Filigree with a Sledge Hammer
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1 Filigree with a Sledge Hammer Self-organized Nanostructures from Ion-Beam Irradiation R. Kree Institut f. Theoretische Physik Georg-August University Göttingen Oldenburg, July 9th 2012
2 Today s menu 1 A failure to begin with 2 A deceptively general explanation 3 Wishful thinking: experiment and theory on the wrong track 4 Unexpected triumph, wrong interpretation 5 Complete failure, the doom of the old is the advent of the new 6 The power of dirt and other surprises 7 Anchors aweigh! New shores ahead! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
3 A holy grail of solid surfaces Before the advent of nanoscience: A perfectly smooth surface after the advent: A surface with perfect nanostructures R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
4 How one fails to polish glass surfaces with an ion beam M.Navez, et.al. (1962) C. R. Acad. Sci Paris 254, p 240 Ion sandblasting effect. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
5 The basics σ Statistics µ Energy of ion kev sledge hammer is distributed in cascades. (Feix, Hartmann, RK, Muñoz-Garcia, Cuerno, PRB, 2005) Average over deposited energy R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
6 The deceptively general explanation Generic curvature instability: Energy of ion kev sledge hammer is distributed in cascades. Valleys (B) get more energy/time than hilltops (A) and are thus eroded faster.. M. Bradley, J. Harper (1988) J. Vac. Sci. Technol. A6, 2390 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
7 The deceptively general explanation, contd. Continuum description Mass conservation h ~ t = Y (θ; h) - divj change in surface height = Sputter yield + surface current Y roughening thermal surface current div ~j = K 4 h smoothing result: universal ripples R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
8 The cornerstone of Bradley-Harper Theory Input Erosion velocity v(x, y) deposited cascade energy/time P(x, y). P available from kinetic theory P. Sigmund (1969) PR 84, 383. Then linearize in height profile. Prediction: Ripple crests to ion beam direction close to normal incidence, and close to grazing incidence. Angle of 90 rotation can be calculated for different materials and ion beam parameters! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
9 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
10 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
11 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
12 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass the ion-beam people s nanostructures in 1990s H.Hofsäß, K. Zhang, 1997 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
13 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass the ion-beam people s nanostructures in 1990s H.Hofsäß, K. Zhang, and some from the shop next door (MBE) from Anupam Madhukar s homepage R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
14 How to get on the wrong track Is the method a player in bottom-up production processes of nanostructures? NO! Mainly because 1 patterns are too blurred 2 nothing but ripples 3 on semiconductors (Si), ripple quality appears worse than on glass the ion-beam people s nanostructures in 1990s H.Hofsäß, K. Zhang, and some from the shop next door (MBE) from Anupam Madhukar s homepage But at least, we have a theory. Let s put it to work and try to improve. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
15 Plenty of room for improvement 1 Non-linear effects? 2 Ion beam parameters? 3 Other materials? 4 Several beam directions, rotated samples? Theorist s point of view Do we understand what s going on? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
16 Plenty of room for improvement 1 Non-linear effects? 2 Ion beam parameters? 3 Other materials? 4 Several beam directions, rotated samples? Theorist s point of view Do we understand what s going on? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
17 Plenty of room for improvement 1 Non-linear effects? 2 Ion beam parameters? 3 Other materials? 4 Several beam directions, rotated samples? Theorist s point of view Do we understand what s going on? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
18 Plenty of room for improvement 1 Non-linear effects? 2 Ion beam parameters? 3 Other materials? 4 Several beam directions, rotated samples? Theorist s point of view Do we understand what s going on? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
19 Plenty of room for improvement 1 Non-linear effects? 2 Ion beam parameters? 3 Other materials? 4 Several beam directions, rotated samples? Theorist s point of view Do we understand what s going on? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
20 Monte Carlo Model Model the current wisdom, see what it gives us. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
21 The Algorithm N e erosion steps + N d Surface diffusion steps Adjust N e /N d to physical time scales. Hartmann, Geyer, Kölbel, R.K.,PR B, 2002 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
22 What can be studied 1 non-linear effects Hartmann, Geyer, Kölbel, R.K.,PR B, ion-beam parameters Yewande, R.K., Hartmann, PR B noise in ion beam, penetration depths, deposited energy R.K. Yasseri, Hartmann NIMB (2009), R.K. T. Yasseri, different single element materials R. K., T. Yasseri geometries like dual beams and rotated samples Yewande, Hartmann, R.K PRB 2006; Yasseri, R.K., NIMB 2010 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
23 BH works Figure: Typical morphologies of ripples obtained from the basic MC model. (a) For smaller θ (50 0 ) ripple wave vectors are parallel (b) for larger θ (80 0 ) they are perpendicular R. K. T. Yasseri, 2012 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
24 First Lessons 1 Yes, we get ripples in accordance with BH-rotation 2 No, they are not nice 3 and they are surprisingly hard to find in parameter space 4 for Si parameters we (and others) didn t find any!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
25 First Lessons 1 Yes, we get ripples in accordance with BH-rotation 2 No, they are not nice 3 and they are surprisingly hard to find in parameter space 4 for Si parameters we (and others) didn t find any!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
26 First Lessons 1 Yes, we get ripples in accordance with BH-rotation 2 No, they are not nice 3 and they are surprisingly hard to find in parameter space 4 for Si parameters we (and others) didn t find any!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
27 First Lessons 1 Yes, we get ripples in accordance with BH-rotation 2 No, they are not nice 3 and they are surprisingly hard to find in parameter space 4 for Si parameters we (and others) didn t find any!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
28 First Lessons 1 Yes, we get ripples in accordance with BH-rotation 2 No, they are not nice 3 and they are surprisingly hard to find in parameter space 4 for Si parameters we (and others) didn t find any!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
29 Dependence on average cascade shape µ 4 2 VI II V IV III 0 0 I 2 4 σ σ µ R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
30 Dependence on average cascade shape µ 4 2 VI II V IV III 0 0 I 2 4 σ σ µ Lots of different pattern types (ripples, dots, holes,...), but none of them nice. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
31 Non-linear effects depend on surface diffusion Three long-time snapshots. Only difference is surface diffusion mechanism Left: based on height differences, Middle: based on path dependent barriers, Right: Wolff-Villain irreversible downhill relaxation. Continuum theory predicts spatio-temporal chaos (Kuramoto-Sivashinski type) as asymptotic behaviour. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
32 General failure None of the trials lead to substantially improved quality of patterns (both in Theory and Experiment) R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
33 The Si ripple desaster R. K., T. Yasseri 2012 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
34 So, we ve come to the end of this pretty lousy show. I must say, I m glad it s over. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
35 But then! SURPRISE!!! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
36 Unexpected triumphs (a) Ripples on Si B. Ziberi et al (b) An array of nanodots on GaSb S. Facsko et al (c) Cones on copper Reiche and W. Hauffe (d) Hexagonal array of nanoholes on Ge Q. Wei et al (e) Square array of nanodots on Si B. Ziberi et al (f) Ripples of two different wave vectors on Si at a 25 degree angle of incidence B. Ziberi et al R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
37 But Why??? 1 because we do it so well controlled 2 because we have special beam parameters 3 because we use special materials (GeSb, GaSb, InP) 4 why did other labs fail to reproduce the results? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
38 But Why??? 1 because we do it so well controlled 2 because we have special beam parameters 3 because we use special materials (GeSb, GaSb, InP) 4 why did other labs fail to reproduce the results? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
39 But Why??? 1 because we do it so well controlled 2 because we have special beam parameters 3 because we use special materials (GeSb, GaSb, InP) 4 why did other labs fail to reproduce the results? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
40 But Why??? 1 because we do it so well controlled 2 because we have special beam parameters 3 because we use special materials (GeSb, GaSb, InP) 4 why did other labs fail to reproduce the results? R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
41 A really clean experiment on Si Köln/Leipzig/Dresden-Rossendorf/: Macko et al (2010), Nanotechnology, 21, R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
42 A really clean experiment on Si Köln/Leipzig/Dresden-Rossendorf/: Macko et al (2010), Nanotechnology, 21, R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
43 The doom of the old dogma No ripples in MC for Si parameters is not a bug, it s a feature! R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
44 New explanations: The power of dirt Discovered by accident H. Hofsäss und K. Zhang Appl. Phys. A, 2008: To create ripples on Si, you need dirt (i.e. a submonolayer concentration of metals like Fe or Mo at the surface) Surfactant sputtering: Dirt, which influences pattern formation (from H. Hofsäss, K. Zhang 2009) R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
45 MC study of surfactant sputtering R.K., T. Yasseri, A. Hartmann, NIMB, 2009 Left: MC, Right: Continuum theory Up: dirt, Down: Topography R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
46 Physical mechanisms 1 Si covered by Fe/Mo has slightly reduced sputter yield. 2 more metal is sputtered from valleys than from crests (BH instability), but it is redeposited homogeneously. Thus metal concentration is enhanced on crests. Thus even less is sputtered from crests etc. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
47 Adatoms: The overlooked major player Now, we can get ripples on Si by dirt. But they are not nice Still, the physical mechanisms are missing, which make ripples nice. Here is the hottest candidate: the cascade particles, which reach the surface but are not sputtered off, i.e. adatoms. Adatoms make up % of cascade at surface. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
48 Adatoms: The overlooked major player Now, we can get ripples on Si by dirt. But they are not nice Still, the physical mechanisms are missing, which make ripples nice. Here is the hottest candidate: the cascade particles, which reach the surface but are not sputtered off, i.e. adatoms. Adatoms make up % of cascade at surface. Ion induced adatom flow is random motion + drift due to remaining ion momentum R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
49 What ion-induced adatoms can do A) Adatom drift leads to smoothing (downhill current) G. Carter, V. Vishnyakov, PR B 1996 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
50 What ion-induced adatoms can do A) Adatom drift leads to smoothing (downhill current) G. Carter, V. Vishnyakov, PR B 1996 B) Adatoms is all you need to create patterns. Sputtering yield zero!! S. Schütz, R.K R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
51 An illuminating physical picture R. Cuerno ion induced flow 2 analogous to flow of a fluid film on an inclined plane 3 well known ripple instability at critical angle 4 adding dirt is like adding a surfactant in the film 5 leads to Marangoni instability (nice ripples) R. Kree, Conf. I.B.S. Bhubaneswar, India, 2011 R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
52 A step closer to the holy grail Adatoms turn ripples into nice ripples Si sputtering parameters, adatom flow parameters fitted to smooth surface stability region R.K R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
53 So, what makes ripples nice? M. Bradley, PR B 2012, S. More, R. K. App. Surf. Sc Do we understand, how adatom flow creates nice ripples? From a theoretical point of view: Changing type II into type I instabilities Θ= B= Γ(q x, q y =0) 0.02 growth rate growth rate Γ(q x =0, q y ) B= qx, qy q x R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
54 Anchors aweigh! New shores ahead! Which combinations of adatom flow, preferential sputtering, chemical forces,... turn the type II (sloppy ripples) instability into a type I (nice ripples, regular dot arrays) instability? This knowledge is the key to technological application. R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
55 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
56 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
57 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
58 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
59 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
60 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
61 Conclusions 1 Nanostructures (ripples, dots) appear spontaneously under ion beam irradiation 2 due to a generic curvature instability 3 on clean Si, you cannot produce clear ripple patterns in this way 4 but with dirt (Fe/Mo), you can 5 adatom flow driven by ions, chemical forces etc can turn ( sloppy ripple ) type II instability nto ( nice ripple ) type I instability 6 adatom flow + dirt may even produce nice dot patterns 7 ion induced nanostructures remain a promising candidate for future production processes R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
62 Many thank s to Alex Hartmann, Martin Feix, Taha Yasseri, Oluwole Emmanuel Yewande, Simon Schütz Hans Hofsäss, Kung Zhang Cynthia Volkerts, Maria Lenius Rodolfo Cuerno, Jorge Muñoz-García SFB 602 Komplexe Strukturen in kondensierter Materie R. Kree (Inst. f. Theoret. Phys.) Oldenburg, 09/07/ / 34
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