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Updated: Jun 20, 2026

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

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Published on: August 6, 2018

Laser tunnel ionization from multiple orbitals in HCl.

H Akagi¹, T Otobe, A Staudte

¹Joint Laboratory for Attosecond Science, University of Ottawa and National Research Council, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.

Science (New York, N.Y.)

|September 12, 2009

Summary

This summary is machine-generated.

Researchers observed electrons tunneling from lower-lying states in hydrogen chloride (HCl) molecules, challenging previous assumptions and highlighting the importance of considering multiple orbitals in quantum tunneling.

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Area of Science:

Quantum mechanics
Atomic and molecular physics
Physical chemistry

Background:

Quantum tunneling is a fundamental quantum mechanical phenomenon influencing molecular electronic structure and radioactive decay.
Electron tunneling from atoms and molecules initiates the interaction of intense light pulses with matter.
Previously, tunneling was assumed to originate exclusively from the highest occupied orbital.

Purpose of the Study:

To investigate and observe electron tunneling from lower-lying electronic states in hydrogen chloride (HCl).
To challenge the prevailing assumption that tunneling initiates solely from the highest occupied orbital.
To quantify the contribution of lower-lying orbitals to molecular tunneling currents.

Main Methods:

Experimental observation of electron tunneling from hydrogen chloride (HCl).
Analysis of fragment ions to isolate tunneling pathways.
Measurement of molecular frame photoelectron angular distributions to identify tunneling origins.
Ab initio simulations to quantify tunneling contributions.

Main Results:

Direct observation of electron tunneling from a lower-lying electronic state in hydrogen chloride (HCl).
Isolation and identification of tunneling contributions from specific molecular orbitals.
Quantification of the impact of lower-lying orbitals on the total and angle-dependent tunneling current.
Experimental evidence supporting the role of coherent interactions between orbitals in tunneling.

Conclusions:

Tunneling processes can originate from electronic states lower than the highest occupied orbital.
The coherent interaction between different orbitals significantly influences tunneling phenomena.
A comprehensive understanding of molecular tunneling requires consideration of multiple electronic states and their interactions.