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Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization

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Double ionization of nitrogen from multiple orbitals.

Zhifeng Wu¹, Chengyin Wu, Xianrong Liu

¹State Key Laboratory for Mesoscopic Physics, Department of Physics, Peking University, Beijing 100871, People's Republic of China.

The Journal of Physical Chemistry. A

|June 4, 2010

Summary

This summary is machine-generated.

Intense femtosecond laser pulses cause nitrogen molecules to form doubly charged ions. Some ions are metastable, while others dissociate into charged fragments, revealing insights into molecular electronic states.

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Area of Science:

Quantum mechanics
Atomic and molecular physics
Laser physics

Background:

Molecules in intense laser fields can undergo tunnel ionization from multiple valence orbitals.
This process leads to the formation of molecular ions in various electronic states.
Understanding these states is crucial for controlling molecular responses to light.

Purpose of the Study:

To investigate the double ionization of nitrogen molecules using intense femtosecond laser pulses.
To characterize the dissociation dynamics of doubly charged nitrogen molecular ions (N2(2+)).
To identify the electronic states involved and the contributions of different valence orbitals.

Main Methods:

Utilizing a reaction microscope to study molecular ion dissociation.
Analyzing kinetic energy releases and angular distributions of fragment ions.
Performing computational chemistry calculations (CASSCF and MRCI) to identify electronic states.

Main Results:

Observed both metastable doubly charged nitrogen molecular ions and dissociating ions.
Identified charge-symmetric (N(+) + N(+)) and charge-asymmetric (N2(+) + N) dissociation channels.
Correlated dissociation pathways with specific electronic states of the molecular dication.

Conclusions:

Femtosecond laser-induced double ionization of nitrogen produces a complex mixture of ionic states.
Dissociation dynamics are strongly dependent on the electronic state of the N2(2+) ion.
Computational methods are essential for interpreting experimental observations and understanding electronic structure contributions.