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Abstract The carrier excitation, relaxation, energy transport, and conversion processes during light‐nanocrystal (NC) interactions have been intensively investigated for applications in optoelectronics, photocatalysis, and photovoltaics. However, there are limited studies on the non‐equilibrium heating under relatively high laser excitation that leads to NCs sintering. Here, the authors use femtosecond laser two‐pulse correlation and in‐situ optical transmission probing to investigate the non‐equilibrium heating of NCs and transient sintering dynamics. First, a two‐pulse correlation study reveals that the sintering rate strongly increases when the two heating laser pulses are temporally separated by <10 ps. Second, the sintering rate is found to increase nonlinearly with laser fluence when heating with ≈700 fs laser pulses. By three‐temperature modeling, the NC sintering mechanism mediated by electron induced ligand transformation is suggested. The ultrafast and non‐equilibrium process facilitates sintering in dry (spin‐coated) and wet (solvent suspended) environments. The nonlinear dependence of sintering rate on laser fluence is exploited to print sub‐diffraction‐limited features in NC suspension. The smallest feature printed is ≈200 nm, which is ≈¼ of the laser wavelength. These findings provide a new perspective toward nanomanufacturing development based on probing and engineering ultrafast transport phenomena in functional NCs.
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Burst laser-induced pitting (BLIP): Transient defect-field interplay in ultrafast surface structuring
Abstract This study examines burst laser-induced pitting (BLIP), an understudied surface modification phenomenon driven by ultrafast laser bursts with sub-picosecond to picosecond inter-pulse delays. Through SEM and AFM analysis, we characterize BLIP as sub-micron pits with polarizationdependent oval shapes, alongside high-fluence melting zones and localized ripple-like structures. Unlike conventional LIPSS, BLIP demonstrates exceptional energy coupling efficiency, evidenced by 10× greater damage areas and a steeper fluence-scaling expansion rate than LIPSS, attributed to transient carrier-mediated processes. Pit density decays exponentially with delay (τ ≈ 6.6-8.9 ps), matching the timescale of self-trapped exciton (STE) relaxation, while spatial statistics reveal a delay-driven transition from field-guided ordering (1-5 ps) to randomized distributions (>10 ps). The resonant-like angular distributions and delay-dependent ellipticity reduction indicate competing mechanisms: optical field enhancement dominates at short delays, while energy dissipation and structure disordering prevail at longer delays. Simulation of nanoplasma excitation reveals near-field optical field enhancements responsible for the ellipticity and ripple-like structures. Beyond their fundamental significance, these BLIP nanostructures offer practical functionalities, including use as anti-reflection coatings and hydrophobic surfaces. These findings establish BLIP as a new paradigm in ultrafast laser-material interactions, where burst parameters selectively activate defect-mediated or field-driven modification pathways in dielectrics.
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- PAR ID:
- 10654335
- Publisher / Repository:
- IOP Publishing
- Date Published:
- Journal Name:
- Journal of Physics: Photonics
- ISSN:
- 2515-7647
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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