Absence of Triplets in Single-Photon Double Ionization of Methanol

Krishnendu Gope, Ester Livshits, Dror M. Bittner, Roi Baer, Daniel Strasser*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

8 Scopus citations


Despite the abundance of data concerning single-photon double ionization of methanol, the spin state of the emitted electron pair has never been determined. Here we present the first evidence that identifies the emitted electron pair spin as overwhelmingly singlet when the dication forms in low-energy configurations. The experimental data show that while the yield of the CH2O+ + H3+ Coulomb explosion channel is abundant, the metastable methanol dication is largely absent. According to high-level ab initio simulations, these facts indicate that photoionization promptly forms singlet dication states, where they quickly decompose through various channels, with significant H3+ yields on the low-lying states. In contrast, if we assume that the initial dication is formed in one of the low-lying triplet states, the ab initio simulations exhibit a metastable dication, contradicting the experimental findings. Comparing the average simulated branching ratios with the experimental data suggests a >3 order of magnitude enhancement of the singlet:triplet ratio compared with their respective 1:3 multiplicities.

Original languageAmerican English
Pages (from-to)8108-8113
Number of pages6
JournalJournal of Physical Chemistry Letters
Issue number19
StatePublished - 1 Oct 2020

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Copyright © 2020 American Chemical Society.


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