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Spatial Separation of Molecular Conformers and Clusters

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Ultrafast Proton Transfer and Contact Ion-Pair Formation in Formic Acid Clusters.

Shaun F Sutton^1,2, Chase H Rotteger^1,2, Carter K Jarman^1,2

¹School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United States.

The Journal of Physical Chemistry Letters

|September 8, 2023

Summary

Ultrafast proton transfer in formic acid clusters (FA) shows ion pair formation increases with size. Rearrangement and transfer times grow linearly with cluster size, becoming significant in small clusters.

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Area of Science:

Physical Chemistry
Chemical Physics
Spectroscopy

Background:

Proton transfer is fundamental in chemical reactions.
Understanding cluster dynamics is key to molecular interactions.
Formic acid clusters serve as model systems for hydrogen-bonded networks.

Purpose of the Study:

Investigate ultrafast proton transfer dynamics in homogeneous formic acid clusters (FA) with n < 10.
Elucidate the relationship between cluster size and proton transfer efficiency.
Determine the timescale of rearrangement and proton transfer within these clusters.

Main Methods:

Femtosecond time-resolved mass spectrometry to monitor dynamics.
Ab initio calculations to model excitation/relaxation pathways.
Analysis of ion pair formation and rearrangement lifetimes.

Main Results:

Successful ion pair formation increases logarithmically with cluster size.
A contact ion pair forms before formate anion dissociation.
Rearrangement and proton transfer times increase linearly with cluster size (approx. 67 fs per additional molecule).
Times ranged from 213 ± 51 fs (trimer) to 667 ± 116 fs (FA9).

Conclusions:

Proton transfer is minimal in formic acid dimers.
Proton transfer becomes prominent in small formic acid clusters.
Cluster size significantly influences proton transfer dynamics and timescales.