Ultrafast on-demand exciton formation in a single-molecule junction by tailored terahertz pulses

• 成果类型: Article
• 署名作者: Kimura, Kensuke; Tamaki, Ryo; Lee, Minhui; Ouyang, Xingmei; Kusaba, Satoshi; Jaculbia, Rafael B.; Kawada, Yoichi; Jung, Jaehoon; Muranaka, Atsuya; Imada, Hiroshi; Katayama, Ikufumi; Takeda, Jun; Kim, Yousoo
• 署名单位: RIKEN; Yokohama National University; University of Tokyo; RIKEN; RIKEN; Institute for Basic Science - Korea (IBS); Hamamatsu Photonics; University of Ulsan; Gwangju Institute of Science & Technology (GIST); Yokohama National University
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-13788
• DOI: 10.1126/science.ads2776
• 发表日期: 2025-03-07
• 页码: 1077-1082
• 关键词: basis-sets; DYNAMICS; charge; Visualization; spectroscopy; manipulation; currents; DESIGN; motion; atoms

摘要

The ultrafast manipulation of molecular states by charge transfer is essential for characterizing and controlling molecular dynamics. In this study, we demonstrated exciton formation in a single molecule through ultrafast electron tunneling processes between a molecule and a metal tip of a scanning tunneling microscope (STM) using a phase-controlled terahertz (THz) pulse. The pronounced luminescence of the well-defined molecular system under the distinct carrier-envelope phase of the THz pulse revealed that sequential state-selective electron-tunneling processes to the frontier molecular orbitals promoted ultrafast exciton formation in the molecule at the STM junction. Furthermore, ultrafast control of exciton formation was achieved using phase- and delay-controlled THz pulse pairs, providing a route for the regulation of molecular dynamics and the emergence of new molecular functions.