Details
| Originalsprache | Englisch |
|---|---|
| Aufsatznummer | 9196 |
| Fachzeitschrift | Nature Communications |
| Jahrgang | 15 |
| Ausgabenummer | 1 |
| Publikationsstatus | Veröffentlicht - 25 Okt. 2024 |
Abstract
Ultraviolet (UV) light that penetrates our atmosphere initiates various photochemical and photobiological processes. However, the absence of extremely short UV pulses has so far hindered our ability to fully capture the mechanisms at the very early stages of such processes. This is important because the concerted motion of electrons and nuclei in the first few femtoseconds often determines molecular reactivity. Here we investigate the dissociative dynamics of iodomethane following UV photoexcitation, utilizing mass spectrometry with a 5 fs time resolution. The short duration of the UV pump pulse (4.2 fs) allows the ultrafast dynamics to be investigated in the absence of any external field, from well before any significant vibrational displacement occurs until dissociation has taken place. The experimental results combined with semi-classical trajectory calculations provide the identification of the main dissociation channels and indirectly reveal the signature of a conical intersection in the time-dependent yield of the iodine ion. Furthermore, we demonstrate that the UV-induced breakage of the C-I bond can be prevented when the molecule is ionized by the probe pulse within 5 fs after the UV excitation, showcasing an ultrafast stabilization scheme against dissociation.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Allgemeine Chemie
- Biochemie, Genetik und Molekularbiologie (insg.)
- Allgemeine Biochemie, Genetik und Molekularbiologie
- Physik und Astronomie (insg.)
- Allgemeine Physik und Astronomie
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in: Nature Communications, Jahrgang 15, Nr. 1, 9196, 25.10.2024.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Few-femtosecond time-resolved study of the UV-induced dissociative dynamics of iodomethane
AU - Colaizzi, Lorenzo
AU - Ryabchuk, Sergey
AU - Månsson, Erik P.
AU - Saraswathula, Krishna
AU - Wanie, Vincent
AU - Trabattoni, Andrea
AU - González-Vázquez, Jesús
AU - Martín, Fernando
AU - Calegari, Francesca
N1 - Publisher Copyright: © The Author(s) 2024.
PY - 2024/10/25
Y1 - 2024/10/25
N2 - Ultraviolet (UV) light that penetrates our atmosphere initiates various photochemical and photobiological processes. However, the absence of extremely short UV pulses has so far hindered our ability to fully capture the mechanisms at the very early stages of such processes. This is important because the concerted motion of electrons and nuclei in the first few femtoseconds often determines molecular reactivity. Here we investigate the dissociative dynamics of iodomethane following UV photoexcitation, utilizing mass spectrometry with a 5 fs time resolution. The short duration of the UV pump pulse (4.2 fs) allows the ultrafast dynamics to be investigated in the absence of any external field, from well before any significant vibrational displacement occurs until dissociation has taken place. The experimental results combined with semi-classical trajectory calculations provide the identification of the main dissociation channels and indirectly reveal the signature of a conical intersection in the time-dependent yield of the iodine ion. Furthermore, we demonstrate that the UV-induced breakage of the C-I bond can be prevented when the molecule is ionized by the probe pulse within 5 fs after the UV excitation, showcasing an ultrafast stabilization scheme against dissociation.
AB - Ultraviolet (UV) light that penetrates our atmosphere initiates various photochemical and photobiological processes. However, the absence of extremely short UV pulses has so far hindered our ability to fully capture the mechanisms at the very early stages of such processes. This is important because the concerted motion of electrons and nuclei in the first few femtoseconds often determines molecular reactivity. Here we investigate the dissociative dynamics of iodomethane following UV photoexcitation, utilizing mass spectrometry with a 5 fs time resolution. The short duration of the UV pump pulse (4.2 fs) allows the ultrafast dynamics to be investigated in the absence of any external field, from well before any significant vibrational displacement occurs until dissociation has taken place. The experimental results combined with semi-classical trajectory calculations provide the identification of the main dissociation channels and indirectly reveal the signature of a conical intersection in the time-dependent yield of the iodine ion. Furthermore, we demonstrate that the UV-induced breakage of the C-I bond can be prevented when the molecule is ionized by the probe pulse within 5 fs after the UV excitation, showcasing an ultrafast stabilization scheme against dissociation.
UR - http://www.scopus.com/inward/record.url?scp=85207816279&partnerID=8YFLogxK
U2 - 10.1038/s41467-024-53183-8
DO - 10.1038/s41467-024-53183-8
M3 - Article
C2 - 39455555
AN - SCOPUS:85207816279
VL - 15
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 9196
ER -