Femtosecond Heating as a Sufficient Stimulus for Magnetization Reversal

1. Theoretical/Modelling Contributions T. Ostler, J. Barker, R. F. L. Evans and R. W. Chantrell Dept. of Physics, The University of York, York, United Kingdom. U. Atxitia and O. Chubykalo-Fesenko Instituto de Ciencia de Materiales de Madrid, CSIC, Cantoblanco, Madrid, Spain.D. Afansiev and B. A. IvanovInstitute of Magnetism, NASU Kiev, Ukraine. Femtosecond Heating as a Sufficient Stimulus for Magnetization Reversal HGST, San Jose, August 2012

2. Experimental Contributions S. El Moussaoui, L. Le Guyader, E. Mengotti, L. J. Heyderman and F. NoltingPaul ScherrerInstitut, Villigen, SwitzerlandA. Tsukamoto and A. ItohCollege of Science and Technology, Nihon University, Funabashi, Chiba, Japan. A. M. Kalashnikova , K. Vahaplar, J. Mentink, A. Kirilyuk, Th. Rasing and A. V. KimelRadboud University Nijmegen, Institute for Molecules and Materials, Nijmegen, The Netherlands. Femtosecond Heating as a Sufficient Stimulus for Magnetization Reversal HGST, San Jose, August 2012

3. Ostleret al.,Nature Communications, 3, 666 (2012).

4. Outline • Model outline: atomistic LLG of GdFeCo and laser heating • Static properties of GdFeCo and comparison to experiment • Transient dynamics under laser heating • Deterministic switching using heat and experimental verification • Mechanism of reversal

5. Background σ- • Inverse Faraday[1,2] effect relates E-field of light to generation of magnetization. • Can be treated as an effective field with the chirality determining the sign of the field. σ+ M(0) Inverse Faraday effect • Control of magnetization of ferrimagneticGdFeCo[3] • High powered laser systems generate a lot of heat. • What is the role of the heat and the effective field from the IFE? [1] Hertel, JMMM, 303, L1-L4 (2006). [2] Van derZielet al., Phys Rev Lett15, 5 (1965). [3] Stanciuet al. PRL, 99, 047601 (2007).

6. A model of laser heating Laser input P(t) two temperature model energy transfers • Recall for circularly polarised light, magnetization induced is given by: • For linearly polarized light cross product is zero. Energy transferred as heat. • Two-temperature[1]model defines an electron and phonon temperature (Te and Tl) as a function of time. • Heat capacity of electrons is smaller than phonons so see rapid increase in electron temperature (ultrafast heating). Electrons Lattice Gel e- e- e- e- Two temperature model [1] Chen et al. International Journal of Heat and Mass Transfer.49, 307-316 (2006)

7. Model: Atomistic LLG • We use a model based on the Landau-Lifshitz-Gilbert (LLG) equation for atomistic spins. • Time evolution of each spin described by a coupled LLG equation for spin i. • Hamiltonian contains only exchange and anisotropy. • Field then given by: • is a (stochastic) thermal term allowing temperature to be incorporated into the model. For more details on this model see Ostleret al. Phys. Rev. B.84, 024407 (2011)

8. Model: Exchange interactions/Structure • GdFeCo is an amorphous ferrimagnet. • Assume regular lattice (fcc). • In the model we allocate Gd and FeCo spins randomly. Fe-Gd interactions are anti-ferromagnetic (J<0) Fe-Fe and Gd-Gd interactions are ferromagnetic (J>0) Fe Gd Atomic Level Sub-lattice magnetization For more details on this model see Ostleret al. Phys. Rev. B.84, 024407 (2011)

9. Bulk Properties • Exchange values (J’s) based on experimental observations of sublattice magnetizations as a function of temperature. • Compensation point and TC determined by element resolved XMCD. • Variation of J’s to get correct temperature dependence. • Validation of model by reproducing experimental observations. compensation point Figure from Ostler et al. Phys. Rev. B.84, 024407 (2011)

10. Bulk Properties • Experimental hysteresis loops (measured for both Fe and Gd species) show out-of-plane magnetisation (see reference below for sample loops). • Experiments of various compositions of GdFeCo (with different compensation points) show diverging coercive field at compensation point. • Qualitative agreement with atomistic model. Figure from Ostler et al. Phys. Rev. B.84, 024407 (2011)

11. Summary so far Atomic level model of a ferrimagnet with time A way of describing heating effect of fs laser • We investigate dynamics of GdFeCo and show differential sublattice dynamics and a transient ferromagnetic state. • Then demonstrate heat driven reversal via the transient ferromagnetic state. • Outline explanation is given for reversal mechanism.

12. Transient Dynamics in GdFeCo by XMCD & Model • Femtosecond heating in a magnetic field. • Gd and Fe sublattices exhibit different dynamics. • Even though they are strongly exchange coupled. Experiment Model results Figures from Raduet al.Nature 472, 205-208 (2011).

13. (an aside) Demagnetisation in ferromagnetic Ni50Fe50 • Femtosecond heating shows decoupled behaviour in NiFe. • Sublattice magnetizations are measured by element specific XMCD. • Each sublattice demagnetises on a different timescale. Experiment Model results Experiments performed by I. Radu

14. Demagnetisation in ferrimagnetic GdFeCo • High fluence completely demagnetises GdFeCo as temperature quickly increases over the Curie temperature. • Again, dispite strong antiferromagnetic exchange coupling the two sublattices demagnetise at different rates. Experiment Model results Experiments performed by I. Radu

15. Timescale of Demagnetisation Experiment • Characteristic demagnetisation time can be estimated as[1]: • GdFeCo has 2 sublattices with different moment (µ). • Even though they are strongly exchange coupled the sublattices demagnetise at different rates (with µ). Model results [1] Kazantsevaet al. EPL, 81, 27004 (2008). Figures from Raduet al.Nature 472, 205-208 (2011).

16. Transient Ferromagnetic-like State Laser heating in applied magnetic field of 0.5 T • System gets into a transient ferromagnetic state at around 400 fs. • Transient state exists for around 1 ps. • As part of a systematic investigation we found that reversal occuredin the absence of an applied field. Figure from Raduet al.Nature 472, 205-208 (2011).

17. Numerical Results of Switching Without a Field • Very unexpected result that the field plays no role. • Is this determinisitic? No magnetic field GdFeCo

18. Sequence of pulses • Do we see the same effect experimentally?

19. Experimental Verification: GdFeCo Microstructures Initial state - two microstructures with opposite magnetisation - Seperated by distance larger than radius (no coupling) 2mm XMCD Experimental observation of magnetisation after each pulse.

20. Experimental Verification: GdFeCo Thin Films • After action of each pulse the magnetization switches, independently of initial state. Fe Initially film magnetised “up” Gd MOKE • Similar results for film initially magnetised in “down” state. • Beyond regime of all-optical reversal, i.e. cannot be controlled by laser polarisation. Therefore it must be a heat effect.

21. What about the Inverse Faraday Effect? • Orientation of magnetization governed by light polarisation. Stanciuet al. PRL, 99, 047601 (2007) Does not depend on chirality (high fluence) Depends on chirality (lower fluence)

22. What about the Inverse Faraday Effect?

23. The Effect of Compensation • Previous studies have tried to switch using the changing dynamics at the compensation point[ref]. • Simulations show starting temperature not important. • Supported by experiments on different compositions of GdFeCo support the numerical observation.

24. Effect of a stabilising field • What happens now if we apply a field to oppose the formation of the transient ferromagnetic state? • Is this a fragile effect? 10 T Bz=10,40,50 T 40 T 50 T GdFeCo • Suggests probable exchange origin of effect (more later).

25. Mechanism of Reversal FMR Exchange • After heat pulse TM moments more disordered than RE (different demagnetisation rates). • On small (local) length scale TM and RE random angles between them. • The effect is averaged out over the system. • Exchange mode is excited when sublattices are not exactly anti-parallel.

26. Mechanism of Reversal end of pulse RE • If we decrease the system size then we still see reversal via transient state. • For small systems a lot of precession is induced. • Frequency of precession associated with exchange mode. • For systems larger than 20nm3 there is no obvious precession induced (averaged out over system). • Further evidence of exchange driven effect. TM TM end of pulse TM sublattice

27. Importance of Moments • As previously stated, the short time-scale demagnetisation time is governed by the magnitude of the correlator. • If we artificially make the local magnetic moments equal, the correlators are equal and no switching occurs. μTM=μRE

28. Summary • Demonstrated numerically switching can occur using only a heat pulse without the need for magnetic field. • Switching is deterministic. • Verified the mechanism experimentally in microstructures (and thin films, see paper). Shown that stray fields play no role. • The magnetic moments are important for switching. • Demonstrated a possible explanation via a local excitation of exchange mode by decreasing system size and observing induced precession.

29. Acknowledgements • Experiments performed at the SIM beamline of the Swiss Light Source, PSI. • Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO), de Stichting voor Fundamenteel Onderzoek der Materie (FOM). • The Russian Foundation for Basic Research (RFBR). • European Community’s Seventh Framework Programme (FP7/2007-2013) Grants No. NMP3-SL-2008-214469 (UltraMagnetron) and No. 214810 (FANTOMAS), • Spanish MICINN project FIS2010-20979-C02-02 • European Research Council under the European Union’s Seventh Framework Programme (FP7/2007- 2013)/ ERC Grant agreement No 257280 (Femtomagnetism). • NASU grant numbers 228-11 and 227-11. • Thank you for listening.

30. Mechanism of Reversal FMR Exchange • After heat pulse TM moments more disordered than RE (different demagnetisation rates). • On small (local) length scale TM and RE random angles between them. • The effect is averaged out over the system. • Exchange mode is excited when sublattices are not exactly anti-parallel.

31. Numerical Model • Dynamics of each spin given by Landau-Lifshitz-Gilbert Langevin equation. • Effective field given by: • Moments defined through the fluctuation dissipation theorem as: • Energetics of system described by Hamiltonian:

32. Landau-Lifshitz-Bloch equation of motion • So far we have used a model for each atomic magnetic moment. • A macro-spin approach should show the same behaviour. • We write a Landau-Lifshitz-Bloch (LLB) equation for the TM and RE sublattices. Usual precession and damping term Longitudinal relaxation of magnetisation (submitted) Full details of model from Atxitia el al. Arxiv 1206.6672

33. Relaxation Rates • Temperature dependent relaxation rates are important for ultrafast switching. • Sign in highlighted area below changes sign. • However, this change in sign alone cannot result in switching! • Different longitudinal relaxation is very important but does not produce switching. (submitted) Full details of model from Atxitia el al. Arxiv 1206.6672

34. Experimental Prediction • Could we see reversal via this dynamical path experimentally? • Effect is averaged out over large systems. LLG

35. Linearising the LLB Equation • From the atomistic simulations, after the pulse is turned off we assume that. Linearise Note: to simplify the analysis we have assumed a square pulse from 0K->1500K->0K

36. Perpendicular Component no transverse component, no switching (dashed) • LLB analysis shows that we require a perpendicular component to induce switching. LLB simulation small transverse component leads to switching (solid) • In LLG simulations, high thermal fluctuations give rise to local perpendicular component. • Note: high frequency of oscillations associated with exchange mode.

37. System Close to Reversal • Analysis shows that when the temperature is lowered there is a transfer of angular momentum from the (unstable) linear (mz) component to transverse (ρ). • Requires a small initial transverse component. T Different pulse heights lead to different state before pulse turned off. t LLB LLG

38. Transient Ferromagnetic-like State Laser heating in applied magnetic field of 0.5 T • For short time sublattices align against TM-RE exchange interaction • “State” exists for around 1ps Figure from Raduet al.Nature 472, 205-208 (2011).

39. Importance of moments μTM=μRE

40. Linear Reversal • Usual reversal mechanism (in a field) below TC via precessional switching • At high temperatures, magnetisation responds quickly without perpendicular component (linear route[1]). • Laser heating results in linear demagnetisation[2].

41. The Effect of Heat • Ordered ferromagnet • Uniaxial anisotropy E Heat E E 50% 50% Cool θ M+ M- M+ M- M+ M- Cool below TC Heat (slowly) through TC System demagnetised Equal chance of M+/M-

42. Inverse Faraday Effect • Magnetization direction governed by E-field of polarized light. • Opposite helicities lead to induced magnetization in opposite direction. • Acts as “effective field” depending on helicity (±). σ+ z σ- z http://en.wikipedia.org/wiki/Circular_polarization Hertel, JMMM, 303, L1-L4 (2006)

43. Outlook • Currently developing a macro-spin model based on the Landau-Lifshitz-Bloch (LLB) formalism to further support reversal mechanism. • How can our mechanism be observed experimentally? Time/space/element resolved magnetisation observation → spin-spin correlation function/structure factor. • Once we understand more about the mechanism, can we find other materials that show the same effect?

44. Differential Demagnetization • Atomistic model agrees qualitatively with experiments • Fe and Gd demagnetise in thermal field (scales with μ via correlator) Kazantsevaet al. EPL, 81, 27004 (2008). Gd slow, ~1ps Fe fast, loses magnetisation in around 300fs Raduet al.Nature 472, 205-208 (2011).

45. What’s going on? 0 ps - Ground state -T>TC Fe disorders more quickly (μ) 0.5 ps -T<TCprecessional switching (on atomic level) -Exchange mode between TM and RE - Transient state 1.2 ps 10’s ps time

46. Reversal • Trivial solution in which transverse component is zero is unstable in regime of reversal. • Perturbations from zero lead to generation of perpendicular component in TM. This triggers the same motion of RE via angular momentum transfer. LLB • This process occurs on small length scales so effect can be averaged out in atomistic model. • By decreasing system size we see this effect. LLG

48. Differential demagnetization times

49. How Can Magnetization Be Reversed? Magnetic Field Circularly Polarised Spin Injection E E Bz Bz M+ M- M+ M-

50. The Effect of Heat E E 50% 50% M+ M- M+ M- M+ M- E E ? M+ M- M+ M-