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Partial fulfillment of the requirement for the award of the degree of Doctor of Philosophy in Physics. A careful review of the literature on CoFeB-based thin films indicates that the magnetic properties of the films are strongly dependent on film thickness.

Prologue Introduction

Prologue

Introduction

This postulation opens the door to new effects and futuristic spintronics devices based on the manipulation and control of the spin degrees of freedom by means of electric and magnetic fields. One of the most important milestones in the young field of spintronics is the discovery of giant magnetoresistance (GMR) in thin-film structure consisting of two ferromagnetic layers separated by a metallic non-magnetic spacer [BAIB1988, BINA1989, REIG2013], which find application in hard disks, where the magnetoresistive (MR) read heads convert information stored in recording media by a small magnetic stray field into electrical signal with a high spatial resolution [WOLF2001, PIRA2007, PIRA2011, MALL2012, HIRO2013].

Figure 1.01: Conceptual diagram of spintronics [ANDO2015].
Figure 1.01: Conceptual diagram of spintronics [ANDO2015].

Motivation behind the work

As can be seen from the literature review, the magnetic properties of the amorphous CoFeB thin films deteriorate as the film thickness increases. To tune the magnetic properties of thick CoFeB films by controlling the development of effective magnetic anisotropy at larger thicknesses, the following methods are generally employed: (i) fabricating multilayer structured thin films with ferromagnetic layers separated by non -magnetic (metallic and non-magnetic) -metallic) layer [NAKA1997, NAOE1998, HUAN2001, NAKA2001, TANA2003, SING2013] and (ii) performing a controlled heat treatment of the amorphous precursor under different annealing environments [HERZ2013, DANI2014].

Objective of the thesis work

A summary of the conclusions of this thesis and a brief description of the future scope of research on these types of materials is presented in Chapter 7. The list of publications resulting from this thesis and other research works is summarized at the end of the thesis.

Fundamental Aspects and Theoretical Modeling

Introduction

Although the history of magnetism is as old as the history of science, the underlying principles and mechanisms that explain the magnetic properties of materials are still complex and mysterious. Therefore, (i) understanding the development of magnetic properties in new materials in new shapes, (ii) tuning the magnetic properties based on thickness, composition and artificially layered structure and (iii) optimizing the magnetic properties for different applications very essential. .

Origin of magnetism

  • Diamagnetism
  • Paramagnetism
  • Ferromagnetism
  • Antiferromagnetism

Some materials have a permanent magnetic moment, which is the result of a strong interaction between magnetic moments even in the absence of an external field. At this point, some magnetic flux remains in the material even at zero magnetic field.

Figure 2.02: Magnetic hysteresis loop of a ferromagnetic material.
Figure 2.02: Magnetic hysteresis loop of a ferromagnetic material.

Intrinsic properties of magnetic materials

  • Exchange Interaction

Some materials follow a structure that results from the coupling of two types of magnetic structures. The origin of the Heisenberg exchange interaction is electrostatic, but the explanation involves quantum mechanics.

Therefore, the electrostatic energy of a system depends on the relative orientation of the spins: the difference in energy determines the exchange energy. The energy of interaction between the atoms i and j carrying the electron spins Si and Sj is defined from the Heisenberg model as [OHAN, where Jij is the exchange integral and related to the overlap of the charge distribution of the.

2.17) Thus, the discrete, pairwise interaction can be replaced by assuming that the magnetic

It is clear from Figure 2.05 that the value of J and thus the short-range exchange interaction strongly depends on the interatomic distance. After treating the Weiss molecular field that TC = C with 𝐶 = 𝑁𝑣𝜇𝑚2𝜇0/3𝑘𝐵, the expression for TC can be obtained from Eq. (2.21) as.

2.23) where a is the distance between the spins, A is called the exchange stiffness constant having

Anisotropy

  • Magnetocrystalline anisotropy
  • Shape anisotropy
  • Induced anisotropy
  • Magnetostrictive anisotropy
  • Magnetic surface anisotropy

If  is positive, applying a tensile stress to the rod creates an easy axis in the direction of the applied stress. When compressive stress is applied, the direction of the easy axis created will be perpendicular to the stress direction.

Figure 2.07: Magnetization of single crystals of iron, nickel and cobalt [HTTP2].
Figure 2.07: Magnetization of single crystals of iron, nickel and cobalt [HTTP2].

Magnetic domains and domain walls

On the other hand, the shape anisotropy dominates over the surface anisotropy above critical thickness, leading to in-plane orientation of the magnetization [PESC1987, GARR2005, YILD20091, YILD20092, HIND2011]. For small Q (< 0.1), the critical thickness for the formation of stripe domains is approximately 𝑡𝑐𝑟𝑖𝑡𝑖𝑐𝑎𝑙 = 2𝜋√𝐴/𝐾 in zero applied field.

Figure 2.13: Comparison of domain wall energies for a (a) Bloch, (b) Néel and (c) Cross-tie  wall  for  a  permalloy  film  as  function  of  film  thickness  [PRUT1964]  and  illustrative  diagrams of the respective domain wall spin configuration
Figure 2.13: Comparison of domain wall energies for a (a) Bloch, (b) Néel and (c) Cross-tie wall for a permalloy film as function of film thickness [PRUT1964] and illustrative diagrams of the respective domain wall spin configuration

Magnetic properties of amorphous and nanocrystalline materials

However, they exhibit low TC due to the lack of long-range ferromagnetic ordering and weak ferromagnetic exchange interaction.

Interlayer coupling in multilayer thin films

  • Exchange coupling
    • Direct exchange coupling
    • Indirect exchange coupling
  • Magnetostatic coupling 1. Topological coupling
    • Stray field coupling
    • Domain wall stray field coupling

Another magnetostatic coupling that arises due to magnetic poles at the edges of the film is stray field coupling. The stray field created by the edges of one magnetic layer magnetostatically couples the other layers as shown in Figure 2.17(a).

Figure 2.17: (a) Schematic drawing of two dominant interlayer coupling mechanisms, and  (b)  variations  of  Néel  coupling  with  spacer  layer  thickness  for  different  multilayer  films  [SCHR2000]
Figure 2.17: (a) Schematic drawing of two dominant interlayer coupling mechanisms, and (b) variations of Néel coupling with spacer layer thickness for different multilayer films [SCHR2000]

Experimental Methods

  • Introduction
  • Techniques used for sample preparation 1. Sputtering technique
  • Their transport in the atmospheric condition to the substrate, and 3. Eventual condensation on the substrate
    • DC sputtering technique
    • Magnetron sputtering technique
    • Calibration of deposition rate
    • Structural property characterization 1. X-ray diffraction
  • ray diffraction (XRD) technique is useful to identify the existence of various phases, degree of crystalline order and quantitative analysis of secondary phases present in a two-

The sputtering yield increases with a) energy, b) mass of the bombarding atoms and c) decrease in angle of attack on the target. To increase the deposition rate and control the thermal stress, magnetron sputtering is used to fabricate the films, as described below in Figure 3.03. The deposition of the films was carried out after stabilizing the plasma and completing the pre-sputtering process.

The deposition rate of the films studied in the present investigations was calibrated using a surface profilometer (Vecco, Dektak-150), as illustrated in Figure 3.05.

Figure 3.01: Schematic diagram of the sputtering process [HTTP3].
Figure 3.01: Schematic diagram of the sputtering process [HTTP3].

CULL2001]

X-ray reflectivity

The period of the interference fringes and the decrease in intensity are related to the thickness and roughness of the layer(s). For incident angles greater than C ( > C) the X-ray beam penetrates the film and therefore reflection occurs at the top and bottom of the film. The interference between the rays reflected from the top and bottom of the film surfaces produces interference fringes.

Plotting 𝜃𝑚2 versus m2 yields a straight line and fitting the experimental data to linear fit provides thickness of the films from the slope and critical angle from the intercept.

Transmission electron microscope

The bright field image is obtained by deliberately excluding all diffracted rays and allowing only the central ray to pass through the specimen. This is done by placing appropriately sized apertures in the back focal plane of the objective lens. Atoms can be identified by analyzing their energies, and the concentration of atoms in the specimen can be determined by counting the number of X-rays emitted.

In the present study, as-deposited films were mechanically polished from substrate side using Gatan Disc grinder to reduce the thickness to 10 m and then thinned using precision ion polishing system (PIPS) to suitable thickness for the TEM observation.

Magnetic property characterization

  • Vibrating sample magnetometer

When a sample is placed in a uniform magnetic field, a dipole moment is induced in the sample proportional to the product of the susceptibility of the sample and the applied field. This signal has an amplitude proportional to the sample's magnetic moment, vibrational amplitude, and vibrational frequency. The exciter vibrates at a frequency of 72 Hz (Lakeshore model 7410) and the signal received by the hall probe and pickup coils is converted to the magnetic moment of the sample.

The oven was flushed with nitrogen gas to avoid oxidation of the sample at high temperature.

Figure 3.11: Schematic diagram of a vibrating sample magnetometer [HTTP6].
Figure 3.11: Schematic diagram of a vibrating sample magnetometer [HTTP6].

Magnetic domain structure analysis 1. MOKE microscope

  • Magnetic force microscope

The heating rate and M–T sequences were programmed using IDEASVSM software. magnetization that is parallel to the plane of the film but perpendicular to the plane of light incidence. As a simple rule, the Kerr rotation is proportional to the component of magnetization parallel to the reflected light beam. The Kerr amplitude is then proportional to the sine of the angle of incidence ϑ, and therefore vanishes for perpendicular incidence.

Additionally, tip shape is important due to the long-range nature of magnetic forces.

Figure 3.14: Schematic drawing of Kerr microscope [HTTP6].
Figure 3.14: Schematic drawing of Kerr microscope [HTTP6].

Thickness dependent properties of single-layer CoFeB

  • Introduction
  • Experimental details
  • Results and discussion 1. Structural properties
    • Magnetic properties
  • Summary

The average size of magnetic domains decreases with increasing Fe content in CoFeB films. Considering thick amorphous CoFeB films, the magnetic anisotropy is expected to be mainly due to magnetoelastic effects caused by the stress induced during the deposition of the films. To study the magnetic properties of the films up to the Curie temperature, high temperature M-T data were measured at a constant applied field of 500.

These results indicate that the low value of TC in the currently investigated films can be correlated with the completely amorphous form of the films [LIUY2008, SAKU2013].

Figure 4.01: Room temperature XRD patterns of 200 nm thick CoFeB442 and CoFeB262  films
Figure 4.01: Room temperature XRD patterns of 200 nm thick CoFeB442 and CoFeB262 films

Magnetic interactions in trilayer structured CoFeB films

  • Introduction
  • Experimental details
  • Results and Discussion 1. Structural properties
    • Magnetic properties
  • Summary

However, symmetric trilayer films with xCr < 1 nm show oscillatory MR/MS behavior. Temperature-dependent M-H loops for symmetric three-layer films with Cr spacer layer (Figure 5.11) reveal that (i) the buckling observed in the first quadrant gradually disappears with decreasing temperature, but the temperature at which the buckling disappears varies with xCr for films with xCr≤ 1, (ii) as xCr > 1 increases, the shape of the loop does not change with temperature, (iii) however, For symmetric three-layer films with Ta spacer layer (Figure 5.12), (i). the shape of the loops does not change with decreasing temperature for all values ​​of xTa.

All symmetric three-layer films (y = 20) show single magnetization reversal process at room temperature (i) with a kink in the first quadrant for films with xCr<1 and (ii).

Figure 5.01: Schematic representation of trilayer [CoFeB262 (y nm) /Cr (x nm) /CoFeB262  (20 nm)] films with (a) y = 20 (symmetric) and (b) y = 100 (asymmetric) along with the  magnetic domain structures
Figure 5.01: Schematic representation of trilayer [CoFeB262 (y nm) /Cr (x nm) /CoFeB262 (20 nm)] films with (a) y = 20 (symmetric) and (b) y = 100 (asymmetric) along with the magnetic domain structures

Tuning magnetic properties of thick CoFeB films by

  • Introduction
  • Experimental details
  • Results and discussion 1. Structural properties
    • Magnetic properties
  • Summary

In order to further explore the possibility of tailoring the magnetic properties of thick CoFeB films with dense The observed changes in the magnetic properties of the trilayer films compared to the monolayer film can be explained based on the nature of the coupling between the CoFeB262 films through the spacer layers. Since the magnetic properties of the films are affected by the measurement temperature, it is very important to understand the change of magnetic interaction and interlayer coupling between CoFeB262 layers in trilayer films as a function of T.

For three-layer films with xCr = 0.75 [see Figure 6.09], (i) with decreasing T, the shape of the loops does not change for y up to 5 nm.

Figure 6.01: Schematic representation of trilayer structured thin films of Substrate/
Figure 6.01: Schematic representation of trilayer structured thin films of Substrate/

Summary and scope for future work

  • Summary of the results
  • Scope for future work

The magnetic properties of CoFeB(t nm) single-layer films revealed a strong thickness dependence in the thickness range between 7 nm and 200 nm. Effects of composition, thickness and temperature on the magnetic properties of amorphous CoFeB thin films. Tuning the magnetic properties of CoFeB thick film by interlayer coupling in three-layer structured thin films.

The role of nanostructure on the magnetic properties of new materials and its application in future magnetoelectronic devices.

Gambar

Figure 2.03: Typical magnetic hysteresis loops of soft and hard ferromagnetic materials
Figure 2.06: Schematic diagram of magnetization, applied field, and easy axis for a given  material
Figure  2.09:  Magnetization  of  a  prolate  ellipsoid  of  revolution  with  c  &gt;  a  and  no  magnetocrystalline anisotropy
Figure 2.11: Schematic drawing of bars to demonstrate inducing an easy-axis in a material  with the positive magnetostriction
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