An ultrafast thermal spike within a time interval of a few pico-seconds generated by intense ionizing energy deposited using 100 MeV Ag ions is utilized to study the atomistic details of damage recovery in 4H-SiC. Sequential single ion irradiations were performed using 300 keV Ar and 100 MeV Ag in ⟨0001⟩ 4H-SiC to invoke swift heavy ion (SHI) beam induced epitaxial recrystallization in samples with different degrees of pre-damaged conditions. SHI irradiation was carried out at both room temperature and a low temperature of ∼80K. Low-temperature irradiation was carried out to arrest thermal diffusion of defects and to isolate ionization-induced defect migration in 4H-SiC. Insights into the thermal spike generated by ionizing events in crystalline and amorphous regions at both the temperatures predict a SiC response to SHI. The results emphasize the role of different degrees of pre-damage induced physico-chemical conditions and irradiation temperatures against SHI-induced recrystallization as evaluated by Rutherford backscattering/channeling, Raman spectroscopy, and hard x-ray photoelectron spectroscopy. Understanding the dependence of ion-beam damage accumulation and their recovery on the inelastic to elastic energy loss ratio is important for the performance prediction of SiC intended for extreme environments such as space, defense, and nuclear radiation. We report substantial damage recovery even at a near liquid nitrogen temperature of ∼80K. The recovery gets impeded mainly by the formation of complex defects having homonuclear bonds. The results are explained in the framework of the inelastic thermal spike model, and the role of phonon in the damage recovery process is emphasized.
The recovery effect of isochronal thermal annealing and inelastic energy deposited during 100 MeV Ag swift heavy ion (SHI) irradiation is demonstrated in the case of 4H-SiC pre-damaged by elastic energy deposition of 300 keV Ar ion. The Ar-induced fractional disorder follows a nonlinear two-step damage build-up. The fractional disorder level of 0.3 displacements per atom (dpa) is established as the threshold above which the lattice rapidly enters the amorphous phase, characterized by the presence of highly photo-absorbing defects. The SHI-induced recovery suggests that the damage annealing, in the pre-damaged region (∼350 nm) where the Se for 100 MeV Ag is almost constant (∼16.21 keV/nm), is more pronounced than the damage creation by SHI. This allows the disorder values to saturate at a lower value than the present initial disorder. Furthermore, the thermal effect due to SHI irradiation of an amorphous nano-zone embedded in a crystalline host matrix has been evaluated using the 3D implementation of the thermal spike. The recovery process by SHI is ascribed to the thermal spike-induced atomic movements resulting from the melting and the resolidification of the crystalline–amorphous interface.
Defects in SiC have shown tremendous capabilities for quantum technology-based applications, making it necessary to achieve on-demand, high-concentration, and uniform-density defect ensembles. Here, we utilize 100 MeV Ag swift heavy ion irradiation on n-type and semi-insulating 4H-SiC for the controlled generation of the defects that have attracted a lot of attention. Photoluminescence spectroscopy shows strong evidence of VSi emitters in semi-insulating 4H-SiC. Additionally, irradiation generates photo-absorbing centers that enhance the optical absorption, suppressing the luminescence intensity at higher fluences (ions/cm2). In n-type 4H-SiC, irradiation drastically increases the inter-conduction band transitions, attributed to absorption from trap centers. A clear correlation is found between (i) loss in the intensity of E2 (TO) Raman signal and the enhancement in absorbance at 532 nm and (ii) decoupling of the longitudinal optical phonon–plasmon coupled Raman mode and the reduction in carrier concentration. The optical bandgap decreases with irradiation fluence for semi-insulating 4H-SiC. This is attributed to the formation of disorder and strain-induced localized electronic states near the band edges.
Ultrasmall nanoparticles (NPs) with a high active surface area are essential for optoelectronic and photovoltaic applications. However, the structural stability and sustainability of these ultrasmall NPs at higher temperatures remain a critical problem. Here, we have synthesized the nanocomposites (NCs) of Ag NPs inside the silica matrix using the atom beam co-sputtering technique. The post-deposition growth of the embedded Ag NPs is systematically investigated at a wide range of annealing temperatures (ATs). A novel, fast, and effective procedure, correlating the experimental (UV−vis absorption results) and theoretical (quantum mechanical modeling, QMM) results, is used to estimate the size of NPs. The QMM-based simulation, employed for this work, is found to be more accurate in reproducing the absorption spectra over the classical/modified Drude model, which fails to predict the expected shift in the LSPR for ultrasmall NPs. Unlike the classical Drude model, the QMM incorporates the intraband transition of the conduction band electrons to calculate the effective dielectric function of metallic NCs, which is the major contribution of LSPR shifts for ultrasmall NPs. In this framework, a direct comparison is made between experimentally and theoretically observed LSPR peak positions, and it is observed that the size of NPs grows from 3 to 18 nm as AT increases from room temperature to 900 °C. Further, in situ grazing-incidence small-& wide-angle X-ray scattering and transmission electron microscopy measurements are employed to comprehend the growth of Ag NPs and validate the UV + QMM results. We demonstrate that, unlike chemically grown NPs, the embedded Ag NPs ensure greater stability in size and remain in an ultrasmall regime up to 800 °C, and beyond this temperature, the size of NPs increases exponentially due to dominant Ostwald ripening. Finally, a three-stage mechanism is discussed to understand the process of nucleation and growth of the silica-embedded Ag NPs.
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