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Spin chemistry of photogenerated spin-correlated radical pairs (SCRPs) offers a practical approach to control chemical reactions and molecular emissions using weak magnetic fields. This capability to harness magnetic field effects (MFEs) paves the way for developing SCRPs-based molecular qubits. Here, we introduce a new series of donor-chiral bridge-acceptor (D-χ-A) molecules that demonstrate significant MFEs on fluorescence intensity and lifetime in solution at room temperature – critical for quantum sensing. By precisely tuning the donor site through torsional locking, distance extension, and planarization, we achieved remarkable control over key quantum properties, including field-response range and linewidth. In the most responsive systems, emission lifetimes increased by over 200%, and total emission intensity was modulated by up to 30%. This level of tunability, and rational design principle of optically addressable molecular qubits, represents a major leap toward functional synthetic molecular qubits, advancing the field of molecular quantum technologies. 

Abstract The interface between the hole transport layer (HTL) and perovskite in p‐i‐n perovskite solar cells (PSCs) plays a vital role in the device performance and stability. However, the impact of this interface on the vertical phase segregation of mixed halide perovskite remains insufficiently understood. This work systematically investigates the impact of chemical and electronic properties of HTL on vertical halide segregation of mixed‐halide perovskites. This work shows that incorporating a poly[bis(4‐phenyl) (2,4,6‐trimethylphenyl) amine] (PTAA)/CuI_xBr_1‐xbilayer as the HTL significantly suppresses light‐induced vertical phase segregation in MAPb(I_0.7Br_0.3)₃. This work uses grazing‐incidence X‐ray diffraction (GIXRD) to capture the depth‐resolved composition change of MAPb(I_0.7Br_0.3)₃at the interface and within the bulk under illumination. By changing the illumination direction and the electronic properties of HTL, this work elucidates the roles of charge carrier extraction and interfacial defects on vertical phase segregation. The PTAA/CuI_xBr_1‐xbilayer, with its synergistic passivation and efficient hole extraction ability, stabilizes the interface and bulk of the mixed halide perovskite layer and prevents phase segregation. This work underscores that synergetic passivation and efficient hole extraction pack a more powerful punch for arresting the vertical phase segregation in mixed‐halide perovskite.