B.3
Result and discussion
Here, we investigate the role of H implantation on the bonding environment and structural properties of embedded NPs. Figure B.2 shows the XANES spectra for
LPCVD layers of Ge and H+Ge implantation samples, annealed at 900 ◦C at the
Ge K-edge. The spectra of samples implanted with H is almost identical to sam-
1 1 0 8 0 1 1 1 0 0 1 1 1 2 0 1 1 1 4 0 1 1 1 6 0 1 1 1 8 0 1 1 2 0 0 0 . 0 0 . 2 0 . 4 0 . 6 0 . 8 1 . 0 1 . 2 1 . 4 H + G e G e A b so rp ti o n ( ar b . u n it s) E n e r g y ( e V ) A f t e r a n n e a l i n g a t 9 0 0 ° C
Figure B.2: XANES spectra at the Ge K-edge for Ge and H+Ge implanted LPCVD layers.
ples without H. For both cases the bonding environments are very similar to the
c-Si33Ge66 standard. No obvious correlation between H implantation and NP bond-
ing environment can be seen. Quantification of the H bonding from XANES analysis would necessitate an appropriate measurement of Si-H and Ge-H standards, lacking in our system. Hence, more investigation is needed for a better understanding of the system.
Figure B.3 (a) shows k3-weighted EXAFS spectra, and figure B.3 (b) correspond-
ing non-phase-corrected FTs for samples implanted with Ge and H+Ge annealed at
900 ◦C. Refined fitting parameters for the first NN shell are listed in Table B.2. A
Table B.2: Rifined EXAFS fitting parameters.
System CNGe RGe (Å) CNSi RSi(Å) σ2(Å2)
Ge+H 1.5±0.2 2.457±0.005 1.7±0.1 2.402±0.006 0.0033±0.0004
Ge 1.5±0.2 2.45±0.005 1.9±0.1 2.402±0.005 0.0036±0.0005
single scattering path for SiGe random structure was used similar to that for fitting the SiGe NP EXAFS data. The values of amplitude and energy shift were obtained for crystalline Ge standard and kept fixed for examined samples. Details of the fit- ting procedure can be found in Section 3.2. It can be seen that the two spectra are
112 H implantation effect 0 2 4 6 8 1 0 1 2 - 8 - 6 - 4 - 2 0 2 4 6 8 0 2 4 0 2 4 6 8 1 0 1 2 1 4 G e + H w i n d o w G e a ) 9 0 0 ° C k 3 * χ(k )( Å -3 ) W a v e n u m b e r K (Å - 1) F T [ k 3 * χ (k)( Å -3 ) ] b ) 9 0 0 ° C G e + H G e R a d i a l d i s t a n c e ( Å )
Figure B.3: (a) k3-weighted EXAFS spectra and (b) corresponding non-phase-corrected FT spectra of Ge and H+Ge samples.
identical. Also, it can be concluded H implantation did not affect the NP structural properties or bonding preference. In summary, no clear changes can be observed from the results.
Appendix C
XANES spectra of crystalline
standards
XANES spectra of NPs were compared to XANES spectra of different crystalline and amorphous standards. As mentioned in the text, no indication of Ge-O or Ge-N
was apparent. Figure C.1 shows XANES spectra of c-Ge, GeO2 and Ge66Si34 spectra.
The XANES spectra of Ge3N4is also presented for further comparison(adopted from
Ref.[[140]]).
Figure C.1:XANES spectra of crystalline Ge, GeO2and Ge66Si34standards. XANES spectra
of crystalline Ge3N4standard adopted from Ref.[[140].
For a quantitative analysis the bond lengths value of the first nearest neighbour of Ge with Si, O and N - achieved from the FT spectra of examined standards- are also summarized in Table C.1. For the presented study, no indication of Ge-O or Ge-N bonds was apparent for Ge implanted samples in PECVD nitride matrices.
However, Si-Ge bonds were analysed for LPCVD Si3N4 matrix. We expected forma-
tion of Ge NPs in LPCVD matrix due to its higher purity and less contamination and stoichiometric structure. Hence, in order to identify the cause of the formation of GeSi NP further systematic study is required. The Ge only composition of the NPs in PECVD nitride matrices is consistent with the bond energy values as given
114 XANES spectra of crystalline standards
Table C.1: Bond length of first nearest neighbour derived from EXAFS data for crys- talline standards. R(Å) Ref. Ge-O 1.73 [141] Ge-N 1.87 [140] Ge-Si 2.01 [99] Ge-Ge 2.44 [45]
in Table C.2. While Si and Ge are completely miscible and readily alloy, clearly Si preferentially bonds to O and/or N.
Table C.2: Bond energies for Si- and Ge- bonds[7]
System Si-Si Si-N Si-O Ge-N Ge-O Ge-Ge Ge-Si
Appendix D
Quantitative analyse of Raman
measurements
Peak position of Ge-Ge Raman-active mode for Ge NPs in PECVD Si3N4and SiO1.67N0.14
matrices were analysed quantitatively and the results are summarized in Table D.1. The Ge-Ge peak position was fitted using the Voigt profile in Multipeak Fit package1. The Ge-Ge signal from amorphous and crystalline Ge standards are associated at 297
and 300 cm−1, respectively[143]. Raman measurements in addition to XANES data
were used to predict the dominant phase of Ge NPs. Noticeably, as the concentration and annealing temperature increases the measured values of peak position for NPs become closer to crystalline component.
Table D.1: Peak frequency for the main Raman-active mode (Ge-Ge) for Ge embed-
ded NPs in PECVD Si3N4 and SiO1.67N0.14 matrices. The frequencies are in units
of cm−1. Samples are referred first by their atomic concentration (at.%) followed by their annealing temperature (◦C)
Matrix Sample Ge-Ge
Si3N4 6-700 6-900 9-700 9-900 12-700 12-900 266.5±1.2 277.8±0.3 285.3±0.1 285.7±0.4 290.8±0.4 292±0.1 SiO1.67N0.14 9-700 9-900 9-1100 12-700 12-900 12-1100 280.2±0.4 285.6±0.8 286.7±0.5 287.3±0.7 294±0.5 295±0.5
1More details can be found in Ref.[[142]]
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