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
Surface and Interface Science Laboratory, RIKEN Cluster for Pioneering Research, Wako, Saitama, Japan.
Department of Physics, Graduate School of Engineering Science, Yokohama National University, Yokohama, Kanagawa, Japan.
Science. 2025 Mar 7;387(6738):1077-1082. doi: 10.1126/science.ads2776. Epub 2025 Mar 6.
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.
通过电荷转移对分子态进行超快操控对于表征和控制分子动力学至关重要。在本研究中，我们利用相位控制的太赫兹（THz）脉冲，通过扫描隧道显微镜（STM）的分子与金属尖端之间的超快电子隧穿过程，证明了单分子中的激子形成。在太赫兹脉冲独特的载波包络相位下，定义明确的分子系统发出的显著发光表明，向前沿分子轨道的顺序态选择性电子隧穿过程促进了STM结处分子中激子的超快形成。此外，利用相位和延迟控制的太赫兹脉冲对实现了激子形成的超快控制，为调节分子动力学和新分子功能的出现提供了一条途径。
