Transforming achiral semiconductors into chiral domains with exceptional circular dichroism

• 成果类型: Article
• 署名作者: Ugras, Thomas J.; Carson, River B.; Lynch, Reilly P.; Li, Haoyang; Yao, Yuan; Cupellini, Lorenzo; Page, Kirt A.; Wang, Da; Arbe, Arantxa; Bals, Sara; Smieska, Louisa; Woll, Arthur R.; Arteaga, Oriol; Javorfi, Tamas; Siligardi, Giuliano; Pescitelli, Gennaro; Weinstein, Steven J.; Robinson, Richard D.
• 署名单位: Cornell University; Cornell University; University of Pisa; Cornell University; University of Antwerp; University of Barcelona; Diamond Light Source; Rochester Institute of Technology; CIC biomaGUNE
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-10730
• DOI: 10.1126/science.ado7201
• 发表日期: 2025-01-31
• 关键词: optical-activity; orientation; polarization; rotation; metal

摘要

Highly concentrated solutions of asymmetric semiconductor magic-sized clusters (MSCs) of cadmium sulfide, cadmium selenide, and cadmium telluride were directed through a controlled drying meniscus front, resulting in the formation of chiral MSC assemblies. This process aligned their transition dipole moments and produced chiroptic films with exceptionally strong circular dichroism. G-factors reached magnitudes as high as 1.30 for drop-cast films and 1.06 for patterned films, approaching theoretical limits. By controlling the evaporation geometry, various domain shapes and sizes were achieved, with homochiral domains exceeding 6 square millimeters that transition smoothly between left- and right-handed chirality. Our results uncovered fundamental relationships between meniscus deposition processes, the alignment of supramolecular filaments and their MSC constituents, and their connection to emergent chiral properties.