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Studying the growth, formation, and morphology of do this by an evolution equation for hx vs x, for a cer-
interfaces has been one of the recent interesting fields of tain time.
study because of its high technical and rich theoretical For this purpose, a copper film was deposited on a
advantages [1]. One of the main problems in this area is polished Si(100) substrate by the resistive evaporation
the scaling behavior of the moments of height difference method in a high vacuum chamber. The pressure during
h hx1 hx2 and the evolution of the probability evaporation was 106 Torr. The thickness of the growing
density function (PDF) of h, i.e., Ph; x in terms of films was measured in situ by a quartz crystal thickness
the length scale x. Recently, Friedrich and Peinke have monitor. We performed all depositions at room tempera-
been able to obtain a Fokker-Planck equation describing ture, with a deposition rate about 20–30 nm= min. The
the evolution of the probability distribution function in substrate temperature was determined using a chromel/
terms of the length scale, by analyzing some stochastic alumel thermocouple mounted in close proximity of
phenomena, such as a turbulent-free jet, etc. [2 – 4]. They samples. The surface topography of the films was inves-
noticed that the conditional probability density of field tigated using Park Scientific Instruments model Auto-
increments (velocity field, etc.) satisfies the Chapman- probe CP. The images were collected in a constant force
Kolmogorov equation. Mathematically this is a necessary mode and digitized into 256 256 pixels with scanning
condition for the fluctuating data to be a Markovian frequency of 0.6 Hz. The cantilever of 0:05 N m1 spring
process in the length scales [5]. constant with a commercial standard pyramidal Si3 N4
In this Letter, using the method proposed by Friedrich tips was used. A variety of scans, each with size L, were
and Peinke, we measure the Kramers-Moyal (KM) recorded at random locations on the Cu film surface.
coefficients for the fluctuating fields h and hx of It is a common procedure to characterize the complex-
a deposited copper film. It is shown that the first and ity of a rough surface by checking the scaling behavior of
second KM coefficients have well-defined values, while the moments Cq hjhx1 hx2 jq i in terms of the
the third and fourth order coefficients tend to zero. length scale x jx1 x2 j. We investigated the scaling
Therefore, by addressing the implications dictated by behavior of the qth moment Cq and observed that all of
the theorem [5], a Fokker-Planck evolution operator has the moments (up to q 20) behave as jx1 x2 jq within
been found. The Fokker-Planck equation for Ph; x is the scaling region 10 to 150 nm. This shows that the
used to give information on changing the shape of the height fluctuations are intermittent or multifractal (see
PDF as a function of the length scale x. By using this [8,9] and references therein). The roughness exponent is
strategy, the information of the observed intermittency related to the exponent 2 as 2 =2 [1]. For the sta-
of the height fluctuation is verified [6]. The first and tionary samples with thickness 440 nm, the roughness
second KM coefficients for the fluctuations of hx en- exponent was found to be 0:83
0:03. From the sto-
able us to write a Langevin equation for the evolu- chastic point of view, one has to remark that multifrac-
tion of height with respect to x. Using this equation, tality is based on properties of the roughness on distinct
we regenerate the surface with similar statistical prop- length scales. However, checking the scaling behavior
erties, compared with the observed morphology by does not explain possible correlation between the rough-
atomic force microscopy. The regeneration of a surface ness measures on different scales. Also, it is noted that the
is known as the inverse method. There are other inverse methods based on multifractality are limited to the sub-
method approaches introduced in the literature [7]. In class of rough surfaces which show scaling properties.
the previous attempts, to regenerate the surface, an evo- The method introduced by Friedrich and Peinke is a
lution equation for hx; t vs t has been evaluated. Here we general method, which explains the complexity of the
surface roughness, with no scaling feature to be explicitly Chapman-Kolmogorov equation formulated in differen-
required. Their method yields an estimation of an effec- tial form yields a master equation, which can take the
tive stochastic equation in the form of a Fokker-Planck form of a Fokker-Planck equation [5]:
equation (also known as Kolmogorov equation). The con-
d @
nection between the multifractality and Markovianity has ph; r D1 h; r
dr @h
been discussed in [4].
A complete characterization of the statistical proper- @2 2
D h; r ph; r; (2)
ties of the height fluctuation requires the evaluation of @h2
joint PDFs PN h1 ; x1 ; . . . ; hN ; xN , for any arbi-
where r : x. The drift and diffusion coefficients
trarily N. If the process is a Markov process (a process
D1 h; r, D2 h; r can be estimated directly from
without memory), an important simplification arises. For
the data and the moments Mk of the conditional proba-
this type of process, the N-point joint PDF, PN , is gen-
bility distributions:
erated by a product of the conditional probabilities
Phi1 ; xi1 jhi ; xi , for i 1; . . . ; N 1. As a nec- 1
Dk h; r lim Mk ;
essary condition for being a Markov process, the k! r!0
Chapman-Kolmogorov equation,
1 Z
Z Mk d h0 h0 hk ph0 ; r rjh; r:
r
ph2 ;x2 jh1 ;x1 dh3 ph2 ;x2 jh3 ;x3
(3)
ph3 ;x3 jh1 ;x1 ; (1) The coefficients Dk h; r are known as Kramers-
Moyal coefficients. The drift and diffusion coefficients
should hold for any value of x3 , in the interval x2 < D1 and D2 are displayed in Fig. 2. It turns out that the
x3 < x1 [5]. We checked the validity of the Chapman- drift term D1 is a linear function of h, whereas the
Kolmogorov equation for different h1 triplets by com- diffusion term D2 is a function quadratic in h. For
paring the directly evaluated conditional probability dis- large values of h, our estimation becomes poor and thus
tributions ph2 ; x2 jh1 ; x1 with the ones calculated uncertainty increases. From the analysis of the data set,
according to the right-hand side of Eq. (1). In Fig. 1, the we obtain the following approximation:
two direct and integrated PDFs are superimposed for the
purpose of illustration. The bold and open symbols rep-
0.3
resent directly evaluated PDF and integrated PDF, re- ∆x= 300 (nm)
∆x=
spectively. Assuming a statistical error of the square 0.2 ∆x=
400 (nm)
500 (nm)
root of the number of events of each bin, we find that ∆ x = 600 (nm)
both PDFs are statistically identical (see also [10], an- 0.1
other interesting and carefully presented example of ap-
D (∆h)
0.08 -50 0 50
∆ h (nm)
0.06
0.04
∆ x = 300 (nm)
0.004 ∆ x = 400 (nm)
∆ x = 500 (nm)
p ( ∆ h2 | ∆ h1)
0.003
D (∆ h)/∆x
2
0.002
0.001
-50 -40 -30 -20 -10 0 10 20 30 40 50
∆ h2 (nm)
-50 -25 0 25 50
FIG. 1 (color online). Test of Chapman-Kolmogorov equation ∆h (nm)
for different values h1 21 nm, h1 0, and h1
21 nm. The bold and open symbols represent directly evaluated FIG. 2 (color online). Drift and diffusion coefficients D1 h
PDF and the integrated PDF, respectively. The length scales and D2 h are estimated from Eq. (3). The D1 and D2 present
x1 , x2 , and x3 are 180, 320, and 260 nm, respectively. the linear and quadratic behavior, respectively.
226101-2 226101-2
PHYSICA L R EVIEW LET T ERS week ending
VOLUME 91, N UMBER 22 28 NOVEMBER 2003
D1 h; x 0:0055:2h; The height field is measured in units of the standard
deviation of h. Analogous to Eq. (2), we can write a
D2 h; x 2:9 104 h2 (4) Fokker-Planck equation for the PDF of h by replacing r
and h with x and h, respectively. We note that this
0:015x0:45 =x;
Fokker-Planck equation is equivalent to the following
Langevin equation (using the Ito interpretation) [5]:
where h is measured in units of the standard deviation
q
of h at x 200 nm. According to Pawula’s theorem, d
the Kramers-Moyal expansion stops after the second hx D1 h D2 hfx: (6)
dx
term, provided that the fourth order coefficient
D4 h; x vanishes [5]. The fourth order coefficient Here, fx is a random force, zero mean with Gaussian
D4 in our analysis was found to be about D4 ’ statistics, correlated in x, i.e., hfxfx0 i x x0 .
104 D2 . In this approximation, we can ignore the co- Furthermore, with this last expression, it becomes clear
efficients Dn for n 3. To perform a quantitative test of that we are able to separate the deterministic and the
the result with these coefficients, we solve the Fokker- noisy components of the surface height fluctuations in
Planck equation for the PDF at scales x L with a terms of the coefficients D1 and D2 . Equation (6)
given distribution at sample size L [6,11]. Figure 3 shows enables us to regenerate rough surfaces which are similar
a comparison between the analysis of the atomic force to the original one (in the statistical sense). In Fig. 4, the
microscopy (AFM) image and the solutions of the ob- AFM and regenerated images are demonstrated. The
tained Fokker-Planck equation for the copper surface for regenerated surface is very similar in statistical sense to
the length scales x 200, 300, and 500 nm. The figure the original one. All regenerated patterns are statistically
shows that the solutions of our model fit the experimen- similar. To ensure this fact, for instance, in Fig. 5 we have
tally determined PDFs with good precision. In the inte- plotted the second moment of the structure function C2
gral scale our measured PDF is nearly a Gaussian for the AFM and regenerated surfaces and their rough-
distribution. In our approximation, the stochastic process ness exponents were found 0:83
0:03 and 0:83
0:01,
underlying the height fluctuation changes is a linear sto- respectively.
chastic process with multiplicative noise.
By the same procedure, we checked the Markovian
nature of the fluctuations of the height h hx h
and found the following expression for the D1 h and
D2 h:
∆ x = 200 (nm)
∆ x = 300 (nm)
∆ x = 500 (nm)
∆ x = 200 (nm)
∆ x = 300 (nm)
∆ x = 500 (nm)
p (∆h, ∆ x)
-2 0 2
∆h
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