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

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Author(s)
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
Type
Article
Citation
Science (New York, N.Y.), v.387, no.6738, pp.1077 - 1082
Issued Date
2025-03
Abstract
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.
Publisher
American Association for the Advancement of Science
ISSN
0036-8075
DOI
10.1126/science.ads2776
URI
https://scholar.gist.ac.kr/handle/local/9005
Appears in Collections:
Department of Chemistry > 1. Journal Articles
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