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Creators/Authors contains: "Guo, Peijun"

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  1. Abstract

    In two-dimensional chiral metal-halide perovskites, chiral organic spacers endow structural and optical chirality to the metal-halide sublattice, enabling exquisite control of light, charge, and electron spin. The chiroptical properties of metal-halide perovskites have been measured by transmissive circular dichroism spectroscopy, which necessitates thin-film samples. Here, by developing a reflection-based approach, we characterize the intrinsic, circular polarization-dependent complex refractive index for a prototypical two-dimensional chiral lead-bromide perovskite and report large circular dichroism for single crystals. Comparison with ab initio theory reveals the large circular dichroism arises from the inorganic sublattice rather than the chiral ligand and is an excitonic phenomenon driven by electron-hole exchange interactions, which breaks the degeneracy of transitions between Rashba-Dresselhaus-split bands, resulting in a Cotton effect. Our study suggests that previous data for spin-coated films largely underestimate the optical chirality and provides quantitative insights into the intrinsic optical properties of chiral perovskites for chiroptical and spintronic applications.

     
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  2. Free, publicly-accessible full text available December 1, 2024
  3. Abstract

    The layer stacking order in 2D materials strongly affects functional properties and holds promise for next-generation electronic devices. In bulk, octahedral MoTe2possesses two stacking arrangements, the ferroelectric Weyl semimetal Tdphase and the higher-order topological insulator 1T′ phase. However, in thin flakes of MoTe2, it is unclear if the layer stacking follows the Td, 1T′, or an alternative stacking sequence. Here, we use atomic-resolution scanning transmission electron microscopy to directly visualize the MoTe2layer stacking. In thin flakes, we observe highly disordered stacking, with nanoscale 1T′ and Tddomains, as well as alternative stacking arrangements not found in the bulk. We attribute these findings to intrinsic confinement effects on the MoTe2stacking-dependent free energy. Our results are important for the understanding of exotic physics displayed in MoTe2flakes. More broadly, this work suggestsc-axis confinement as a method to influence layer stacking in other 2D materials.

     
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    Free, publicly-accessible full text available December 1, 2024
  4. Abstract

    The combined effects of compact TiO2(c‐TiO2) electron‐transport layer (ETL) are investigated without and with mesoscopic TiO2(m‐TiO2) on top, and without and with an iodine‐terminated silane self‐assembled monolayer (SAM), on the mechanical behavior, opto–electronic properties, photovoltaic (PV) performance, and operational‐stability of solar cells based on metal‐halide perovskites (MHPs). The interfacial toughness increases almost threefold in going from c‐TiO2without SAM to m‐TiO2with SAM. This is attributed to the synergistic effect of the m‐TiO2/MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine‐terminated silane SAM. The combination of m‐TiO2and SAM also offers a significant beneficial effect on the photocarriers extraction at the ETL/MHP interface, resulting in perovskite solar cells (PSCs) with power‐conversion efficiency (PCE) of over 24% and 20% for 0.1 and 1 cm2active areas, respectively. These PSCs also have exceptionally long operational‐stability lives: extrapolatedT80 (duration at 80% initial PCE retained) is ≈18 000 and 10 000 h for 0.1 and 1 cm2active areas, respectively.Postmortemcharacterization and analyses of the operational‐stability‐tested PSCs are performed to elucidate the possible mechanisms responsible for the long operational‐stability.

     
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  5. null (Ed.)