Search for: All records

Abstract The structure and dynamics of polystyrene (PS)‐b‐poly(ethylene oxide) block copolymers (BCPs) are studied. The BCPs exhibit microphase‐separated cylindrical and lamellar morphologies. Structural dynamics are measured with X‐ray photon correlation spectroscopy in the small‐angle regime. Morphologies and domain sizes are evaluated using small‐angle X‐ray scattering (SAXS), scanning electron microscopy, and atomic force microscopy. Different solvent processing conditions are investigated. Grain sizes evaluated using SAXS are found to depend on processing only for the rubbery majority BCP. The structural relaxation times are examined as a function of PS volume fraction, temperature, morphology, and structural sizes. Well above the glass transition temperature (T_g) of PS, all samples exhibit stretched autocorrelation decays and diffusive dynamics. NearT_gof PS, the dynamics of all samples are anomalous with compressed autocorrelation decays and hyperdiffusive dynamics. This transition occurs at 153 °C or 1.13T_gof PS. In the diffusive regime (at high temperature), structural relaxation times are dependent on the processing method. Near PST_g(at low temperature), structural relaxation times scale with the PS volume fraction. Structural relaxation times do not correlate with grain size, indicating that the out‐of‐equilibrium state of PS dominates the structural dynamics of these strongly phase‐segregated BCPs. 

Abstract Chirality has been a property of central importance in physics, chemistry and biology for more than a century. Recently, electrons were found to become spin polarized after transmitting through chiral molecules, crystals, and their hybrids. This phenomenon, called chirality-induced spin selectivity (CISS), presents broad application potentials and far-reaching fundamental implications involving intricate interplays among structural chirality, topological states, and electronic spin and orbitals. However, the microscopic picture of how chiral geometry influences electronic spin remains elusive, given the negligible spin-orbit coupling (SOC) in organic molecules. In this work, we address this issue via a direct comparison of magnetoconductance (MC) measurements on magnetic semiconductor-based chiral molecular spin valves with normal metal electrodes of contrasting SOC strengths. The experiment reveals that a heavy-metal electrode provides SOC to convert the orbital polarization induced by the chiral molecular structure tospinpolarization. Our results illustrate the essential role of SOC in the metal electrode for the CISS spin valve effect. A tunneling model with a magnetochiral modulation of the potential barrier is shown to quantitatively account for the unusual transport behavior. 

Abstract Zero‐dimensional (0D) organic metal halide hybrids (OMHHs) have recently emerged as a new class of light emitting materials with exceptional color tunability. While near‐unity photoluminescence quantum efficiencies (PLQEs) are routinely obtained for a large number of 0D OMHHs, it remains challenging to apply them as emitter for electrically driven light emitting diodes (LEDs), largely due to the low conductivity of wide bandgap organic cations. Here, the development of a new OMHH, triphenyl(9‐phenyl‐9H‐carbazol‐3‐yl) phosphonium antimony bromide (TPPcarzSbBr₄), as emitter for efficient LEDs, which consists of semiconducting organic cations (TPPcarz⁺) and light emitting antimony bromide anions (Sb₂Br₈²⁻), is reported. By replacing one of the phenyl groups in a well‐known tetraphenylphosphonium cation (TPP⁺) with an electroactive phenylcarbazole group, a semiconducting TPPcarz⁺cation is developed for the preparation of red emitting 0D TPPcarzSbBr₄single crystals with a high PLQE of 93.8%. With solution processed TPPcarzSbBr₄thin films (PLQE of 86.1%) as light emitting layer, red LEDs are fabricated to exhibit an external quantum efficiency (EQE) of 5.12%, a peak luminance of 5957 cd m⁻², and a current efficiency of 14.2 cd A⁻¹, which are the best values reported to date for electroluminescence devices based on 0D OMHHs. 

Abstract Metal halide perovskite nanocrystals (NCs) have emerged as highly promising light emitting materials for various applications, ranging from perovskite light‐emitting diodes (PeLEDs) to lasers and radiation detectors. While remarkable progress has been achieved in highly efficient and stable green, red, and infrared perovskite NCs, obtaining efficient and stable blue‐emitting perovskite NCs remains a great challenge. Here, a facile synthetic approach for the preparation of blue emitting CsPbBr₃nanoplatelets (NPLs) with treatment by an organic sulfate is reported, 2,2‐(ethylenedioxy) bis(ethylammonium) sulfate (EDBESO₄), which exhibit remarkably enhanced photoluminescence quantum efficiency (PLQE) and stability as compared to pristine CsPbBr₃NPLs coated with oleylamines. The PLQE is improved from ≈28% for pristine CsPbBr₃NPLs to 85% for EDBESO₄treated CsPbBr₃NPLs. Detailed structural characterizations reveal that EDBESO₄treatment leads to surface passivation of CsPbBr₃NPLs by both EDBE²⁺and SO₄^2–ions, which helps to prevent the coalescence of NPLs and suppress the degradation of NPLs. A simple proof‐of‐concept device with emission peaked at 462 nm exhibits an external quantum efficiency of 1.77% with a luminance of 691 cd m⁻²and a half‐lifetime of 20 min, which represents one of the brightest pure blue PeLEDs based on NPLs reported to date. 

Abstract Surface passivation of perovskite solar cells (PSCs) using a low‐cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA,N,N‐bis(tert‐butyloxycarbonyl)‐quinacridone (TBOC‐QA), followed by thermal annealing to convert TBOC‐QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI₃) showed significantly improved performance with remarkable stability. A PCE of 21.1 % was achieved, which is much higher than 18.9 % recorded for the unmodified devices. The QA coating with exceptional insolubility and hydrophobicity also led to greatly enhanced contact angle from 35.6° for the pristine MAPbI₃thin films to 77.2° for QA coated MAPbI₃thin films. The stability of QA passivated MAPbI₃perovskite thin films and PSCs were significantly enhanced, retaining about 90 % of the initial efficiencies after more than 1000 hours storage under ambient conditions.