X-ray Diffraction: Principles and Practice Ashish Garg and Nilesh Gurao Department of Materials Science and Engineering Indian Institute of Technology Kanpur Layout of the Lecture Materials Characterization Basics Diffraction X-ray Diffraction Crystal Structure and X-ray Diffraction Different Methods Importance of X-ray Diffraction Phase Analysis Texture Analysis Stress Analysis Particles Size Analysis ……….. Summary Materials Characterization Essentially to evaluate the structure and properties Structural Characterization Diffraction X-ray and Electron Diffraction Microscopy Spectroscopy Property Evaluation Mechanical Electrical Anything else Time Line 1665: Diffraction effects observed by Italian mathematician Francesco Maria Grimaldi 1868: X-rays Discovered by German Scientist Röntgen 1912: Discovery of X-ray Diffraction by Crystals: von Laue 1912: Bragg’s Discovery Electromagnetic Spectrum Generation of X-rays Commercial X-ray Tube X-ray Spectrum from an Iron target Short Wavelength Limit SW L ( nm ) Continuous spectrum I CS AiZV Characteristic X-ray Moseley’s Law C (Z ) I K Bi (V V k ) λSWL n m 12400 V Use of Filter Ni filter for Cu Target Crystal Systems and Bravais Lattices Structure of Common Materials Metals Copper: FCC -Iron: BCC Zinc: HCP Silver: FCC Aluminium: FCC Ceramics SiC: Diamond Cubic Al2O3: Hexagonal MgO: NaCl type Diffraction A diffracted beam may be defined as a beam composed of a large number of scattered rays mutually reinforcing each other Scattering Interaction with a single particle Diffraction Interaction with a crystal Scattering Modes Random arrangement of atoms in space gives rise to scattering in all directions: weak effect and intensities add By atoms arranged periodically in space In a few specific directions satisfying Bragg’s law: strong intensities of the scattered beam :Diffraction No scattering along directions not satisfying Bragg’s law Diffraction of light through an aperture d 1 0.9 0.8 0.7 0.6 Intensity 0.5 0.4 0.3 0.2 0.1 0 -15 -10 -5 0 5 10 15 1 0.9 0.8 0.7 0.6 Intensity 0.5 0.4 0.3 0.2 0.1 0 -15 -10 -5 0 Minima sin θ λ 10 15 Maxima sin n a 5 n = 0, 1,.. 2n 1 2a n = 1, 2,.. Young’s Double slit experiment d sinθ = mλ, m = 1,2,3….. Constructive Interference d sinθ = (m+½)λ, m = 1,2,3….. Destructive Interference Interference Phase Difference = 0˚ Phase Difference = 180˚ Phase Difference = 90˚ Interference and Diffraction Bragg’s Law n=2d.sin n: Order of reflection d: Plane spacing a = h k l : Bragg Angle 2 2 in out 2 2 Path difference must be integral multiples of the wavelength in=out Braggs Law d n 2 sin 1 sin d 2 Geometry of Bragg’s law The incident beam, the normal to the reflection plane, and the diffracted beam are always co-planar. The angle between the diffracted beam and the transmitted beam is always 2 (usually measured). Sin cannot be more than unity; this requires nλ < 2d, for n=1, λ < 2d λ should be less than twice the d spacing we want to study Order of reflection Rewrite Bragg’s law λ=2 sin d/n A reflection of any order as a first order reflection from planes, real or fictitious, spaced at a distance 1/n of the previous spacing Set d’ = d/n λ=2d’ sin An nth order reflection from (hkl) planes of spacing d may be considered as a first order reflection from the (nh nk nl) plane of spacing d’ = d/n *The term reflection is only notional due to symmetry between incoming and outgoing beam w.r.t. plane normal, otherwise we are only talking of diffraction. Reciprocal lattice vectors Used to describe Fourier analysis of electron concentration of the diffracted pattern. Every crystal has associated with it a crystal lattice and a reciprocal lattice. A diffraction pattern of a crystal is the map of reciprocal lattice of the crystal. Real space Reciprocal space Crystal Lattice Reciprocal Lattice Crystal structure Diffraction pattern Unit cell content y x y’ x’ Structure factor y’ x’ Reciprocal space a* b* c* bc a (b c ) Reciprocal lattice of FCC is BCC and vice versa ca a (b c ) ab a (b c ) 001 a 010 b c 100 Ewald sphere 1 k' hkl 1 2 d hkl 2 hkl k Ewald sphere Limiting sphere Ewald sphere J. Krawit, Introduction to Diffraction in Materials Science and Engineering, Wiley New York 2001 Two Circle Diffractometer For polycrystalline Materials Four Circle Diffractometer For single crystals 2 Circle diffratometer 2 and 3 and 4 circle diffractometer 2θ, ω, φ, χ 6 circle diffractometer θ, φ, χ and δ, γ, µ www.serc.carleton.edu/ Hong et al., Nuclear Instruments and Methods in Physics Research A 572 (2007) 942 NaCl crystals in a tube facing X-ray beam Powder Diffractometer (400) (410) (220) (330)(221) (310) (311) (222) (320) (321) (211) (210) (200) (111) (110) (100) Calculated Patterns for a Cubic Crystal Structure Factor N Fhkl fne 2 i ( hu n kv n lw n ) Intensity of the diffracted beam |F|2 1 − − − − h,k,l : indices of the diffraction plane under consideration u,v,w : co-ordinates of the atoms in the lattice N : number of atoms fn : scattering factor of a particular type of atom Bravais Lattice Reflections possibly present Reflections necessarily absent Simple All None Body Centered (h+k+l): Even (h+k+l): Odd Face Centered h, k, and l: mixed h, k, and l unmixed i.e. all odd or all even Systematic Absences Permitted Reflections Simple Cubic BCC (100), (110), (111), (200), (210), (211), (220), (300), (221) ……… (110), (200), (211), (220), (310), (222)…. FCC (111), (200), (220), (311)….. Diffraction Methods Method Wavelength Angle Laue Variable Fixed Rotating Crystal Powder Fixed Fixed Specimen Single Crystal Variable (in Single part) Crystal Variable Powder Laue Method Transmission Zone axis Reflection Zone axis crystal crystal Film Incident beam • • • Incident beam Film Uses Single crystal Uses White Radiation Used for determining crystal orientation and quality Rotating Crystal Method Determination of unknown crystal structures Powder Method Sample Incident Beam Film • Useful for determining lattice parameters with high precision and for identification of phases Indexing a powder pattern Bragg’s Law n = 2d sin For cubic crystals a d hkl 2 2 2 h k l w hich gives rise to 2 sin θ θ S1 h k l 2 (for front reflections) or 2W S2 θ 1 (for back reflections) 2 W 2 2 2 4a 2 w hich is a constant Indexing SS1 (mm) () () sin2 1 (mm) 38 19.0 38 19.0 0.11 45 22.5 45 22.5 0.15 66 33.0 66 33.0 0.30 78 39.0 78 39.0 0.40 83 41.5 83 41.5 0.45 97 49.5 97 49.5 0.58 113 56.5 113 56.5 0.70 118 59.0 118 59.0 0.73 139 69.5 139 69.5 0.88 168 84.9 168 84.9 0.99 FCC; wavelength=1.54056Å Simple BCC Cubic 2 2 h22+k sin +l 2/ +l2 22/ Lattice 22+k 22+lh 22 2+k2sin hsin h22+k22+l22Parameter, a (Å) 0.11 3 0.15 4 0.30 8 0.40 11 0.45 12 0.58 16 0.70 19 0.73 20 0.88 24 0.99 27 21 0.037 42 0.038 63 0.038 84 0.036 5 10 0.038 6 12 0.036 8 14 0.037 9 16 0.037 10 18 0.037 11 20 0.037 0.055 0.11 0.038 0.75 0.050 0.10 0.050 0.10 0.045 0.09 0.048 0.097 4.023 3.978 3.978 4.039 3.978 Not NotSimple BCC Cubic 4.046 But what is the lattice 4.023 0.046 0.081 parameter? 4.023 0.049 0.088 4.023 0.050 0.09 4.023 Not Constant 0.050 0.0925 Constant; so it is FCC Diffraction from a variety of materials (From “Elements of X-ray Diffraction”, B.D. Cullity, Addison Wesley) Reality Crystallite size can be calculated using Scherrer Formula t 0.9 B cos B Instrumental broadening must be subtracted (From “Elements of X-ray Diffraction”, B.D. Cullity, Addison Wesley) Intensity of diffracted beam • • • • • • polarization factor structure factor (F2) multiplicity factor Lorentz factor absorption factor temperature factor For most materials the peaks and their intensity are documented JCPDS ICDD Name and formula Reference code: 00-001-1260 PDF index name: Nickel Empirical formula: Ni Chemical formula: Ni Crystallographic parameters Crystal system: Cubic Space group: Fm-3m Space group number: 225 a (Å): 3.5175 b (Å): 3.5175 c (Å): 3.5175 Alpha (°): 90.0000 Beta (°): 90.0000 Gamma (°): 90.0000 Measured density (g/cm^3): 8.90 Volume of cell (10^6 pm^3): 43.52 Z: 4.00 RIR: Status, subfiles and quality Status: Marked as deleted by ICDD Subfiles: Inorganic Quality: Blank (B) References Primary reference: Hanawalt et al., Anal. Chem., 10, 475, (1938) Optical data: Data on Chem. for Cer. Use, Natl. Res. Council Bull. 107 Unit cell: The Structure of Crystals, 1st Ed. Stick pattern from JCPDS http://ww1.iucr.org/cww-top/crystal.index.html Actual Pattern Lattice parameter, phase diagrams Texture, Strain (micro and residual) Size, microstructure (twins and dislocations) Bulk electrodeposited nanocrystalline nickel Powder X-ray diffraction is essentially a misnomer and should be replaced by Polycrystalline X-ray diffraction Information in a Diffraction Pattern Phase Identification Crystal Size Crystal Quality Texture (to some extent) Crystal Structure Intensity (a.u.) Analysis of Single Phase 2(˚) d (Å) (I/I1)*100 27.42 3.25 10 31.70 2.82 100 45.54 1.99 60 53.55 1.71 5 56.40 1.63 30 65.70 1.42 20 76.08 1.25 30 84.11 1.15 30 89.94 1.09 5 I1: Intensity of the strongest peak Procedure Note first three strongest peaks at d1, d2, and d3 In the present case: d1: 2.82; d2: 1.99 and d3: 1.63 Å Search JCPDS manual to find the d group belonging to the strongest line: between 2.84-2.80 Å There are 17 substances with approximately similar d2 but only 4 have d1: 2.82 Å Out of these, only NaCl has d3: 1.63 Å It is NaCl……………Hurrah Specimen and Intensities Substance File Number 2.829 1.999 2.26x 1.619 1.519 1.499 3.578 2.668 (ErSe)2Q 19-443 2.82x 1.996 1.632 3.261 1.261 1.151 1.411 0.891 NaCl 5-628 2.824 1.994 1.54x 1.204 1.194 2.443 5.622 4.892 (NH4)2WO2Cl4 22-65 2.82x 1.998 1.263 1.632 1.152 0.941 0.891 1.411 (BePd)2C 18-225 Caution: It could be much more tricky if the sample is oriented or textured or your goniometer is not calibrated Presence of Multiple phases d (Å) I/I 4 1 More Complex Pattern of Cu2O Remaining 3.01 Lines 5 Several permutations combinations possible 2.47 I/I1 72 d d (Å) I/I1 e.g. d1; d2; and d3, the first three strongest lines (Å) 2.13 28 Observed Normalized 3.020 9 show several alternatives 2.09 * 100 3.01 5 7 2.465 and 100 match Then take any of the two lines together 1.80 * 52 20 2.47 72 1.50 100 It turns out that 1st and 3rd strongest lies belong 2.135 37Patternto for Cu 1.29 9 Cu and then all other peaks for Cu1.743 can be 1d (Å) 2.13I/I1 28 39 1.28 * 18 separated out 2.088 100 1.50 20 28 1.510 27 1.22 4 Now separate the remaining lines and normalize 1.808 46 9 1.08 * 13 20 1.287 171.278 1.29 the intensities 20 36 17 4 1.04 * 1.233 4 1.09the1.22 Look for first three lines and it turns out that 0.98 5 1.0436 5 phase is Cu2O 0.98 5 7 1.0674 2 If more phases, more pain to solve0.9795 0.9038 3 0.91 4 0.8293 9 0.83 0.8083 8 0.81 * * 8 10 Lattice Strain do No Strain 2 Uniform Strain d strain 2 Non-uniform Strain B roadeing b 2 2 d d 2 tan Texture in Materials Grains with in a polycrystalline are not completely randomly distributed Clustering of grains about some particular orientation(s) to a certain degree Examples: Present in cold-rolled brass or steel sheets Cold worked materials tend to exhibit some texture after recrystallization Affects the properties due to anisotropic nature Texture Fiber Texture A particular direction [uvw] for all grains is more or less parallel to the wire or fiber axis Double axis is also possible e.g. [111] fiber texture in Al cold drawn wire Example: [111] and [100] fiber textures in Cu wire Sheet Texture Most of the grains are oriented with a certain crystallographic plane (hkl) roughly parallel to the sheet surface and certain direction [uvw] parallel to the rolling direction Notation: (hkl)[uvw] Texture in materials [uvw] i.e. perpendicular to the surface of all grains is parallel to a direction [uvw] Also, if the direction [u1v1w1] is parallel for all regions, the structure is like a single However, the direction crystal [u1v1w1] is not aligned for all regions, the structure is like a mosaic structure, also called as Mosaic Texture Pole Figures (100) pole figures for a sheet material (a) Random orientation (b) Preferred orientation Thin Film Specimen Grazing angle (very small, ~1-5) B B Film or Coating Substrate Smaller volume i.e. less intensity of the scattered beam from the film Grazing angle Useful only for polycrystalline specimens Thin Film XRD Precise lattice constants measurements derived from 2- scans, which provide information about lattice mismatch between the film and the substrate and therefore is indicative of strain & stress Rocking curve measurements made by doing a q scan at a fixed 2 angle, the width of which is inversely proportionally to the dislocation density in the film and is therefore used as a gauge of the quality of the film. Superlattice measurements in multilayered heteroepitaxial structures, which manifest as satellite peaks surrounding the main diffraction peak from the film. Film thickness and quality can be deduced from the data. Glancing incidence x-ray reflectivity measurements, which can determine the thickness, roughness, and density of the film. This technique does not require crystalline film and works even with amorphous materials. Thin Films Specimens B1B (hkl) plane of the substrate B2 B B1B2 Diffraction from hkl plane i.e. No Diffraction from hkl occurs plane Single Crystal Substrate If the sample and substrate is polycrystalline, then problems are less But if even if one of them is oriented, problems arise In such situations substrate alignment is necessary 30 40 0028 0024 0026 0022 0020 0018 50 60 70 80 90 2216 20 10 △ △ SrTiO3 (110) 40 50 60 70 80 90 30 4016/ 0416 20 10 014 △ △ Log Intensity (a.u.) Bismuth Titanate thin films on oriented SrTiO3 substrates Only one type of peaks It apparent that films are highly oriented SrTiO3 (100) * △ 0016 0012 0014 008 0010 006 004 Oriented thin films △ SrTiO3 (111) 10 20 30 40 50 60 o 2 ( ) 70 80 90 Degree of orientation [uvw] corresponding to planes parallel to the surface Film Substrate Side view But what if the planes when looked from top have random orientation? Top view Pole Figure SrTiO3 (110) SrTiO3 (100) SrTiO3 (111) 1 2 1 1 2 1 3 1 2 3 2 1 1 4 Peaks at ~50 Excellent in-plane orientation 2 sets of peaks at ~ 5, 65 and 85° Indicating a doublet or opposite twin growth 2 2 1 3 2 2 3 3 sets of peaks at ~ 35 and 85° indicating a triplet or triple twin growth (117) Pole Figures for Bismuth Titanate Films Texture Evolution 3 (100) planes inclined at 54.7° to (110) plane, separated by 120° Film SrTiO3 (100) Two (100) planes inclined at 45° to (110) plane in opposite directions BNdT(001) STO [100] STO(111) 45 54.7° STO(110) STO(111) STO(100) BNdT/SrTiO3 (100) BNdT/SrTiO3 (110) BNdT/SrTiO3 (111) Rocking Curve An useful method for evaluating the quality of oriented samples such as epitaxial films is changed by rocking the sample but B is held constant Width of Rocking curve is a direct measure of the range of orientation present in the irradiated area of the crystal (0010) Rocking curve of (001)(2212) SrBi Rocking (116)oriented film 2Ta2Ocurve 9 thin of oriented SrBi2Ta2O9 thin film Normal B FWHM = 0.07° (a.u.) Intensity (a.u.) Intensity 17.4 FWHM = 0.171° 32.432.4 17.5 32.6 32.832.8 17.6 17.7 () () 17.6 32.6 17.8 33.0 18.0 33.0 17.833.233.2 18.2 Order Disorder Transformation Structure factor is dependent on the presence of order or disorder within a material Present in systems such as Cu-Au, Ti-Al, NiFe Order-disorder transformation at specific compositions upon heating/cooling across a critical temperature Examples: Cu3Au, Ni3Fe Order Disorder Transformation Structure factor is dependent on the presence of order or disorder within a material. Complete Disorder Example: AB with A and B atoms randomly distributed in the lattice Lattice positions: (000) and (½ ½ ½) Atomic scattering factor favj= ½ (fA+fB) Structure Factor, F, is given by F = Σf exp[2i (hu+kv+lw)] = favj [1+e( i (h+k+l))] = 2. favj when h+k+l is even = 0 when h+k+l is odd The expected pattern is like a BCC crystal A B Order Disorder Transformation Complete Order Example: AB with A at (000) and B at (½ ½ ½) Structure Factor, F, is given by F = fA e[2i (h.0+k.0+l.0)]+ fA e[2i (h. ½+k. ½+l. ½)] = fA+fB when h+k+l is even = fA-fB when h+k+l is odd The expected pattern is not like a BCC crystal, rather like a simple cubic crystal where all the reflections are present. Extra reflections present are called as superlattice reflections A B Order-Disorder Transformation Disordered Cu3Au Ordered Cu3Au Instrumentation Diffractometer Source Optics Detector Incident Beam Part Diffracted Beam Part Sample Source Incident Beam Optics Diffracted Beam Optics Detector Geometry and Configuration Theta-Theta Source and detector move θ, sample fixed Theta-2Theta Sample moves θ and detector 2θ , source fixed Vertical configuration Horizontal configuration Incident Beam Part Source Incident Beam Optics Horizontal sample Vertical sample Diffracted Beam Part Sample Diffracted Beam Optics Detector Sample translation XYZ translation Z translation sample alignment Sample exactly on the diffractometer circle Knife edge or laser Video microscope with laser XY movement to choose area of interest X-ray generation X-ray tube (λ = 0.8-2.3 Ǻ) Rotating anode (λ = 0.8-2.3 Ǻ) Liquid metal Synchrotron (λ ranging from infrared to X-ray) X-rays X-ray tube Be window W cathode Rotating anode Electrons Metal anode Small angle anode Small focal spot Large angle anode Large focal spot Rotating anode of W or Mo for high flux Microfocus rotating anode Liquid anode for high flux and small beam size 10 times brighter 100 times brighter Gallium and Gallium, indium, tin alloys Synchrotron provides intense beam but access is limited Brighter than a thousand suns Synchrotron High brilliance and coherence X-ray bulb emitting all radiations from IR to X-rays http://www.coe.berkeley.edu/AST/srms Moving charge emits radiation Electrons at v~c Bending magnet, wiggler and undulator Straight section wiggler and undulator Curved sections Bending magnet Filter to remove Kβ For eg. Ni filter for Cu Kβ Reduction in intensity of Kα Choice of proper thickness Slits To limit the size of beam (Divergence slits) To alter beam profile (Soller slit angular divergence ) Narrow slits Lower intensity + Narrow peak Mirror focusing and remove Kα2 Mono-chromator Si remove Kα2 Graphite Beam Profile Mirror Parallel beam Source Soller slit Detector Mirror Sample Para-focusing Detector Sample Source Point focus Detector Sample Source Comparison Parallel beam Para-focusing X-rays are aligned X-rays are diverging Lower intensity for bulk samples Higher intensity Higher intensity for small samples Lower intensity Instrumental broadening independent of orientation of diffraction vector with specimen normal Instrumental broadening dependent of orientation of diffraction vector with specimen normal Suitable for GI-XRD Suitable for Bragg-Brentano Texture, stress Powder diffraction Detectors Single photon detector (Point or 0D) scintillation detector NaI proportional counter, Xenon gas semiconductor Position sensitive detector (Linear or 1D) gas filled wire detectors, Xenon gas charge coupled devices (CCD) Area detectors (2D) wire CCD 3D detector X-ray photon Photoelectron or Electron-hole pair Photomultiplier tube or amplifier Electrical signal Resolution: ability to distinguish between energies Energy proportionality: ability to produce signal proportioanl to energy of x-ray photon detected Sensitivity: ability to detect low intensity levels Speed: to capture dynamic phenomenon Range: better view of the reciprocal space Data collection and analysis Choose 2θ range Step size and time per step Hardware: slit size, filter, sample alignment Fast scan followed with a slower scan Look for fluorescence Collected data: Background subtraction, Kα2 stripping Normalize data for comparison I/Imax Summary X-ray Diffraction is a very useful to characterize materials for following information Phase analysis Lattice parameter determination Strain determination Texture and orientation analysis Order-disorder transformation and many more things Choice of correct type of method is critical for the kind of work one intends to do. Powerful technique for thin film characterization