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  1. Helical Complex Ladder Polymer with Amplification of Asymmetry

    Here, we report a Cu–salen helical complex ladder polymer (HLP-Cu) built from covalently fused Cu(Salen) units. Point chirality from enantiopure diamines directs the formation of a rigid, π-conjugated helix. Compared with a planar analogue (LLP-Cu) and the Cu(Salen) monomer, HLP-Cu exhibits up to 5-fold stronger circular dichroism and a maximum dissymmetry factor of 7.4 × 10–3. Titration experiments suggest a cooperative amplification of asymmetry arising from extended conjugation and helical geometry during helix formation. Time-dependent density functional theory calculations are employed to support this hypothesis, showing that increasing conjugation length and helical order enhance the rotational strength of contributing excitedmore » states via elevated magnetic transition moments and improved alignment of electric and magnetic transition moments. Our findings provide a new polymer platform for designing functional chiral materials with tunable chiroptical and spin-dependent properties.« less
  2. High-performance 2D electronic devices enabled by strong and tough two-dimensional polymer with ultra-low dielectric constant

    As the feature size of microelectronic circuits is scaling down to nanometer order, the increasing interconnect crosstalk, resistance-capacitance (RC) delay and power consumption can limit the chip performance and reliability. To address these challenges, new low-k dielectric (k < 2) materials need to be developed to replace current silicon dioxide (k = 3.9) or SiCOH, etc. However, existing low-k dielectric materials, such as organosilicate glass or polymeric dielectrics, suffer from poor thermal and mechanical properties. Two-dimensional polymers (2DPs) are considered promising low-k dielectric materials because of their good thermal and mechanical properties, high porosity and designability. Here, we report amore » chemical-vapor-deposition (CVD) method for growing fluoride rich 2DP-F films on arbitrary substrates. We show that the grown 2DP-F thin films exhibit ultra-low dielectric constant (in plane k = 1.85 and out-of-plane k = 1.82) and remarkable mechanical properties (Young’s modulus > 15 GPa). We also demonstrated the improved performance of monolayer MoS2 field-effect-transistors when utilizing 2DP-F thin films as dielectric substrates.« less
  3. Evidence of high-temperature exciton condensation in a two-dimensional semimetal

    Electrons and holes can spontaneously form excitons and condense in a semimetal or semiconductor, as predicted decades ago. This type of Bose condensation can happen at much higher temperatures in comparison with dilute atomic gases. Two-dimensional (2D) materials with reduced Coulomb screening around the Fermi level are promising for realizing such a system. Here we report a change in the band structure accompanied by a phase transition at about 180 K in single-layer ZrTe2 based on angle-resolved photoemission spectroscopy (ARPES) measurements. Below the transition temperature, gap opening and development of an ultra-flat band top around the zone center are observed.more » This gap and the phase transition are rapidly suppressed with extra carrier densities introduced by adding more layers or dopants on the surface. The results suggest the formation of an excitonic insulating ground state in single-layer ZrTe2, and the findings are rationalized by first-principles calculations and a self-consistent mean-field theory. Our study provides evidence for exciton condensation in a 2D semimetal and demonstrates strong dimensionality effects on the formation of intrinsic bound electron–hole pairs in solids.« less

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"Wang, Yuzhe"

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