Selective subsurface absorption of hydrogen in palladium using laser distillation

Area of Science:

• Surface science
• Physical chemistry
• Theoretical chemistry

Background:

• Selective subsurface absorption of hydrogen in palladium is crucial for catalysis.
• Controlling adsorbate dynamics at the quantum level is challenging.

Purpose of the Study:

• To develop a theoretical model for selective subsurface absorption of atomic hydrogen on Pd(111) using IR laser pulses.
• To investigate the use of laser pulses and dissipation for controlling adsorbate dynamics.

Main Methods:

• Theoretical modeling using the reduced density matrix approach.
• Treatment of energy and phase relaxation via the semigroup formalism.
• Utilizing rationally designed and on-the-fly optimized IR laser pulses for vibrational excitation.

Main Results:

• Demonstrated selective subsurface absorption of hydrogen on Pd(111) via IR laser excitation.
• Showcased
• laser distillation
• as a mechanism to transfer population to inaccessible states using dissipation.
• Revealed differences in laser control strategies between 1D and 3D treatments of the system.

Conclusions:

• Infrared laser pulses can selectively drive atomic hydrogen into the subsurface of Pd(111).
• Dissipation is a viable tool for controlling quantum dynamics and achieving selective state population.
• The dimensionality of the system significantly impacts optimal laser control strategies.