Ultrafast on-demand exciton formation in a single-molecule junction by tailored terahertz pulses
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.
Authors
- Rafael Jaculbia (ORCID: https://orcid.org/0000-0003-3156-2404)
- Xing‐Mei Ouyang
- Ikufumi Katayama (ORCID: https://orcid.org/0000-0001-6788-7732)
- Atsuya Muranaka (ORCID: https://orcid.org/0000-0002-3246-6003)
- Kensuke Kimura (ORCID: https://orcid.org/0000-0003-1270-5289)
- Jun Takeda (ORCID: https://orcid.org/0000-0002-1197-6821)
- Satoshi Kusaba (ORCID: https://orcid.org/0000-0002-5313-4817)
- Jaehoon Jung (ORCID: https://orcid.org/0000-0001-6550-139X)
- Yousoo Kim (ORCID: https://orcid.org/0000-0001-7730-0704)
- Ryo Tamaki (ORCID: https://orcid.org/0000-0003-3687-7245)
- Hiroshi Imada (ORCID: https://orcid.org/0000-0001-8508-8563)
- Minhui Lee (ORCID: https://orcid.org/0000-0001-7217-5334)
- Y. Kawada
Institutions
- Pioneer (United States) (US)
- Hamamatsu Photonics (Japan) (JP)
- Yokohama National University (JP)
- Gwangju Institute of Science and Technology (KR)
- University of Ulsan (KR)
- RIKEN Center for Sustainable Resource Science (JP)
- Institute for Basic Science (KR)
- RIKEN Center for Emergent Matter Science (JP)
- Korea Basic Science Institute (KR)
- Kanagawa Industrial Technology Center (JP)
- The University of Tokyo (JP)
Publication Details
- Journal
- Science
- Published
- 2025-03-06
- DOI
- https://doi.org/10.1126/science.ads2776
- Citations
- 14
- Primary Topic
- Molecular Junctions and Nanostructures
- Type
- article
- Field-Weighted Citation Impact
- 10.23