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Roughness and Growth Characteristics of

Self-Affine Thin Gold Films

T.W.J. de Wild (S2961830) & L. Grosse (S2983710)


Rijksuniversiteit Groningen
May, 2017

Contents 1
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2 Mathematical Description of Rough Surfaces . . . . . . . . . . . . . . . . . . 1
3 Experimental Approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
5 Discussion and Suggestions for Further Studies . . . . . . . . . . . . . . . . . 12
6 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

Bibliography 15

1 Introduction
The development of scanning probe microscopy (SPM) unlocked the possibility to study the
structure of materials in particular metals on distance scales smaller than ever before.
This paper describes the empirical study on the microstructure of thin film gold samples
using a scanning probe microscope (SPM). Thin films of different thicknesses ranging from
100 to 1000 nm are considered at ambient conditions. In the performed experiment, particular
attention is payed to characterising (a) the microscopic structure or roughness of the gold
surfaces and (b) the growth behaviour of the gold films.
This paper is organised as follows. In section 2 the mathematical and statistical descrip-
tion of rough surfaces and their growth behaviour is reviewed. Subsequently, the experimental
approach is briefly explained in section 3. Following up on this, the results and corresponding
analysis is given in section 4. The obtained results are discussed and possibilities for future
extensions of this work are proposed in section 5. Finally, conclusions are drawn and findings
are summarised in section 6.

2 Mathematical Description of Rough Surfaces


In this section, the mathematical characterisation of rough surfaces and their growth be-
haviour will be treated. Section 2.1 starts with a discussion of the height distribution and cor-

1
2. Mathematical Description of Rough Surfaces 2

responding parameters. Then, in section 2.2, the height-height correlation function (HHCF)
and growth characteristics of (self-affine) rough surfaces will be introduced.

2.1 The Height Distribution Function


The structure of a rough surface can be described by a single random variable h(r), describing
the height of the surface at a position r relative to a (arbitrarily chosen) reference height
level. In this work the convention will that the reference height which is set to the value
zero is the lowest height value present in the considered dataset. The position vector r is
defined in the surface plane. That is, if the height of the surface is measured along the z-axis,
the position vector r is defined on xy-plane: r = (rx x , ry y).
The random variable h(r) is completely specified by the height probability density func-
tion (h) (PDF), or simply height distribution (HD). This function gives the probability for
a random height value to lie in the interval h and h + dh. Furthermore, the distribution (h)
is normalized to unity, that is: Z +
(h)dh 1. (1)

To proceed, it usually assumed that the height distribution function is well-described by a
Gaussian distribution. Setting the average hhi to zero, the variance 2 = hh2 i hhi2 is
equal to the expectation value of h2 , whose square root is usually called the RMS roughness
amplitude w. That is, (h) is given by:
1 2 /2w 2
(h) = eh . (2)
2w2
Indeed, the Gaussian form of the height distribution function is to be confirmed by empirical
determination of the distribution function: this will be one of the core aims of the experiment.
Various higher order moments of (h) will be introduced below that allow for convenient
comparison between the empirically determined height distribution function and the Gaussian
assumption of Eq. 2.

2.1.1 RMS Roughness Amplitude


As mentioned above, RMS roughness amplitude w is defined as the square root of the ex-
pectation value hh2 i and forms an important parameter in the characterisation of a rough
surface. Formally, w is given by:
Z + 1/2
p 2
w hh2 i = h (h) dh (3)

The RMS roughness amplitude describes the spread of (h) around the average or mean,
which is set to zero.

2.1.2 Skewness
The 3-th order moment of the height distribution, usually called the skewness, is a measure
for (a)symmetry of the distribution. Skewness is denoted by 3 and defined by:
Z +
1
3 = 3 h3 (h) dh (4)
w
3

For a Gaussian distribution, the skewness equals zero since it is symmetric around the peak
value (which is set to h 0). The skewness is positive or negative if the distribution has a
tail extending towards the right or left (relative to the peak), respectively.

2.1.3 Kurtosis
Kurtosis (4 ), the 4-th order moment of the height distribution is a measure for the sharpness
of the height distribution function. It is given by:
Z +
1
4 = 4 h4 (h)dh, (5)
w

For a Gaussian, 4 = 3 and for a mildly and sharply peaked distributions are indicated by
4 < 3 and 4 > 3, respectively. In addition, the so-called excess kurtosis is also regularly
considered in favor of the standard definition of kurtosis. The excess kurtosis is defined as:
Z +
1
4 = 4 h4 (h)dh 3, (6)
w

such that a Gaussian satisfies 4 = 0 and mildly (sharply) peaked distributions have 4 < 0
(> 0). This convention will be used from now on. Also, explicit reference to the excess
kurtosis will not always be made: whenever kurtosis is mentioned in the remain parts of this
paper, strictly speaking the excess kurtosis is meant.

2.2 Second Order Statistics and Growth Concepts of Rough Surfaces


In this subsection the growth of rough surfaces will be reviewed. First, three different types
or modes of surface growth will be introduced. Subsequently, the focus will be contrained to
a particular type of surface growth: the growth of self-affine rough surfaces. Using second
order statistics, which is formally captured by a height-height correlation function (HHCF),
the mathematical characteristics of these self-affine surfaces will be derived. Finally, by
inducing time dependence in the HHCF, the growth behaviour of self-affine surfaces will be
described.

2.2.1 Types or Modes of Surface Growth


Rough surfaces, or more specifically thin films, can generally grow in three different ways.
The first growth type is the so called layer by layer growth, which is also known as Frank van
der Merwe growth. This type of growth results in relatively smooth surfaces, since different
mono-layers are formed on top of each other. The second growth type is unstable growth (or
Volmer-Weber growth). If this growth behaviour occurs, small mounds are usually formed,
causing the growth to be unstable. The third and final general growth type is self-affine
or Stransky-Karastanov growth, which essentially refers to a combination of the two growth
modes mentioned above. In case of self-affine growth the amount of roughness grows with
time and/or the length scale of observation.

2.2.2 Self-Affine Rough Surfaces


A self-affine rough surface is as a surface that remains statically invariant (unchanged) under a
self-affine transformation. A self-affine transformation is defined as a dilatation with different
2. Mathematical Description of Rough Surfaces 4

ratios in different direction. Under such a transformation, a self-affine surface statistically


recovers its initial form, i.e. the form it possessed before the transformation. For a self-affine
rough surface, the random height variable h(x) is forced to obey the constraint:

h(x) = h(x). (7)

This equation mathematically formalises the statement that a self-affine surface is scale invari-
ant under the effect of re-scaling the height variable h(x) by a factor (that is h h)
and shrinking the x-axis according to x x/.

2.2.3 The Height-Height Correlation Function


Now that the concept of a self-affine surface is introduced, its second order statistics can be
discussed. The second order statistics is generically described by a height-height correlation
function (HHCF), denoted as:

H(r) = h[h(r) h(0)]2 i = 2w2 f (r/) (8)

with f (r/) a scaling function depending on the described system: in this case a self-affine
surface. The quantity is called the lateral correlation length and serves, in addition to the
RMS roughness amplitude w, as an important parameter to characterise a rough surface.
Note that, by assumption of in-plane rotational invariance, the position vector r is replaced
by its magnitude r |r| in the HHCF. Intuitively, the HHCF H(r) may be considered as
a measure for the probability that the random height value at r is the same as the random
height value at r 0. The location on the surface corresponding to r 0 is arbitrary. For
self-affine rough surfaces, the small and large scale behavior of the HHCF is given by:
(
x2 x  1
f (x) = , (9)
1 x1

where is know as the Hurst or roughness exponent, x r/ and is the in-plane lateral
correlation length mentioned above. The Hurst exponent can take values in the range 0
1 and is a measure for the amount of height-variation on small scales (length scales smaller
than the lateral correlation length ). By construction, -values close to zero correspond to
large height-variation on small scales and -values close to one indicate small height-variation
on small scales. Using the above scaling function f (x), the asymptotic behaviour of H(r)
can be written as: (
mr2 x  1
H(r) = , (10)
2w2 x1

where m w2 / 2 is referred to as the local surface slope.

2.2.4 Growth and the Dynamical Scaling Hypothesis


Using the HHCF, the growth of self-affine rough surfaces can now be described in a mathe-
matical way. Since the self-affine growth is (obviously) related to the time evolution of the
self-affine surfaces, it is evident that time dependence should be induced in the HHCF for it
to govern growth effects. In particular, the time dependence is assumed to manifest in the
5

RMS roughness amplitude w and the lateral correlation length by means of power laws in
time:
w = w(t) t and = (t) t1/z , (11)
where is called the growth exponent and z is the dynamic exponent. Including the time-
dependence in w and , the HHCF becomes:

H(r, t) = 2 [w(t)]2 f [r/(t)] . (12)

Consequently, the time-dependence in the asymptotic behaviour of H(r) reads:


(
r2 t22/z r  (t)
H(r, t) 2 . (13)
t r  (t)

Now, so-called dynamical scaling hypothesis requires the dynamic exponent z to be related to
and via z = /. When this condition is satisfied, the time-exponent of H(r, t) becomes
zero at small scales r  (t). To see this explicitly, plug the dynamical scaling condition
z = / into the time exponent:

2 2/z = 2 2/(/) = 0. (14)

Hence, in case of dynamical scaling the time dependence drops out of the small scale expres-
sion for the HHCF. Growth behaviour obeying the dynamical scaling hypothesis is referred
to as stationary growth, whereas dynamical scaling breakdown (z 6= /) is called non-
stationary growth.

3 Experimental Approach
In the performed experiment thin gold films of thicknesses ranging from 100 to 1000 nm are
analysed using aSPM scanning probe microscope. During all data-acquisitions (gaining the
SPM images), the resolution of the SPM is set to 512 points per line scan. Subsequently,
the selected SPM images see section 4.1 for the selection criteria are analysed using the
computer software Gwyddion [1]. Using Gwyddion, all characterising parameters (e.g. w,
and ) could be obtained from the SPM images.
Since it is assumed that the thickness of the samples grows linearly over time (d t), the
samples of different thicknesses may equivalently be considered as the same thin gold film,
but at different times in its growth evolution. To this end, the analysis on the time-evolution
of the HHCF performed in the previous section can be applied to the empirical data by
replacing t by d.

4 Results
4.1 Selected Samples
SPM images of size 0.5 um 0.5 um are taken multiple times for the different sample thick-
nesses. However, the used samples were damaged at some places due to scratches. For that
reason, only SPM images showing a smooth patch of the samples are taken into consideration.
From these images, a further selection is made based on the visibility of the grains. In some
4. Results 6

(a) 100 nm (b) 400 nm (c) 1000 nm



(d) 700 nm

Figure 1: Selected SPM images of gold for analysis (thicknesses 100, 400 and 1000
nm). In subfigure (d) the SPM image of the 700 nm sample is shown. Observe
that the structure of the sample is indeed different from the samples shown in (a),
(b) and (c).

cases, SPM images of smooth sample patches were obtained, but the visibility of the grains
was rather low. Based on this selection criteria, the analysed SPM images are chosen. Before
the analysis, the SPM images are adjusted and corrected. In particular, the minimum height
value is set to zero in each sample. The images are corrected using the Align Rows option in
Gwyddion.1
The selected images are shown in Fig. 1. It should be noted that the initial plan was
to analyse images of a 700 nm thickness sample as well. Unfortunately, it seems that the
analysed sample was accidentally taken from a second set of gold samples that was not aimed
for this experiment. This presumption is based on the fact that the observed structure in the
700 nm SPM image is completely different from the SPM images of the other thicknesses.
For comparison, a SPM image of the 700 nm sample is also shown in Fig. 1 (d). Observe that
for this sample the size of the faces surrounded by grains is significantly bigger compared to
the samples shown in subfigures (a) to (c). Furthermore, the height variation is bigger as can
be seen from the gradient scale to right to the image. For these reasons, the 700 nm sample
is excluded from the analysis described below.

4.2 The Height Distribution Function


For the analysed images, the height distribution function (h) is determined using the 1D
Statistical Functions tool in Gwyddion. In the left panel of Fig. 2, the height distribution
1
This is a basic correction algorithm that includes different techniques, the details can be found in Ref.
[1].
7

0.5 0.5

0.4 0.4

0.3 0.3

(nm-1 )
(nm-1 )

100 nm
0.2 0.2 400 nm
1000 nm
0.1 0.1

0.0 0.0
-4 -2 0 2 4 -4 -2 0 2 4
h (nm) h (nm)

Figure 2: Left: Measured height distribution function for 100 nm sample (rep-
resented by red dots) and Gaussian PDF fitted by Gwyddion (blue) with RMS
roughness amplitude w = 0.92 0.15 nm. The data is normalised to the peak
value of the fitted Gaussian. Right: fitted Gaussian PDFs (h) for the different
thicknesses (100, 400 and 1000 nm). The fitted values for w are given in Tab. 1.

function data obtained by Gwyddion is shown using the red dots. It should be noted that
the number of data points is somewhat low, certainly when compared to typical height dis-
tribution functions obtained by others using the same setup and samples. Nevertheless, the
obtained data fits the Gaussian PDF reasonably well, as shown by the blue solid line. The
fitted Gaussian is solely based RMS roughness amplitude w, since the height value of the
peak is set to zero hp 0. The fitting value for w is obtained via the Statistical Quantities
tool. Similarly, this is done for the 400 and 1000 nm images. The right panel in Fig. 2 shows
the fitted Guassian distributions for all thicknesses.
Besides the RMS roughness amplitude w, the full-width-at-half-maximum FWHM and
the skewness 3 and (excess) kurtosis 4 are also obtained for all analysed thicknesses. To
compute the FWHM from the RMS roughness amplitude, a Gaussian distribution function
is assumed:

FWHM = 2 2 ln 2 w. (15)

The values for the roughness amplitude w, FWHM, skewness 3 and kurtosis 4 are presented
in Tab. 1. For a height distribution function to be a Gaussian distribution, both the skewness
and kurtosis should satisfy the constraints that they are close to zero. This condition is met
to reasonable extent for all obtained values of 3 and 4 . The only value that deviates
considerably from zero is the skewness value for thickness d = 100 nm. Hence, it may
be concluded that the height distribution function for the analysed samples is fairly well
described by a Gaussian distribution.

d (nm) w (nm) FWHM (nm) 3 4


100 0.92 0.15 2.18 0.35 0.437 0.0917
400 1.11 0.16 2.62 0.37 0.0408 0.0898
1000 1.22 0.18 2.87 0.42 0.0110 0.257

Table 1: Parameters characterising the height distribution function (PDF) (h).


The data presented in this table will be referred to as the HD method, since it is
obtained via the measured height distributions.
4. Results 8

2.0 3.0

2.5
1.5
2.0
H (nm2 )

H (nm2 )
1.0 1.5
100 nm
400 nm
1.0 1000 nm
0.5
0.5

0.0 0.0
20 40 60 80 100 120 140 20 40 60 80 100 120 140
r (nm) r (nm)

Figure 3: Left: measured HHCF (blue dashed) and fit (Eq. 16) (black) for a
thickness of 100 nm. Right: measured HHCFs for all analyzed sample thicknesses.

4.3 The Height-Height Correlation Function

The height-height correlation functions (HHCFs) are obtained for the different thicknesses,
again using the 1D Statistical Functions tool in Gwyddion. The obtained HHCFs are shown
in the right panel of Fig. 3. From these data, the Hurst or roughness exponent , lateral
correlation length are obtained. Furthermore, the large scale behaviour (r/  1) of
the HHCF also provides a second independent approach to determine the RMS roughness
amplitude w. The HHCFs are analysed via two approaches. In the first, Gwyddion fits a
Gaussian HHCF to the data, from which and w can be determined. This approach will
be referred to as the HHCF Fit method. The second approach employs the short and large
range behaviour of the HHCF to determine and in the so-called slope method (SM).

HHCF Fit Method

Using the Graph Fitting Tool in Gwyddion, a Gaussian HHCF fit is made to the obtained
HHCFs. The Gaussian HHCF fit, denoted below as fHHCF (r), is part of Gwyddions
standard fitting function library and has the form:
h 2
i
fHHCF (r) = 2w2 1 e(r/) , (16)

where w is the RMS roughness amplitude and is the lateral correlation length. For the
HHCF corresponding to the sample of 100 nm thickness, the HHCF data and the fit fHHCF (r)
are shown in the left panel of Fig. 3.
Similarly, the fits are also performed for 400 and 1000 nm thickness. The fitted values and
corresponding errors, which are automatically calculated by the Gwyddion fitting algorithm,
are tabulated in Tab. 2 for all thicknesses. The obtained values for the roughness amplitude
w are in reasonable agreement with values obtained via the HD method (see Tab. 1).
Contrary to the roughness amplitude w, the fitted values for the lateral correlation length
should be regarded with caution. As can be seen from the left panel of Fig. 3, the r-
value of the transition point from an increasing HHCF to a flat HHCF is systematically
underestimated by the fit (black solid) as compared with the data (blue dashed). To be more
specific, the HHCF fit gives = 12.0 0.3 nm, whereas the data suggests that the transition
point lies somewhere around ' 25 nm.
9

0.25
2 low 2 high 0.4
0.20

0.3
log H (nm2 )

log H (nm2 )
0.15
100 nm
0.2
0.10 400 nm
1000 nm
0.05 0.1

log rk
0.00 0.0
1.0 1.1 1.2 1.3 1.4 1.5 0.6 0.8 1.0 1.2 1.4 1.6
log r (nm) log r (nm)

Figure 4: Close up of the HHCF at small scales (log r . 1.6). Left: Visualisation
of the slope method. Note the presence of the two linear portions with slopes 2low
and 2high . Right: Close up of the HHCFs at small scales for all thicknesses.

Slope Method
The slope method conveniently employs the advantage of plotting the data logarithmically.
That is, the datasets are analysed in the form (log H(r), log r), instead of (H(r), r). In this
way, the small and large scale behaviour of the HHCF becomes:
(
2 log r + log m r/  1
log H(r) = . (17)
log 2w2 r/  1

This explicitly shows the advantage of using the logarithmic representation of the data:
plotting log H(r) as a function of log r will yield a straight line with slope 2 in the small
scale regime r/  1.
To find these slopes and hence the value of , the data is transformed to the logarithmic
form and plotted for the small scale regime in Fig. 4. The right panel shows the data for all
thicknesses. The left panel shows only the data for 100 nm thickness. Furthermore, this panel
serves as a visual clarification for the discussion below. In fact, it is observed that, in the
logarithmic representation, the linearly growing part of the HHCF can be divided into two
portions, referred to as the low and high parts. These two portions have a slightly different
slope, denoted by 2low and 2high , respectively (see the left panel of Fig. 4). The transition
point between the two linear portions is denoted with log rk . The invoked terminology of
the high and low linear portions is based on this transition point log rk : the low and high
portions lie to the left and right of this value, respectively.

d (nm) w (nm) (nm)


100 0.914 0.003 12.0 0.3
400 1.049 0.003 12.3 0.3
1000 1.172 0.002 12.7 0.3

Table 2: HHCF fit parameters (Eq. 16) for all sample thicknesses. Note that
the roughness parameter w is in reasonable agreement with values obtained via
the HD method. The fitted values for the lateral correlation length should
be regarded with caution, since they are systematically and significantly lower
compared to the values obtained via the SM approach.
4. Results 10

Lastly, the value for the lateral correlation length (or rather log ) is determined from the
intersection of the linear fit with slope high and the horizontal line log 2w2 . The log r value
at which the intersection occurs is identified with log . The used values for w to determine
the horizontal line log 2w2 are the ones obtained via the HHCF Fit and tabulated in Tab. 2.
The determined values for the Hurst exponents in the low and high portion (low and high ),
the transition point log rk and the lateral correlation length log are given in Tab. 3.
The errors are also provided in this table and are determined for the different quantities as
follows. The errors in the Hurst exponents low and high are calculated automatically by the
used fitting software (gnuplot). Since the values for log rk and log are obtained graphically,
the errors have been estimated manually and are not computed using an automised algorithm.
The errors in and log 2w2 are calculated using the known errors in log and w, respectively.
As can be seen from the right panels in Fig. 3 and Fig. 4, for r . 20 nm (corresponding
to log r . 1.3) the HHCFs have approximately the same slope. This statement is true to
high degree for the studied samples of 100 and 1000 nm, but less so for the 400 nm sample.
Therefore, it is justified to consider the average Hurst exponents over all thicknesses. The
averages will be denoted as hii , where the subscript i = {low, high, total} refers to the
averages of the low, the high and the total (low plus high) Hurst exponents. Including all
analysed thicknesses, the following averages are obtained:

hilow = 0.308 0.010,


hihigh = 0.248 0.012,
hitotal = 0.278 0.011. (18)

Excluding the 400 nm case, since its slope differs reasonably from the 100 and 1000 nm cases,
the averages become:

hilow = 0.343 0.010,


hihigh = 0.288 0.011,
hitotal = 0.316 0.010. (19)

The above values (Eq. 19, excluding 400 nm thickness) are in approximate agreement with
previous work on the roughness and growth characteristics of gold by R.C. Salvarezza and
collaborators [2]. They find that, in the high linear portion, the value high is constrained
by:
0.32 0.03 < high < 0.39 0.01, (20)
using gold samples of thicknesses 30, 170, 500 and 850 nm. The transition point log rk is found
to be 1.5, independent of sample thickness, compared to our obtained value of log rk ' 1.25.

d (nm) low high log rk (nm) log (nm) (nm) log 2w2 (nm)
100 0.356 0.009 0.323 0.012 1.23 0.02 1.405 0.006 25 1 0.223 0.002
400 0.237 0.011 0.167 0.014 1.27 0.01 1.541 0.007 34 1 0.343 0.002
1000 0.330 0.010 0.253 0.009 1.30 0.02 1.602 0.006 40 1 0.438 0.003

Table 3: Obtained values for the Hurst exponents in the low and high portion
(low and high ), the transition point log rk and the lateral correlation length
log . The origin of the stated errors is explained in the text.
11

0.10 0.10

0.08 0.08

0.06 0.06

0.04 0.04
log w (nm)

log w (nm)
0.02 0.02

0.00 0.00

-0.02 -0.02

-0.04 -0.04

1.8 2.0 2.2 2.4 2.6 2.8 3.0 3.2 1.8 2.0 2.2 2.4 2.6 2.8 3.0 3.2
log d (nm) log d (nm)

(a) HHCF Fit Method (b) HD Method

Figure 5: Determination of the growth exponent . Left: Linear fit (blue solid)
based on HHCF Method data (red dots). Right: Linear fit based on HD Method
data.

However, the low portion Hurst exponent low is constrained by:

0.71 0.03 < low < 0.77 0.03. (21)

Unfortunately, this constraint is quite different from our values obtained for low .

4.4 Growth Exponents


Now that all required data is presented, the growth parameters and z can be determined.
Since the sample thichness grows linear with time (d t), the RMS roughness amplitude w
and lateral correlation length scale with the thickness d as:

w d d1/z . (22)

To determine the exponent , the RMS roughness amplitudes corresponding to the different
thicknesses are plotted logarithmically and the slope (which equals ) is extracted. Since
two sets of w-values are obtained via the HHCF Fit method and the HD method, two slopes
could be determined from the data. The linear fits (in the logarithmic representation of the
data) give:

log w = 0.1209 log d 0.2733 (HD Method)


log w = 0.1070 log d + 1.009 (HHCF Fit Method) (23)

For both methods, the data (red dots) and fits (solid blue lines) are presented in Fig. 5,
the left panel and right panel corresponding to the HHCF Fit and HD method, respectively.
The fitted values for are also presented in Tab. 4, including the errors which are again
determined automatically by the fitting software.
The growth exponent z related to the time evolution of the lateral correlation length is
extracted from the (d, ) data obtained via the Slope Method (SM), see Tab. 3. Based on the
fact that the HHCF Fit Method systematically underestimates the lateral correlation length
for all thicknesses, this data is disregarded (as indicated in Tab. 4). The linear fit that is
found is given by:

log = 0.2001 log d + 1.0089, (Slope Method) (24)


5. Discussion and Suggestions for Further Studies 12

1.65

1.60

1.55

log (nm)
1.50

1.45

1.40

1.35
1.8 2.0 2.2 2.4 2.6 2.8 3.0 3.2
log d (nm)

Figure 6: Linear fit through (d, ) data obtained via the Slope Method (SM). The
slope of the fit equals 1/z. Note that a fit on the values for obtained via the
HHCF Fit Method is not performed, since the HHCF Fit Method systematically
underestimates the lateral correlation length, as discussed in the text.

where the slope 0.2001 equals 1/z. The data and linear fit are also shown in Fig. 6. The
obtained values for 1/z and z including their errors are given in Tab. 4. The last column is
table shows the ratio of hitotal = 0.278 0.011 (including 100, 400 and 1000 nm data) and
the determined -values via the HHCF Fit Method and the HD Method. It should be noted
that this ratio differs from the value for z determined via the Slope Method by approximately
a factor of two. Therefore, based on the data presented in Tab. 4 it can be concluded that
the dynamical scaling condition is not satisfied, since according to the data z 6= hitotal /.
In other words, the gold samples obey non-stationary growth.
It is worthwhile to mention that the non-stationary growth behaviour also manifests in
the HHCF Fits given by Eq. 16 and tabulated in Tab. 2, although the lateral correlation
length determined by this fit is systematically underestimated. The HHCF fits are plotted for
all thicknesses in Fig. 7. The non-stationary growth is visible in the plot since in the small
scale regime r/  1, the curves corresponding to the different thicknesses do not overlap.
For stationary growth, i.e. for dynamical scaling, overlap of the different curves at small
scales is a requirement [3]. Based on the fact that this is not the case, one concludes that the
gold samples show non-stationary growth.

5 Discussion and Suggestions for Further Studies


In relation to the performed experiment and the obtained results, the following comments
on possible future extensions and improvement are in order. First and arguably most im-
portant, to confirm the validity of the results presented in this work, the experiment should

Method 1/z z hitotal /


HHCF Fits Disregarded 0.1070 0.004 2.59 0.14
SM 0.2001 0.005 4.99 0.01
HD 0.1209 0.006 2.29 0.16

Table 4: Obtained values for the growth parameters and z. The last column
gives the ratio for /, which must equal z for the dynamical scaling condition
to be satisfied, this is clearly not the case. The average value used for is
hitotal = 0.278 0.011 as obtained taking all thicknesses into account.
13

0.50

H (nm2 )
100 nm
0.10 400 nm
0.05 1000 nm

0.01

1 5 10 50 100
r (nm)

Figure 7: Manifestation of the non-stationary growth or non-dynamical scaling


condition by means of the HHCF Fits according to Eq. 16. For dynamical scaling
or stationary growth, the curves should overlap at small scales r/  1. However,
as shown this is not the case and the growth is concluded to be non-stationary.

be repeated in which the analysis of a correct 400 nm gold sample is included. Furthermore,
the experiment could be extended by considering more gold samples of various thicknesses
or other type of samples (e.g. silver (Ag) or silicon (Si)).
It should also be mentioned that in the current experiment, only one SPM image for
each thickness was analysed. However, the statistical accuracy of the results would increase
if multiple scans of the same (part of a) sample would be combined. Furthermore, such an
approach would also give a more conclusive answer to the question whether the obtained
values for the higher order moments of the height distribution (3,4 ) are indeed in line with
a Gaussian distribution. Currently, this conclusion is made based on values extracted from
only three SPM images (one for each analysed thickness). In fact, the skewness 3 of the
100 nm image is 0.437 (see Tab. 1), which deviates rather significantly from the Gaussian
value (3 = 0). Combining multiple scans would allow to determine whether this deviation
is accidental or systematic.
Then, there are some aspects about the analysis of the HHCF to be mentioned. The first
point is related to the determination of the lateral correlation via the HHCF Fit. Compared
to the -values obtained via the Slope Method (SM), the values from the HHCF Fit are found
to be systematically lower for all thicknesses. Using the multiple scans approach mentioned
in the previous paragraph, it could be examined whether this apparent underestimation is
indeed a shortcoming of the applied fit (Eq. 16) as suggested in Section 4.3 or that the
underestimation is only characteristic for the particular SPM images used in this work.
Secondly, it was found that the linear rise of the HHCF at small scales could be subdivided
into two regimes, called the low and high portion, with different values for the Hurst exponent
(hilow and hihigh ). As stated in the Results, the high portion Hurst exponent hihigh agrees
fairly well with values stated in literature. However, this is not the case for hilow . This
discrepancy could be subject of study in future extensions to this experiment. Also, the
-values obtained for 400 nm thickness seem to deviate from the general trend in the 100 and
1000 nm cases. In future experiments this apparent deviation could be resolved or examined
in more detail. Lastly, let us mention that from are more fundamental and theoretical
perspective the physical origin of the division into two linear portions could be studied.
Lastly, the experiment described in this work could be repeated under a variety of different
conditions. For instance, one could construct this experiment, but cool or heat the gold
samples and examine the effect of temperature on the surface growth behaviour.
6. Conclusion 14

6 Conclusion
This work describes the empirical determination of the roughness and growth characteristics
of gold samples by means of Scanning Probe Microscopy (SPM). It is found that gold surfaces
can be described fairly well by a Gaussian height probability density function (h) (PDF)
and the RMS roughness amplitude w, since the 3-th and 4-th order moments 3 and 4
(skewness and kurtosis) determined from the measured height distributions are reasonably
close to the values corresponding to a Gaussian distribution. In addition, the second order
statistics as governed by the height-height correlation function (HHCF) is also examined.
The corresponding lateral correlation length is determined, as well as the surfaces Hurst
exponent , which measures the amount of height-variation on small scales. It was found
that in fact two Hurst exponents can be identified, consistent with literature [2]. However,
the obtained values for only partially agree with the values provided in literature. Finally,
the growth exponents z and are obtained. It is found that the dynamical scaling condition
z = / is not fulfilled and hence it can be concluded that the gold samples show non-
stationary growth behaviour.
Bibliography

[1] P. Klapetek, D. Necas, and C. Anderson, Gwyddion user guide, Czech Metrology Insti-
tute, vol. 2007, p. 2009, 2004.

[2] L. Vazquez, R. Salvarezza, P. Herrasti, P. Ocon, J. Vara, and A. Arvia, Stm study of
fractal scaling in evaporated gold films, Applied surface science, vol. 70, pp. 413417,
1993.

[3] Unkown, Manual: Scanning probe microscopy, RUG Phys. Lab. 3 Course Material,
2015.

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