Robert T. Sang | Searcharxiv

arXiv2022

Laser-Induced Graphitisation of Diamond Under 30 fs Laser Pulse Irradiation

The degree of laser-induced graphitisation from a sp3-bonded to a sp2-bonded carbon fraction in a single crystal chemical vapour deposited (CVD) diamond under a varying fluence of an ultrashort pulsed laser (30 fs, 800 nm, 1 kHz) irradiation has been studied. The tetrahedral CVD sp3-phase was found to transition to primarily an sp2-aromatic crystalline graphitic fraction below the critical fluence of 3.9 J/cm2, above which predominantly an amorphous carbon was formed. A fractional increase of fluence from 3.3 J/cm2 to 3.9 J/cm2 (~ 20 %) resulted in a substantial (~ three-fold) increased depth of the sp2-graphitised areas owing to the non-linear interactions associated with an fs-laser irradiation. Additionally, formation of C=O carbonyl group was observed below the critical threshold fluence; the C=O cleavage occurred gradually with the increase of irradiation fluence of 30 fs laser light. The implications for these findings on enhancement of fs-driven processing of diamond are discussed.

physics.chem-ph↗

arXiv2020

Observation of Dynamic Stark Resonances in Strong-Field Excitation

We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.

physics.atom-ph↗