Theoretical Insights into Energy Absorption and Charge Draining during Field Evaporation Assisted by Femtosecond Laser Pulses.

Manipulation of laser-assisted field evaporation taking place at a sub-picosecond time scale relies on a full understanding of the dynamics at a microscopic level. We use first-principles methods to investigate the mechanism of energy absorption and charge draining during fast evaporation of silicon in a high electrostatic field with ultrafast-laser illumination. The results show that laser energy absorption to trigger field evaporation can be described by an effective cross section, which depends on the photon frequency and the static field strength. The cross section is not affected by pulse duration or laser intensity, indicating that the absorption is first-order. It is found that the charge state of the evaporating ion fluctuates due to the collective excitation of electrons. The average charge state does not depend on laser parameters but only on the static field strength, in agreement with experimental observations. Our work provides theoretical insights into the manipulation of modern atom probe tomography and other ultrafast-laser-induced phenomena in high electric fields.