200aW. We describe criteria for measuring P(sub D) that requires accurate knowledge of TC. Ultimately, we fabricated superconducting thermistors from Ir (T(sub c) >= 135mK) and Mo/Cu proximitized bilayers, where T(sub c) is the thermistor transition temperature. We measured the Ir TES arrays in our 50mK adiabatic demagnetization refrigerator test system, which can measure up to eight 1x32 arrays simultaneously using a time-division multiplexer, as well as our single-pixel test system which can measure down to 15mK. In our previous Ir array measurements our best reported performance was NEP=2.5x10(exp -19) W/Hz(sub 1/2) and Tau approximately equals 5ms for straight-beam TESs. In fact, we expected NEP approximately equals 1.5x10(exp -19)?W/Hz(sup 1/2) for meander beam TESs, but did not achieve this previously due to 1/f noise. Here, we detail improvements toward measuring the expected NEP and demonstrate NEP=(1.3+0.2)x10 (sup -19)W/Hz(exp 1/2) in our single-pixel test system and NEP=(1.6+/-0.3)x10(sup -19)W/Hz(sup 1/2) in our array test system.

infrared spectrometer↗

Pressure dependence of the magnetic ground state in CePtSi 2

CePtSi 2 was reported to exhibit an antiferromagnetic order below T*=1.8 K at ambient pressure, a valence state change at ~1.2 GPa, and superconductivity in the range between 1.4 and 2.1 GPa with a maximum transition temperature of 0.14 K [T. Nakano et al., Phys. Rev. B 79, 172507 (2009)]. We have performed polycrystalline and single-crystal neutron diffraction experiments to determine the magnetic structure under ambient and high pressures. We found incommensurate magnetic peaks with a magnetic propagation vector of (0.32,0,0.11) at ambient pressure below T SDW ~ 1.25 K. Those magnetic peaks originate from a spin-density-wave order with the easy axis along the c axis and an averaged ordered moment of 0.45(5) μB , suggesting that there may be an intermediate phase between T* and T SDW . Applying pressures, the magnetic propagation vector shows no change and the magnetic order disappears around 1.0 GPa, which is much lower than the critical pressure for the superconducting phase. The results suggest that other than magnetic fluctuations may play a primary role in the superconducting pairing mechanism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Mapping the structural, magnetic and electronic behavior of (Eu 1-x Ca x ) 2 Ir 2 O 7 across a metal-insulator transition

In this study, we employ bulk electronic properties characterization and x-ray scattering/spectroscopy techniques to map the structural, magnetic and electronic properties of (Eu 1-x Ca x ) 2 Ir 2 O 7 as a function of Ca-doping. As expected, the metal-insulator transition temperature, T-MIT, decreases with Ca-doping until a metallic state is realized down to 2 K. In contrast, T-AFM becomes decoupled from the MIT and (likely short-range) AFM order persists into the metallic regime. This decoupling is understood as a result of the onset of an electronically phase separated state, the occurrence of which seemingly depends on both synthesis method and rare earth site magnetism. PDF analysis suggests that electronic phase separation occurs without accompanying chemical phase segregation or changes in the short-range crystallographic symmetry while synchrotron x-ray diffraction confirms that there is no change in the long-range crystallographic symmetry. X-ray absorption measurements confirm the $J_{eff}$ = 1/2 character of (Eu 1-x Ca x ) 2 Ir 2 O 7 . Surprisingly these measurements also indicate a net electron doping, rather than the expected hole doping, indicating a compensatory mechanism. Lastly, XMCD measurements show a weak Ir magnetic polarization that is largely unaffected by Ca-doping. Keywords: term, term, term.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Coexistence of Synchronization and Stochasticity in Thermally Coupled Mott Oscillators

Synchronization is conventionally regarded as a mechanism for suppressing variability and enforcing order in coupled systems, from pendula and lasers to neurons and electronic oscillators. Here, we show that synchronization can also embed stochasticity at finer scales. We observe this phenomenon in thermally coupled VO 2 neuristors, where robust in-phase synchronization at the microsecond scale coexists with spike onset fluctuations at the nanosecond scale, with no fixed leader. The coexistence of order and disorder originates from stochastic domain-level physics of the insulator–metal and metal–insulator transitions, where local variations in transition temperature drive cycle-to-cycle randomness in nucleation, percolation, and relaxation. A stochastic domain model reproduces this effect by generating synchronized spike trains with random lead–lag jitter, and experimental interspike interval statistics confirm the persistence of fine-scale variability despite macroscopic phase locking. These findings establish that synchronization and stochasticity can coexist within the same physical platform, revealing hidden disorder within collective order. Furthermore, this insight reframes synchronization as not purely deterministic, but as a universal context where microscopic variability can persist, with implications for electronics, cryptography, and the fundamental physics of order–disorder coexistence.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

X-Ray Missions Based on LTD Technologies

Microcalorimeter arrays used as imaging spectrometers will enable ground-breaking science in X-ray astrophysics. Their development has been one of the driving applications of the low temperature detector community since the early 1980s. While their application in space remains in relative infancy, we are on the verge of an era in which microcalorimeter spectrometers are likely to dominate instrumentation for high-energy astrophysics missions. NASA sounding rocket experiments such as the X-ray Quantum Calorimeter (XQC) and Micro-X have now paved the way for orbital observatories. JAXA’s Astro-H gave us a glimpse of this fantastic new capability before its unfortunate demise. The launch of XRISM later this year should finally demonstrate the sort of large suite of observations that X-ray microcalorimeter arrays will make major contributions to. In the mid-2030s, we will see the launch of ESA’s flagship Athena mission, that will further advance the imaging and spectroscopic capabilities for the high-energy X-ray community enormously. Numerous other potential new mission concepts using X-ray microcalorimeters have been studied in detail such as NASA’s Lynx and the Light Element Mapper (LEM), JAXA’s Super-DIOS, and China’s Hot Universe Baryon Surveyor (HUBS). In the first half of this presentation, I will review the development and desired requirements of the X-ray microcalorimeter missions and concepts, and describe the current progress and status missions being implemented and proposed. In the second half of this presentation, I will focus on The Line Emission Mapper (LEM) which is a probe-class mission concept under study by NASA that is designed to provide unprecedented insight into the physics of galaxy formation, including stellar and black-hole feedback and flows of baryonic matter into and out of galaxies. LEM incorporates a light-weight X-ray optic with 10” angular resolution and a large-format microcalorimeter array with a 15” pixel pitch over a 29’ field of view (FOV). The main microcalorimeter array and readout design takes advantage of mature technology that has been developed for Athena X-IFU. The central 7’ region of the array consists of ~ 800 transition-edge sensors (TESs), optimized for a bandpass of 0.3-2 keV and with an energy resolution of 1.2 eV at 1 keV. The rest of the FOV is covered by 4-pixel TES hydras with 2.5 eV energy resolution at 1 keV. Hydras are position-sensitive (‘thermally multiplexed’) detectors that enable extremely large numbers of effective pixels in an array, without a commensurate increase in the number of wires, bias circuit, and readout components. In total the array will have ~ 4k TESs with ~ 14k imaging elements on a 290 micron-pitch. The array will be read out with state-of-the-art time-division multiplexing (TDM), implement with 59 pixels (and 1 dark pixel) in each of the 69 TDM columns. Here we present a detailed overview of the baseline microcalorimeter detector design and present first results from both single pixel TESs and 4-pixel hydras. Our prototype LEM pixels utilize 15um x 50um Mo/Au TESs with a transition temperature of around 58 mK. These pixels incorporate high-fill-factor Au absorbers of thickness 0.54um. We have demonstrated an energy resolution of 0.90+/-0.02 eV and 1.90 +/-0.02 eV at 1.5 keV for single pixel and 4-pixel hydras, respectively, meeting the performance requirements of LEM. We show how the position discrimination in the hydra pixels can be achieved, down to energies of a few 100 eV, using the measured pulse rise-times. Finally, we will show that the properties of the LEM pixels are well optimized for the proposed TDM read out architecture.

Simon Richard Bandler↗

Pressure dependence of intermediate-range order and elastic properties of glassy Baltic amber

Amber is a unique example of a fragile glass that has been extensively aged below its glass transition temperature, thus reaching a state that is not accessible under normal experimental conditions. In this paper, we studied the medium-range order of Baltic amber by x-ray diffraction (XRD) at high pressures. The pressure dependences of the low-angle XRD intensity between 0 and 5 Å -1 were measured from 0 to 7.3 GPa by the energy-dispersive XRD. The first diffraction peak at 1.1 Å -1 and ambient pressure has a doublet structure consisting of the first sharp diffraction peak (FSDP) at 1.05 Å -1 and the second feature at 1.40 Å -1 . The peak position and the width of the FSDP increase as the pressure increases, while the intensity of the FSDP decreases. Below P 0 = 2.4 GPa, the rapid increase of the FSDP peak position was observed, while above P 0 , the gradual increase was observed. Below P 0 , voids and holes in a relatively low-density state are suppressed, whereas above P 0 , the suppression becomes mild. Such a change suggests the crossover from the low- to high-density state at P 0 . There is a close correlation between the pressure dependence of XRD and previously reported sound velocity results. The correlation between the mean-square fluctuation of the shear modulus on the nanometer scale and fragility in amber and other glass formers is also discussed.

36 MATERIALS SCIENCE↗

Anisotropic field-induced changes in the superconducting order parameter of UTe 2

UTe 2 is a newly discovered unconventional superconductor, where electron Cooper pairs combine into a spin-triplet ground state. We study the specific heat C( H,T ) of a high-quality UTe 2 single crystal, with a single anomaly at a high superconducting transition temperature T c = 2.1 K and a low residual Sommerfeld coefficient γ 0 . Applying magnetic fields up to 12 T along the crystallographic axes a, b , and c , we observe highly anisotropic behavior in γ 0 ( H ). Below 4 T, γ 0 ( H ) ≈ γ 0 + λi √H (i = a, b, c) , which is expected for an unconventional superconductor with nodes on the Fermi surface away from the direction of the magnetic field. At 4 T ( a and b axes) and 5.5 T ( c axis), distinctive changes in the behavior of γ 0 (H) suggest that a stable low-field ground state begins to evolve above 4 T. The data analysis indicates that the nodes are located near the a–b plane, with possible order parameters d B2u + iεd B1u or d B2u + iεd Au . Our findings support B 2u as the primary superconducting order parameter in UTe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structures of glass-forming liquids by x-ray scattering: Glycerol, xylitol, and D-sorbitol

In this work, synchrotron X-ray scattering has been used to investigate three liquid polyalcohols of different sizes (glycerol, xylitol and D-sorbitol) from above the glass transition temperatures $T_g$ to below. We focus on two structural orders: the association of the polar OH groups by hydrogen bonds (HBs) and the packing of the non-polar hydrocarbon groups. We find that the two structural orders evolve very differently reflecting the different natures of bonding. Upon cooling from 400 K, the O$\cdots$O correlation at 2.8 Å increases significantly in all three systems, indicating more HBs, until kinetic arrest at $T_g$; the increase is well described by an equilibrium between bonded and non-bonded OH with ΔH = 9.1 kJ/mol and ΔS = 13.4 J/mol/K. When heated above $T_g$, glycerol loses the fewest HBs per OH, followed by xylitol and by D-sorbitol, in the same order the number of OH groups per molecule increases (3, 5, and 6). The pair correlation functions of all three liquids show exponentially damped density modulations of wavelength 4.5 Å, which are associated with the main scattering peak and with the intermolecular C$\cdots$C correlation. In this respect, glycerol is the most ordered with the most persistent density ripples, followed by D-sorbitol and by xylitol. Heating above $T_g$ causes faster damping of the density ripples with the rate of change being the slowest in xylitol, followed by glycerol and by D-sorbitol. Given the different dynamic fragility of the three liquids (glycerol being the strongest and D-sorbitol the most fragile), we relate our results to the current theories of the structural origin for the difference. We find that the fragility difference is better understood on the basis of the thermal stability of HB clusters than that of the structure associated with the main scattering peak.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In-Plane Anisotropy of Charge Density Wave Fluctuations in 1⁢𝑇−TiSe 2

We report measurements of anisotropic triple-𝑞 charge density wave (CDW) fluctuations in the transition metal dichalcogenide 1⁢𝑇−TiSe 2 over a large volume of reciprocal space with x-ray diffuse scattering. Above the transition temperature, 𝑇 CDW , the in-plane diffuse scattering is marked by ellipses which reveal that the in-plane fluctuations are anisotropic. In addition, the out-of-plane diffuse scattering is characterized by rodlike structures which indicate that the CDW fluctuations in neighboring layers are largely decoupled. Furthermore, our analysis of the diffuse scattering line shapes and orientations suggests that the three charge density wave components contain independent phase fluctuations with a hierarchy of length scales, leading to intricate fluctuation patterns that go beyond the conventional 2D-to-3D crossover picture.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Probing Defects and Spin‐Phonon Coupling in CrSBr via Resonant Raman Scattering

Abstract Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, defects in mono‐ to multilayer CrSBr are correlated with structural, vibrational, and magnetic properties. Resonant Raman scattering is used to reveal distinct vibrational defect signatures. In pristine CrSBr, it is shown that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. Environmental exposure is shown to cause drastic degradation in monolayers, with the formation of intralayer defects. This is in contrast to multilayers that predominantly show bromine surface defects. Through deliberate ion irradiation, the formation of defect modes is tuned: these are strongly polarized and resonantly enhanced, reflecting the quasi‐‐1D electronic character of CrSBr. Strikingly, pronounced signatures of spin‐phonon coupling of the intrinsic phonon modes and the ion beam‐induced defect modes are observed throughout the magnetic transition temperature. Overall, defect engineering of magnetic properties is possible, with resonant Raman spectroscopy serving as a direct fingerprint of magnetic phases and defects in CrSBr.

2D magnetic semiconductors↗

High‐Pressure Synthesis of Ultra‐Incompressible, Hard and Superconducting Tungsten Nitrides

Abstract Transition metal nitrides, particularly those of 5 d metals, are known for their outstanding properties, often relevant for industrial applications. Among these metal elements, tungsten is especially attractive given its low cost. In this high‐pressure investigation of the W–N system, two novel ultra‐incompressible tungsten nitride superconductors, namely W 2 N 3 and W 3 N 5 , are successfully synthesized at 35 and 56 GPa, respectively, through a direct reaction between N 2 and W in laser‐heated diamond anvil cells. Their crystal structure is determined using synchrotron single‐crystal X‐ray diffraction. While the W 2 N 3 solid's sole constituting nitrogen species are N 3‐ units, W 3 N 5 features both discrete N 3‐ as well as N 2 4‐ pernitride anions. The bulk modulus of W 2 N 3 and W 3 N 5 is experimentally determined to be 380(3) and 406(7) GPa, and their ultra‐incompressible behavior is rationalized by their constituting WN 7 polyhedra and their linkages. Importantly, both W 2 N 3 and W 3 N 5 are recoverable to ambient conditions and stable in air. Density functional theory calculations reveal W 2 N 3 and W 3 N 5 to have a Vickers hardness of 30 and 34 GPa, and superconducting transition temperatures at ambient pressure (50 GPa) of 11.6 K (9.8 K) and 9.4 K (7.2 K), respectively. Additionally, transport measurements performed at 50 GPa on W 2 N 3 corroborate with the calculations.

Chemistry↗

Searching Materials Space for Hydride Superconductors at Ambient Pressure

Abstract A machine‐learning‐assisted approach is employed to search for superconducting hydrides under ambient pressure within an extensive dataset comprising over 150 000 compounds. The investigation yields ≈50 systems with transition temperatures surpassing 20 K, and some even reaching above 70 K. These compounds have very different crystal structures, with different dimensionality, chemical composition, stoichiometry, and arrangement of the hydrogens. Interestingly, most of these systems display slight thermodynamic instability, implying that their synthesis will re quire conditions beyond ambient equilibrium. Moreover, a consistent chemical composition is found in the majority of these systems, which combines alkali or alkali‐earth elements with noble metals. This observation suggests a promising avenue for future experimental investigations into high‐temperature superconductivity within hydrides at ambient pressure.

Cerqueira, Tiago F. T.↗

Efficient and Photostable Organic Solar Cells Achieved by Alloyed Dimer Acceptors with Tailored Linker Structures

Abstract High power conversion efficiency (PCE) and long‐term stability are prerequisites for commercialization of organic solar cells (OSCs). Herein, two dimer acceptors (DYTVT and DYTCVT) are developed with different properties through linker engineering, and study their effects as alloy‐like acceptors on the photovoltaic performance and photostability of OSCs. These ternary OSCs effectively combine the advantages of both dimer acceptors. DYTVT, characterized by its high backbone planarity, ensures elevated electron mobility and high glass‐transition temperature (T g ), leading to efficient charge transport and enhanced photostability of OSCs. Conversely, DYTCVT, with its significant dipole moment and electrostatic potential, enhances compatibility of the alloy acceptors with donors and refines the blend morphology, facilitating efficient charge generation in OSCs. Consequently, D18:DYTVT:DYTCVT OSCs exhibit higher PCE (18.4%) compared to D18:MYT (monomer acceptor, PCE = 16.5%), D18:DYTVT (PCE = 17.4%), and D18:DYTCVT (PCE = 17.0%) OSCs. Furthermore, owing to higherT g of alloy acceptors (133 °C) than MYT (T g = 80 °C) and DYTCVT (T g = 120 °C), D18:DYTVT:DYTCVT OSCs have significantly higher photostability (t 80% lifetime = 4250 h under 1‐sun illumination) compared to D18:MYT (t 80% lifetime = 40 h) and D18:DYTCVT OSCs (t 80% lifetime = 2910 h).

Chemistry↗

Enhanced Ion Transport and Molecular Packing Stability in Asymmetric 2D Nanostructured π‐Conjugated Thieno[3,2‐b]Thiophene‐Based Liquid Crystal

Organic semiconductors based on liquid crystal (LC) molecules have attracted increasing interest. Here, in this work, two linear LCs based on 2,5‐bis(thien‐2‐yl)thieno[3,2‐b]thiophene (BTTT) mesogen are designed and synthesized, including BTTT/dEO3 with two symmetrically attached tri(ethylene oxide) groups and BTTT/mEO6 with one asymmetrically attached hexa(ethylene oxide) group. These two molecules have comparable functional‐group compositions but different molecular geometries, leading to their moderately different material performances. Both LCs show smectic mesophases with relatively low transition temperatures as confirmed by differential scanning calorimetry and polarized optical microscopy. A combination of experimental grazing incidence wide‐angle X‐ray scattering and molecular dynamics (MD) simulations reveals a herringbone packing motif of BTTT segments in both LCs while a smaller molecular tilt angle in BTTT/mEO6. Ionic conductivities are measured by doping LCs with different amounts of ionic dopants, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). BTTT/mEO6 shows better smectic phase stability to higher LiTFSI doping ratios. Both LCs exhibit similar ionic conductivities in the smectic phases, but BTTT/mEO6 outperforms BTTT/dEO3 by a factor of three in the amorphous phase at higher temperatures. MD simulations, performed to examine the ion solvation environment, reveal that BTTT/mEO6 is more efficient in coordinating Li‐ions and screening their interactions with TFSI‐ions which further promote ionic transport.

grazing incidence wide-angle X-ray scattering↗

Unconventional Anomalous Hall Effect in Hexagonal Polar Magnet Y 3 Co 8 Sn 4

A rare realization of unconventional anomalous Hall effect (UAHE) both below and above the magnetic transition temperature (T C ) in a hexagonal noncentrosymmetric magnet Y 3 Co 8 Sn 4 , using a combined experimental and ab initio calculations. Occurrence of such UAHE is mainly attributed to the reciprocal ($\mathscr{KS}$) topology (i.e., the presence of topological Weyl points at/near the Fermi level), along with some contribution from the topological magnetic texture (at low temperatures), as inferred from the measured field-dependent ac susceptibility. The effect of UAHE on the measured transport behavior however evolves differently with temperature above and below T C = 53 K, suggesting different physical mechanism responsible in the two phases. A unique planar ferrimagnetic ordering is found to be the most stable state with ab-plane as the easy plane below T C . The simulated net magnetization and the moment per Co atom agrees fairly well with the experimentally measured values. A reasonably large anomalous Hall conductivity (AHC) is also observed in both the phases (above and below T C ) of the present compound, which is again not so ubiquitous. In conclusion, the results underscore the family of R 3 Co 8 Sn 4 (R = rare earth) polar magnets as a compelling backdrop for exploring the synergy of magnetism and topological non-trivial electronic states, pivotal for spintronic applications.

Density functional theory calculations↗

The Evolution of Magnetism in a Thin Film Pyrochlore Ferromagnetic Insulator

The pyrochlore vanadates are compelling candidates for next-generation dissipationless devices. Lu 2 V 2 O 7 and Y 2 V 2 O 7 are ferromagnetic insulators (T c ~ 70 K) that are believed to exhibit the magnon Hall effect and are expected to host topological magnons. Their completely dissipationless magnon edge states could be harnessed to realize low-power information transport in spintronic or magnonic devices. As a crucial step in the realization of devices, we synthesize the first thin films of pyrochlore Y 2 V 2 O 7 on isostructural Y 2 V 2 O 7 substrates and explore the evolution of their magnetic properties down to the ultrathin limit. All films are insulating ferromagnets with transition temperatures of up to the bulk value (T c ~ 68 K) that decrease with thickness according to finite-size effects. Our films also exhibit a change in anisotropy from in-plane to out-of-plane easy axis coincident with the development of partial strain relaxation and nonzero magnetic hysteresis in an applied field. Furthermore, this evolution demonstrates the impact of strain on magnetic anisotropy and paves the way to tunable magnon topology.

Anderson, Margaret A. [Harvard University, Cambrid↗

Tethered Small-Molecule Acceptors Simultaneously Enhance the Efficiency and Stability of Polymer Solar Cells

For polymer solar cells (PSCs), the mixture of polymer donors and small-molecule acceptors (SMAs) is fine-tuned to realize a favorable kinetically trapped morphology and thus a commercially viable device efficiency. However, the thermodynamic relaxation of the mixed domains within the blend raises concerns related to the long-term operational stability of the devices, especially in the record-holding Y-series SMAs. Here, a new class of dimeric Y6-based SMAs tethered with differential flexible spacers is reported to regulate their aggregation and relaxation behavior. In their polymer blends with PM6, it is found that they favor an improved structural order relative to that of Y6 counterpart. Most importantly, the tethered SMAs show large glass transition temperatures to suppress the thermodynamic relaxation in mixed domains. For the high-performing dimeric blend, an unprecedented open circuit voltage of 0.87 V is realized with a conversion efficiency of 17.85%, while those of regular Y6-base devices only reach 0.84 V and 16.93%, respectively. Most importantly, the dimer-based device possesses substantially reduced burn-in efficiency loss, retaining more than 80% of the initial efficiency after operating at the maximum power point under continuous illumination for 700 h. In conclusion, the tethering approach provides a new direction to develop PSCs with high efficiency and excellent operating stability.

14 SOLAR ENERGY↗