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$In Situ Neutron Powder Diffraction Using Custom-made Lithium-ion Batteries$

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Published on: November 10, 2014

Predissociation dynamics of lithium iodide.

H Schmidt¹, J von Vangerow¹, F Stienkemeier¹

¹Physikalisches Institut, Universität Freiburg, 79104 Freiburg, Germany.

The Journal of Chemical Physics

|February 2, 2015

Summary

Lithium iodide (LiI) predissociation dynamics were studied. Femtosecond spectroscopy revealed LiI predissociation occurs at the X-A potential curve crossing, while helium nanodroplets rapidly quench vibrational excitation.

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Area of Science:

Physical Chemistry
Molecular Spectroscopy
Quantum Dynamics

Background:

Predissociation dynamics govern molecular decay pathways.
Understanding excited-state dynamics is crucial for molecular control.
Lithium iodide (LiI) serves as a model system for studying these processes.

Purpose of the Study:

To investigate the predissociation dynamics of LiI in the A-state.
To compare gas-phase dynamics with LiI embedded in helium nanodroplets.
To elucidate the mechanism of vibrational wave packet decay.

Main Methods:

Femtosecond pump-probe photoionization spectroscopy.
High-level ab initio electronic structure calculations.
Simulations of wave packet dynamics.

Main Results:

Gas-phase LiI exhibits damped oscillations in ion signals, indicating vibrational wave packet excitation and decay.
Signal decay is attributed to predissociation at the avoided X-A potential curve crossing.
A coupling constant V_XA = 650(20) cm(-1) was inferred for the X-A crossing.
LiI in helium nanodroplets shows no pump-probe delay dependence, suggesting rapid droplet-induced relaxation.

Conclusions:

The primary predissociation pathway for LiI in the A-state involves the X-A potential curve crossing.
Helium nanodroplets effectively suppress vibrational excitation, leading to rapid relaxation.
Femtosecond spectroscopy provides insights into ultrafast molecular dynamics and environmental effects.