Resonant Inelastic X-ray Scattering on elementary excitations

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1 Resonant Inelastic X-ray Scattering on elementary excitations Jeroen van den Brink Ament, van Veenendaal, Devereaux, Hill & JvdB Rev. Mod. Phys. 83, 705 (2011) Autumn School in Correlated Electrons Jülich

2 Outline 1. Introducing RIXS 2. Magnetic RIXS on low dimensional magnets

3 1. Introducing RIXS Basic Scattering Process Direct & Indirect RIXS 5 features of RIXS Elementary Excitations Accessible to RIXS Progress in past decade

4 2. Magnetic RIXS on low dimensional magnets Quasi 2D cuprates Quasi Some 1D theory cuprates Quasi Some 2D experiments iron pnictide A (big) Quasi open 2D iridate problem Doped Cu & Fe systems

5 2. Magnetic RIXS on low dimensional magnets Quasi 2D cuprates Some theory Some experiments A (big) open problem

6 Basic Scattering Process Direct and Indirect RIXS

7 What is Resonant Inelastic X-ray scattering RIXS X-ray scattering: photon in! solid! photon out inelastic: ω out < ω in Cu K-edge resonant: tune ω in to an atomic absorption edge 4 p ~9 KeV 1 s

8 What is Resonant Inelastic X-ray scattering RIXS X-ray scattering: photon in! solid! photon out inelastic: ω out < ω in Cu K-edge resonant: tune ω in to an atomic absorption edge 4 p ~9 KeV 1 s

9 What is Resonant Inelastic X-ray scattering RIXS X-ray scattering: photon in! solid! photon out inelastic: ω out < ω in Cu K-edge resonant: tune ω in to an atomic absorption edge 4 p ~9 KeV INDIRECT Momentum transfer: q Energy loss 1 s

10 What is Resonant Inelastic X-ray scattering RIXS Cu L-edge X-ray scattering: photon in! solid! photon out inelastic: ω out < ω in resonant: tune ω in to an atomic absorption edge 3 d ~900 ev 2 p DIRECT Momentum transfer: q Energy loss resolution < 100 mev

11 Direct and Indirect RIXS DIRECT scattering via absorptionemission matrix elements scattering via intermediate state core-hole shake-up INDIRECT

12 RIXS = GS XAS INTERMEDIATE XES FS Local atomic transition Complicated state with strong core-hole potential Local atomic transition Contains chemical detail and atom specific physics But: RIXS = GS... FS Carries low energy, long wavelength, elementary excitations Universal effective low energy (magnetic) behavior

13 RIXS amplitude F and intensity I Intensity Amplitude ω loss momentum in out q loss =k -k

14 RIXS amplitude F and intensity I polarization in out Intensity Amplitude ω loss momentum in out energy conservation final energy ω out initial energy ω in

15 2nd Order: Resonant Scattering RIXS amplitude Kramers-Heisenberg expression RIXS transition operator H.A. Kramers and W. Heisenberg, Z. Phys. 31, 681 (1925)

16 Greens function expression for RIXS amplitude RIXS amplitude Greens function with =intermediate state propagator so that:

17 5 distinguishing features of RIXS

18 Why X-rays: Inelastic Scattering momentum ~ Å -1 with X-rays at a resonance probe charged excitations have angular momentum l=1 polarization dependence Solid: Lattice spacings ~ Å Brillouin zone ~ Å -1 Visible Photons: momentum ~ 10-3 Å -1 X-rays at 10 kev momentum ~ 5 Å -1 several BZ s

19 ' =50 ' z~ y~ x~ =69 z(a) y(c) x(b)

20

21 Why At resonance: enhanced loss features Inelastic Scattering with X-rays at a resonance choose element & electronic shell X-ray Absorption Edges K-edges L-edges TM X-ray penetration depth: ~microns RIXS is bulk sensitive Atomic #

22 Tunable X-ray sources synchrotron ESRF Grenoble

23 Tunable X-ray sources synchrotron X-ray laser ESRF Grenoble LCLS, Stanford

24 X-ray spectrometers ESRF ID32 Soft RIXS: TM L-edges

25

26

27 Elementary Excitations accessible to RIXS

28 Elementary Excitations in TMO: Schematic dipolar Couple to Charge quadru polar dipolar Couple to Angular Momentum

29 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p

30 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p

31 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p

32 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p

33 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p s=1/2 l=1

34 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p s=1/2 l=1 l s

35 Direct TM L-edges Cu L-edge 3 d ~900 ev Momentum transfer Energy loss 2 p s=1/2 l=1 l s

36 Direct TM L-edges dd excitation Cu L-edge spin flip 3 d ~900 ev Momentum transfer Energy loss 2 p

37 Direct TM L-edges dd excitation Cu L-edge spin flip 3 d ~900 ev Momentum transfer Energy loss 2 p Ir L-edge ~11.2 kev

38

39 Progress in the Past Decades

40 Cu L-edge resolution dd zero-loss magnon

41 Cu L-edge resolution dd zero-loss magnon phonon COURTESY Lucio Braicovich ESRF Beamline ID

42 Summary part I Direct and Indirect RIXS RIXS measures excitation energy & momentum Polarization in/out dependence can be studied Element and orbital sensitive Bulk sensitive & needs small sample volumes Measures charge neutral elementary excitations spin, orbital, lattice, charge excitons Great progress in resolution in the past decade

43 2. Magnetic RIXS on low dimensional magnets Quasi 2D cuprates Quasi 1D cuprates Quasi 2D iron pnictide Quasi 2D iridate Doped Cu & Fe systems

44 Quasi 2D cuprates

45 La 2 CuO 4 crystal structure CuO 2 layer (LaO) 2 layer CuO 2 layer (LaO) 2 layer CuO 2 layer

46 La 2 CuO 4 magnetic structure strongly correlated antiferromagnet spin 1/2 insulator gap ~2 ev U ~ 6 ev

47 Atomic Model: Local d-d orbital splitting: Cu 2+ Cubic Crystal field splitting Cu 2+ 3d9 e g orbitals t 2g orbitals e g 5x t 2g

48 Ultra-short Core-hole Life-time expansion RIXS amplitude short life-time τ of the high energy core-hole large core-hole broadening Γ=ħ/τ large constant RIXS response governed by (dipole) transition operators

49 RIXS transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

50 RIXS transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

51 RIXS transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

52 RIXS transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

53 RIXS transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

54 Orbital excitations by direct RIXS on La 2 CuO 4 d-d excitations Moretti, Bisogni, Aruta, Balestrino, Berger, Brookes, Luca, Castro, Grioni, Guarise, Medaglia, Miletto, Minola, Perna, Radovic, Salluzzo, Schmitt, Zhou, Braicovich & Ghiringhelli, NJP 13, (2011)

55 RIXS spin-flip transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

56 RIXS spin-flip transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

57 RIXS spin-flip transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

58 RIXS spin-flip transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) Marra, Wohlfeld & JvdB, PRL 109, (2012)

59 RIXS spin-flip transition metal L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) x 2 -y 2 spin NOT // z: pure spin flip Marra, Wohlfeld & JvdB, PRL 109, (2012)

60 High Magnetic resolution RIXS on Cu La L-edge 2 CuO 4 Cu spectrum L-edge In special cases direct spin-flip scattering is allowed at Cu L-edge CuO s are such special cases... magnon phonon zero-loss bimagnon

61 Magnetic direct RIXS on La 2 CuO Cu L-edge Ament, Ghiringhelli, Moretti, Braicovich & JvdB, PRL 103, (2009) magnon dispersion Braicovich, JvdB et al., PRL 104, (2010)

62 RIXS magnon dispersion of Sr 2 CuO 2 Cl 2 deviation from simple Heisenberg > transferred momentum q Guarise et al., PRL 105, (2010)

63 Magnetic L-edge RIXS on 8% doped La 2-x Sr x CuO 4 Tc = 21K d-d excitation paramagnon Braicovich, JvdB et al. PRL 104, (2010)

64

65 magnon paramagnon

66 Dynamical structure factor Hubbard model, QMC magnon paramagnon U=8t Jia, Nowadnick, Wohlfeld, Kung, Chen, Johnston, Tohyama, Moritz & Devereaux Nat. Comm. 5, 3314 (2014)

67 Summary part 2 RIXS sensitive to magnetic excitations of e.g. low D cuprates, iron pnictides and iridates Magnons, spinons and paramagnons are observed Dispersion of these modes can be determined Observed paramagnons are challenge for theory It can reasonably be assumed that the future of RIXS is even brighter than its past More and better experiments, instruments, theory

68 RIXS amplitude/intensity Interaction light & matter

69 RIXS amplitude F and intensity I Intensity Amplitude ω loss momentum in out q loss =k -k

70 RIXS amplitude F and intensity I polarization in out Intensity Amplitude ω loss momentum in out energy conservation final energy ω out initial energy ω in

71 Interaction of light and matter: Hamiltonian kinetic Zeeman Darwin electron-nucleus electron-electron free photons vector potential spin-orbit coupling plane wave

72 Lowest order perturbing Hamiltonian: small A small Fermi Golden Rule, to second order: transition rate

73 2nd Order... Fermi Golden Rule, to second order: transition rate

74 2nd Order... Fermi Golden Rule, to second order: transition rate

75 2nd Order: Resonant Scattering I RIXS amplitude small RIXS amplitude RIXS transition operator Kramers-Heisenberg expression H.A. Kramers and W. Heisenberg, Z. Phys. 31, 681 (1925)

76 2nd Order: Resonant Scattering II RIXS amplitude RIXS intensity: This expression is essentially exact (non-relativistic limit)

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