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ISSN 1063-7761, Journal of Experimental and Theoretical Physics, 2019, Vol. 129, No. 2, pp. 258–276.

© Pleiades Publishing, Inc., 2019.


Russian Text © The Author(s), 2019, published in Zhurnal Eksperimental’noi i Teoreticheskoi Fiziki, 2019, Vol. 156, No. 2, pp. 310–330.

ORDER, DISORDER, AND PHASE TRANSITION


IN CONDENSED SYSTEM

Magnetic and Superconducting Properties of the Heterogeneous


Layered Structures V/Fe0.7V0.3/V/Fe0.7V0.3/Nb and
Nb/Ni0.65(0.81)Cu0.35(0.19)
V. D. Zhaketova, Yu. V. Nikitenkoa,*, Yu. N. Khaidukovb, O. V. Skryabinac,
A. Csikd, M. M. Borisove, E. Kh. Mukhamedzhanove, S. N. Vdovichevf,
E. I. Litvinenkoa, A. V. Petrenkoa, and A. V. Churakova
a Joint
Institute for Nuclear Research, Dubna, Moscow oblast, 141980 Russia
b
Skobeltsyn Institute of Nuclear Physics, Moscow State University, Moscow, 119992 Russia
c
Institute of Solid State Physics, Russian Academy of Sciences, Chernogolovka, Moscow oblast, 142432 Russia
d Institute for Nuclear Research, Hungarian Academy of Sciences, Debrecen, H-4026 Hungary
e Russian Research Centre Kurchatov Institute, Moscow, 123182 Russia
f Institute for Physics of Microstructures, Russian Academy of Sciences, Nizhny Novgorod, 603087 Russia

*e-mail: nikiten@nf.jinr.ru
Received December 3, 2018; revised February 1, 2019; accepted February 14, 2019

Abstract—The heterogeneous ferromagnetic–superconducting layered heterostructures


V/Fe0.7V0.3/V/Fe0.7V0.3/Nb and Nb/Ni0.65(0.81)Cu0.35(0.19), which contain magnetic clusters and ferromag-
netic domains, are studied. The magnetic and superconducting properties of the structures depend on the
magnetic-layer thickness, the magnetic field, and the time elapsed from structure preparation. We detected
the interaction of clusters with a domain structure, diamagnetism and magnetization reversal of the magnetic
layer during the superconducting transition in a ferromagnetic–superconducting heterostructure, and a
superconducting transition in the magnetic layer. The magnetic and resistive properties of the heterostruc-
tures changed in several weeks and months.

DOI: 10.1134/S1063776119070136

1. INTRODUCTION sists in the determination of the spatial magnetic and


A number of new phenomena caused by the inter- superconducting profiles of the entire structure as
action of ferromagnetic and superconducting order functions of external parameters. To determine the
parameters have been predicted for ferromagnetic– spatial magnetization vector profile of a layered struc-
superconducting (FS) layered heterostructures. These ture, researchers use nanometer-resolved reflectome-
are cryptoferromagnetism [1–6], the inverse proxim- try of polarized neutrons [15].
ity effect [7–9], a spontaneous vortex phase [10–12],
and triplet superconductivity [13, 14]. These phenom- The authors of [16, 17] noted that the characteris-
ena were detected and studied in many experimental tics of FS structures change substantially in time,
works, which usually applied macroscopic methods, which hinders their experimental investigation and
such as the measurement of the magnetic moment and further application. Therefore, it is important to deter-
the resistance of a structure. The interaction of ferro- mine the time-induced changes of a structure and to
magnetism and superconductivity manifests itself in a reveal the causes of time instability. The purpose of
simultaneous change in the magnetic and supercon- this work is to study FS structures of various composi-
ducting properties of contacting ferromagnetic and tions by various experimental techniques in several
superconducting layers. The interface between the months and to compare their characteristics. As a
layers in real structures is rather long and comparable result, we revealed significant changes in magnetic
with the ferromagnetic and superconducting coherent and nuclear spatial profiles across a structure, a mag-
lengths. Therefore, the properties of the region in the netic structure in the plane of the magnetic layer, the
vicinity of the interface change along with changes in critical superconducting transition temperature (STT)
the properties of contacting ferromagnetic and super- of the structure and its magnetic layer, and the resis-
conducting layers. Hence, the problem mainly con- tance of the structure.

258
MAGNETIC AND SUPERCONDUCTING PROPERTIES 259

Concentration, % bium boundary is 20 nm. The magnetic layer (two FeV


Nb Si layers and V layer between them) has a thickness of
100 V 20 nm, which is larger than the thickness calculated
from the amounts of the deposited elements by a factor
of 6.3. As a result of mutual penetration of the ele-
Fe ments, the layer of iron atoms turn out to be addition-
Ta
10 O ally diluted by niobium and vanadium atoms by 14
times, so that the iron atom content is 7% within the
C spatial distribution width. As a result, the structure
consists of an inhomogeneous diluted ferromagnet
H surrounded by superconducting niobium and vana-
1
dium layers.

0.1 2.2. Synchrotron Measurements


0 50 100 150 200 250 300 350 Synchrotron radiation scattering intensity I(Q) at
z, nm
glancing angle θ was approximated by the relationship
[21–23]
Fig. 1. (Color online) Depth profile of the
V/FeV/V/FeV/Nb structure: coordinate z = 0 corresponds N (Qy ,G1, R1, B1, P1, R2, G2, B2, P2, C )
to the structure surface. −P1
 
 
2. INVESTIGATION OF THE STRUCTURE
Ta(20 nm)/V(150 nm)/Fe0.7V0.3(1 nm)/ 3 (
= G1 exp − 1 R12Qy2 + B1  ) Qy
 Qy R1 3 

V(1.2 nm)/Fe0.7V0.3(1 nm)/Nb(150 nm)/Si  erf   


  6  
The results of studying the Ta(20 nm)/
V(150 nm)/Fe0.7V0.3(1 nm)/V(1.2 nm)/Fe0.7V0.3(1 nm)/ ( ) (
× exp − 1 R22Qy2 + G2 exp − 1 R22Qy2
3 3 )
Nb(150 nm)/Si structure (for brevity, V/FeV/V/FeV/ −P3
 
Nb) were presented in [18, 19]. Here, we present some  
new data. The structure was prepared at the Helm-  Qy  + C.
+ B2
holtz center (Berlin, Germany). To prepare the struc-  Qy R2 3 
ture, we deposited Fe0.7V0.3, V, and Fe0.7V0.3 layers  erf   
sequentially onto a 150-nm-thick niobium layer in the   6  
amount that corresponds to a layer thickness of 1, 1.2, Figure 2 shows the experimental (black) and calcu-
and 1 nm at the density of the bulk material. A vana- lated (red) dependences of the synchrotron radiation
dium 150-nm-thick layer was then deposited, and a scattering intensity for a wavelength of 1.4 Å and a
20-nm-thick tantalum layer was finally deposited to glancing angle θ = 10 mrad on transferred wavevector
prevent oxidation of the structure. Qy directed in the structure plane normal to an inci-
dent beam. At the given glancing angle, radiation
2.1. Spatial Profile reaches the magnetic layer and is scattered by its struc-
tural heterogeneities. As a result of fitting the calcula-
Figure 1 shows the spatial profile of the tion to the experimental data, the following values
V/FeV/V/FeV/Nb structure measured by neutral- were obtained: R1 = 11 nm, R2 = 4.7, P1 = 1, and P2 =
atom mass spectrometry at a spatial resolution of 1 nm 3. Parameter 2R2 = 9.4 nm is identified with the cluster
[20]. As is seen from these curves, the two Fe0.7V0.3 diameter along axis y (normal to incident beam in the
magnetic layers are unresolved and form one layer. sample plane). Parameter 2R1 = 22 nm is the linear
Nevertheless, neutron investigations demonstrate that size of a cluster system.
the magnetic structure consists of two separate mag-
netic moments.
2.3. Magnetic Measurements
The boundaries of the niobium and vanadium lay-
ers have the depth that is close to the magnetic layer Figure 3 shows the temperature dependences of the
thickness, and the boundary depth increases with the zero-field cooled (ZFC) and field-cooled (FC, H =
distance from the silicon substrate. For example, the 20 Oe) magnetic moments. It is seen that, in contrast
depth of the boundary with niobium that is nearest to to the transition in vanadium, the superconducting
the substrate, which is determined as the distance at transition in the niobium layer substantially changes
which the element concentration changes in the range the magnetic moment of the structure. At T = 8 K
50–100%, is 10 nm, and the depth of the farthest nio- (which is higher than Tc), the magnetic moment is

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


260 ZHAKETOV et al.

I, s−1 M × 106, CGS units


0
105
–1

104 –2

–3
M × 106, CGS units
103 –4 10
2
–5 5
2 1
0
102 –6
1 –5
–7 –10
0 2 4 6 8 10
101 0.1 1 T, K
–8
Qy, nm−1 40 80 120 160 200 240 280
T, K
Fig. 2. (Color online) Experimental (black) and calculated Fig. 3. (Color online) Temperature dependence of the
(red) dependences of the synchrotron radiation scattering magnetic moment of the V/FeV/V/FeV/Nb structure tL =
intensity for θ = 10 mrad. 33 months after structure preparation under (1) ZFC and
(2) FC (H = 20 Oe) conditions.

only created by the magnetic layer: the ZFC magnetic σm = σs = 1 at T < Tc. Then, the magnetic moment of
moment is Mm(ZFC, 8 K) = –7.2 × 10–6 CGS units. the magnetic layer is Mm(ZFC, 6 K) = 0 and the
This magnetic moment corresponds to a magnetic change in the moment during the transition is ΔMm =
induction Bm(8 K) = 180 G for a 20-nm-thick mag- 7.2 × 10–6 CGS units. The diamagnetic moment of the
netic layer and to 1.8 kG for two iron layers of a total superconducting layer is Ms(ZFC, 6 K) = 0.
nominal thickness of 2 nm. The ZFC magnetic
moment of the structure at T = 6 K, which is lower In the third case, we assume that the ferromagnetic
than Tc, is Mst (ZFC, 6 K) ≈ 0. At T < Tc, the magnetic layer is not superconducting and σs = 1; as a result, we
moment of the structure Mst is the sum of the magnetic have Mm(ZFC, 6 K) = –Ms(ZFC, 6 K) = 2.8 × 10–6 CGS
moments of the magnetic layer (Mm) and the super- units and ΔMm = 10 × 10–6 CGS units.
conducting layer (Ms). The following condition should
be met because of the diamagnetism of the supercon- Obviously, the first and second cases do not take
ducting layers to an applied magnetic field and the place. The third case, where the magnetic moments of
diamagnetism to the moment of the ferromagnetic the superconducting and magnetic layers change, is
layer: most probable. The results of FC measurements make it
possible to understand what happens. In the FC mea-
M st (ZFC,6 K) = M m(ZFC,6 K) + M s (ZFC,6 K) surements, we have Mst(FC, 6 K) = 6.2 × 10–6 CGS
= M m(ZFC,8 K)(1 − σmε) − HVs σ s = 0. units = –Mm(FC, 8 K). If the magnetic flux in the
superconducting layer is assumed to be frozen in the
Here, σm(s) = 0–1 is the diamagnetism of the magnetic FC mode because of pinning and to be not rejected
(superconducting) layer; ε is the fraction of the mag- during the superconducting transition, the magnetic
netic layer, which becomes superconducting because moment of the magnetic layer turns out to be reversed
of the proximity effect; and Vs is the superconducting at the critical temperature and to remain its absolute
layer volume. value. As will be seen further from neutron data, both
We now consider the case where the moment of the the total moment and the oppositely directed moment
magnetic layer does not change (ΔMm = 0). Then, the of the domain structure are reversed. This behavior of
moment of the superconducting layer should be para- the magnetic moment can be explained if we take into
magnetic with respect to a magnetic field and be account that the magnetic moment of the magnetic
layer is mainly determined by clusters. During the
Ms(ZFC, 6 K) = 7.2 × 10–6 CGS units. Note that the
transition, clusters pass from the state opposite to a
maximum diamagnetic moment of the superconduct- field to the state along a field as a result of a magnetic
ing layer to a field H = 20 Oe is 2.8 × 10–6 CGS units. perturbation. The system of magnetic moments of
We consider the second case, where the entire clusters is known to have two minima in the energy of
magnetic layer becomes superconducting (ε = 1) and interaction of the clusters with a magnetic field, and

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 261

M × 106, CGS units of this interaction also follows from the data of neu-
10 tron relaxation measurements [19], where correlation
2
was detected between the behavior of the magnetic
moments of clusters and the density of domain walls.
9
It also follows from the data in Fig. 3 that the tem-
1 perature of merging the FC and ZFC dependences
8
(blocking temperature) is Tb(20 Oe) = 150 K. Further,
7 we will use Tb to determine the magnetization of mag-
M × 106, CGS units netic clusters.
6 0
2 Figure 4 shows the temperature dependences of the
–400 magnetic moment in a field of 1 kOe. The FC magnetic
5
1
moment at T = 10 K > Tc is seen to be 9.5 × 10–6 CGS
–800 units. It could be thought that this is the saturated
4 –1200 moment in such a high field. However, the data
2 4 6 8 obtained in a field of 100 Oe, where the moment is
T, K
3 higher, cannot be explained on this assumption.
40 80 120 160 200 240 280 Therefore, we have to assume that the moment in a
T, K field of 1 kOe is oriented at a certain angle to magnetic
field direction. This assumption has a double substan-
Fig. 4. (Color online) Temperature dependence of the tiation. First, the too high moment in the ZFC super-
magnetic moment of the V/FeV/V/FeV/Nb structure conducting state can be explained in this case. This
under (1) ZFC and (2) FC (H = 1 kOe) conditions at tL = moment is explained by the appearance of an addi-
33 months. tional diamagnetic moment to the perpendicular com-
ponent of the scattered magnetic field of the magnetic
layer magnetization. Second, as will be shown below,
they are determined by the angles between the direc- the magnetic moment of the ferromagnetic layer in
tions of the magnetic moments and a field, which dif- Nb/CuNi structures is oriented at an angle close to
fer from each other by angle π [24]. 90° in a magnetic field of 5 kOe.
If a finite diamagnetic moment appears in the super- We now consider the data of measurements in a
conducting layer in the ZFC mode, the magnetic layer magnetic field of 100 Oe (Fig. 5). Moment Mst(ZFC,
should be additionally magnetized by 2.8 × 10–6 CGS 6 K) = –24 × 10–6 CGS units appears in the ZFC
units. The additional ZFC magnetization is likely to be superconducting state. If we assume that the moment
related to the fact that a magnetic field under ZFC
conditions is applied at T < Tc and a magnetic field of the magnetic layer (–6.5 × 10–6 CGS units) exist-
ing at T = 8 K does not change, the diamagnetic
under FC conditions is applied at T = 300 K. The moment of the superconducting layer is Ms(6 K) =
problem also concerns the mechanism of changing the
orientations of the moments. For example, this change ‒17.5 × 10–6 CGS units, which is close to the calcu-
can be explained by the fact that the cluster-surround- lated maximum value (Ms, max = –14 × 10–6 CGS
ing medium with domains is superconducting. In this units). The excess of the experimental value over the
case, the magnetic field at clusters that is scattered by calculated one can be related to the accuracy of loca-
a diamagnetic moment would be along an applied tion of the structure with respect to the magnetic field
magnetic field. direction [25, 26]. The FC magnetic moment at T =
Thus, the ZFC and FC experimental data indicate 8 K is 9 × 10–6 CGS units and increases to 20 ×
that the magnetic moment of the magnetic layer 10‒6 CGS units at T = 6 K. The positive change in the
changes in both direction and the absolute value magnetic moment (11 × 10–6 CGS units) is compara-
during the superconducting transition. ble with the maximum diamagnetic moment (14 ×
10‒6 CGS units), and it cannot be associated with the
The problem of the diamagnetism of the magnetic appearing magnetic moment of the superconducting
layer in a residual magnetic field H ≈ 1 Oe near the layer [27]. Therefore, we have to assume that the fer-
STT at T > Tc is important. This diamagnetism is romagnetic layer is magnetized during the supercon-
assumed to be related to the interaction of a system of ducting transition.
clusters with ferromagnetic domains, which create a
local magnetic field at clusters that is opposite to an We now estimate the magnetic moment and the
applied magnetic field. This interaction is supported magnetization of clusters. The authors of [28, 29]
by the fact that the moments of the clusters and the derived the following relation between blocking tem-
moment of the domain structure are opposite to each perature Tb(H) and the magnetic field:
other and simultaneously change their directions
during the superconducting transition. The presence Tb (H ) = Tb (0)(1 − H /H c )m, (1)

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


262 ZHAKETOV et al.

M × 106, CGS units Ny ×10−6


10 180 5.0
2 160 4.5
140 4.0
5 3.5
120
M × 106, CGS units 3.0
1 40 100 2.5
0 20 2.0
2 80
0 1.5
60
1.0
–5 –20 40
1 0.5
–40
0 2 4 6 8 10 40 60 80 100 120 140 160 180
T, K
Nz
–10
40 80 120 160 200 240 280
T, K Fig. 6. (Color online) Neutron scattering intensity for the
V/FeV/V/FeV/Nb structure detected on the plane (Ny,
Fig. 5. (Color online) Temperature dependence of the Nz), which is perpendicular to a horizontal neutron beam,
magnetic moment of the V/FeV/V/FeV/Nb structure for polarization P0 = +1 and neutron wavelength λ =
under (1) ZFC and (2) FC (H = 100 Oe) conditions at tL = 3.8 Å. Here, Ny and Nz are the spatial channel numbers
33 months. along y and z, respectively.

where Tb(0) = kV/25kB, Hc = 2k/Jcl, k = HcJcl/2 is the pictures in the plane normal to a neutron beam for the
crystalline anisotropy constant, V is the cluster vol- V/FeV/V/FeV/Nb structure in a magnetic field of
ume, kB = 1.38 × 10–16 erg/K is the Boltzmann con- 1 kOe at a temperature of 10 K. Magnetic domains are
stant, Jcl is the saturation magnetization of the cluster, along the magnetic field. These intensity pictures are
and m = 2 for a relatively low field. caused by magnetic structures with characteristic sizes
Using Eq. (1), we find Hc at m = 2, L1, 2, 3 = 6.5, 21, and 57 nm [18, 19]. L1 = 6.5 nm is the
interplanar spacing in the cluster lattice. The first
H c = (H1 − ηH 2 )/(1 − η), (2) (Ny = 140, Nz = 130), third (Ny = 90, Nz = 95; Ny =
where η = (Tb(H1)/Tb(H2))1/2. 110, Nz = 55; Ny = 60, Nz = 120), and fifth (Ny = 15,
For magnetization, we have Nz = 35) orders of reflection from the lattice are clearly
visible. This interplanar spacing (L1 = 6.5 nm) can be
J cl = 2k /H c = 50kBTb (0)/(VH c ). (3) used to estimate the intercluster distance (9.3 ±
Using the cluster diameter (9.4 nm) determined 0.3 nm), which indicates a close cluster packing.
from synchrotron measurements, we obtain Hc = Recall that the cluster diameter determined from syn-
0.9 kOe, Tb(0) = 183.5 K, and Jcl = 2.35 ± 0.2 kG, chrotron scattering data is 9.4 ± 0.2 nm. Parameter
L2 = 21 nm is close to 2R2 = 22 nm obtained from syn-
which corresponds to the magnetization of a 2-nm-
thick Fe0.7V0.3 layer (2.25 ± 0.1 kG) determined by chrotron scattering. Parameter L3 = 57 nm was only
magnetic measurements within the limits of experi- determined by neutron scattering and is a parameter of
mental error. a purely magnetic structure, which is likely to be the
domain wall thickness. In a low magnetic field H =
25 Oe at T = 10 K, the magnetic moments of clusters
2.4. Neutron Measurements are opposite to the magnetic field direction. The total
magnetic moment measured by a SQUID magnetom-
As synchrotron radiation scattering, neutron scat- eter is directed identically (Fig. 3). Therefore, the
tering can be used to determine the parameters of scat- magnetization is mainly determined by clusters rather
tering objects from the dependence of the scattering than the magnetic medium surrounding them [18].
intensity on the transferred momentum. However, the
use of neutrons is limited because of a low neutron Low-temperature neutron measurements have
beam intensity as compared to synchrotron radiation. been performed for 3.5 years. The first measurements
On the other hand, neutrons are irreplaceable in were carried out 3 months after sample preparation.
studying magnetic (ferromagnetic walls) and nuclear– Figure 8 displays the results of these measurements,
magnetic (clusters) objects due to their magnetic namely, the temperature dependence of the scattering
moment. Figures 6 and 7 show the neutron scattering coefficient S(T) = 1 – (R(T) + Tr(T))/(R(150 K) +

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 263

Ny ×10−6 S
180 0.7
4.5 S
0.6
160 4.0 0.6 P0 = −1
0.4
140 3.5 0.5 +1 0.2 17 Oe, P0 = +1
120 3.0 17 Oe
0.4 0 2 4 6 8 10 12
2.5 T, K
100
2.0 0.3
80 9.5 kOe
1.5
0.2
60
1.0
40 0.1 +1
0.5
40 60 80 100 120 140 160 180 0
Nz 1 10 100 1000
T, K

Fig. 7. (Color online) Neutron scattering intensity for the


V/FeV/V/FeV/Nb structure detected on the plane Fig. 8. (Color online) Temperature dependence of the
(Ny, Nz), which is perpendicular to a horizontal neutron neutron scattering coefficient S(T) for the
V/FeV/V/FeV/Nb structure at tL = 3 months for H = 17 Oe
beam, for polarization P0 = –1 and neutron wavelength
and 9.5 kOe.
λ = 3.8 Å.

Tr(150 K)) of polarized neutrons with a wavelength perature because of a decrease in the domain wall
λ = 1.28 ± 0.015 Å (scattering at T = 150 K is zero), density and the disordering of the magnetic moments
where R and Tr are the neutron reflection and trans- of clusters [18]. A comparison of Figs. 8–10 demon-
mission coefficients, respectively. strates that, in time, the scattering intensity decreases
At T = 8 K, the neutron scattering is maximal (55– threefold within 15 months and almost vanishes in
59%) and the polarization of scattered neutrons is the following 2 years. This behavior demonstrates
negative (–0.035). The neutron scattering intensity at that the clusters degrade in time and the magnetic
H = 17 Oe and T = 8 K (Fig. 8) in comparison with
that at H = 5 kOe and T = 300 K increased sevenfold layer becomes more homogeneous.
and the magnetization increased only by a factor of
1.5. Note that the nonzero polarization of scattered
S
neutrons is determined by the magnetization of clus- 0.24
ters with respect to the magnetization of the cluster- 3
surrounding medium. Therefore, the negative polar-
ization at T = 8 K points to the fact that the magnetic 0.20
moments of clusters are opposite to a magnetic field.
The magnetic moment of the surrounding medium 0.16
undergoes reorientation simultaneously with the 2
reorientation of the magnetic moments of clusters
during the superconducting transition, which is indi- 0.12
cated by the spin asymmetry of specular neutron
reflection SR(T) = (R+ – R–)/(R+ + R–) presented in 0.08
1
Fig. 11 for a temperature of (1) 8 and (2) 3 K. Here, the
moments of the clusters and the surrounding 0.04
medium are opposite to each other. When tempera-
ture decreases to 1.5 K, the magnetization (moment 0
along the magnetic field direction) of the clusters 1 10 100 1000
decreases in absolute value, the magnetization of the T, K
surrounding medium increases, and the total magne-
tization of the magnetic layer decreases. The Fig. 9. (Color online) Temperature dependence of the
decrease in the magnetization of the magnetic layer neutron scattering coefficient S(T) for the
with decreasing temperature below Tc ref lects the V/FeV/V/FeV/Nb structure at tL = 1.5 months: magnetic
action of superconductivity. Simultaneously, the states at (1) H = 17 Oe, (2) H = 17 Oe after preliminary
neutron scattering decreases with decreasing tem- magnetization in a field of 2 kOe, and (3) H = 1 kOe.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


264 ZHAKETOV et al.

S SR
0.05 0.2
5
0.04
6
0.03 0.1 1

0.02 3
4 0
0.01

0 –0.1 2
1
–0.01 2

1 2 3 4 5 6 7 8 9 10 11 12 –0.2
1 2 3 4 5 6 7
T, K
λ, Å
Fig. 10. (Color online) Temperature dependence of the neu-
tron scattering coefficient S(T) for the V/FeV/V/FeV/Nb
structure at tL = 3.5 years for H = 28 Oe: (1) λ = 2 ± 0.2 Å, Fig. 11. (Color online) Spin asymmetry of reflection
P0 = +1; (2) λ = 2 ± 0.2 Å, P0 = –1; (3) λ = 4.6 ± 0.46 Å, SR(T) = (R+ – R–)/(R+ + R–) for a temperature of (1) 8
P0 = +1; (4) λ = 4.6 ± 0.46 Å, P0 = –1; (5) λ = 7.2 ± 0.72 Å, and (2) 3 K.
P0 = +1; and (6) λ = 7.2 ± 0.72 Å, P0 = –1.

3. STUDY OF THE STRUCTURES Table 1 gives the layer parameters for the structures
Nb(70 nm)/Ni0.65Cu0.35(4 nm)/Si V/FeV/V/FeV/Nb, Nb/Ni0.65Cu0.35, and
AND Nb(70 nm)/Ni0.81Cu0.19(h)/Si, h = 2, 3, 4 nm Nb/Ni0.81Cu0.19 at various times after their fabrication.
These structures were prepared by magnetron sput- As follows from Table 1, the change in the copper
tering in the Institute for Physics of Microstructures and nickel layer thicknesses is maximal for the
and the sputtering technique was described in detail in
[17]. From here on, we will designate these structures Nb/Ni0.81Cu0.19(2) structure, where the magnetic layer
as Nb/Ni0.65Cu0.35(4) and Nb/Ni0.81Cu0.19(h), where is thinnest. The magnetic layer thickness increased by
h = 2, 3, 4 is the Ni0.81Cu0.19 layer thickness in nano- 69% for copper and by 80% for nickel within half a
meters. year after structure preparation. Simultaneously, the
decrease in the copper and nickel concentrations at

3.1. Spatial Profiles


Concentration, %
Figures 12 and 13 show the spatial profiles of the 100
Nb/Ni0.65Cu0.35(4) structure measured by neutral Nb
mass spectrometry (NMS) at various times. The
structure elements are seen to penetrate each other
significantly. The niobium and silicon content is sig-
nificant (30% in total) even at the center of the distri-
bution of Ni and Cu, which make up the ferromag-
netic layer of a calculated thickness of 4 nm. Nine 10 Ni
months after preparation, the copper and nickel pro- Si
files are seen to become asymmetric with respect to O Cu
each other, and the copper profile moves toward the C Si
niobium layer more strongly (Fig. 12). Half a year
later, the nickel and copper distributions changed
again (Fig. 13). For example, the magnetic layer thick- 1
ness increased from 6.5 nm by 35% to 8.8 nm (Fig. 12). 0 20 40 60 80 100
As compared to nickel, copper diffused toward the z, nm
niobium layer more strongly. As a result, a 1.5-nm-
thick layer of a niobium–copper solution and a 5-nm- Fig. 12. (Color online) Depth profiles of the elements in
thick layer of a nickel–silicon solution formed. the Nb/Ni0.65Cu0.35(4) structure at tL = 9 months.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 265

Concentration, % R, Ω
100 101
Nb

100

3
10–1
10 2
Si Ni
O Cu 10–2
C Si
10–3
1
1
0 20 40 60 80 100
z, nm 10–4
4 5 6 7 8 9
T, K
Fig. 13. (Color online) Depth profiles of the elements in
the Nb/Ni0.65Cu0.35(4) structure at tL = 15 months. Fig. 14. (Color online) Temperature dependence of the
electrical resistance of the Nb/Ni0.81Cu0.19(4) structure at
H = 0: (1) two weeks after structure preparation, (2) one
the center of the magnetic layer in this structure is month after preparation, and (3) two months after prepa-
maximal (30%). ration.

3.2. Resistance Measurements Nb/Ni0.81Cu0.19(4) structure in the absence of a mag-


Low-temperature resistance measurements were netic field (H = 0) at various values of tL. Critical tem-
carried out in a He-4 cryostat using the four-probe perature Tc is seen to change substantially in time: Tc is
method in the Institute of Solid State Physics. A 8.4 K for the as-prepared structure, 8.2 K after two
Keithley 6220 precision power supply was used as a weeks, 7.5 K, after a month, and only 6.85 K after two
source of current passing through a structure, and a months. The change in the critical temperature in two
Keithley 2182 nanovoltmeter was used to measure the months was 18.5%. Apart from Tc, the resistance also
voltage. The temperature was measured with a therm-
change at temperatures both above and below Tc, and
istor located under a sample.
the ratio ρ = R(T > Tc)/R(T < Tc) changed from 10 4 to
In time, the critical STT decreases because of the
separation of nickel and copper and an increase in the 101 within two months. Since the rate of change of Tc
magnetization. Figure 14 shows the temperature and ρ is higher than the rate of change of the spatial
dependences of the resistance of the profiles in the structure (Figs. 12, 13), the change in Tc

Table 1. Layer parameters in various structures


C1CuNi, C2CuNi,
Structure H1Cu, nm H2Cu, nm H2Cu/H1Cu H1Ni, nm H2Ni, nm H2Ni/H1Ni C1CuNi/C2CuNi
% %

V/FeV/V/FeV/Nb 20 (FeV) 7(Fe)


Nb/Ni0.65Cu0.35(4) 6.4 8.4 1.31 8 9.1 1.14 40 35 0.88
Nb/Ni0.81Cu0.19(2) 2.9 4.9 1.69 3.0 5.4 1.8 70.5 49.1 0.7
Nb/Ni0.81Cu0.19(3) 3.9 4.8 1.23 4.3 5.2 1.21 69.8 65.6 0.94
Nb/Ni0.81Cu0.19(4) 5.9 6.4 1.085 6.1 5.8 0.95 70.9 62.8 0.89
V/FeV/V/FeV/Nb (tL = 18 months), Nb/Ni0.65Cu0.35 (subscript 1, tL = 9 months; subscript 2, tL = 15 months), Nb/Ni0.81Cu0.19 (sub-
script 1, tL = 2 weeks, subscript 2, tL = 6 months). H1Cu(Ni) and H2Cu(Ni) are the Cu(Ni) layer thickness for the first and second time,
respectively; C1CuNi and C2CuNi are the total copper and nickel concentrations at the center of the magnetic layer at the first and second
time, respectively.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


266 ZHAKETOV et al.

R, Ω R, Ω
101 5
1

2, 3 4
100
2, 3
3 5 4 1 3 2
10–1
2

10–2
1

10–3 0
4 5 6 7 8 9 6 7 8 9 10
T, K T, K
Fig. 16. (Color online) Temperature dependences of the
Fig. 15. (Color online) Temperature dependence of the electrical resistances of the structure (1)
electrical resistance of the Nb/Ni0.81Cu0.19(4) structure at Nb/Ni0.81Cu0.19(4), (2) Nb/Ni0.81Cu0.19(3), and (3)
H = 100 Oe: (1) two weeks after structure preparation, (2) Nb/Ni0.81Cu0.19(2) two weeks after structure preparation
one month after preparation, and (3) two months after and the structure Nb/Ni0.81Cu0.19(2) one month after
preparation. Tc = 6.85 K. preparation at H = (4) 0 and (5) 100 Oe.

and ρ is assumed to be caused by a change in the het- 3.3. Synchrotron Measurements


erogeneous magnetic structure in the layer plane.
The Nb/Ni0.81Cu0.19(h) structure is characterized
Figure 15 depicts the temperature dependences of by three size parameters R1, R2, and R3. In this case,
resistance in a magnetic field H = 100 Oe. As follows
from a comparison of Tc at H = 0 and 100 Oe, the fer- the dependence of the radiation scattering intensity on
transferred wavevector Qy can be written as follows
romagnetic layer magnetized by a magnetic field
decreases Tc of the structure by 0.65 K in comparison [21–23]:
with the demagnetized layer. As time, a magnetic field N (Qy ,G1, R1, B1, P1, R2, G2, B2, P2, R3, G3, B3, P3, C )
is seen to decrease Tc. In time, a fraction of pure −P1
nickel, the magnetization of which is higher than that  
 
( )
of a nickel–copper solution, was found to form. Thus, Qy
the change in Tc in both cases is likely to be caused by
1
= G1 exp − R1 Qy + B1
2 2  
3  Qy R1 3 
the magnetization.  erf   
Figure 16 displays the temperature dependences   6  
of resistance for structures with various magnetic-
layer thicknesses. The STT of the as-prepared struc- ( )
× exp − 1 R2 Qy + G2 exp − 1 R2 Qy
3
2 2

3
2 2
( )
tures (curves 1–3) is seen to decrease with increasing −P2
magnetic-layer thickness. For example, this tem-  
 
( )
perature of the Nb/Ni0.81Cu0.19(4) structure is lower
Qy
+ B2   exp − 1 R3 Qy
2 2
than that of the Nb/Ni0.81Cu0.19(3) and
Nb/Ni0.81Cu0.19(2) structures (8.52 K) by 0.3 K. The  Qy R2 3  3
STT of Nb/Ni0.81Cu0.19(2) at H = 0 decreased by  erf   
  6  
0.64 K one month after preparation. −P2
 
For comparison, the decrease in the STT of the  
Nb/Ni0.81Cu0.19(4) structure at H = 0 in two weeks was
almost the same, 0.73 K. One month after prepara-
1
(
+ G3 exp − R3 Qy B3
3
2 2 
) Qy
 Qy R3 3 
 + C.
tion, the STT of Nb/Ni0.81Cu0.19(2) in a magnetic field  erf   
of 100 Oe was lower than that at H = 0 by 0.96 K.   6  
Thus, the STT was found to depend on the mag- Figures 17 and 18 show the dependences of the syn-
netic-layer thickness, the magnetic field, and the time chrotron radiation scattering intensity of the
elapsed from structure preparation. Nb/Ni0.81Cu0.19(2) structure at glancing angles θ = 5

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 267

I, s–1 I, s–1
103 101

102
100

101

10–1
100

10–1 –2 10–2 –2
10 10–1 100 101 10 10–1 100 101
Qy, nm–1 Qy, nm–1

Fig. 17. (Color online) Experimental (black) and calcu- Fig. 18. (Color online) Experimental (black) and calcu-
lated (red) dependences of the synchrotron radiation scat- lated (red) dependences of the synchrotron radiation scat-
tering intensity for the Nb/Ni0.81Cu0.19(2) structure at θ = tering intensity for the Nb/Ni0.81Cu0.19(2) structure at θ =
5 mrad. The parameters obtained upon fitting the experi- 10 mrad. The parameters obtained upon fitting the exper-
mental data are as follows: G1 = 500, R1 = 100, B1 = 0.06, imental data are as follows: G1 = 10, R1 = 100, B1 = 0.03,
P1 = 2, G2 = 5, R2 = 5.1, B2 = 0, P2 = 0, G3 = 3, R3 = 2, P1 = 1, G2 = 0.8, R2 = 5.7, B2 = 0, P2 = 0, G3 = 0.3, R3 =
B3 = 2.1, P3 = 1.2, and C = 0.028. 4, B3 = 0.015, P3 = 3, and C = 0.028.

and 10 mrad and fitting curves, which well describe Parameter 2R1 significantly exceeds parameter 2R2.
the experimental data. At θ = 5 mrad, total specular This parameter is the linear fractal size for the
reflection from the niobium layer preceding the mag- Nb/Ni0.81Cu0.19(4) and Nb/Ni0.81Cu0.19(2) structures
netic layer takes place (radiation penetration depth is and is the linear size of a structure of randomly located
1 nm), and the scattering at 10 mrad is mainly deter- clusters for the Nb/Ni0.81Cu0.19(3) structure.
mined by the magnetic layer (radiation penetration
depth is 100 nm). As a result, the dependence is
smooth at θ = 5 mrad and is quasi-periodic at θ = 3.4. Magnetic Moment at H = 0
10 mrad. Figure 19 displays the temperature dependences of
Table 2 gives the parameters obtained by fitting the the magnetic moment of the Nb/Ni0.65Cu0.35(4) struc-
calculated data to the experimental results. The ele- ture in the absence of magnetic field. At T = 10 K, the
mentary cluster size is R3 = 3–4 nm. Structures of moment is negative, 3.5 × 10–6 CGS units. During the
clusters of characteristic size R2 were also observed. superconducting transition (Tc = 6 K) and the first

Table 2. Structure parameters obtained from the synchrotron radiation scattering intensity for various structures
V/FeV/V/FeV/Nb Nb/Ni0.65Cu0.35(4) Nb/Ni0.81Cu0.19(4) NB/Ni0.81Cu0.19(3) Nb/Ni0.81Cu0.19(2)

R1 – – 65 65 100
R2 11 9 5 5.3 5.7
R3 4.7 3.3 3 4 4
P1 – – 1.3 – 1
P2 1 1.3 4 – –
P3 3 2.9 3 3 3
V/FeV/V/FeV/Nb at tL = 22 months, Ni0.65Cu0.35 at tL = 3 months, and Ni0.81Cu0.19 at tL = 5 months.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


268 ZHAKETOV et al.

M × 106, CGS units M × 106, CGS units


15 20
4
1 2
3 0
10
3 M × 106, CGS units
2 20
1 4
–20 2
0
5 1
–20

–40 –40
0 –60 3
0 5 10 15 20 25
–60 T, K
–5
0 50 100 150 0 25 50 75 100 125 150
T, K T, K

Fig. 19. (Color online) Temperature dependence of the Fig. 20. (Color online) Temperature dependence of the
magnetic moment of the Nb/Ni0.65Cu0.35(4) structure at magnetic moment of the Nb/Ni0.65Cu0.35(4) structure at
H = 0 and tL = 7 months: (1) first cooling from T = 300 K tL = 3 months upon cooling under (1, 3) ZFC and (2, 4)
(black), (2) heating after cooling to T = 3 K < Tc (red), and FC conditions at H = (1, 2) 20 and (3, 4) 100 Oe.
(3) second cooling after heating (blue).

cooling (curve 1), the absolute value of the magnetic value) negative magnetic moment. As a result, the
moment changes threefold and becomes M1(T < Tc) = magnetic moment becomes stable, decreasing from
11 × 10–6 CGS units (Bm = 1390 G at a layer thickness 11 × 10–6 CGS units to 7 × 10–6 CGS units and
of 4 nm). This large change in the moment cannot be remaining positive. Upon repeated cooling (curve 3)
explained by the electrodynamic effect [30]. The to the minimum temperature, the moment becomes
entire magnetic layer is thought to be superconduct- almost equal to the moment having appeared upon the
ing. We now trace how the change in the magnetiza- first cooling (curve 1).
tion can be explained in this case. The magnetic field Similar behavior of the magnetic moment was
of the superconducting current that appears as a reac- observed in other structures. Table 3 gives the mag-
tion to the negative magnetic moment of the layer is netic moments of the Ni0.65Cu0.35 and Ni0.81Cu0.19
directed in the positive direction, and this field mag- structures at H = 0.
netizes the magnetic layer. As a result, the absolute
value of the magnetic moment exceeds the value As follows from Table 3, the magnetization of the
before the transition. In turn (see Fig. 14), an increase structure increases in absolute value with the mag-
in the magnetization degrades the superconducting netic-layer thickness at both T > Tc and T < Tc. As the
properties of the magnetic layer; as a result, the dia- Ni0.81Cu0.19 magnetic-layer thickness, the relative
magnetic moment to the new positive moment is change in the magnetic moment during the transition
smaller than in the first case of a smaller (in absolute increases, which is related to the fact that, when the

Table 3. Magnetic moment of the magnetic layer in the Ni0.65Cu0.35 and Ni0.81Cu0.19 structures at H = 0 for T > Tc and T < Tc
and saturation moment Msat
Magnetic-layer M(T > Tc), M(T < Tc), Msat,
Structure ΔM/M (T > Tc), %
thickness, nm 10–6 CGS units 10–6 CGS units 10–6 CGS units

Nb/Ni0.65Cu0.35(4) 6.5 −3.5 11 214 6 (H = 100 Oe)


Nb/Ni0.81Cu0.19(2) 2.95 −1.5 4 167 6.5
Nb/Ni0.81Cu0.19(3) 4.1 −6 8 33 9
Nb/Ni0.81Cu0.19(4) 6 −12 18 50 18

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 269

M × 106, CGS units layer is assumed to unchanged during the supercon-


2 ducting transition, the ratio of the field-induced
changes in the moment of the superconducting layer
during transition is ηs = ΔM2/ΔM1 = (63 – 3)/(14.5 –
1 4) = 5.7. However, ηs cannot be larger than H2/H1 = 5.
Therefore, the moment of the magnetic layer changes
0 during the transition. Moments M1 and M2 are seen to
be almost equal to moment M(H = 0, 10 K), which is
M × 106, CGS units
–1 50 reversed during the transition and becomes 7 ×
2 1 10‒6 CGS units. Assuming that the magnetic moment
25 is reversed and becomes 7 × 10–6 CGS units (as in the
–2 2
case H = 0), we find the ratio of the diamagnetic
0 moments of the superconducting layer ηs = (63 +
1 7)/(14.5 + 7) = 3.25, which is an allowed value. ηs will
–3
–25 be even lower if the magnetic layer is magnetized in a
0 5 10 15 20 25
–4
T, K magnetic field. Thus, in a magnetic field of 20–
20 40 60 80 100 120 140 100 Oe, the magnetic layer also undergoes magnetiza-
T, K tion reversal during the ZFC superconducting transi-
tion. Under the FC conditions, the moment is positive
Fig. 21. (Color online) Temperature dependence of the
at both T > Tc and T < Tc, as in the V/FeV/V/FeV/Nb
magnetic moment of the Nb/Ni0.65Cu0.35(4) structure structure. The ZFC and FC dependences are inter-
upon cooling under (1) ZFC and (2) FC conditions for sected in a field of H = 20 Oe at T = 40 K and in a field
H = 20 Oe at tL = 7 months. of 100 Oe at T = 25 K, which indicates the presence of
magnetic clusters in the magnetic layer, as in the
V/FeV/V/FeV/Nb structure.
magnetic-layer thickness decreases, the layer becomes Figure 21 shows the (1) ZFC and (2) FC tempera-
more strongly demagnetized at T > Tc. ture dependences of the magnetic moment of the
Ni0.65Cu0.35(4) structure in a magnetic field H = 20 Oe
that were obtained later, at tL = 7 months. Tc is seen to
3.5. Magnetic Moment at H ≠ 0
remain unchanged as compared to the earlier mea-
Figures 20 and 21 depict the temperature depen- surement. However, the dependences of the magnetic
dences of the magnetic moment of the Nb/Ni0.65Cu0.35 moment changed substantially. For example, at T =
structure upon cooling in a magnetic field of 20 and 10 K, the ZFC magnetic moment changed by a factor
100 Oe (FC) and upon zero-field cooling (ZFC) at of 1.5 in absolute value and the FC magnetic moment
tL = 3 and 7 months. even became negative. At T < Tc, the moment is posi-
The transition at tL = 3 months is seen to occur at a tive for both regimes, increases in absolute value by a
temperature of 8.5 K (Fig. 20; Hall effect measure- factor of 3–10, and the ZFC moment is higher than
ments of the as-prepared structure gave 8.8 K). This the FC moment. The fact that the ZFC moment is
temperature differs from the temperature (6.85 K) higher than the FC moment at T < Tc is likely not be
determined in earlier (tL = 2 months) resistance mea- experimentally observed earlier. Thus, we can state
surements. This difference is likely to be related to dif- that the change in the spatial profile of the structure
ferent contributions of different structural regions to within four months substantially changes its magnetic
the resistance and the magnetic moment. The pres- characteristics.
ence of a standard diamagnetic response to a change in The ZFC and FC dependences at H = 20 Oe merge
the ZFC magnetic moment indicates that the diamag- at a higher temperature (T = 60 K) than in the first
netic moment of the superconducting layer dominates measurements, which points to a decrease in the mag-
over the moment of the magnetic layer. At T = 10 K, netization of clusters. Therefore, we can conclude that
the moment is related to the magnetic layer and is nickel leaves the clusters.
M1(20 Oe, 10 K) = –4 × 10–6 CGS units (induction of Table 4 gives the magnetization of the clusters Jcl
309 G in a 6.5-nm-thick layer) and M2(100 Oe, 10 K) = calculated by Eq. (3) using the blocking temperature at
–3 × 10–6 CGS units under ZFC conditions. The two magnetic fields and the data on the magnetic clus-
magnetic-field dependence of the diamagnetic ter size dm. This table also presents saturation magne-
response is nonlinear. For example, the moment is tization Jlay for a layer of a calculated thickness using
M(20 Oe, 6 K) = –14.5 × 10–6 CGS units in a field the magnetic moment in a high magnetic field at T ≥
H1 = 20 Oe and is M(100 Oe, 6 K) = –63 × 10–6 CGS Tc. Note that the saturation magnetization is Jsol =
units (450 G for 70-nm-thick layer) in a fivefold field 2 kG for the Ni0.65Cu0.35 solution and is 3.75 kG for the
H2 = 100 Oe. If the magnetic moment of the magnetic Ni0.81Cu0.19 solution [31]. The inequality Jcl ≥ Jlay is

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


270 ZHAKETOV et al.

Table 4. Parameters of the clusters in the magnetic layer of the structures


Structure dcl, nm Tb(0), K Hc, kOe Jlay, kG Jcl, kG
Ni0.65Cu0.35(4)
6.6 44.1 0.422 0.75 ± 0.1 3.5 ± 1.0
tL = 1 month
Ni0.81Cu0.19(2)
6 35 0.983 1.6 ± 0.2 1.4 ± 0.5
tL = 4 month
Ni0.81Cu0.19(3)
8 90 0.451 2.2 ± 0.2 4.9 ± 1.5
tL = 4 month
Ni0.81Cu0.19(4)
8 142 0.403 3.0 ± 0.3 10.5 ± 4.0
tL = 4 month
V/FeV/V/FeV/Nb
9.4 183.5 0.9 2.25 ± 0.2 2.35 ± 0.2
tL = 33 month

seen to be met, which indicates that the nickel content Nb/Ni0.81Cu0.19(2) and Nb/Ni0.81Cu0.19(3) structures,
with respect to the cooper content is higher in clusters the ZFC moment at H = 5 kOe is negative at T < Tc,
than in the layer of the calculated thickness. The mag- which points to the fact that the diamagnetic moment
netization of the layer Jlay turns out to be lower than of the superconducting layer is higher than the
that of the solution Jsol and increases with the layer moment of the superconducting layer. First, this find-
thickness. ing is related to the fact that the magnetic moment of
Figures 22–24 show the temperature dependences a thin layer is low in absolute value. Second, in this
of the magnetic moment of the Nb/Ni0.81Cu0.19 struc- case, the diamagnetic moment of the superconducting
tures for a magnetic field H = (1) 25, (2) 150, and (3) layer increases with the magnetic field more strongly
5000 Oe. For comparison, we also present the tem- than the magnetic moment of the magnetic layer. As a
perature dependence at H = 0 (4). For the result, when the magnetic field increases, the diamag-

M × 106, CGS units


M × 106, CGS units
20 10
5

3 80 5 3 M × 106, CGS units


5
10 5
CGS units

60 4 3 20
M × 106,

4 40 3 2 1 3
20 0
0 1 4 –20
–20 –40
0 2 6 10 14 T, K 0 –60 2
7 –80
2 2 4 6 8 10 12 14
2
T, K 1
6 –5
–10 M × 106, CGS units 6, 7
CGS units

1200 6 200 5 7
M × 106,

1 800 7 0
400 –200 6 4
0 –10 –400
–20 2 6 10 14 –600
T, K 2 6 10 14 T, K
50 100 150 200 250 300 50 100 150 200 250 300
T, K T, K

Fig. 22. (Color online) Temperature dependences of the Fig. 23. (Color online) Temperature dependences of the
magnetic moment of the Nb/Ni0.81Cu0.19(4) structure magnetic moment of the Nb/Ni0.81Cu0.19(3) structure
under ZFC and FC conditions 3.5 months after structure under ZFC and FC conditions 3.5 months after structure
preparation: (1) H = 0; (2) ZFC, H = 25 Oe; (3) FC, H = preparation: (1) H = 0; (2) ZFC, H = 25 Oe; (3) FC, H =
25 Oe; (4) ZFC, H = 150 Oe; (5) FC, H = 150 Oe; (6) 25 Oe; (4) ZFC, H = 150 Oe; (5) FC, H = 150 Oe; (6)
ZFC, H = 5 kOe; and (7) FC, H = 5000 Oe. Upper inset: ZFC, H = 5 kOe; and (7) FC, H = 5000 Oe. Upper inset:
(1) H = 0; (2) ZFC, H = 25 Oe; (3) FC, H = 25 Oe; (4) (1) ZFC, H = 0; (2) ZFC, H = 25 Oe; and (3) FC, H =
ZFC, H = 150 Oe; and (5) FC, H = 150 Oe. Lower inset: 25 Oe. Lower inset: (1) ZFC, H = 150 Oe; (2) FC, H =
(1) ZFC, H = 5 kOe; (2) FC, H = 5 kOe. 150 Oe; (3) ZFC, H = 5000 Oe; and (4) FC, H = 5 kOe.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 271

M × 106, CGS units I, s–1


212
5 4 3 5

2
210
0
M × 106, CGS units M × 106, CGS units
1 100 3 1
01 0 5
–100 –800
–5 –200 208 2
–1600 6
–300 2
6 –400 –2400
4
4
2 4 6 8 10 12 14 2 4 6 8 10 12 14
T, K T, K
–10 206
3
20 40 60 80 100 0 40 80 120 160
T, K T, K

Fig. 24. (Color online) Temperature dependences of the Fig. 25. (Color online) Temperature dependences of the
magnetic moment of the Nb/Ni0.81Cu0.19(2) structure neutron intensities I(T) reflected from and transmitted
under ZFC and FC conditions 3.5 months after structure through the Nb/Ni0.81Cu0.19(4) structure under ZFC and
preparation: (1) ZFC, H = 0; (2) ZFC, H = 25 Oe; (3) FC, FC conditions at H = 25 Oe for λ = 2 Å ± 10% at tL =
H = 25 Oe; (4) ZFC, H = 150 Oe; (5) FC, H = 150 Oe; and
(6) ZFC, H = 5 kOe. Left-hand inset: (1) ZFC, H = 0; 3.5 months: (1) ZFC, P0 = +1; (2) ZFC, P0 = –1; (3) FC,
(2) ZFC, H = 25 Oe; (3) FC, H = 25 Oe. Right-hand inset: P0 = +1; and (4) FC, P0 = –1.
(4) ZFC, H = 150 Oe; (5) FC, H = 150 Oe; and (6) ZFC,
H = 5 kOe.
characteristic temperatures at which the ZFC and FC
curves are intersected. The dependences of the posi-
netic moment of the superconducting layer becomes tive and negative neutron polarizations are slightly dif-
higher than the moment of the magnetic layer in abso- ferent, which indicates that neutrons are scattered by
lute value, which eventually leads to a negative total
moment. These data are analogous to the data
obtained for the V/FeV/V/FeV/Nb structure in a mag-
netic field of 1 kOe (Fig 4). The moment of the I, s–1
Nb/Ni0.81Cu0.19(4) and Nb/Ni0.81Cu0.19(3) structures is
lower than that in a magnetic field of 150 Oe by an
order of magnitude. The ZFC and FC dependences 178
coincide, which points to the absence of hysteresis 2
(elastic regime of changing the magnetization). Obvi-
ously, the magnetic moment in this case is normal to a
magnetic field. 176
1
3
3.6. Neutron Measurements
The authors of [32] performed detailed neutron 174
investigations of the magnetic behavior of layered 4
Nb/Ni0.65Cu0.35(4) structure. Here, we present the
results of new studies of the Nb/Ni0.65Cu0.35(4) struc-
172
ture and the Nb/Ni0.81Cu0.19(4) structure. We now 20 40 60 80 100
compare data on the temperature of merging the ZFC T, K
and FC dependences obtained in magnetic and neu-
tron measurements. Figures 25 and 26 show the tem- Fig. 26. (Color online) Temperature dependences of the
perature dependences of the total ZFC and FC inten- neutron intensities I reflected from and transmitted
sities of neutrons I reflected from and transmitted through the Nb/Ni0.81Cu0.19(4) structure under ZFC and
through the Nb/Ni0.81Cu0.19(4) structure. Note that FC conditions at H = 150 Oe for λ = 2 ± 0.2 Å at tL =
the intensity I = I0 – Is is determined by neutron scat- 2 months: (1) ZFC, P0 = +1; (2) ZFC, P0 = –1; (3) FC,
tering intensity Is. The dependences are seen to have P0 = +1; and (4) FC, P0 = –1.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


272 ZHAKETOV et al.

SR I, s–1
0.08
2
152
0.04 3

148
0
1 2
144
–0.04

–0.08 140 1
10 100
T, K 0 2 4 6 8 10
Fig. 27. (Color online) Temperature dependence of the T, K
polarization asymmetry of the specular neutron reflection
from the Nb/Ni0.81Cu0.19(2) structure under (1) ZFC and Fig. 28. (Color online) I(T) for the Nb/Ni0.65Cu0.35(4)
(2) FC conditions in a magnetic field H = 70 Oe. The structure at λ = 2 Å and P0 = +1 in (1) E1, (2) E2, and (3)
blocking temperature is found to be 25 K, which is lower
than the magnetometric value (in contrast to the neutron E3. The errors do not exceed the circle sizes.
scattering data).

both domain walls and nuclear–magnetic clusters. It ments, the contribution of the surface during neutron
is also seen that the polarization dependences of neu- reflection is higher as compared to that of the struc-
tron scattering are different for both the FC and ZFC ture volume. The neutron scattering intensity is also
conditions and two different magnetic fields. In the determined by clusters and domain walls. However,
ZFC mode, the magnetic moments are along a mag- when the magnetic field increases, the neutron scat-
netic field; in the FC mode, the magnetic moments tering is most strongly determined by clusters.
are opposite to a magnetic field. The blocking tem- Figure 28 shows the temperature dependence of
perature is 150 K at H = 25 K (Fig. 25) and 70 K at the total neutron intensity I(T) of the
150 Oe (Fig. 26). These values are higher than the val- Nb/Ni0.65Cu0.35(4) structure beginning from 10 to
ues of 125 and 56 K obtained in the magnetic measure- 1.5 K for three experiments (curves 1–3). In the first
ments by 20–25%. The blocking temperature weakly experiment, a magnetic field of 25 Oe was used at 10 K
depends on the neutron polarization and, hence, is (E1 (1)). In the second experiment at T = 10 K (E2,
mainly determined by the domain wall density. (2)), the structure was magnetized in a field of 500 Oe,
Figure 27 depicts the temperature dependences of a field was changed to 25 Oe, and measurements were
the polarization asymmetry of the ZFC and FC spec- carried out when temperature was changed from 10 to
ular neutron reflections in a magnetic field H = 70 Oe 1.5 K. Curve 3 (E3) was obtained in an experiment
for the Nb/Ni0.81Cu0.19(2) structure. The blocking with a magnetic field of 200 Oe similarly to curve 1. It
temperature was found to be 25 K, which is lower than is seen that, in the temperature range 5–8 K, curve 2 is
that obtained in the magnetometric measurements above curve 1 and curve 3 is above curve 2. This
(29 K) unlike the neutron scattering data. behavior is explained by the fact that the structure in
The neutron and magnetic methods are seen to give experiments E2 and E3 is magnetized. At T = 4 K for
the blocking temperatures that coincide accurate to all experiments and at T = 9 K in experiment E2, the
20–25%. Obviously, the difference between the block- intensity decreases because of neutron scattering by
ing temperatures determined in the magnetic and neu- magnetization fluctuations during the superconduct-
tron measurements is determined by measurable val- ing transition and an increase in the domain wall den-
ues. For example, the magnetic moment that is the sity. At T = 9 K, the transition occurs due to the prox-
sum of the moments of clusters and domains is deter- imity effect in the magnetic layer adjacent to the nio-
mined in the magnetic measurements. The contribu- bium layer; at T = 4 K, the transition takes place
tion of domains to the total moment increases with the throughout the magnetic layer.
magnetic field. The asymmetry of neutron reflection The fact that the superconducting transition takes
is proportional to the magnetization, which in turn is place is also indicated by the fact that, at T = 4 and
proportional to the magnetic moment of the structure. 9 K, the transfer of the momentum of neutrons
However, as compared to the magnetic measure- increases toward an increase in the glancing angle of

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 273

+ +
SR SR
0.10 0.20

0.15
0.05
0.10

0.05
0
0
–0.05 –0.05

–0.10
–0.10
2 3 4 5 6
–0.15
λ, Å 2 3 4 5 6
λ, Å
Fig. 29. Asymmetry of neutron reflection in “plus” spin Fig. 30. Asymmetry of neutron reflection in “plus” spin
state SR+ (5 K, 10 K) for the Ni0.65Cu0.35(4) structure. state SR+ (1.5 K, 10 K) for the Ni0.65Cu0.35(4) structure.

reflected neutrons and a decrease in the glancing angle whole, the scattering increases with decreasing tem-
of refracted neutrons. This behavior is explained by perature. The scattering intensity changes periodi-
inelastic neutron scattering by magnetization fluctua- cally. The scattering is seen to be polarization sensi-
tions. The energy transferred normal to the interfaces tive, i.e., cluster related, only at certain temperatures
is 0.2 neV. It should be noted that the real energy trans- in the temperature ranges 8–8.5 and 3–4 K, where the
fer can be slightly higher because of a 100% inelastic scattering is maximal. Therefore, as for the
scattering probability and momentum transfer toward V/FeV/V/FeV/Nb structure, we can conclude that a
other directions. change in the domain structure leads to the motion of
When the temperature decreases beginning from the magnetic moments of clusters due to a change in
T = 4 K, the asymmetry of specular neutron reflec- the interaction of two systems.
tion,

SR+ (T ,T0 ) = (R + (T ) − R+(T0 ))/(R + (T ) + R+(T0 )) I, s–1


increases in the “plus” spin state (neutron polarization
toward magnetic field vector). Figures 29 and 30 dis-
play the SR+ dependences for T0 = 10 K at H = 25 Oe 315
and T = 5 and 1.5 K, respectively. The increase in the
asymmetry of specular neutron reflection in a fixed
spin state when the temperature decreases demon-
strates the magnetization of the medium surrounding 2
310
clusters increases. However, as follows from Fig. 28,
the neutron scattering by domain walls at T = 1.5 K 1
remains almost unchanged as compared to T = 5 K.
Thus, the action of superconductivity in this case is 305
reduced to the rotation of the magnetic moments of
domains toward the magnetic field direction.
Recall that, in contrast to this structure, the mag-
netization of the surrounding medium in the 2 4 6 8 10
V/FeV/V/FeV/Nb structure increased due to an T, K
increase in the domain size.
Figure 31 shows the temperature dependence of the Fig. 31. (Color online) Temperature dependence of the
neutron scattering coefficient of the neutron intensity for the Nb/Ni0.81Cu0.19(4) structure in a
Nb/Ni0.81Cu0.19(4) structure in a magnetic field of magnetic field of 25 Oe at a neutron wavelength λ = 2 Å
25 Oe toward a decrease in the temperature. On the and polarization P0 = (1) +1 and (2) –1.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


274 ZHAKETOV et al.

SR SR
0.15 0.10

0.10
0.05

0.05

0
0

–0.05 –0.05
1 2 3 4 5 6 1 2 3 4 5 6
λ, Å λ, Å

Fig. 32. Spin asymmetry of reflection SR(T) for the Fig. 33. Spin asymmetry of reflection SR(T) for the
Nb/Ni0.81Cu0.19(4) structure at T = 9 K and H = 25 Oe. Nb/Ni0.81Cu0.19(4) structure at H = 25 Oe and T = 1.5 K.

Figures 32 and 33 depict the spin asymmetry of 150 Oe are different. As follows from the temperature
reflection SR(T) for a temperature of 9 (Fig. 32) and dependences of asymmetry SR(T), the magnetization
1.5 K (Fig. 33). It is seen that SR(1.5 K) ≈ 0.7SR(9 K). of the cluster-surrounding medium decreases in a field
Therefore, the magnetization of the medium sur- of 75 Oe and increases in a field of 150 Oe. Thus, the
rounding clusters decreases by 30% when the tem- behaviors of clusters and domains are different for all
perature decreases from 9 to 1.5 K. As follows from the magnetic fields. The simultaneous decrease in the
data shown in Figs. 32 and 33, the domain size
decreases with decreasing temperature. This behavior magnetization and the increase in the dissociation in a
of the domain structure differs radically from the field of 75 Oe are unusual. The saturation magnetiza-
behavior of the domain structures in tion is likely to decrease in this case as well. It should
V/FeV/V/FeV/Nb and Nb/Ni0.65Cu0.35(4). The mag-
netization decreases beginning from T = 4 K. There-
fore, 4 K is thought to be the STT in the magnetic layer I, s–1
at H = 25 Oe.
Figures 34 and 35 depict the coherent propagation 180
(reflection + transmission) intensity I(T) in a mag-
netic field of 75 and 150 Oe, respectively. In contrast
to a field of 25 Oe, the scattering decreases with
decreasing temperature in a magnetic field of 75 or 178
150 Oe. Obviously, this is related to an increase in the 1
domain size, when the domain wall density decreases
(as in the case of V/FeV/V/FeV/Nb). At T = 2.5 K, the 2
scattering is identical to that at T = 4 K and H = 25 Oe 176
for the Nb/Ni0.65Cu0.35(4) and Nb/Ni0.81Cu0.19(4)
structures. Temperature T = 2.5 K was taken to be the
STT in the magnetic layer at H = 75 and 150 Oe. 174
Polarization-dependent neutron scattering caused by
scattering by clusters is observed in the curves in
Figs. 34 and 35 before T = 2.5 K. As follows from 2 4 6 8 10
Fig. 34, the moments of clusters at H = 75 Oe are T, K
either normal to and along a magnetic field (T = 3.25,
6, 7 K) or opposite to a field (T = 1.75, 4.5, 7.5 K). At Fig. 34. (Color online) Temperature dependence of the
H = 150 Oe, the moments are either normal or oppo- neutron intensity for the Ni0.81Cu0.19(4) structure in a
site to a magnetic field (T = 4.5, 6.5 K). The behaviors magnetic field of 75 Oe at a neutron wavelength λ = 2 Å
of the magnetization of the magnetic layer at 75 and and neutron polarization P0 = (1) +1 and (2) –1.

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


MAGNETIC AND SUPERCONDUCTING PROPERTIES 275

I, s–1 the magnetic field. The superconducting transition in


the structure is accompanied by the magnetization
164
reversal of the magnetic layer and the reverse of its
magnetic moment in a low magnetic field or even in
163
the absence of a field.
1 In time, the clusters degrade, the layers in the
V/FeV/V/FeV/Nb structure become more homoge-
162 neous, and the magnetic and superconducting proper-
ties of the structures change substantially. In time, Ni
and Cu atoms in the Nb/NiCu structures separate in
161 depth to form individual layers. As a result of the sep-
aration of Ni and Cu, the STT in the
2
Nb/Ni0.81Cu0.19(4) structure decreases.
160 The superconducting properties changed rather
rapidly, within one–two weeks after structure prepa-
159 ration, which is likely to be related to a change in the
0 5 10 15 20 heterogeneous structure in the magnetic-layer plane.
T, K The magnetic properties of the structure changed in a
few months, which correlated with the changes in the
Fig. 35. (Color online) Temperature dependence of the
depth profiles of the element concentrations.
neutron intensity for the Ni0.81Cu0.19(4) structure in a
magnetic field of 150 Oe at a neutron wavelength λ = 2 Å ACKNOWLEDGMENTS
and neutron polarization P0 = (1) +1 and (2) –1.
We thank V.L. Aksenov and L.Ya Vinnikov for their help
in the investigations and helpful discussions and
be noted that, at the wavelengths that are longer than a M.V. Avdeeva and A.V. Tomchuk for the useful discussions
critical wavelength (4 Å for H = 25 Oe and 5 Å for H = of the small-angle synchrotron radiation scattering data.
75, 150 Oe), a neutron wave is split in the angle of
reflection, which is caused by neutron transitions REFERENCES
between spin states in a magnetic field because of
magnetic noncollinearity [33]. This process was found 1. P. W. Anderson and H. Suhl, Phys. Rev. 116, 898
to occur near the surface of a structure in a magnetic (1959).
field of a few kilooersteds. This field at the surface of 2. A. I. Buzdin and L. N. Bulaevskii, Sov. Phys. JETP 67,
the niobium layer can only be induced by clusters, the 576 (1988).
magnetic moments of which are either perpendicular 3. F. S. Bergeret, K. B. Efetov, and A. I. Larkin, Phys.
to the interface or oriented at a nonzero angle to the Rev. B 62, 11872 (2000).
interface. 4. A. I. Buzdin, Rev. Mod. Phys. 77, 935 (2005).
5. E. B. Sonin, Phys. Rev. B 66, 100504 (2002).
6. E. B. Sonin and N. A. Logoboy, J. Phys.: Conf. Ser.
4. CONCLUSIONS 150, 052245 (2009).
7. F. S. Bergeret, A. F. Volkov, and K. B. Efetov, Eur.
The main conclusions of studying three types of FS Phys. Lett. 66, 111 (2004).
structures are as follows. Their magnetic layers are 8. F. S. Bergeret and N. Garcia, Phys. Rev. B 70, 052507
structurally heterogeneous. The magnetic properties (2004).
of the structures are determined by magnetic nano- 9. M. Y. Kharitonov, A. F. Volkov, and K. B. Efetov,
clusters, ferromagnetic domains, and the magnetic Phys. Rev. B 73, 054511 (2006).
layer thickness. Clusters and domains interact with 10. T. K. Ng and C. M. Varma, Phys. Rev. Lett. 78, 330
each other. The action of superconductivity on the (1997).
magnetic state of clusters is reduced to changing the 11. E. B. Sonin and I. Felner, Phys. Rev. B 57, R14000
orientations of their magnetic moments. The action of (1998).
superconductivity on a domain structure leads to a 12. S. V. Dubonos, A. K. Geim, K. S. Novoselov, and
change in the direction of the magnetic moments of I. V. Grigorieva, Phys. Rev. B 65, 220513(R) (2002).
domains and a change in their sizes. The magnetic 13. F. S. Bergeret, A. F. Volkov, and K. B. Efetov, Appl.
field determines the STT in a structure and the action Phys. A 89, 599 (2007).
of superconductivity of its magnetic state. A supercon- 14. G. Novak, H. Zabel, et al., Phys. Rev. B 78, 134520
ducting transition in the magnetic layer of the (2008).
Nb/Ni0.65(0.81)Cu0.35(0.19) structures takes place at a 15. Yu. V. Nikitenko and V. G. Syromyatnikov, Reflectome-
temperature below the STT in the superconducting try of Polarized Neutrons (Fizmatlit, Moscow, 2013) [in
layer. The STT in the magnetic layer also depends on Russian].

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019


276 ZHAKETOV et al.

16. P. V. Leksin, A. A. Kamashev, N. N. Garif’yanov, et al., 24. R. Prozorov, Y. Yeshurun, T. Prozorov, and A. Gedan-
in Proceedings of the 20th Symposium on Nanophysics ken, Phys. Rev. B 59, 6956 (1999).
and Nanoelectronics, March 14–18, Nizh. Novgorod, 25. S. Monton, F. de la Cruz, and J. Guimpel, Phys. Rev. B
2016, Vol. 1, p. 77. 75, 064508 (2007).
17. S. N. Vdovichev, Yu. N. Nozdrin, E. E. Pestov, 26. S. W. Han, J. Farmer, H. Kaiser, et al., Phys. Rev. B 62,
P. A. Yunin, and A. V. Samokhvalov, JETP Lett. 104, 9784 (2000).
329 (2016). 27. A. E. Koshelev and A. I. Larkin, Phys. Rev. B 52, 13559
18. V. D. Zhaketov, Yu. V. Nikitenko, F. Radu, A. V. Pet- (1995).
renko, A. Csik, M. M. Borisov, E. Kh. Mukhamedzha- 28. E. P. Wohltarth, J. Phys. 10, 241 (1980).
nov, and V. L. Aksenov, J. Exp. Theor. Phys. 124, 114 29. L. E. Wenger and J. D. Mydosh, Phys. Rev. B 29, 4156
(2017). (1984).
19. V. D. Zhaketov, Yu. V. Nikitenko, A. V. Petrenko, 30. S. Mironov, A. S. Melnikov, and A. Buzdin, Appl.
A. Csik, V. L. Aksenov, and F. Radu, J. Exp. Theor. Phys. Lett. 113, 022601 (2018).
Phys. 125, 480 (2017). 31. C. G. Robbins, H. Claus, and P. A. Beck, Phys. Rev.
20. K. Vad, A. Csik, and G. A. Langer, Spectrosc. Eur. 21, Lett. 22, 1307 (1969).
13 (2009). 32. V. D. Zhaketov, Yu. V. Nikitenko, A. V. Petrenko,
S. N. Vdovichev, A. V. Churakov, and A. Csik, J. Exp.
21. G. Beaucage, J. Appl. Crystallogr. 28, 717 (1995). Theor. Phys. 127, 508 (2018).
22. G. Beaucage, H. K. Kammler, and S. E. Pratsinis, 33. V. L. Aksenov, Yu. V. Nikitenko, and S. V. Kozhevnikov,
J. Appl. Crystallogr. 37, 523 (2004). Phys. B (Amsterdam, Neth.) 297, 94 (2001).
23. C. M. Sorensen and G. C. Roberts, J. Coll. Interf. Sci.
186, 447 (1997). Translated by K. Shakhlevich

JOURNAL OF EXPERIMENTAL AND THEORETICAL PHYSICS Vol. 129 No. 2 2019

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