Journal: Journal of Chemical Physics
DOI: 10.1063/1.5125145
PubMed: 31703493
Open Access: Publisher link
Published: November 5, 2019
Authors
János Sarka, C. Petty, B. Poirier
Abstract
Exact quantum dynamics calculations are performed for the bound rovibrational states of the neon tetramer (Ne4) in its ground electronic state, using pair-wise Lennard-Jones potentials and the ScalIT suite of parallel codes.
The vibrational states separate into two groups:
- A low-lying group mostly localized to a single potential well
- A higher-energy delocalized group lying above the isomerization threshold
This structure is a testament to the “intermediate” quantum nature of Ne4 — neon is light enough for significant quantum effects but heavy enough not to be purely quantum like helium.
To accurately and efficiently represent both groups of states, the phase-space optimized discrete variable representation (PSO-DVR) approach was used as implemented in ScalIT. Rovibrational energy levels for all total angular momentum values J = 1–5 were also computed, treating all Coriolis coupling exactly.
Notes
- Neon clusters sit at the fascinating boundary between classical and quantum behavior — heavier than helium (quantum), lighter than argon (classical)
- The isomerization dynamics are particularly interesting: fluxional clusters that tunnel between geometries
- Collaboration with János Sarka (then at Budapest, now widely published in molecular spectroscopy)
- Likely the last paper from Corey’s academic chemistry career before the full pivot to blockchain/security