DUAL SOLUTION SYNTHESIS AND CHARACTERIZATION OF MULTILAYER SULPHIDE THIN FILMS FOR POSSIBLE APPLICATIONS

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ABSTRACT

CuS:ZnS, CdS:ZnS, AlS:ZnS and SnS:ZnS multilayer thin films were synthesized on glass substrates using two solution based methods: successive ionic layer adsorption and reaction (SILAR) and solution growth technique(SGT). The deposited alloyed samples were annealed between 373K and 523K using Master Chef Annealing Machine. The crystallographic studies were done using X-ray diffractometer (XRD) and scanning electron microscope (SEM). The XRD pattern of CuS:ZnS alloyed thin films of samples P5 and P6show well defined peaks. The XRD pattern of CdS:ZnS alloyed thin films of sample Q5 show well defined peaks. The XRD pattern of AlS:ZnS alloyed thin films of samples R1 and R6 show well defined peaks. The XRD pattern of SnS:ZnS alloyed thin films of sample T6 show well defined peaks which reveals the samples are polycrystalline in nature. Their grain sizes were calculated. Rutherford backscattering spectroscopy (RBS) analysis confirmed the percentage of the elements of copper, cadmium, aluminium, tin, zinc and sulphur in the alloyed thin films. The surface electron microscopy result indicates the microstructure of the deposited alloyed thin films. The optical characterization was carried out using spectrophotometer. The spectral transmittance of samples P0, P1, P2, P3, and P4 show maximum transmissions of 44%, 98%, 78%, 96% and 57% at wavelength of about 900nm throughout the studied region and band gap of 3.98eV, 4.20eV, 4.18eV, 4.21eV and 4.15eV respectively. The spectral transmittance of samples Q0, Q1, Q2, Q3, and Q4 show maximum transmissions of 80%, 90%, 95%, 88% and 97% at wavelength of about 900nm, 900nm, 400nm, 650nm and 470nm within the studied region and band gap of 4.20eV, 4.21eV, 4.15eV and 4.19 respectively. The spectral transmittance of samples R0, R2, R3, R4, and R5 show maximum transmissions of 67%, 82%, 88%, 97% and 70% at wavelength of about 900nm within the studied region and band gap of 4.02eV, 4.20eV, 4.25eV, 4.35eV and 4.15eV respectively. The spectral transmittance of samples T0, T2, T3, T4, and T5 show maximum transmissions of 35%, 40%, 37%, 80% and 82% at wavelength of about 900nm within the studied region and band gap of 3.68eV, 3.8eV, 3.7eV, 3.98eV and 3.9eV respectively. Other optical properties that were investigated are; absorbance, reflectance, absorption coefficient, extinction coefficient, refractive index, optical conductivity and dielectric constants. From the qualities, these sulphide multilayer thin films may be found useful in window coating, vulcanization, etc.







TABLE OF CONTENTS

Title Page                                                                                                                    i

Declaration                                                                                                                  ii

Certification                                                                                                                iii

Dedication                                                                                                                  iv

Acknowledgement                                                                                                      v

Table of Content                                                                                                         vi

List of Tables                                                                                                              ix

List of Figures                                                                                                             x

Abstract                                                                                                                      xiii

 

CHAPTER 1:                        INTRODUCTION

1.1       Preamble                                                                                                         1

1.2       Alloy                                                                                                               2

1.3       Aim/Objectives                                                                                               3

1.4       Motivation of Study                                                                                       3

1.5       Significance of the Study                                                                               4

1.6       Scope of Study                                                                                               4

 

CHAPTER 2: LITERATURE REVIEW

2.1       Energy Bands                                                                                                 6

2.1.1    Conduction energy band                                                                                6

2.1.2    Insulator energy bands                                                                                    7

2.1.3    Semiconductor energy band                                                                           7

2.2       Solar energy                                                                                                    12

2.2.1    The solar spectrum                                                                                          13

2.2.2    Solar Radiation                                                                                               15

2.3       Photovoltaic Effect                                                                                         16

2.3.1    Solar cell                                                                                                         17

2.3.2    Types of solar cells                                                                                          18

2.3.3    The solar panel                                                                                                18

2.4       Thin Film Science                                                                                           19

2.4.1    Description of thin film materials                                                                   19

2.4.2    Types of thin film                                                                                           20

2.4.3    Applications of thin films                                                                               23

2.5       Deposition Techniques of Sulphide Alloy Thin Films                                    27

2.5.1    Chemical deposition techniques                                                                   28

2.5.1.1  Chemical bath deposition (CBD)                                                                28

2.5.1.2 Successive ionic layer adsorption and reaction (SILAR) method             29

2.5.1.3 Chemical vapor deposition (CVD)                                                                 30

2.5.1.4 Plating                                                                                                                        31

2.5.1.5 Spray pyrolysis                                                                                              31

2.5.1.6 Electrodeposiition                                                                                          32

2.5.2 Physical deposition                                                                                            34

2.5.2.1 Sputtering                                                                                                       35

2.5.2.2 Pulsed laser deposition                                                                                   35

2.5.2.3 Thermal evaporatoion                                                                                              35

2.5.2.4 Electron beam evaporation                                                                             36

2.5.2.5 Electrohydrodynamic deposition                                                                 36

2.6       Description of Materials Characterization Techniques                                   37

2.6.1    Structural and morphological property studies                                               37

2.6.1.1 X-ray diffraction (XRD)                                                                                37

2.6.1.2 Scanning electron microscopy (SEM)                                                 38

2.6.2    Optical property studies                                                                                  39

2.6.2.1 UV- Visible spectroscopy                                                                               39

2.7       Annealing                                                                                                        44

2.8       Effect of Material Properties on Transmitting Thin Films                              45

 

CHAPTER 3:                        MATERIALS AND EXPERIMENTAL METHODS

3.1       Description of Deposition Techniques Used                                                  47

3.2       Preparation of Sulphide Alloy Thin Films                                                      47

3.2.1    Apparatus used for the deposition                                                                  47

3.2.2    Substrate preparation                                                                                      48

3.2.3    Deposition of sulphide multilayer thin films using dual solution synthesis   

(SGT and SILAR)                                                                                          48

3.2.3.1 Deposition of CuS:ZnS thin films                                                                  49

3.2.3.2 Deposition of CdS:ZnS thin films                                                                  50

3.2.3.3 Deposition of AlS:ZnS thin films                                                                   50

3.2.3.4 Deposition of SnS:ZnS thin films                                                                   51

3.3       Characterization of Deposited Thin Films                                                      52

3.3.1     Optical characterization                                                                                  52

3.3.2    X-ray diffractometer (XRD)                                                                          52

3.3.3    Scanning electron microscopy (SEM)                                                 52

3.3.4    Rutherford backscattering spectrometry (RBS)                                             53

 

CHAPTER 4:                        RESULTS AND DISCUSSION

4.1       Composition and Thickness of the Deposited Thin Films                              54

4.2       Structural Properties                                                                                       82

4.2.1    Crystallographic studies of the deposited samples                                         82

4.2.2    Microstructure of the Deposited Samples                                                      91

4.3       Optical Properties                                                                                           95

4.3.1    CuS:ZnS thin films                                                                                         95

4.3.2    CdS:ZnS thin films                                                                                         103

4.3.3    AlS:ZnS thin films                                                                                          111

4.3.4    SnS:ZnS thin films                                                                                          118

4.4       Possible Areas of Application of the Deposited Thin Films                           125

 

CHAPTER 5:                        CONCLUSION AND RECOMMENDATIONS

5.1       Conclusion                                                                                                      126

5.2       Recommendations                                                                                          127

5.3       Contribution to Knowledge                                                                            127

 

REFERENCES                                                                                                        128





 

LIST OF TABLES


4.1:      The elements in sample P1 of CuS:ZnS                                                          55

4.2:      The elements in sample P2 of CuS:ZnS                                                          57

4.3:      The elements in sample P3 of CuS:ZnS                                                          59

4.4:      The elements in sample Q2 of CdS:ZnS                                                         62

4.5:      The elements in sample Q3 of CdS:ZnS                                                         64

4.6:      The elements in sample Q4 of CdS:ZnS                                                         66

4.7:      The elements in sample R3 of AlS:ZnS                                                          69

4.8:      The elements in sample R4 of AlS:ZnS                                                          71

4.9:      The elements in sample R5 of AlS:ZnS                                                          73

4.10:    The elements in sample T2 of SnS:ZnS                                                          76

4.11:    The elements in sample T3 of SnS:ZnS                                                          78

4.12:    The elements in sample T4 of SnS:ZnS                                                          80

4.13:    XRD results of CuS:ZnS alloyed thin film                                                    83

4.14:    XRD results of CuS:ZnS alloyed thin film                                                    85

4.15:    XRD results of AlS:ZnS alloyed thin film                                                     87

4.16:    XRD results of SnS:ZnS alloyed thin film                                                     89





LIST OF FIGURES

2.1:      Schematic energy bands of (a) a conductor, (b) an insulator, and (c) a semiconductor                                        10

2.2(a):  Schematic Diagram of a p-n junction                                                                     11

2.2(b):  Energy band diagram of a p-n junction                                                    11

2.3:      The Spectral irradiance                                                                                   14

2.4:      Path length of sunlight through the atmosphere                                             15

2.5:      Schematic diagram of chemical bath deposition (CBD)                            29

2.6:      Schematic diagram of CVD technique                                                           30

2.7:      Schematic diagram of spray pyrolysis                                                            32

2.8(a): Typical set-up of three electrode system of electrodeposited             technique(wikipedia.org, 2021)                                                                        33

2.8(b):  Pictorial view of a typical two electrode set-up of electrodeposited

technique                                                                                                         33

2.9:      Thermal evaporation technique set-up                                                            36

2.10:    Basic schematic diagram for construction of a spectrophotometer                      39

4.1:      The composition of sample P1 with thickness 247.5nm, of CuS:ZnS

measured by RBS                                                                                           56

4.2:      The composition of sample P2 with thickness 238nm, of CuS:ZnS

measured by RBS                                                                                           58

4.3:      The composition of sample P3 with thickness 247.5nm, of CuS:ZnS

measured by RBS                                                                                           60

4.4:      The composition of sample Q2 with thickness 298.6nm, of CdS:ZnS

measured by RBS                                                                                           63

4.5:      The composition of sample Q3 with thickness 160nm, of CdS:ZnS

measured by RBS                                                                                           65

4.6:      The composition of sample Q4 with thickness 190nm, of CdS:ZnS

measured by RBS                                                                                           67

4.7:      The composition of sample R3 with thickness 140nm, of CdS:ZnS

measured by RBS                                                                                           70

4.8:      The composition of sample R4 with thickness 171nm, of CdS:ZnS

measured by RBS                                                                                           72

4.9:      The composition of sample R5 with thickness 300nm, of CdS:ZnS

measured by RBS                                                                                           74

4.10:    The composition of sample T2 with thickness 360nm, of SnS:ZnS

measured by RBS                                                                                           77

4.11:    The composition of sample T3 with thickness 440nm, of SnS:ZnS

            measured by RBS                                                                                           79

4.12:    The composition of sample T4 with thickness 440nm, of SnS:ZnS

            measured by RBS                                                                                           81

4.13:    XRD pattern of CuS:ZnS alloyed thin films of samples P5 and P6

annealed at 150◦C and 200◦C respectively                                                    84

4.14     XRD pattern of CdS:ZnS alloyed thin film of samples Q5 annealed at 200◦C                                                                                             86

4.15:    XRD pattern of AlS:ZnS alloyed thin films of samples R1 and R6

annealed at 200◦C and 250◦C respectively                                                    88

4.16:    XRD pattern of SnS:ZnS alloyed thin film of samples T6 annealed at

200◦C                                                                                                              90

4.17:    Optical micrograph of CuS:ZnS alloyed thin films of samples P5 and P6     91

4.18:    Optical micrograph of CdS:ZnS alloyed thin films of samples Q5 and Q6   92

4.19:    Optical micrograph of AlS:ZnS alloyed thin films of samples R1 and R6    93

4.20:    Optical micrograph of SnS:ZnS alloyed thin films of samples T1 and T6     94

4.21:    Transmittance spectra of CuS:ZnS thin films annealed at different

temperatures                                                                                                    97

4.22:    Absorbance spectra of CuS:ZnS thin films annealed at different

temperatures                                                                                                    97

4.23:    Reflectance spectra of CuS:ZnS thin films annealed at different

temperatures                                                                                                    98

4.24:    Plot of real dielectric constant versus photon energy for CuS:ZnS

thin films                                                                                                         98

4.25:    Plot of optical conductivity versus photon energy for CuS:ZnS thin

films                                                                                                                99

4.26:    Plot of optical imaginary dielectric constant versus photon energy for

CuS:ZnS thin films                                                                                         99

4.27:    Plot of extinction coefficient versus photon energy for CuS:ZnS thin

films                                                                                                                100

4.28:    Plot of (αhυ)2 versus photon energy for CuS:ZnS thin films                          101

4.29:    Plot of absorption coefficient versus photon energy for CuS:ZnS thin        

films                                                                                                                102

4.30:    Plot of refractive index versus photon energy for CuS:ZnS thin films          102

4.31:    Transmittance spectra of CdS:ZnS thin films annealed at different

temperatures                                                                                                    105

4.32:    Absorbance spectra of CdS:ZnS thin films annealed at different

temperatures                                                                                                    105

4.33:    Reflectance spectra of CdS:ZnS thin films annealed at different

temperatures                                                                                                    106

4.34:    Plot of real dielectric constant versus photon energy for CdS:ZnS thin

films                                                                                                                106

4.35:    Plot of optical conductivity versus photon energy for CdS:ZnS thin

films                                                                                                                107

4.36:    Plot of optical imaginary dielectric constant versus photon energy for

CdS:ZnS thin films                                                                                         107

4.37:    Plot of extinction coefficient versus photon energy for CdS:ZnS thin

films                                                                                                                108

4.38:    Plot of (αhυ)2 versus photon energy for CdS:ZnS thin films                         109

4.39:    Plot of absorption coefficient versus photon energy for CdS:ZnS thin

films                                                                                                                110

4.40:    Plot of refractive index versus photon energy for CdS:ZnS thin

films                                                                                                                110

4.41:    Transmittance spectra of AlS:ZnS thin films annealed at different

temperatures                                                                                                    112

4.42:    Absorbance spectra of AlS:ZnS thin films annealed at different

temperatures                                                                                                    112

4.43:    Reflectance spectra of AlS:ZnS thin films annealed at different

temperatures                                                                                                    113

4.44:    Plot of real dielectric constant versus photon energy for AlS:ZnS

            thin films                                                                                                         113

4.45     Plot of optical conductivity versus photon energy for AlS:ZnS thin

films                                                                                                                114

4.46     Plot of optical imaginary dielectric constant versus photon energy for

CuS:ZnS thin films                                                                                         114

4.47:    Plot of extinction coefficient versus photon energy for AlS:ZnS thin

films                                                                                                                115

4.48:    Plot of (αhυ)2 versus photon energy for AlS:ZnS thin films                          116

4.49:    Plot of absorption coefficient versus photon energy for AlS:ZnS thin

films                                                                                                                117

4.50:    Plot of refractive index versus photon energy for AlS:ZnS thin films           117

4.51:    Transmittance spectra of SnS:ZnS thin films annealed at different

temperatures                                                                                                    119

4.52:    Absorbance spectra of SnS:ZnS thin films annealed at different

temperatures                                                                                                    119

4.53:    Reflectance spectra of SnS:ZnS thin films annealed at different

temperatures                                                                                                    120

4.54:    Plot of real dielectric constant versus photon energy for SnS:ZnS

thin films annealed at different temperatures                                                 120

4.55:    Plot of optical conductivity versus photon energy for SnS:ZnS thin films    121

4.56:    Plot of optical imaginary dielectric constant versus photon energy for

SnS:ZnS thin films                                                                                          121

4.57:    Plot of extinction coefficient versus photon energy for SnS:ZnS thin films 122

4.58:    Plot of (αhυ)2 versus photon energy for SnS:ZnS thin films                          123

4.59:    Plot of absorption coefficient versus photon energy for CuS:ZnS thin

films                                                                                                                124

4.60:    Plot of refractive index versus photon energy for CuS:ZnS thin films          124

 

 


 

 

 

 

CHAPTER 1

INTRODUCTION

1.1       PREAMBLE

Thin films now occupy a prominent place in research and solid state technology. In an expanding variety of applications in the various electronic and optoelectronic devices, much interest has been attracted as a result of the use of thin film semi-conductors due to their low cost of production. A variety of methods has been used to prepare a high quality transition metal chalcogenides. Each technology has its limitation. Therefore, in order to grow sulphide multilayer thin films with desirable shape and structure, solution growth and successive ionic layer absorption and reaction technique were employed, which combine simplicity and low cost with potential for large scale production (it does not require sophisticated equipment)

Transition metal chalcogenites: oxides, sulfides, selinides and tellurides are important technological materials. In this study the effect of varying annealing temperature was investigated in order to broaden the range of application. Although there have been numerous papers published reporting the preparation of chalcogenide thin films using solution growth and successive ionic layer absorption and reaction technique respectively, Kaur et al. pointed out that the process has remained recipe oriented with little understanding of the kinetics of the process. There is therefore, a need for careful investigation of a substrate using two techniques - solution growth technique and successive ionic layer absorption and reaction to identify the condition that favours high quality coherent deposits.


 

1.2       ALLOY

An alloy is a mixture of metal(s) and another element. The metal is usually called the primary metal or the base metal, and the name of this metal may also be the name of the alloy. Alloys are defined by metallic bonding character. An alloy may be a solid solution of metal elements (a single phase) or a mixture of metallic phases (two or more solutions). An alloy is distinct from an impure metal in that, with an alloy, the added elements are well controlled but are often considered useful. The mechanical properties of alloys will often be quite different from those of its individual constituents. Although the elements of an alloy usually must be soluble in the liquid state, they may not always be soluble in the solid state (Callister and Rethwisch, 2010). If the metals remain soluble when solid, the alloy forms a solid solution, becoming a homogeneous structure consisting of identical crystals, called a phase. As the mixture cools, the constituents becomes solids, they may separate to form two or more different types of crystals, creating a heterogeneous microstructure of different phases, some with one or more constituent than the other phase has.

However, in other alloys, the insoluble elements may not separate until after crystallization occurs. If cooled very quickly, they crystallize as a homogeneous phase, but they are supersaturated with the secondary constituents. As time passes, the atom of these supersaturated alloys can separate from the crystal lattice, becoming more stable, and form a second phase that serve to reinforce the crystals internally. Some alloys such as electrum which is an alloy consisting of silver and gold, occur naturally.

The primary metal is called the base, the matrix, or the solvent. The secondary constituents are often called solutes. If there is a mixture of only two types of atoms (not regarding impurities) such as copper-nickel alloy, it is called a binary alloy. If there are three types of atoms forming the mixture, such as iron, nickel and chromium, then it is called a ternary alloy. An alloy with four constituents is a quaternary alloy, while a five part alloy is termed quinary alloy.


1.3       AIM/OBJECTIVES

The aim of this study is the to investigate the influence of varying annealing temperature on solution growth and successive ionic layer absorption and reaction depostited multilayer sulphide (CuS:ZnS, CdS:ZnS, AlS:ZnS and SnS:ZnS)thin films to deduce a suitable thin film for possible applications.

In order to achieve the aim of this study, the following objectives were adopted:

i           prepare ZnS bath by Solution growth technique.

ii          grow other sulphide alloy (CuS, SnS, CdS, AlS) thin films by Successive ionic layer absorption and reaction technique and dip into already prepared ZnS bath.

iii         anneal the deposited samples at various temperatures.          

iv         characterize the deposited samples.

v          study the influence of varying annealing temperature.

vi         identify possible applications of the films deposited.


1.4       MOTIVATION OF STUDY

Energy is the pre-requisite for creation of wealth and sustainability of development. The importance of energy in economic development has been recognised historically but the equitable distribution of energy amongst the masses has always been a matter of great concern. Sustainability of development can be ensured by use of sustainable energy resources which are environment-friendly and available in abundance. And the only possible answer to this problem is Renewable Energy. Renewable Sources include wind, biomass, geothermal, hydro-power, ocean thermal and last but not the least solar energy. Owing to the exponential growth of global population, the need for energy is going to be doubled in coming fifty years. But this huge demand can be met by solar energy alone if properly harnessed. With the advancement in the field of nanotechnology and material science, a huge number of motivated researchers are exploring this vast area of science and making great contribution towards different fabrication techniques to produce a cheap, sustainable, environment friendly, highly efficient solar cell and other nanoelectronic devices.


1.5       SIGNIFICANCE OF THE STUDY

The need and the desire to produce high quality sulphide thin films with combinational qualities in the areas of applications led to the choice of the study on dual solution synthesis and characterization of CuS:ZnS, CdS:ZnS, AlS:ZnS and SnS:ZnS multilayer thin films for possible applications.

The outcome of the study will provide appropriate process for large scale production of high quality multilayer thin films.


1.6       SCOPE OF STUDY

This study encompasses the preparation of multilayer sulphide (CuS:ZnS, CdS:ZnS, AlS:ZnS and SnS:ZnS) thin films using two solution based methods: solution growth and SILAR technique. Reagents required include: copper sulphate (CuSO4), cadmium chloride (CdCl2), aluminium chloride (AlCl2), tin chloride (SnCl2), zinc chloride (ZnCl2), ammonia (NH3) and thiourea (CS(NH3)). The deposited samples were annealed using Master Chef annealing machine at varying temperatures. X-ray diffractometer (XRD) and scanning electron microscope (SEM) were used to determine the structural properties of the samples, Rutherford Backscattering Spectroscope (RBS) was used to determine the composition and thickness of the deposited samples and spectrophotometer was used to determine the optical properties of the samples.


 

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