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- Title
Molecular ground-state dissociation in the condensed phase employing plasmonic field enhancement of chirped mid-infrared pulses.
- Authors
Morichika, Ikki; Murata, Kei; Sakurai, Atsunori; Ishii, Kazuyuki; Ashihara, Satoshi
- Abstract
Selective bond cleavage via vibrational excitation is the key to active control over molecular reactions. Despite its great potential, the practical implementation in condensed phases have been hampered to date by poor excitation efficiency due to fast vibrational relaxation. Here we demonstrate vibrationally mediated, condensed-phase molecular dissociation by employing intense plasmonic near-fields of temporally-shaped mid-infrared (mid-IR) pulses. Both down-chirping and substantial field enhancement contribute to efficient ladder climbing of the carbonyl stretch vibration of W(CO)6 in n-hexane solution and to the resulting CO dissociation. We observe an absorption band emerging with laser irradiation at the excitation beam area, which indicates that the dissociation is followed by adsorption onto metal surfaces. This successful demonstration proves that the combination of ultrafast optics and nano-plasmonics in the mid-IR range is useful for mode-selective vibrational ladder climbing, paving the way toward controlled ground-state chemistry. There is a growing interest in controlling the chemical process at molecular level. Here the authors show the mid-IR chirped pulse driven ground-state dissociation of condensed phase tungsten hexacarbonyl using efficient vibrational ladder climbing process by employing plasmonic near-field enhancement.
- Subjects
CONDENSED matter; PLASMONICS; CHEMICAL process control; DISSOCIATION (Chemistry); SERS spectroscopy; METALLIC surfaces; SCISSION (Chemistry); LASER beams
- Publication
Nature Communications, 2019, Vol 10, Issue 1, pN.PAG
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-019-11902-6