Edith Cowan University Research Online ECU Presentations 2011 Nano-engineered high-performance magnetooptic garnet materials Mohammad Nur-E-Alam Edith Cowan University, m.nur-e-alam@ecu.edu.au Mikhail Vasiliev Edith Cowan University, m.vasiliev@ecu.edu.au Viacheslav Kotov Institute of Radio Engineering and Electronics, Russian Academy of Sciences Kamal Alameh Edith Cowan University, k.alameh@ecu.edu.au Presented at the 2011 International Conference on Materials for Advanced Technologies (ICMAT), 26th June-1st July, 2011, Suntec, Singapore. This Presentation is posted at Research Online. http://ro.ecu.edu.au/ecupres/8 Nano-engineered high-performance magneto-optic garnet materials Mohammad Nur-E-Alam1, Mikhail Vasiliev1, Viacheslav Kotov2 and Kamal Alameh1 1Electron Science Research Institute, Edith Cowan University, 270 Joondalup Dr, Joondalup, WA 6027, Australia 2Institute of Radio Engineering and Electronics, Russian Academy of Sciences, 11 Mohovaya St, Moscow 125009, Russia OUTLINE • Introduction Introduction to Bismuth- and rare-earth-substituted iron garnets and application examples • Material synthesis and characterization RF magnetron sputtering technology Conventional oven annealing for crystallizing the amorphous layers • Thin-film engineered garnet materials, properties & applications (Bi, Dy)3(Fe, Ga)5O12 and (Bi, Lu)3(Fe, Al)5O12 Introduction to Rare Earth Iron garnets Rare-earth iron garnets: R3Fe5O12 where R is a rare earth atom • Commonly known garnet materials are: Yttrium Iron garnet (YIG = Y3Fe5O12), Gadolinium Gallium garnet (GGG= Gd3Ga5O12) and Bismuth Iron garnet (BIG = Bi3Fe5O12 ) Crystal structure of magnetic garnets • The two very important subclasses of garnets for use in magneto-optic (MO) applications are described by: (Bi, Dy)3(Fe, Ga)5O12 and (Bi, Lu)3(Fe, Al)5O12 - Bismuth-substituted rare-earth iron garnets doped with Ga or Al, of importance due to the strong Faraday effect and a large variety of possible properties adjustable through • Still considered to be the best transparent MO material for material composition non-reciprocal optical components magnetic recording media magnetic field sensors MO imaging media MO planar waveguides magnetically-tunable photonic crystal structures Background theory: Faraday effect Magneto-optical phenomenon = interaction between light and magnetic field β=VBd β = Faraday rotation angle V = Verdet constant d = material thickness MO material For thin-film materials, we use specific Faraday rotation: θF [ °/µm] = β / d (at B = Bsat) Extraordinary magneto-optical properties of Bi-substituted iron garnets first reported in 1969 (C. F. Buhrer, J. Appl. Phys. 40(11), 4500–4502, 1969). • Highest specific Faraday rotation in the visible and near-IR regions (of all semi-transparent dielectric materials) Thin film materials synthesis & characterization Optical characterization MO characterization Magnetic and microstructural characterization RF Magnetron sputtering (a common method & very suitable for integratedoptics devices) Our system at ESRI, ECU • The parameters of importance are: film thickness, absorption spectra, specific Faraday rotation, coercive force, switching field, saturation field, and magnetization direction • Optimization of magnetic properties is crucial for the development of new functional materials and for many emerging technologies in integrated optics and photonics MO thin films & process parameters Photographs of a correctly annealed garnet-Bi2O3 nanocomposite thin film and of two other nanocomposite films of similar type, but over-annealed • Amorphous films: High optical absorption + no magnetism ⇒ Zero Faraday rotation • Crystallized films: Low optical loss + magnetization ⇒ High MO figures of merit are possible Q [°] = 2 * |ΘF| [°/µm] / α [µm-1] The optimized annealing regimes for highly Bi-substituted garnet materials are strongly dependent on the film composition Transmission(%) Absorption coefficient (cm-1) Bi2Dy1Fe5-xGaxO12 : Bi2O3 thin film materials and engineering of their optical properties Wavelength (nm) Wavelength (nm) • The parameters of importance are: absorption coefficient and specific Faraday rotation spectra. Co-deposition from a garnet-stoichiometric target + Bi2O3 target reduces absorption significantly (M. Vasiliev, M. N. Alam et al, Opt. Express 17(22), 19519–19535, 2009). • Correctly annealed films with optimized Bi2O3 content also show increased Faraday rotation (M. Vasiliev, M. Nur-E-Alam, K. Alameh et al, J. Phys. D Appl. Phys. 44(7), 075002, 2011). Bi2Dy1Fe5-xGaxO12 : Bi2O3 thin film materials and their properties – Faraday rotation Specific remnant magnetization SpecificFaraday Faraday rotation rotation, atat remnant magnetisation (deg/ (deg/ µ m) µm) 11 GGG \ Bi2Dy1Fe4Ga1O12, specific Faraday rotation measured in thin (150 nm) films 532, 10.12 10 532, 9.8 GGG \ Bi2Dy1Fe4Ga1O12, specific Faraday rotation measured in thick (> 500 nm) films 9 8 Material’s phase content depends on the process parameters Composite 300 W Bi2Dy1Fe4Ga1O12 + 90 W Bi2O3 layers on GGG measured specific Faraday rotation data points in films with t > 500 nm 7 Composite 200 W Bi2Dy1Fe4.3Ga0.7O12 + 25 W Bi2O3 layers on GGG measured specific Faraday rotation data points in films with t > 500 nm 6 MO Figure of Merit, GGG \ Bi2Dy1Fe4.3Ga0.7O12, specific Faraday rotation data points measured in thick (> 500 nm) films 5 Q = 2 * |ΘF| / A; ΘF = 0.1 – 10 °/µm; 4 A = 0.01 – (> 7000) cm-1 532, 4 3 We achieved: 635, 2.6 2 Q (green) ≈ 30° 670, 1.9 635, 1.66 670, 1.54 780, 0.89 Q (red) ≈ 50° 1 780, 0.67 635, 1.1 670, 0.79 780, 0.47 0 500 Optical properties of garnet layers depend significantly on the material phase 520 540 560 580 600 620 640 660 680 700 720 Wavelength (nm) Wavelength (nm) 740 760 780 800 820 Q (1550 nm range) is expected to be > 1000 Crystal structure properties of Bi2Dy1Fe5-xGaxO12 thin film materials 1600 (420) 1400 Intensity (arb. units) 1200 (422) Fe3O4 (642) 1000 Bi2Dy1Fe4Ga1O12: Bi2O3 composite film on glass, annealed at 580 °C (211) 800 (400) Fe3O4 (640) (444) (842) (800) (220) 600 Bi2Dy1Fe4.3Ga0.7O12: Bi2O3 composite film on glass, annealed at 560 °C (321) 400 Fe3O4 (521) 200 Bi2Dy1Fe4Ga1O12 film on glass, annealed at 620 °C 0 10 20 30 40 50 60 70 2Θ (degs) Stronger garnet-phase reflection peaks and weaker iron oxide peaks observed in high-performance oxide-mixed composites •Garnet phase with bcc cubic lattice type • Crystal lattice parameters have been calculated from XRD data • Average grain size 37 nm (agrees with TEM imaging results) 80 Magnetic properties of Bi2Dy1Fe5-xGaxO12 thin film materials 10 Downwards from "+" saturation Upwards from "-" saturation 8 Return path to memory state from point at 1580 Oe Coercive force (1.25 kOe) Faraday rotation (deg/mm) 6 Return path to memory state from point at 910 Oe back to near demagnetized state and into virgin magnetization loop Return path to memory state from point at 582 Oe 4 2 0 -3000 -2000 -1000 0 1000 2000 -2 -4 -6 -8 -10 Magnetic field (He) • Control over the magnetic hysteresis loop properties of garnet layers – an area of our ongoing research; crucial for the design of integrated optic devices using Faraday effect • Multiple remnant magnetization levels demonstrated in films with perpendicular magnetization (M. Nur-E-Alam, M. Vasiliev, and K. Alameh, Opt. Quantum Electron. 41(9), 661–669, 2009). 3000 Bi1.8Lu1.2Fe3.6Al1.4O12 Magneto-soft thin films • Low absorption coefficients observed Error due to all sources • High specific Faraday rotation 5.9 deg/µm at 532 nm 1.6 deg/µm at 635 nm 1.07 deg/µm at 660 nm • Measured MO quality factors (2ΘF/A) 13.9° (±1.6°) at 532 nm 15.7° (±2°) at 635 nm 12.7° (±0.7°) at 660 nm RF sputtered Bi1.8Lu1.2Fe3.6Al1.4O12 magnetically-soft thin films are very attractive for different magneto-optic applications and for designing novel magnetically-controlled photonic components Faraday-effect hysteresis loops Faraday rotation (deg/mm) Faraday rotation (deg/µm) Garnet layer on GGG, deposited @ 250 C -500 Garnet layer on GGG, deposited @ 680 C 6 Hc = (45 ± 5) Oe Hsat ~350 Oe 5 4 Hc = (10 ± 2) Oe Hsat ~200 Oe 3 2 1 0 -400 -300 -200 -100 -1 0 100 200 300 400 500 -2 -3 -4 • Strong substrate dependency of coercive force observed • Hc ~ 45 Oe for the films on GGG substrates deposited at 250 °C and Hc below 10 Oe obtained in films deposited at high substrate temperatures (680 °C). •Measured Faraday-effect magnetic field sensitivity at 532 nm: > 100 °/(cm·Oe) -5 -6 Magnetic field (Oe) (Oe) Magnetic field Hysteresis loop of Bi1.8Lu1.2Fe3.6Al1.4O12 MO films deposited onto (GGG) substrates •Low coercive force ⇒ lower external magnetic field required to control light through polarisation Magnetic domain structures: polarization microscopy (a) (b) 20 µm Substrate T=250° C Substrate T=680° C Domain structures observed in the absence of external magnetic fields using transmission-mode polarization microscopy Regular maze-type domains were observed in sputtered Bi1.8Lu1.2Fe3.6Al1.4O12 films deposited onto GGG at (a) 250 °C and (b) 680 °C substrate temperature Films deposited at high T(sub) are almost domain-free ⇒ almost in-plane magnetization Good crystalline quality, low coercive force values and high magnetic sensitivity achieved in our magnetically-soft garnet materials which are attractive for the development of reconfigurable nanophotonic devices and garnet waveguides Bi1.8Lu1.2Fe3.6Al1.4O12 : Bi2O3 nanocomposites and engineering of the material properties (BiLu)3(FeAl)5O12 + 4.5 vol% Bi2O3 annealed for 3 hrs @ 620 °C Composition type (BiLu)3(FeAl)5O12 + 4.5 vol% Bi2O3 annealed for 20 hrs @ 615 °C 34.5 20.85 25.6 18.03 (BiLu)3(FeAl)5O12 + 4.5 vol% Bi2O3 annealed for 5 hrs @ 615 °C 22.17 (BiLu)3(FeAl)5O12 + 4.5 vol% Bi2O3 annealed for 10 hrs @ 610 °C 22.1 (BiLu)3(FeAl)5O12 + 4.5 vol% Bi2O3 annealed for 5 hrs @ 610 °C 42.8 50.2 The effects of adjusting the garnet stoichiometry by cosputtering extra Bi2O3 have been studied; significantly improved material properties were achieved 27.5 20.6 High Faraday rotations 11.9 observed 635 nm MO figure of merit 15.7 Very low absorption Bi1.8Lu1.2Fe3.6Al1.4O12 532 nm MO figure of merit 13.9 deposited at T sub = 250 °C, coefficients measured annealed for 1 hr @ 650 °C (below 1000 cm-1 at 0 20 40 60 635 nm). MO figure of merit (degrees) High MO figures of merit measured at MO figures of merit measured in garnet and garnet-oxide 635 nm (more than composite films of type Bi1.8Lu1.2Fe3.6Al1.4O12 : Bi2O3 50°) Bi1.8Lu1.2Fe 3.6Al1.4O12 C Substrate T=250° deposited at T sub = 680 °C, annealed for 3 hrs @ 630 °C 42.8 Improved optical transparency achieved in nanocomposites Left: 650 nm-thick film of Bi1.8Lu1.2Fe3.6Al1.4O12 on a Gd3Ga5O12 (GGG) substrate; Right: 1150 nm-thick film of (Bi1.8Lu1.2Fe3.6Al1.4O12 + 20 vol.% co-sputtered Bi2O3) on a GGG substrate - both films are asdeposited Annealed (crystallized) films: Left: 1030 nm-thick (Bi2Dy1Fe4Ga1O12 +24 vol.% Bi2O3) on glass; Right: 1080 nm-thick Bi2Dy1Fe4.3Ga0.7O12 on GGG. Surface morphology and magnetic properties of Bi1.8Lu1.2Fe3.6Al1.4O12 : Bi2O3 nanocomposite thin films 2D image of garnet-oxide composite film Substrate T=250° C 3D image of garnet-oxide composite film Comparatively lower coercive force has been achieved for nanocomposite oxide-mixed films Nano-crystalline structure of garnet materials has been observed Applications of MO garnet films The garnet and garnet-oxide thin film materials possess an excellent combination of optical, magnetic and MO properties. Suitable for use in a wide range of emerging application areas • Nano-structured magnetic photonic crystals (MPC) for magneto-optic polarization controllers in a wide angular range (up to ± ΘFmax) • Ultrafast spatial or temporal modulators of light intensity • Non-reciprocal waveguide components • Dielectric permanent magnets with adjustable magnetic field landscapes over the film surface • Nano-engineered high-contrast magnetic field sensors and visualisers • Potential applications in biology (cell manipulation) 100 µm X 1000 Magnetic lattices for trapping ultra-cold atoms High resolution images of magnetic data tracks have been acquired using visible and UV polarisation microscopy Asymmetrical 2D magnetic lattice formed using a film of Bi2Dy1Fe4Ga1O12 sputtered onto a Si substrate (A. Abdelrahman et al, Phys. Rev. A 82(1), 012320, 2010). Ultra-fast spatial light modulators and image recognition systems CONCLUSION Bi-substituted MO garnet thin-film materials (both magnetically-soft and hard) with excellent optical and record-high MO quality have been demonstrated Sputter-deposition and oven annealing processes required for the manufacture of high-quality garnet films have been studied and the process parameters were optimized The combination of material properties achieved is of interest for the development of different emerging types of reconfigurable nano-photonic devices Our research work will be continued to further optimize the material properties and demonstrate the potential of garnets in a range of new applications Thank you Electron Science Research Institute, Edith Cowan University