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Volume averaging effect in nonlinear processes of focused laser fields.

Yuzhong Yao¹, William M Freund¹, Jie Zhang¹

¹Department of Chemistry, Oregon State University, Corvallis, Oregon 97331-4003, USA.

The Journal of Chemical Physics

|August 15, 2021

Summary

Volume averaging in focused laser fields can obscure nonlinear process intensity dependence. However, simple power-law relationships remain unaffected, while multi-photon saturation effects require advanced techniques like z-scans for accurate characterization.

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Area of Science:

Nonlinear optics
Laser-matter interactions
Atomic physics

Background:

Focused laser fields exhibit intensity variations across the sampled volume.
This volume averaging effect can hinder the accurate determination of nonlinear process intensity dependence.
Understanding these effects is crucial for precise measurements in laser spectroscopy and material processing.

Purpose of the Study:

To theoretically derive and experimentally investigate the impact of volume averaging on nonlinear optical processes.
To determine conditions under which volume averaging does not affect the extracted intensity dependence exponent.
To establish the necessity and methodology for advanced techniques like z-scans to probe saturation effects in multi-photon processes.

Main Methods:

Theoretical analysis of volume averaging for power-law dependent nonlinear processes.
Implementation of spatial filtering and laser focus displacement (z-scan) techniques.
Experimental measurements using a nanosecond laser and multiphoton ionization of argon atoms.
Characterization of beam waist and Rayleigh range for a non-ideal Gaussian beam profile.

Main Results:

Volume averaging does not alter the derived exponent for simple power-law intensity dependencies when the entire volume is sampled.
Z-scan techniques are essential for revealing saturation effects in multi-photon processes.
Careful modeling of spatial discrimination and z-scan range is required for accurate intensity dependence measurements.
Experimental results for argon multiphoton ionization showed remarkable agreement with theoretical predictions.

Conclusions:

The study clarifies the influence of volume averaging on nonlinear optical measurements.
It highlights the importance of advanced scanning techniques for detailed analysis of multi-photon processes.
Accurate characterization of laser beam parameters and detection limitations is vital for reliable experimental outcomes.