A linearly polarised 10 ps pulse laser at nm with a repetition rate of kHz Talisker Ultra, Coherent was used as an excitation source for the SHG measurements. The measurements were performed in transmission geometry with the nm fundamental beam focused at normal incidence on the MGN sample surfaces. The SH signal was collected with a 75 mm focal length lens L 4 and the fundamental beam was filtered out with a long-pass dichroic mirror M LP , nm cut-off wavelength.
The accumulated signal total four accumulations, each 1 s integration time was analysed. Figure 2. First, the dependence of SH intensity on the polarisation plane orientation of the laser operating at its fundamental harmonic of nm was investigated in the MGN-II sample containing mechanically reshaped Ag NPs. Since its SPR band position coincided well with the excitation wavelength, the highest incident field coupling and local field enhancement was expected.
The SH signal reached maximum for the fundamental harmonic polarised parallel to the long axis of the Ag NPs, i. The SH signal polarisation components, denoted as p-pol SH and s-pol SH in figure 3 b , were selected by placing a rotating polariser at the entrance slit of the spectrometer while keeping the polarisation plane of the fundamental beam parallel to the long axis of Ag NPs p-pol fundamental harmonic.
Figure 3. Corresponding schematics of the experimental conditions are also shown for clarity. The SH signal peaked at nm accompanied by strong photo-induced luminescence can be seen in the spectra. The observed photoluminescence is attributed to the excitation via multiphoton absorption. Indeed, MAIL has been observed in a number of noble metal-based structures upon irradiation with ultra-short pulsed lasers [ 23 — 28 ]. For bulk metals the light emission follows the excitation of electron transition from 5 d - to 6 ps -bands [ 29 ]. It is known that in low dimensional systems the light emission is considerably enhanced by the local fields associated with the surface plasmons.
Furthermore, the dielectric environment can play a significant role in the efficiency of MAIL, quenching or enhancing the signal due to different energy transfer processes. Figure 4. Note that this band is suppressed in FEM D sample. This band was also observed in the single-photon luminescence studies on laser-induced ionisation and photo-modification of Ag NPs in soda lime glass [ 30 ]. The laser-assisted reshaping, described in detail elsewhere [ 5 ], results in formation of the cationic shell in the vicinity of the Ag NPs.
The density of this cationic shell is higher around the Ag nano-ellipsoids with large aspect ratios. This explains the nm band intensity increase observed with increase in the aspect ratio of laser-reshaped MGNs and the fact that the band is not pronounced in the MAIL spectrum of the mechanically stretched MGN-II.
As shown in [ 24 ], the difference in observed nonlinear responses from Ag nano-ellipsoids with different aspect ratios can be associated with the relative strength of scattering and absorption in NPs. Since SHG and two-photon-induced luminescence scale quadratically with intensity of the incident light, observed slope deviations may suggest that three-photon-induced processes are also present in the MAIL signal around nm.
Figure 5. The Ag dielectric constant was adopted from [ 20 ]. The host medium refractive index of 1. The effective radius a eff used for the NPs in the simulations was taken to be 15 nm. The incident radiation in the model was assumed to be linearly polarised along the long axis of the target reflecting the experimental conditions used. The DDA simulation results confirm that the extinction for Ag NPs at , and nm is dominated by absorption for all aspect ratios under consideration.
The simulation results confirm that MAIL phenomenon is dominant in the Ag nano-ellipsoids with small aspect ratios i. It is worth noting that the spectrally resolved optical response in the laser-reshaped MGNs, registered in transmission geometry and shown in figure 4 , can be substantially modified due to the self-absorption in reshaped and unmodified spherical Ag NPs within the NPs containing layer, as simulation results suggest for the Ag NPs with aspect ratio of 1, in figure 5 c. SHG and MAIL spectra were explained for two different types of nanoparticle reshaping mechanisms: laser reshaped local modification and mechanically stretched global modification.
It was argued that ion species in the vicinity of the laser reshaped NPs and small Ag ions in the volume of the NP containing layer are responsible for the observed MAIL signal in the visible range. Both mechanical stretching and laser-assisted reshaping of the Ag NPs provide a simple and yet effective tool for spectral manipulation of the SPRs.
By subsequent irradiation of MGNs with precisely chosen wavelengths, elongation effects greater than the values presented here can be achieved, leading to higher scattering cross sections and effectively better frequency doubling abilities. Laser reshaping unlike mechanical stretching provides spectral selectivity, and more importantly the much needed spatial selectivity, for fast and local nanoprocessing of MGNs, paving the way for the fabrication of micro-patterned optical elements [ 35 ] in photonics, security and data storage [ 36 ].
All data created during this research are openly available from the University of Dundee Institutional Repository. Crossref Google Scholar.
Publications by PD Dr. Gerhard Seifert
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