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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

Lijun Zhanga,b, Yong Dua, Qing Chenc, Ingo Steinbachb, Baiyun Huanga
a

State Key Laboratory of Powder Metallurgy, Central South University, Hunan, China
Interdisciplinary Centre for Advanced Materials Simulation, Ruhr-Universitt Bochum, Bochum, Germany
c
Thermo-Calc Software AB, Stockholm, Sweden
b

Atomic mobilities and diffusivities in the fcc, L12


and B2 phases of the NiAl system
A phenomenological model was utilized to describe diffusivities in the c (fcc) / c (L12) and A2/B2 phases of the NiAl
system. An effective strategy, which takes the homogeneity
range and defect concentration into account, was developed
in the present work to optimize the atomic mobilities of c
phase. Such a strategy results in a dramatic decrease in the
number of atomic mobility parameters to be evaluated for
the L12 phase. The measured composition- and temperature-dependent diffusivities in the NiAl system have been
well replicated by the present mobility descriptions. For the
L12 phase, comprehensive comparisons show that with fewer
model parameters the presently obtained mobilities yield a
better fit to experimental diffusivities, compared with previous assessments. The mobility descriptions are further validated by comparing calculated and measured concentration
profiles for various diffusion couples. The time-dependent
Al composition profile for the annealed vapor Al / c couple
is accurately described for the first time.
Keywords: NiAl system; Diffusion; Atomic mobility; Order / disorder phenomena; DICTRA

1. Introduction
Knowledge of both thermodynamic and diffusion characteristics in multicomponent alloys is of critical importance
in various materials processes, such as solidification, heat
treatment, recrystallization and protective coatings. To gain
an insight into the above materials processes, an advanced
Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

computational technique is an appropriate underlying tool.


So far, the CALPHAD (CALculation of PHAse Diagram)
technique has made significant progress, and a wide variety
of multicomponent thermodynamic databases have already
been constructed [1]. However, this is not the case for diffusion data. To simulate diffusion-controlled transformations
in multicomponent systems, the DICTRA (DIffusion Controlled TRAnsformations) software package [2] has been
developed, and operates under the CALPHAD framework.
Based on the sharp interface and local equilibrium hypothesis, DICTRA has been successfully utilized to simulate
various phase transformation processes with the so-called
atomic mobility database [3 7]. Moreover, 2D or 3D simulations using the phase-field method including effects of interfacial energy, stress, strain and convective transport in
liquid, in addition to thermodynamic and kinetic data, represent a new class of simulation tools in materials science
[8 11]. The link to real CALPHAD-type thermodynamic
and atomic mobility databases [12 15] is also of invaluable benefit. In phase-field simulations metastable phases
are also addressed, and thus an extrapolation of thermodynamic functions beyond the region of thermodynamic stability are needed resting on a sound model basis. Therefore,
there is an increasing need to establish accurate atomic mobility databases for advanced material research.
In the present work, we examine the atomic mobilities
and diffusivities in the c(fcc), c(L12), and B2 phases of
the NiAl system, which is of great technological importance in many applications, such as high-temperature structural materials, coatings, diffusion barriers etc. In this system, there exists a large amount of experimental data on
1461

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Basic
L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

diffusivities in various phases and composition profiles for


different diffusion couples. The former is the main input of
our CALPHAD-type assessment work and is critically reviewed in Section 3; the latter is used to validate the obtained mobility data in the final part of Section 4. Several
assessments on the atomic mobilities in the NiAl system
can be found in the literature. The earliest one, performed
by Engstrm and gren [16], dealt with the disordered c
phase. Later, Helander and gren [6] introduced a phenomenological model on the basis of Girifalcos theory [17] and
obtained a successful description for the atomic mobilities
and diffusivities in the ordered B2 phase. The work due to
Helander and gren [6] was then updated by Wei et al.
[18], who considered more experimental data. However,
the results by Wei et al. [18] were found to be unreasonable
by Liu and Liang [19]. Most recently, Campbell carefully
assessed [20] and reassessed [21] the mobilities and diffusivities for both the B2 and L12 phases in the NiAl(Cr)
system by adopting the phenomenological model due to
Helander and gren [6]. While these latest modeling results
agree well with most of experimental data, as many as 11
[20] and 12 [21] parameters were employed for the L12
phase in the NiAl system. The introduction of so many parameters was not justified considering the relatively narrow
composition range of the L12 phase. Besides, it is recognized that the self-diffusion parameters for the pure elements are the building blocks for the development of
multicomponent atomic mobility databases. However, only
the self-diffusion coefficients for pure elements at high
temperatures are usually taken into account in most of the
early assessments, such as the assessments by Jnsson [22]
for pure Ni, and Engstrm and gren [16] for pure Al. The
direct extrapolation of these self-diffusion parameters obtained by means of the data at high temperatures into the
low temperature region may result in inaccurate predictions
of diffusivities. Such an extrapolation should be avoided in
various quantitatively numerical simulations. Cui et al.
[23] performed a literature review on the self-diffusivity
data for pure Al over the wide temperature range and suggests that a smaller frequency factor than that assessed by
Engstrm and gren [16] is likely to be more realistic. Consequently, they [23] reassessed the self-diffusion parameter
for pure Al by using more data than those used by Engstrm
and gren [16]. However, they [23] ignored two groups of
literature data, i. e. Fradin and Rowland [24] at high temperatures and Burke and Ramachandran [25] at low temperatures. Using high purity Al (99.9999 wt.%) coupled
with nuclear magnetic resonance (NMR) and radio-frequency field pulse technique, Fradin and Rowland [24]
measured the self-diffusion coefficients of pure Al at a relatively wide temperature range (513 823 K), which show a
certain deviation from those earlier data by Lundy and Murdock [26] and Stoebe et al. [27], but in a good agreement
with those later data by Beyeler and Adda [28] and Messer
et al. [29] and also the only two data at low temperatures
from Burke and Ramachandran [25] and Volin and Balluffi
[30]. Therefore, there is a need to update the self-diffusion
parameters for pure Ni and Al by considering all the experimental data over the entire temperature range before reassessing atomic mobilities in the c and c phases of the present NiAl system.
In the present work, we intend to (I) update the self-diffusion parameters for pure Ni and Al by considering all the
1462

experimental data over the entire temperature range; (II) reassess the atomic mobilities and diffusivities in the fcc, L12
and B2 phases by taking into account almost all available
experimental data and paying special attention to the number of parameters used for the description of L12 phase,
and compare the present results with the previous assessments; and (III) validate the presently obtained atomic mobilities and diffusivities by comparing the calculated and
measured concentration profiles in a variety of diffusion
couples.

2. Models
The thermodynamic description of the fcc, L12 and B2
phases in the NiAl system is directly taken from the work
by Dupin et al. [31]. Since L12 and B2 phases are ordered
structures of fcc and bcc, respectively, they were represented by a two-sublattice model, where Ni and antisite Al
atoms occupy one sublattice, and Al and antisite Ni atoms
the other. For the B2 phase, vacancies were introduced into
both sublattices.
According to the model suggested by Andersson and gren [32] and Jnsson [22], which is based on the absolute
reaction rate theory [33], the atomic mobility for an element
B, MB , can be expressed as:




RT ln MB0
QB 1 mg
exp 
C
1
MB exp
RT
RT RT
where R is the gas constant, T the temperature, MB0 a frequency factor and QB the activation enthalpy. Both MB0
and QB are in general dependent on composition, temperature and pressure. mg C is a factor taking into account the ferromagnetic contribution to the diffusion coefficient, and
can be expressed as [34]


nQB
mg
2
C exp6n exp
RT
in which n represents the state of the magnetic order
(0 < n < 1), and  can be treated as a constant (0.3 for bcc
alloys, while 0 for fcc alloys [35]).
For a disordered phase, in the spirit of the CALPHAD approach [36], the composition dependency of RT ln MB0 and
QB can be represented with the RedlichKister expansion,
namely
"
#
m
X
X
XX

r
r i;j
i
xi U B
xi xj
U B xi  xj
3
UB
i

j>i

r0

where UB represents RT ln MB0 or QB . UiB is the value of UB


for pure i and r Ui;j
B are binary interaction parameters. Obviously, one can simply combine QB and RT ln MB0 into
one parameter, i. e. UB QB RT ln MB0 when the ferromagnetic effect on diffusion is negligible.
Once the atomic mobilities in an alloy are known, various diffusivities including trace diffusivity, intrinsic diffusivity, and chemical diffusivity can be calculated. Assuming the monovacancy mechanism for diffusion and
neglecting correlation factors [22, 32], the tracer diffusivity
DB is related to the mobility MB by the Einstein relation:
DB RTMB

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Basic

L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

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In the volume-fixed frame of reference or number-fixed


frame of reference, the interdiffusion coefficient D~nkj , which
relates the flux of element k with the gradient of component
j and reference component n, is given by [32]:


X
qui qui
n
~
Dkj
dik  xk xi Mi

5
qxi qxn
i
where dik is the Kroneker delta (dik 1 if i k, otherwise
dik 0) and li is the chemical potential of element i. The
intrinsic diffusion coefficient, Dnkj , is defined in the latticefixed frame of reference and can be identified as [32]


quk quk

6
Dnkj xk Mk
qxj qxn
For an ordered phase, the composition dependence of the
atomic mobility should include also the effect of chemical
ordering. Based on Girifalcos conclusion [17] that the increase of the activation energy due to chemical ordering depends quadratically on the long-range order parameter, Helander and gren [6] proposed a phenomenological model
to describe diffusion in phases with the B2 ordering transformation, where the activation energy can be expressed as
ord
QB Qdis
B QB

where Qdis
B represents the contribution from the disordered
state and can be expressed by Eq. (3), while Qord
B denotes
the contribution from chemical ordering. This later quantity
is given by an equation of the form:
h
i
XX
ord  b
8

Q
y
y

x
x
Qord
i
j
j
B
Bij i
i

i6j

where Qord
Bij is a parameter describing the contribution of the
component B as a result of the chemical ordering of the i j
atoms on the two sublattices and yi is the site fraction of
component i on the  sublattice,
yi

Ni

Ntotal

in which Ni is the number of sites on the  sublattice that



is the total number of
are occupied by an i atom and Ntotal
sites on the  sublattice. Although the phenomenological
model developed by Helander and gren [6] was for an
AB-type alloy (B2 structure), it is proved to be applicable
also for the AB3-type alloy (L12 structure) by Tkei et al.
[37].

3. Review of literature data


There exists a large amount of diffusivity data for fcc, L12,
and B2 phases in the NiAl system. To assign suitable
weighting for various data from different sources in the
present assessment, the following geometric relations are
used as an important criterion:
(I) the inter-diffusion coefficient is equivalent to the impurity diffusion coefficient of Al in Ni when xNi ? 1,
and equivalent to the impurity diffusion coefficient of
Ni in Al when xNi ? 0;
(II) the tracer diffusion coefficient of Al is equivalent to
the self-diffusion coefficient of Al when xNi ? 0, and
Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

equivalent to the impurity diffusion coefficient of Al


in Ni when xNi ? 1; and
(III) the tracer diffusion coefficient of Ni is equivalent to
the self-diffusion coefficient of Ni when xNi ? 1, and
equivalent to the impurity diffusion coefficient of Ni
in Al when xNi ? 0.
3.1. Fcc phase
As listed in Table 1, various experimental diffusion coefficients associated with the fcc phase exist in the literature,
includingself-diffusion coefficients of Al [24 30] and Ni
Ni
[38 56] DAl
Al and DNi , impurity diffusion
 Nicoefficients
 of
Al
Al in Ni [57 59] and Ni in Al [60, 61] DAl and DNi , as


well as inter-diffusion coefficients [57, 62 72] D~Ni
AlAl .
Two general criteria were employed in data selection for assessment of atomic mobilities of the fcc phase in the present
work. One is the above mentioned geometric relations, and
the other is that the measured diffusion coefficients at high
temperatures, as well as those at low temperatures but in
single crystals, are used in the assessment. The diffusivities
resulting from poly-crystals at low temperatures are not utilized since the grain boundary diffusion becomes dominant
at low temperatures in poly-crystals. The detailed information for the selection of experimental data is summarized
in Table 1. As for the impurity diffusion coefficients of Ni
in fcc Al, Du et al. [73] conducted a critical assessment by
means of the least-squares method and semi-empirical correlations. Thus, their results [73] are directly utilized in the
present assessment.
3.2. L12 and B2 phases
According to Campbell [20, 21], the experimental data for
Ni diffusion as well as the inter-diffusion in the L12 and
B2 phases are substantial, while limited experimental data
are available for Al diffusion due to the lack of appropriate
isotope. There are two alternative ways to determine the
Al tracer diffusion coefficients in the L12 and B2 phases.
One way is to measure the solute tracer diffusion coefficients of Al-substituting elements (e. g. In, Ga and Ge) in
Ni3Al or NiAl, or measure the tracer diffusion coefficients
in similar systems, i. e. Ge in Ni3Ge and Ga in Ni3Ga. The
other way is to use the DarkenManning relation to determine the Al tracer diffusion coefficients from the inter-diffusion or intrinsic diffusion coefficients. Since critical evaluation of the relevant experimental data have been
performed by Campbell [20, 21], there is only a need to
concisely summarize and categorize all of them in the present work. Besides, some literatures not mentioned by
Campbell [20, 21] are also included. Table 2 lists all the experimental data in the L12 and B2 phases, including tracer
diffusion coefficients of Al and Ni (Refs. [74 89] for L12
phase, while Refs. [92 96] for B2 phase), intrinsic diffusion coefficients for Al and Ni (Refs. [80, 81] for L12 phase,
while Refs. [94, 97] for B2 phase), as well as inter-diffusion
coefficients (Refs. [63, 67 71, 79 82, 90, 91] for L12
phase, while Refs. [63, 70, 71, 90, 94, 97 104] for B2
phase).
According to Helander and gren [6], it is possible to
fully characterize the diffusion in a binary system using
two out of the three usual types of diffusivities, i. e. tracer
1463

L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

diffusion coefficients of two components or tracer diffusion


coefficients for one component plus inter-diffusion coefficients. Thus, the atomic mobilities of Ni and Al in the L12
and B2 phases of the NiAl system are assessed based on
the corresponding tracer diffusion coefficients of Ni and
the inter-diffusion coefficients, while the Al tracer diffusion
coefficients in the L12 and B2 phases are not used because
most of the reported data are not from direct measurements.
The only existing experimental information for Al tracer
diffusion coefficients in L12 phase is from Larikov et al.
[74], who used the radioactive isotope 26Al with specific
activity of approximately 1.7 106 Bq L 1. Their results
[74], however, show certain deviation from those deter-

W 2010 Carl Hanser Verlag, Munich, Germany

mined with other methods [75, 79 84]. Considering their


mutual consistency, the experimentally measured Ni tracer
diffusion coefficients in L12 phase from [85, 86, 88, 89],
as well as those from [75, 87] above 1 173 K, are employed
in the present assessment of mobilities in L12 phase, while
those from [75, 87] below 1 173 K are not because the contribution from grain boundary diffusion cannot be negligible in poly-crystal specimens at low temperatures. Due to
the fact that the inter-diffusion coefficients in the L12 phase
above 1 373 K measured by Watanabe et al. [70, 71] from
various diffusion couples are consistent with each other,
and also in fair agreement with those by Fujiwara and Horita [80, 81], the experimental values above 1 373 K from

Table 1. Summary of various experimental diffusion coefficients in the fcc phase of the NiAl system.
Data

T (K)

DAl
Al

723 923
603 733
513 823
673 883
358 482
403 473
515 785

DNi
Ni

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Basic

DNi
Al

DAl
Ni

D~Ni
AlAl

Methoda
26

Al, thick layer technique, SC


Al, NMR line-narrowing measurement
NMR and radio-frequency field pulse technique
26
Al, sectioning, SC
TEM, void shrinkage investigation
diffusion controlled climb model
NMR and modified SlichterAllion theory
27

Ref.

Codeb

[26]
[27]
[24]
[28]
[30]
[25]
[29]

&

[38]
[39]
[40]
[41]
[42]
[43]
[44, 45]
[46]
[47]
[48]
[49]
[50]
[51]
[52]
[53]
[54]
[55]
[56]

&

&
&
&
&
&
&

1 273
1 143 1 521
1 373 1 448
1 423 1 673
1 423 1 673
953 1 103
973 1 373
1 202 1 576
948 1 023
748 923
1 173 1 473
1 273 1 673
1 253 1 673
1 173 1 473
1 338 1 563
1 163 1 477
813 1 193
873 1 273

63

1 373 1 573
1 073 1 243
914 1 212

pressure-welded DC, spectro photometry


measurement of weight gain by surface oxidation
SIMS, SC

[57]
[58]
[59]

&

623 903
776 924
entire range

63

Ni, sectioning
electrical resistance measurement
the least-squares method

[60]
[61]
[73]

1 373 1 573
1 533
1 273 1 573
1 273 1 573
1 273 1 473
1 073 1 473
1 073 1 473
1 173 1 473
1 173 1 473
1 073, 1 273

pressure-welded DC, lathe sectioning


single-phase DC, BMM
Ni3Al/Ni and NiAl/Ni DC, BMM
vapor/solid single-phase DC, EPMA, BMM
single-phase DC, EPMA, BMM
single-phase DC, AEM and EPMA, BMM
Ni3Al/Ni DC, AEM and EPMA, BMM
NiAl/Ni DC, AEM and EPMA, SFT
various kinds of DC, AEM and EPMA, SFT
single-phase DC, EMPA, BMM

[57]
[62]
[63]
[64]
[65]
[66]
[67 69]
[70]
[71]
[72]

&

Ni, SAM, PC
Ni, sectioning and SAM, PC
63
Ni, activity measurement, PC
63
Ni and 59Ni, sectioning, PC
63
Ni and 59Ni, SAM, PC
63
Ni, surface monitoring technique, SC
63
Ni, sectioning and SAM, SC and PC
63
Ni, layer-by-layer sample taking
63
Ni, SAM, SC and PC
63
Ni, SAM, SC
63
Ni, absorption method, SC and PC
63
Ni, graphs of radioactivity distribution
63
Ni, sectioning and SAM, SC
63
Ni, absorption method
63
Ni, Gruzin method, PC
63
Ni, absorption method
63
Ni, miscrosectioning technique, SC
63
Ni, absorption method, SC
63

&
&
&
&
&
&
&
^
&
&
&
&
&
&
&
&
&

&
&

~
&

&
&
&
&
&
&
&
&
&

SC = single crystals; PC = poly-crystals; NMR = nuclear magnetic resonance; TEM = transmission electron microscopy; SAM = surface
activity method; SIMS = secondary ion mass spectrometry; DC = diffusion couples; BMM = BoltzmannMatano method; EPMA = electron probe microanalyzer; AEM = analytical electron microscope; SFT = Sauer & Freise technique.
Indicates whether the data are used or not used in the atomic mobility assessment: &, used; ~ not directly used because the assessment
work from Du et al. [73] is used; ^, the experimental data from single crystals are used, while those from poly-crystals are not; &, not
used but used to compare with the present assessment.

1464

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Basic

L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

W 2010 Carl Hanser Verlag, Munich, Germany

those from Hancock and McDonnell [95] below 1 273 K


are not employed because there exists considerable grain
boundary diffusion at low temperatures. Due to good agreements among them, the inter-diffusion coefficients above
1 173 K from Watanabe et al. [70, 71] and Paul et al. [93,

Table 2. Summary of various experimental diffusion coefficients in the L12 and B2 phases of the NiAl system.
Data

T (K)

L12

DAl

1 273 1 473
1 173 1 473
974 1 206
1 005 1 422
1 400
1 423 1 523
1 173 1 373
1 172 1 532
1 173 1 373

radioactive Al isotope
114m
In, SSM, PC
68
Ga in Ni3Ga, 67Ga in Ni3Ga, IBSS
69/71
Ga and 74/72/70Ge in Ni3Al, SIMS, SC
DarkenManning equation
Manning equation
DarkenManning equation
extrapolation from ternary systems
67
Ga in Ni3Al, RAM

1 460 1 830
1 273 1 473
1 163 1 477
965 1 625
1 004 1 422

63

DAl , DNi
D~Ni
AlAl

B2

DAl

DNi

DAl , DNi
D~Ni
AlAl

Ref.

Codeb

[74]
[75]
[76]
[77, 78]
[79]
[80, 81]
[82]
[83]
[84]

&

[85]
[74]
[86]
[87]
[88]

&

[75]
[89]

&
&
&
&
&
&
&
&

1 173 1 473
1 183 1 373

Ni, RAM
radioactive Ni isotope
63
Ni, absorption method
63
Ni, RAM & IBSS, PC
63
Ni, SSM, PS (1 223 1 422 K)
64
Ni, SIMS, SC (1 004 1 259 K)
63
Ni, SSM, PC
63
Ni, SSM

1 423 1 523

Darken equation & velocity equation

[80,81]

&

1 273 1 573
1 143 1 373
1 073 1 473
1 173 1 473
1 173 1 473
1 273 1 473
1 223 1 473
1 323 1 523
1 173 1 373

Ni/NiAl DC, EMPA, BMM


various kinds of DC, EPMA, WF
Ni/Ni3Al DC, AEM and EPMA, BMM
Ni/NiAl DC, AEM and EPMA, SFT
various kinds of DC, AEM and EPMA, SFT
single-phase DC, PC, EMPA, BMM
single-phase DC, PC, EMPA, BMM
Ni/NiAl DC, EPMA, SFT
two-phase DC, EPMA, BMM

[63]
[90]
[67 69]
[70]
[71]
[79]
[91]
[80, 81]
[82]

&

1 007 1 373
1 373 1 673
1 273

114m

In, sectioning & RAM


NiAl/NiAlIn DC, EPMA, Halls method
Mannings equation & intrinsic diffusivities

[92]
[93]
[94]

&

1 273 1 623
1 050 1 630

63

Ni, RAM, PC
Ni, SSM for HTM;
64
Ni, SIMS for LTM; SC
Mannings equation & intrinsic diffusivities

[95]
[96]

[94]

&

1 471 1 770
1 273

DC, markers distribution and Darken equation


intrinsic diffusivities and Darken equation

[97]
[94]

&

1 273 1 573
1 143 1 273
1 223 1 423
1 173 1 473
1 173 1 473
1 072 1 572
1 173 1 373
1 223 1 773
1 473 1 773
1 123 1 423
1 273 1 473

Ni/NiAl DC, EPMA, BMM


layer growth in Al coating/Ni
pack-aluminized Ni/NiAl, EPMA, BMM
Ni/NiAl DC, AEM and EPMA, SFT
various kinds of DC, AEM and EPMA, SFT
single-phase vaporsolid DC, EPMA, BMM
single-phase DC, EPMA, WF
single-phase DC, EPMA, SFT
single-phase DC, EPMA, SFT
packing Al/Ni, EPMA, WF
various kinds of DC, EPMA, SFT

[63]
[98]
[90]
[70]
[71]
[99]
[100]
[101]
[97]
[102, 103]
[94, 104]

&

1 273

Methoda

Phase

DNi

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[70, 71] as well as those from [80, 81] are utilized in the
present assessment. As for the B2 phase, the experimental
Ni tracer diffusion coefficients from Frank et al. [96], as
well as those from Hancock and McDonnell [95] above
1 273 K, are employed in the present assessment, while

63

&
&
^
&

&

&
&
^
^
&
&
&
&

&
&

&

&

&
^
^
^
&
^
&
&
&
&

SC = single crystals; PC = poly-crystals; IBSS = ion-beam sputter-sectioning; SIMS = secondary ion mass spectrometry; RAM = residual activity method; SMM = serial sectioning method; DC = diffusion couples; BMM = BoltzmannMatano method; EPMA = electron probe microanalyzer; AEM = analytical electron microscope; SFT = Sauer & Freise technique; WF = Wagners function;
HTM = high temperature measurement; LTM = low temperature measurement.
Indicates whether the data are used or not used in the atomic mobility assessment: &, used; ^, partly used; &, not used but used to compare with the present assessment.

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

1465

Basic
L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

W 2010 Carl Hanser Verlag, Munich, Germany

4. Results and discussion


The assessment of atomic mobilities for the fcc, L12, and
B2 phases in the NiAl system is conducted phase by phase
by means of the PARROT module [105] in the DICTRA

Table 3. Summary of atomic mobility parameters of Al and Ni in the fcc, L12 and B2 phases obtained in the present work. The parameters from the previous assessments [6, 16, 21 23] are also listed for comparison.a
Phases

Mobility

fcc

Mobility of Al

Parameters
UAl
Al 123 111:6  97:34  T
UAl
Ni
0 AlAl
UNi

Sources
This work

268 381:0  71:04  T


308 067:5 111:52  T

UAl
Al 142 000  72:12  T

[16]

UNi
Al 284 000  59:83  T
0 Al;Ni
UAl 41 300  91:2  T
UAl
Al 126 719  95:08  T
Mobility of Ni

[23]

UNi
Ni 271 377:6  81:79  T

This work

b
UAl
Ni 144 600:0  64:85  T

UAl;Ni
29 571:8
Ni

UNi
Ni 287 000  69:8  T

[16, 22]

UAl
Ni 145 900  64:26  T
0

L12

Mobility of Al

UAl;Ni
113 000 65:5  T
Ni

ord
Qord
AlAlNi 0:0, QAlNiAl 30 350:0
ord
Qord
AlAlNi 220 214  50:98  TQAlNiAl 2 780 4:61  T

Qord
AlAlNiAl

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104], those in Ni-rich region from Shankar and Seigle [90],


as well as the inter-diffusion coefficients measured by Kim
and Chang [100] except for those around stoichiometric
composition, are included in the present assessment of
atomic mobilities in B2 phase.

Mobility of Ni

475 293,

Qord
AlAlNiNi

This work
[21]c

435 391

ord
Qord
NiAlNi 0:0, QNiNiAl 55 441:9

Qord
NiAlNi 674 704 42:63  T

This work
[21]c

Qord
NiNiAl 101 347  3:12  T
ord
Qord
NiAlNiAl 222 275, QNiAlNiNi 612 177

B2

Mobility of Al

ord
Qord
AlAlNi QAlNiAl 350 911:2

Qord
AlAlVa
Qord
AlNiVa

Qord
AlVaAl
Qord
AlVaNi

365 062:0
0:0

ord
Qord
AlAlNi QAlNiAl 359 700

Qord
AlAlVa
Qord
AlNiVa
Mobility of Ni

Qord
AlVaAl
Qord
AlVaNi

Qord
NiVaAl
Qord
NiVaNi

0:0

a
b
c

Qord
NiVaAl
Qord
NiVaNi

This work

335 668:5
0:0

ord
Qord
NiAlNi QNiNiAl 314 400

Qord
NiAlVa
Qord
NiNiVa

[6]

1 071 200

ord
Qord
NiAlNi QNiNiAl 329 521:7

Qord
NiAlVa
Qord
NiNiVa

This work

[6]

107 000
0:0

In J (mole-atoms) 1; temperature (T) in Kelvin.


Indicate that this mobility is directly taken from Du et al. [73].
ord
ord
ord
c 0 Al
c 0 Al
c 0 Ni
c 0 Ni
Qord
AlAlNiAl , QAlAlNiNi , QNiAlNiAl , QNiAlNiNi correspond to the interactive parameters D QAl;Ni:Al , D QAl;Ni:Ni , D QAl;Ni:Al , D QAl;Ni:Ni
in Ref. [21], respectively.

1466

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Basic

L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

The assessment of the atomic mobilities


for fcc phase

Ni
and
U
started with the two end-members UAl
Al
Ni on the basis of the experimental self-diffusion coefficients of Al and
Ni, as listed in Table 1. Then the end-member, UAl
Ni , corresponding to the impurity diffusivity of Ni in Al was taken
directly from a recent work by Du et al. [73]. The remaining
end-member, UNi
Al , was optimized with the experimental
data on the impurity diffusivity of Al in Ni [57, 59]. Allison
and Samelsons data [58] were not used in the present as-

sessment because considerable grain boundary diffusion


had been observed in their samples. The interaction parameters in the mobility description were then assessed by
using the experimental inter-diffusion data in Table 1. The
finally obtained mobility parameters for the fcc phase are
listed in Table 3.
Figure 1a d presents the calculated self-diffusion coefficients of Al and Ni, and impurity diffusion coefficients of
Al in fcc Ni and Ni in fcc Al along with the corresponding
experimental data [24 30, 38 61], respectively. The
previous assessment results from Engstrm and gren
[16], Jnsson [22] and Cui et al. [23], as well as those from
the most recent first-principles calculations by Mantina
et al. [106, 107], are also plotted in Fig. 1 for comparison.

(a)

(b)

(c)

(d)

software based on all the literature data critically reviewed


in Section 3.

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4.1. Atomic mobility of disordered fcc phase

Fig. 1. Calculated self-diffusion coefficients of (a) Al, (b) Ni, impurity diffusion coefficients of (c) Al in fcc Ni and (d) Ni in fcc Al, compared with
the corresponding experimental data [24 30, 38 61], the previous assessments from Engstrm and gren [16], Jnsson [22], and Cui et al. [23] as
well as those from the most recent first-principles calculations by Mantina et al. [106, 107].

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

As shown in Fig. 1a, the calculated Al self-diffusion coefficients due to the present work and Cui et al. [23] can noticeably reproduce more experimental data than Engstrm and
gren [16]. But in order to characterize which assessment
is statistically better between the present work and Cui et al.
[23] for Al as well as between the present work and Jnsson
[22] for Ni, the coefficient of determination (R2) are then
employed. R2 is a statistical measure of how well the regression line approximates the real data points, and an R2
of 1.0 indicates that the regression line perfectly fits the
data. In general, all the experimental data are included in
the calculation of R2 except that those from Kalinovich
et al. [50] are not used for Ni because they show noticeable
deviations from all the other data, shown in Fig. 1b. The
calculated R2 from the present work and Cui et al. [23] for
Al are 0.99711 and 0.99030, while those of the present
work and Jnsson [22] for Ni are 0.99068 and 0.98466.
The calculations on R2 indicate that the presently obtained
self-diffusion parameters for Al and Ni are both statistically
better than the previous assessments [22, 23]. It is noteworthy that our calculated self-diffusion coefficients of Al
are nearly the same as those from first-principles calculations by Mantina et al. [106]. Moreover, the presently obtained Al and Ni self-diffusion coefficients have been successfully applied in establishing the atomic mobility
database of the AlCu [108] and NiPt [109] systems. The
comparisons between the measured inter-diffusion coefficients [57, 62 72] and the calculated ones from the present
work and Engstrm and gren [16] are shown in Fig. 2.
Both assessments can describe most of the experimental
data, and are close to each other. In comparison with the
previous assessment [16], more experimental data are considered in the present work. Furthermore, the present evalu-

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Basic

Fig. 2. Comparisons between the measured inter-diffusion coefficients


[57, 62 72] and the calculated ones from the present work and Engstrm and gren [16].

1468

ation utilizes one less parameter, compared with the previous work [16].
4.2. Atomic mobilities of ordered L12 and B2 phases
ord
According to Eqs. (7 9), four end-members, Qord
AlAlNi , QAlNiAl ,
ord
ord
QNiAlNi and QNiNiAl , can be used to describe the order contribution to the activation energy in the L12 phase. Since the diffusion in L12 phase occurs via jumps between two different
sublattices, these contributions are not symmetric, as pointed
out by Campbell [20, 21]. Therefore, no similar simplification
ord
in B2 phase, like Qord
AAB QABA , can be made for the endmembers in L12 phase. However, the selection of parameters
can be made on the basis of different considerations. From a
thermodynamic point of view, it is easy to know that
yNi ybAl  yAl ybNi for Ni3Al since antisite defect concentrations
are very small in the ordered state. This means that the contributions for the Al : Ni configuration could be negligible
ord
provided the corresponding parameters, Qord
AlAlNi and QNiAlNi ,
are not exceptionally large. Furthermore, the homogeneity
range of L12 phase is very narrow [31]. Such a small homogeneity prevents a large number of parameters to be optimized in a meaningful way. Consequently, only Qord
AlNiAl and
Qord
NiNiAl were chosen for the optimization in a preliminary assessment. Firstly, Qord
NiNiAl was determined on the basis of the
experimentally measured Ni tracer diffusion coefficients in
L12 phase [85, 86, 88, 89], as well as those above 1 173 K
[75, 87]. The parameter was then temporarily fixed. Next,
Qord
AlNiAl was assessed by employing the critically reviewed
inter-diffusion coefficients [70, 71, 80, 81]. Finally, Qord
AlNiAl
and Qord
NiNiAl were optimized simultaneously. It was found that
ord
two parameters, Qord
AlNiAl and QNiNiAl , were enough to reproduce all the reliable experimental information. As for the
B2 phase, the assessment procedure in the present work is
the same as those of Helander and gren [6] and Campbell
[20, 21], and thus not described here. In order to make the
mobilities of A2 phase physically reasonable, the mobilities
of A2 phase proposed by Helander and gren [6] were directly employed in the present work according to Liu and
Liang [19]. Table 3 lists all mobility parameters for the L12
and B2 phases.
Figure 3a and b shows the calculated tracer diffusion
coefficients of Ni in L12 phase compared with the experimental data from Refs. [74, 75, 85 89]. The assessment results from Campbell [21] are also superimposed in the plots
for comparison. As shown in Fig. 3a and b, the present results yield more or less the same fit to the experimental data
as those of Campbell [21] although only 2 parameters were
employed in the present work, comparing with 12 parameters by Campbell [21], who also considered the Al tracer
diffusion coefficients in her assessment. In addition, the
model-predicted tracer diffusion coefficients of Al in L12
phase are presented in Fig. 3c and d along with the experimental data from indirect methods [74 84], which were
not used in the present assessment. This plot can be used
to check the reliability of those Al tracer diffusion coefficients measured with indirect methods [74 84]. As can be
seen in Fig. 3c and d, the predicted Al tracer diffusion coefficients based on the presently obtained parameters agree
with those data from indirect measurements [74 84] to a
certain degree, indicating that those data can give a good estimation of the real Al tracer diffusion coefficients. The calculated inter-diffusion coefficients of L12 phase at 1 373,

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

1 423, 1 473 and 1 523 K from the present work and Campbell [21] are compared with the experimental data [63,
67 71, 79 82, 90, 91] in Fig. 4a. It can be seen that more
experimental data can be reproduced by the present work.
The extrapolations from high temperatures into low temperatures based on the assessed atomic mobilities are made

in Fig. 4b, where the model-predicted inter-diffusion coefficients at 1 173 and 1 273 K are compared with the corresponding experimental data [63, 67 71, 79, 82, 90, 91].
As can be seen, the presently calculated inter-diffusion
coefficients agree more or less with the measured ones in
single- and two-phase diffusion couples, but deviate greatly

(a)

(b)

(c)

(d)

Fig. 3. (a) and (b) Calculated tracer diffusion coefficients of Ni in L12 phase compared with the experimental data from [74, 75, 85 89]; (c) and (d)
Model-predicted tracer diffusion coefficients of Al in L12 phase along with the experimental data from indirect methods [74 84]. The previous assessment from Campbell [21] is also appended.

(a)

(b)

Fig. 4. Calculated inter-diffusion coefficients of L12 phase at (a) 1 373, 1 423, 1 473 and 1 523 K, and (b) 1 173 and 1 273 K are compared with the
experimental data [63, 67 71, 79 81, 90, 91] and the previous assessment [21].

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

from those in three-phase diffusion couples. This may be


due to the contribution of grain boundary diffusion to the
formation and diffusion process of c phase in the c / B2
three-phase diffusion couples being comparable to the volume diffusion at temperatures below 1 273 K, and this effect becomes bigger as the temperature decreases according
to Fig. 4b.
Similarly, the calculated Ni and the model-predicted Al
tracer diffusion coefficients in B2 phase are compared with
the corresponding experimental data [92 96] in Fig. 5a d,
respectively. As can be seen in Fig. 5a and b, the presently
calculated Ni tracer diffusion coefficients show a preference to the experimental data from Frank et al. [96] over a
wide temperature range by means of single-crystal alloys,
while the previous assessments [6, 21] prefer to those at
high temperatures from Hancock and McDonnell [95] by
means of poly-crystal alloys. It should be noted that at
the time when Helander and gren [6] performed the assessment only the experimental data from Hancock and
McDonnell [95] were available. The purpose of Fig. 5c
and d is the same as that of Fig. 3c and d, i. e. to check the
reliability of those Al tracer diffusion coefficients measured
via indirect methods [92 94]. Figure 6 shows the calculated inter-diffusion coefficients in the B2 phase along with
the experimental data from [63, 70, 71, 90, 94, 101 104]. It
can be found that the assessments from the present work

To further validate the presently obtained atomic mobilities


of fcc, L12 and B2 phases, comparisons between the calculated and the measured concentration profiles in a series of
single- and multi-phase diffusion couples were performed.
Figure 8a d shows the model-predicted concentration profiles of Ni-8 at.% Al / Ni (c / c), Al / Ni (gas / c), Ni-23.1 at.%
Al / Ni-6.6 at.% Al (c / c) and Ni-48 at.% Al / Ni-54 at.% Al
(B2 / B2) diffusion couples along with the corresponding
experimental ones [64, 66, 79, 100], respectively. The detailed annealing conditions can be found in each plot. In
Fig. 8a, we assumed that two equal c regions each with a

(a)

(b)

(c)

(d)

and Campbell [21] yield almost the same fit to the experimental data, but better than those from Helander and gren
[6]. Again, it should be noted that some recently experimental data, like those from Paul et al. [94, 104], who took
the effect of molar volume into account, were not available
when Helander and gren [6] conducted an assessment.
The comparisons between the experimental intrinsic diffusion coefficients [97, 104] and the calculated ones from
the present work and the previous assessments [6, 21] are
presented in Fig. 7. As can be seen, our results provide the
best fit to the experimental data from Paul et al. [94, 104].
4.3. Simulation of diffusion growth in various diffusion
couples

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Basic

Fig. 5. (a) and (b) Calculated tracer diffusion coefficients of Ni in B2 phase compared with the experimental data from [94 96]; (c) and (d) Modelpredicted tracer diffusion coefficients of Al in B2 phase along with the experimental data from indirect methods [92 94]. The previous assessments
from Helander and gren [6] and Campbell [21] are also appended.

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Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Basic

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

100 lm thickness form the diffusion couple, and a double


geometric grid was employed to define a higher density of
points at the interface. The compositions were defined by
the Ni-8 at.% Al / Ni end members in the mole fraction of

Al using the heavy-side function. For the vapor/solid diffusion couple, Al / Ni (gas Al / c), Yamamoto et al. [64] obtained the experimental data based on two assumptions.
One is that Al concentration in the surface coincides almost

(a)

(a)

(b)

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(b)

(c)
Fig. 6. Calculated inter-diffusion coefficients in the B2 phase (a) along
xAl = 0.38; (b) at 1 173, 1 273, 1 373, 1 473, 1 573, 1 673 and 1 773 K;
(c) at 1 123, 1 223, 1 323, 1 423 and 1 623 K, compared with the corresponding experimental data [63, 70, 71, 90, 94, 101 104], and the previous assessments [6, 21].

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

(c)
Fig. 7. Calculated (a) intrinsic diffusion coefficients rate and intrinsic
diffusion coefficients of (b) Ni and (c) Al in the B2 phase compared with
the experimental data [94, 97, 104] and the previous assessments [6, 21].

1471

L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

with the solubility limit of fcc phase (Ni-rich) in the NiAl


phase diagram, while the other is that the change in molar
volume of fcc phase shows a linear increase with Al concentration, i. e. from 6.586 10 6 m3 mol 1 for pure Ni to
9.995 10 6 m3 mol 1 for pure Al. The above two assumptions were directly adopted in the present simulation to reproduce their experimental results, as shown in Fig. 8b.
The vapor/solid diffusion couple was simulated assuming
single c region with a total 250 lm thickness, and pure Ni
as initial composition. A geometric grid was utilized to set
a higher density of points at the lower side of the diffusion
couple. In accordance with the assumption from Yamamoto
et al. [64] that Al concentration in the surface coincides almost with the solubility limit of fcc-Ni, we fixed the composition at the lower side as 19.2 at.% Al as a boundary
condition over the entire simulation process. For the c / c
diffusion couple shown in Fig. 8c, it consists of one c
region with a 80 lm thickness and another one with a
85 lm thickness. A double geometric grid was employed
to define a higher density of points at the interface, and the
compositions were defined by Heaviside step functions
using the equilibrium site fractions corresponding to the
Ni-23.1 at.% Al / Ni-6.6 at.% Al end members. The same
method as that used for the c / c diffusion couple was also
used to define the simulation condition for the B2/B2 diffusion couple in Fig. 8d except for different couple thicknesses and different compositions. As shown in Fig. 8, all
the model-predicted concentration profiles in various single-phase diffusion couples agree well with the corresponding experimental data.
The comparisons between the calculated concentration
profiles in multi-phase diffusion couples, i. e. Ni-25 at.%
Al / Ni (c / c) and Ni-45 at.% Al / Ni (B2 / c) annealed at

1 173 and 1 473 K, and the experimental ones [63, 68, 69]
are presented in Fig. 9. The c / c diffusion couple in Fig. 9a
was assumed to be made up of one c region with a 70 lm
thickness and another c region with a 90 lm thickness. Each
region has a geometric grid with a higher density of grid
points at the interface. The initial compositions for the two
end-members are represented by the equilibrium site fractions corresponding to 25 and 0 at.% Al, respectively. The
c / c diffusion couple in Fig. 9b was also defined in the similar way as Fig. 9a, but with different region thicknesses. As
for the B2 / c diffusion couple in Fig. 9c, the simulation assumed that one c region with a thickness of 500 lm and another B2 region with a thickness of 800 lm form the diffusion couple, and each region has a geometric grid with a
higher density of grid points at the interface. The initial
end-member compositions are 45 and 0 at.% Al. The compositions are converted into site fractions during the simulation.
The c phase was assumed to be active, and added with a very
thin layer (i. e. 1 lm) at the B2 / c interface. The initial composition of c phase was assumed to be 25 at.% Al, and defined in site fractions. As can be seen in Fig 9, again, all the
model-predicted concentration profiles in various multiphase diffusion couples agree reasonably with the corresponding experimental data. Consequently, the plots in Figs.
8 and 9 clearly indicate that the presently obtained atomic
mobilities of Al and Ni in fcc, L12 and B2 phases are reliable.

5. Conclusions
.

all the related experimental data over the entire temperature range, the self-diffusion parameters for pure
Ni and Al were both updated in the present work. The
comparisons of the coefficient of determination (R2) be-

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Basic

Fig. 8. Model-predicted concentration profiles of (a) solid / solid Ni-8 at.% Al / Ni, (b)
vapor / solid Al / Ni, (c) solid / solid Ni23.1 at.% Al / Ni-26.6 at.% Al and (d) solid /
solid Ni-8 at.% Al / Ni-54 at.% Al diffusion
couples along with the corresponding experimental ones [64, 66, 79, 100].

1472

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Basic

Fig. 9. Comparisons between the calculated


and measured [63, 68, 69] concentration profiles in multi-phase diffusion couples: (a) solid / solid Ni-25 at.% Al / pure Ni at 1 173 K,
(b) solid / solid Ni-25 at.% Al / pure Ni at
1 173 K, and (c) Ni-45 at.% Al / pure Ni annealed at 1 173 and 1 473 K.

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

tween the present work and the previous assessments


[16, 22, 23] clearly indicate that the present assessments
for pure Ni and Al are both statistically better;
On the basis of the phenomenological model proposed
by Helander and gren [6], atomic mobilities in fcc,
L12 and B2 solid phases were reassessed by taking into
account all the reliable experimental data via DICTRA
software. An effective strategy was successfully utilized in the present work to select parameters of ordered contributions, resulting in a dramatic decrease
in parameter usage for the L12 phase. Comprehensive
comparisons between various experimental diffusivities and the presently calculated results, as well as between the previous assessments [6, 16, 21] and the
present assessment, were also made for fcc, L12 and
B2 phases in the present work;
The present mobility descriptions were validated by comparing calculated and measured concentration profiles of
a variety of diffusion couples. Moreover, the time-dependent Al composition profile for the annealed vapor Al
gas / c couple is accurately described in the present work.

The financial support from the Chinesisch-Deutsches Zentrum fr Wissenschaftsfrderung (Grant No. GZ522), the Creative Research Group
of National Natural Science Foundation of China (Grant No. 50721003)
and the Key Program of the National Natural Science Foundation of China (Grant No. 50831007) is acknowledged. One of the authors (Yong Du)
acknowledges Cheung Kong Chair Professorship released by Minister of
Education of China for financial support. The authors would also like to
express their thanks to Dr. Anders Engstrm from the Thermo-Calc Software AB in Sweden for helping us with his valuable calculations. Special
thanks are given to Dr. C.E. Campbell from National Institute of Standards and Technology, USA for her kind communication with her most
recent database, and sharing with the literature on self-diffusion coefficient fore pure Ni.

Int. J. Mat. Res. (formerly Z. Metallkd.) 101 (2010) 12

Appendices
While this manuscript was under review, we were discussing with Dr. C. E. Campbell from NIST, USA about establishment of a reference database for the self-diffusion mobilities in pure materials. She kindly provided us with some
missing literature for Ni self-diffusion coefficients [110
116]. In order to check the reliability of the presently obtained Ni self-diffusion parameters, we compared those experimental self-diffusion coefficients [110 116] with the
presently calculated ones, as shown in Fig. 10. It was found

Fig. 10. Calculated self-diffusion coefficients of Ni compared with the


experimental data [110116] provided by Dr. C.E. Campbell from
NIST, USA.

1473

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L. Zhang et al.: Atomic mobilities and diffusivities in the fcc, L12 and B2 phases of the NiAl system

that the current parameters can describe those experimental


data [110 116] very well though they were not used in our
previous assessment, indicating that the present Ni self-diffusion parameters should be reliable.
Moreover, a statistical analysis was also performed between the present work and Jnssons assessment [22] by
taking into account all the experimental self-diffusion coefficients of pure Ni except those from Kalinovich et al. [50],
which show noticeable deviations from the other data [39
50, 52 56, 110 116]. The calculated coefficient of determination, i. e. R2, for the present work and Jnssons assessment [22] are 0.99019 and 0.98566, respectively. It also
suggests that the present work is statistically better than
Jnssons assessment [22].
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(Received September 9, 2009; accepted September 10, 2010)


Bibliography
DOI 10.3139/146.110428
Int. J. Mat. Res. (formerly Z. Metallkd.)
101 (2010) 12; page 1461 1475
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State Key Laboratory of Powder Metallurgy
Central South University, Changsha, Hunan 410083, P. R. China
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