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Substrate-step-induced effects on the growth of CaF2 on Si (111)

Substrate-step-induced effects on the growth of CaF2 on Si (111)

Substrate-step-induced effects on the growth of CaF2 on Si (111)

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163<strong>the</strong> protrusi<strong>on</strong>s are not distributed homogeneously. Figure 9band c dem<strong>on</strong>strate clearly that some <str<strong>on</strong>g>step</str<strong>on</strong>g>s are decorated by series<strong>of</strong> triangular protrusi<strong>on</strong>s, while o<strong>the</strong>r <str<strong>on</strong>g>step</str<strong>on</strong>g>s are completelyprotrusi<strong>on</strong>-free. In all cases, however, <strong>the</strong>se protrusi<strong>on</strong>s arein fr<strong>on</strong>t <strong>of</strong> CaF 2 -covered terraces, which has been proved byFFM. Therefore, <strong>the</strong> lateral <strong>growth</strong> <strong>of</strong> CaF 2 <strong>on</strong> <strong>the</strong> terrace hasto be previous to <strong>the</strong> formati<strong>on</strong> <strong>of</strong> <strong>the</strong> triangular protrusi<strong>on</strong>sin fr<strong>on</strong>t <strong>of</strong> it. This may be explained by <strong>the</strong> necessity <strong>of</strong> triplesubstrate <str<strong>on</strong>g>step</str<strong>on</strong>g>s which can be overgrown by protrusi<strong>on</strong>s. Thisassumpti<strong>on</strong>, however, cannot be proved strictly because <strong>on</strong>ecan investigate <strong>on</strong>ly <strong>the</strong> <str<strong>on</strong>g>step</str<strong>on</strong>g> heights <strong>of</strong> <strong>the</strong> film, which maydiffer from <strong>the</strong> height <strong>of</strong> <strong>the</strong> underlying substrate <str<strong>on</strong>g>step</str<strong>on</strong>g>.The analysis <strong>of</strong> <strong>the</strong> protrusi<strong>on</strong> densities is presented inFig. 13. First, <strong>the</strong> density and coverage <strong>of</strong> <strong>the</strong>se protrusi<strong>on</strong>sincrease with increasing coverage. In later <strong>growth</strong> stages <strong>the</strong>density <strong>of</strong> protrusi<strong>on</strong>s is almost c<strong>on</strong>stant, while <strong>the</strong> surfacefracti<strong>on</strong> covered with protrusi<strong>on</strong>s increases fur<strong>the</strong>r. This effectis due to <strong>the</strong> over<strong>growth</strong> <strong>of</strong> substrate <str<strong>on</strong>g>step</str<strong>on</strong>g>s.5 Relaxati<strong>on</strong> at <str<strong>on</strong>g>step</str<strong>on</strong>g>sSome <strong>of</strong> <strong>the</strong> largest triangular protrusi<strong>on</strong>s show hole-likestructures. Figure 14 shows a typical example for a film depositedat 630 ◦ C. The large twin protrusi<strong>on</strong> has rims at <strong>the</strong>free-standing edges which do not point to <strong>the</strong> upper terrace<strong>of</strong> <strong>the</strong> vicinal substrate. The small triangular protrusi<strong>on</strong> <strong>on</strong> <strong>the</strong>back side <strong>of</strong> <strong>the</strong> twin protrusi<strong>on</strong>, however, does not show thiseffect. In additi<strong>on</strong>, <strong>the</strong>re are small gaps (arrows in Fig. 14)running preferentially parallel to substrate <str<strong>on</strong>g>step</str<strong>on</strong>g>s. Unfortunately,<strong>the</strong> sample must be at room temperature for <strong>the</strong> AFMmeasurement. Therefore, <strong>on</strong>e has no informati<strong>on</strong> <strong>on</strong> whe<strong>the</strong>r<strong>the</strong>se cracks are formed during <strong>growth</strong> or during <strong>the</strong> coolingfrom <strong>growth</strong> to room temperature.The AFM micrograph shown in Fig. 14 is recorded underambient c<strong>on</strong>diti<strong>on</strong>s. One can distinguish smooth CaF 2 layersand areas covered by small clusters. In a previous report, wehave shown that <strong>the</strong> clusters are formed due to <strong>the</strong> transfer <strong>of</strong><strong>the</strong> sample from UHV c<strong>on</strong>diti<strong>on</strong>s to ambient c<strong>on</strong>diti<strong>on</strong>s [54].The clusters are formed by transformati<strong>on</strong> <strong>of</strong> <strong>the</strong> unstable CaFinterface layer under <strong>the</strong> influence <strong>of</strong> air.Rim-like structures <strong>of</strong> l<strong>on</strong>g CaF 2 stripes are also formedclose to some <strong>of</strong> <strong>the</strong> CaF 2 film <str<strong>on</strong>g>step</str<strong>on</strong>g>s. Figure 15a shows thiseffect for an 8-TL film grown at 630 ◦ C. CaF 2 stripes cover<strong>the</strong> entire <str<strong>on</strong>g>step</str<strong>on</strong>g>s (arrows). The edge <strong>of</strong> <strong>the</strong> stripes pointing to<strong>the</strong> upper terrace is smooth while <strong>the</strong> o<strong>the</strong>r edge pointing to<strong>the</strong> lower terrace is rough. In additi<strong>on</strong>, some small protrusi<strong>on</strong>sare formed at <strong>the</strong> rough edge. Unfortunately, it cannot be determinedusing AFM whe<strong>the</strong>r <strong>the</strong> CaF 2 stripe is formed <strong>on</strong><strong>the</strong> lower or <strong>on</strong> <strong>the</strong> upper terrace. The shape <strong>of</strong> <strong>the</strong> stripe,however, suggests that it is more likely that <strong>the</strong> CaF 2 stripeis formed <strong>on</strong> <strong>the</strong> lower terrace since <strong>the</strong> edge pointing in thisdirecti<strong>on</strong> is rough.A line scan (Fig. 15b taken from <strong>the</strong> white line in Fig. 15a)shows <strong>the</strong> typical height a and width b <strong>of</strong> <strong>the</strong> CaF 2 stripe. Thegeometric dimensi<strong>on</strong>s <strong>of</strong> <strong>the</strong> CaF 2 stripes have been analysedfrom various micrographs. The result <strong>of</strong> <strong>the</strong> analysis is shownby Fig. 16. Although <strong>the</strong> scattering <strong>of</strong> <strong>the</strong> data is not negligible,<strong>the</strong>re is a tendency that <strong>the</strong> stripe height a seems to beindependent from <strong>the</strong> <str<strong>on</strong>g>step</str<strong>on</strong>g> height h while <strong>the</strong> stripe width bincreases with increasing height <strong>of</strong> <strong>the</strong> <str<strong>on</strong>g>step</str<strong>on</strong>g>. CaF 2 stripes areobtained exclusively if <strong>the</strong> <str<strong>on</strong>g>step</str<strong>on</strong>g> height h is larger than 1 nm(equivalent to <str<strong>on</strong>g>step</str<strong>on</strong>g>s <strong>of</strong> triple-layer height). Thus triple-layerhigh<str<strong>on</strong>g>step</str<strong>on</strong>g>s seem to be critical <str<strong>on</strong>g>step</str<strong>on</strong>g> heights for <strong>the</strong> <strong>on</strong>set <strong>of</strong> thisphenomen<strong>on</strong>.One has to c<strong>on</strong>sider <strong>the</strong> small (but not negligible) latticemismatch between CaF 2 and <strong>Si</strong> at <strong>the</strong>se <strong>growth</strong> temperaturesto explain <strong>the</strong> <strong>growth</strong> <strong>of</strong> <strong>the</strong> CaF 2 stripes. <strong>Si</strong>nce CaF 2 hasa larger lattice c<strong>on</strong>stant than <strong>Si</strong> <strong>the</strong> pseudomorphic CaF 2 filmis compressed laterally. At <str<strong>on</strong>g>step</str<strong>on</strong>g>s, however, <strong>the</strong> film <strong>on</strong> <strong>the</strong>upper terrace can relax easily since neighbour molecules are(a)250nmbah(b)Fig. 14. Rim formati<strong>on</strong> at <strong>the</strong> edges <strong>of</strong> a big triangular twin protrusi<strong>on</strong>grownbyCaF 2 depositi<strong>on</strong> at 630 ◦ C (AFM micrograph). The clusters observed<strong>on</strong> <strong>the</strong> terraces close to <strong>the</strong> triangular protrusi<strong>on</strong> are formed after <strong>the</strong>transfer <strong>of</strong> <strong>the</strong> sample from UHV to ambient c<strong>on</strong>diti<strong>on</strong>s due to <strong>the</strong> instability<strong>of</strong> <strong>the</strong> CaF interface layer. Partially, <strong>the</strong>re are cracks in <strong>the</strong> CaF 2 film(see arrows)Fig. 15. a AFM micrograph obtained after depositi<strong>on</strong> <strong>of</strong> 8-TL CaF 2 at630 ◦ C and transfer to ambient c<strong>on</strong>diti<strong>on</strong>s. The arrows mark CaF 2 stripes.b Height pr<strong>of</strong>ile <strong>of</strong> <strong>the</strong> line scan marked in a showing <strong>the</strong> typical geometriclengths to characterize <strong>the</strong> stripes: <str<strong>on</strong>g>step</str<strong>on</strong>g> height, h, stripe height, a, and stripewidth, b

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