Wavelength and decay time tuning of intraband transitions in low spatial frequency laser-induced periodic surface structures

Abstract

We present the study of the alteration of wavelength and decay time of intraband transitions in the laser-induced periodic surface structures (LIPSS) of silver formed by varying the incident laser peak fluence. The studies are performed using a femtosecond laser (λ0 = 800 nm) based ultrafast transient absorption spectroscopy (UFTS)setup. Using the same laser, an array (~2 mm size) of laser-induced periodic surface structures were obtained in a single-step fabrication process in the open air without translating the sample. Each unit cell of the array comprises low spatial frequency LIPSS (LSFL) near the center with nanoparticles/clusters around the edges. As obtained from 2D Fast Fourier Transform, the overall periodicity(Λ) of LSFL is within 0.714λ0–0.723λ0 range. The nanoparticles/clusters show a random size distribution that varies from 50 nm to 300 nm. In UFTS measurement, the LIPSS was excited by a 3.3 eV laser. The SPP/SPR dip in the data is an indication of intraband transition or hot electron generation. The effect of change in structuring due to varying laser fluence on these intraband transitions is also analyzed. It is observed that there is a non-linear redshift (~16 nm) in the SPR peak wavelength with a significant enhancement in the relaxation times of the hot electrons due to localized annealing of shallow defects. Therefore, a large tunability in wavelength of SPP/SPR and lifetime of hot electrons was achieved by varying the laser fluence. The study highlights the suitability of LIPSS in applications requiring efficient energy transfer, enhanced photocatalytic action, and tunable sensors.