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Studies on linear and non linear optical properties of pulsed laser deposited Si, SiOx and SiC nanostructured thin films

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Inset shows static refractive indices (n0) for nc-Si thin films deposited as a function of Ts………. 5.16 (a) Tauc plots for determining the optical band gap (Eg) of a-SiC films deposited at different Ts and (b) variation of, for example, PLD a-SiC thin films with.

Silicon nanostructures and thin films

Si-based materials have also been reported to exhibit nonlinear optical (NLO) properties in both bulk and nanostructured forms. Si-based films have been produced by thermal evaporation [32], RF sputtering [33], variety of chemical vapor deposition (CVD) [34, 35] and pulsed laser deposition (PLD) [36] techniques, etc.

Silicon carbide thin films

Luminescent SiC films can be fabricated by incorporating various defects (dislocations, defects, and surface states related to oxygen and hydrogen) during the growth process [49]. Since then, amorphous SiC (a-SiC) films have continued to be of great interest both for fundamental understanding and technologically in electronic and optoelectronic devices.

Pulsed laser deposition technique

The nucleation and growth of films that are crystalline, amorphous, or both depend on the density, kinetic energy, degree of ionization, and the type of deposition material, as well as on the substrate temperature and its physicochemical properties. Therefore, the substrate temperature and the kinetic energy of the arriving species to the substrate are key factors that determine the degree of crystallinity of the films in PLD.

Characterization of Si-based Thin Films

In a Z-scan experiment, consistent with the Sheik-Bahae formalism (SBF), under the approximation that the sample thickness is less than the Rayleigh length, z0, the measured far-field transmission intensity as a function of sample position (z) w.r.t the focal plane of the lens, simply accounting for nonlinear and nonlinear intensity-dependent absorption. On the other hand, if the peak appears before the valley, then it shows the self-defocusing property corresponding to the negative nonlinear refractive index. n2 can be calculated by fitting the CA Z-scan measurement data to equation (2.18). The inset of Figure 4.8 (b) shows the Tauc plot for α (hν), estimated from the values ​​of k (hν) calculated from ε1 and the best fit.

Open circle and solid lines represent experimental data and fitted data, respectively. f) the variation of ITA/ITO and FWHM of TO Raman peak of SiOx film as a. Both the n(λ) and k(λ) spectra of the Si films showed that their optical properties changed from a-Si-like to poly-Si-like with increasing Ts. The optical band gap, refractive index and film thickness estimated from SE were found to be in good agreement with UV-Vis-NIR results. The third-order NLO properties of Si, SiOx and a-SiC thin films deposited via PLD were investigated using modified Z-scan technique under cw He-Ne laser irradiation. The origin of optical nonlinearity in all these PLD Si-based thin films; Si, SiOx and a-SiC, is due to the thermal effect induced by cw laser illumination.

The TEM images showed an increase in particle size, while the SAED pattern confirmed the improvement in crystallinity of the films with increasing Ts. FESEM images showed uniform nanostructure growth with particle size increasing with increasing Ts.

Third order Nonlinear optical properties of nc-Si, SiOx and a-SiC PLD

Organization of the Present Thesis

Experimental Details

Experimental setup for fabrication of a-Si:SiO 2 via direct laser irradiation of

The laser beam was guided by a 90° prism focused by a convex lens with a focal length of 25 cm and irradiated onto the c-Si wafer at an incidence angle of ~30˚. to avoid back reflection on the laser). Laser ablation was performed for 10 min at all laser fluxes except that at 2.67 Jcm-2 where the ablation time was reduced to 5 min to avoid drilling the Si wafer.

Pulsed laser deposition (PLD) setup for fabrication of Si, SiO x and SiC thin

10-6 mbar before deposition, using a turbomolecular pump (Pfeiffer, Hi Pace 300 C) connected to the bottom 100 CF port of the ablation chamber, as shown in Figure 2.1. For this, the ablation chamber was pressurized with the desired pressure through a separate port via gas flow regulator as shown in Figure 2.2 and also marked in Figure 2.3.

Characterization of thin films

33 | Page where B is the Tauc slope (or B parameter), e.g. is the energy of the optical band gap and m is the power factor that depends on the type of electronic transition (m=1/2, 3/2 and 2 for direct, forbidden and indirect transitions respectively) determined by the nature of the material. Thus, the imaginary part of the dielectric function ε2 ​​in Tauc Lorentz-Lorentz (TLL) model is defined as,.

Modified Z-Scan set-up for measurement of the third order NLO coefficients

But the intensity entering the thin film sample is estimated as R) W/cm2, where R is the reflection coefficient of the sample. The thickness of the films in the present work is less than 600 nm and therefore satisfies the thin film approach. The linear and nonlinear refractive indices (n and n2 respectively) can be expressed as, , where, n and k (extinction coefficient) represent the real and imaginary parts of the complex linear refractive index, while n2 and k2 are those of the real and imaginary part of the complex nonlinear refractive index, respectively.

Optical limiting set-up

The PL spectra of the whitish region of all the samples prepared at different laser fluence are shown in Figure 3.10. The inset shows the variation of (. ) and n0 of the SiOx films (estimated using the envelope method), as a function of O2 pressure. The SAED pattern of the dark region (marked with a rectangular box) is shown in the inset of Figure 4.27(a).

Fabrication of lumunescent Si:SiO 2 nanostructures by direct laser irradiation of Si

Experimental Details

The effect of laser fluence on the production of a-Si:SiO2 was studied by varying the fluence in the range of Jcm-2. The Raman spectra of a-Si:SiO2 were recorded at room temperature (RT) by micro-Raman spectrometer in backscattering geometry. Fourier Transform Infrared (FTIR) transmission spectra of all the samples were recorded to get the confirmation of the presence of SiO2 in the vicinity of the focus area.

Results and discussions

  • Study of morphological, structural and photoluminescence property of
  • Structural characterization of a-Si:SiO 2 nanostructures as a function of laser
  • Surface morphology characterization of a-Si:SiO 2 nanostructures as a
  • TEM analysis of a-Si:SiO 2 nanostructures as a function of laser fluence.58

To study the effect of laser fluence on the formation of a-Si embedded in SiO2. This decrease in particle size with increasing laser fluence can be explained as follows. Figure 3.13(a) shows the variation of the ratio of atomic percentages of oxygen to silicon (O/Si) from the intensity of EDX and PL peak 2 of white micro clusters with increasing laser fluence.

Conclusion

In general, it was observed that the transmittance of the SiOx films increases with increasing O2 pressure. The values ​​of β for the nc-Si films were observed to be of the order of 10 cm/W. The value of β of nc-Si films was observed to be of the order of 10 cm/W.

Fabrication and characterization of PLD Si and SiO x thin films

Experimental Details

Raman spectra of Si and SiOx thin films were recorded using a micro-Raman setup in a backscattering geometry. SEM and EDX of the SiOx films were performed for surface morphology and compositional analysis. In addition, steady-state PL spectra of SiOx films were recorded at RT using a commercial fluorimeter (Thermo Spectronic, FA-357) equipped with a charge-coupled detector.

Effect of substrate temperature and O 2 pressure on Si-based thin films via

  • Effect of substrate temperature on the properties of Si films
    • Structural properties of nc-Si thin films
    • Linear optical properties of Si thin films
  • Effect of background oxygen pressure during deposition on the properties
    • Structural and Compositional properties of SiO x thin films
    • Linear optical properties of SiOx thin films
    • Photoluminescence studies of SiO x films

Refractive index and (b) extinction coefficient as a function of wavelength of Si films deposited at room temperature, 400 and 700 ºC. Raman spectra of the background matrix of all other films, Fig. 4.15 (b-e), also showed similar features. 97 | Page Figure 4.19 (a) Tauc plots for determining optical gaps of SiOx films and (b) variation of optical gaps (Eg) of SiOx films as a function of varying O2 pressure.

Conclusion

The deconvoluted Raman spectra of all a-SiC thin films are shown in Figure 5.5 (a-d). 124 | Page Figure 5.7 FTIR absorption spectra of a-SiC PLD thin films fabricated at Ts from RT to. 144 | Page Figure 6.4 Variation of the nonlinear absorption coefficient (ß) and nonlinear refractive index (n2) of nc-Si thin films as a function of Ts.

Fabrication and characterization of PLD amorphous SiC thin films

Experimental Details

A schematic of PLD system used for the deposition of SiC thin films is shown in Figure 2.1 (Chapter 2). 118 | P a g e Figure 5.3 XRD spectra of PLD SiC thin films produced at different substrate temperatures (Ts) from RT to 750 °C. Effect of substrate temperature on structural and linear and nonlinear optical properties of nanostructured PLD a-SiC thin films', Partha P.

Effect of substrate temperature in properties of SiC films

  • Surface morphology of PLD a-SiC thin films by FESEM images…
  • TEM images and SAED patterns of PLD a-SiC thin films
  • Structural and compositional studies of PLD a-SiC thin films
  • Linear optical properties of PLD a-SiC thin films

Conclusion

Significant third-order optical nonlinear susceptibility was observed in nc-Si thin films in the present case compared to that of bulk Si. But the observed values ​​of these NLO coefficients of SiOx thin films deposited at the lowest O2 pressure of 10-4 mbar, in the present case, were an order of magnitude higher. In this thesis, the third order optical nonlinearity of nc-Si, SiOx and SiC thin films using cw laser is presented.

Third order Non-linear optical properties of PLD Si, SiO x and SiC thin films

Experimental Details

  • Third order NLA and NLR coefficients of PLD nc-Si films
  • Optical limiting in PLD nc-Si thin films

This change in the values ​​of ß and n2 of Si film as a function of Ts can be correlated with the linear absorption coefficient, α (at λ = 632.8 nm), which changes in a similar way with increasing Ts as shown in the inset of Fig. 6.4. This decrease in phonon density reduces the probability of optical absorption in these indirect bandgap Si thin films, resulting in the decrease in the RSA coefficient, ß, with decreasing α and vice versa. In this work, the values ​​of α in these thin films were found to change with the Ts, which explains the similar trend of n2 as a function of Ts.

Effect of oxygen pressure on the third order NLO response and OL property

  • Third order NLA and NLR coefficients by modified Z-scan
  • Optical limiting in PLD SiO x thin films

This decrease in linear absorption with increase in O2 pressure is solely due to the stoichiometric changes of the SiOx films from Si-rich to oxygen-rich. This decrease in phonon density reduces the probability of optical absorption in the indirect band gap of SiOx thin films leading to the decrease in RSA coefficient, ß. The Z-scan for these thin films was performed under cw laser illumination which can cause significant heating in the samples producing thermally induced optical nonlinearities in SiOx thin films as discussed in section 6.4 and equation (6.1).

Effect of substrate temperature on the third order NLO properties of a-SiC

The values ​​of α of these thin films were found to decrease with increasing Ts, Figure 5.15, Chapter 5, due to the transition of the film from Si-rich to nearly stoichiometric a-SiC, and thus resulting in the decrease of the n2 (equation 6.1) of the a-SiC films with increasing Ts. These values ​​of χ(3) depended solely on the linear absorption coefficient controlled by. 156 | Page stoichiometry and crystallinity of the films, two of which later depended on the deposition parameters of the PLD technique.

Conclusion

A large third-order NLO sensitivity of the order of 10-1 esu was observed in these PLD nc-Si films, which is 109 times higher compared to that of a bulk Si. The significantly large NLO sensitivity of the order of 10-1-10-3 esu was observed in these films. The amorphous nature of the clusters, which were composed of a-Si as well as amorphous SiO2, was confirmed by Raman spectra, FTIR spectra, and SAED patterns.

Conclusions

Effect of He pressure on structural, optical and photoluminescence properties of nanostructured PLD a-SiC thin films. 169 | P a g e National Symposium on Pulsed Laser Deposition of Thin Films and Nanostructured Materials (PLD 2013), organized by Dept. Dey and Alika Khare, conference presentation from International Conference on Nanotechnology (ICNT 2013), organized by Dept.

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Alika Khare Thesis Submitted to the Department/ Center : Physics Date of completion of Thesis Viva-Voce Exam : 27/05/2022 Key words for description of Thesis Work : Fabrication of

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