Picosecond Fickian Proton Diffusion in a Deep Eutectic Solvent Revealed by Backscattering QENS
Abstract We report anomalous continuous Fickian proton diffusion in the 40 mol % imidazole/levulinic acid deep eutectic solvent, a transport signature lacking a resolvable jump length or residence time and marking the first observation in a liquid proton conductor. In every hydrogen-bonded proton conductor previously characterized by quasi-elastic neutron scattering (QENS), Grotthuss-type transport manifests as jump diffusion with a finite step length set by the hydrogen-bond spacing. Using isotopic contrast QENS difference-spectrum analysis to isolate the acidic proton dynamics from molecular background, we find that molecular species undergo conventional jump diffusion. In contrast, the acidic proton exhibits purely quadratic q dependence (Γ ∝ q2) across the entire picosecond time scale measurement window.
Authors
- Thomas Simunovic
- Bhavya Sharma (ORCID: https://orcid.org/0000-0003-4388-5702)
- Eugene Mamontov (ORCID: https://orcid.org/0000-0002-5684-2675)
- Mark Dadmun (ORCID: https://orcid.org/0000-0003-4304-6087)
- Adam E. Imel (ORCID: https://orcid.org/0000-0002-3177-7846)
- Brian Andrew Barth (ORCID: https://orcid.org/0000-0002-3887-6054)
- Shane Foister (ORCID: https://orcid.org/0009-0008-7780-0301)
- Thomas A. Zawodzinski (ORCID: https://orcid.org/0000-0002-2690-8784)
- Kevin J. Ledford (ORCID: https://orcid.org/0009-0005-9948-2656)
- Katherine D. Vogel
- Mrinalini Ayilliath Kolaprath
Institutions
- Oak Ridge National Laboratory (US)
- University of Tennessee Health Science Center (US)
- University of Tennessee at Knoxville (US)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2026-09-25
- DOI
- https://doi.org/10.1021/acs.jpclett.6c02172
- Primary Topic
- Fuel Cells and Related Materials
- Type
- article
- Field-Weighted Citation Impact
- 0.00