Ultrashort Lifetime Expansion for Resonant Inelastic X-ray Scattering. Luuk Ament
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1 Ultrashort Lifetime Expansion for Resonant Inelastic X-ray Scattering Luuk Ament In collaboration with Jeroen van den Brink and Fiona Forte
2 What is RIXS? Resonant Inelastic X-ray Scattering Synchrotron radiation Interesting sample Momentum transfer q Energy loss 4p 1s Core-hole res (5-10 kev)
3 Why RIXS? Complementary to Raman and neutrons Momentum dependence Tune X-rays to different resonances Small samples Why not?
4 Outline 1. Framework: the UCL expansion What can one measure? 2. Charge excitations 3. Magnetic RIXS on La 2 CuO 4 Coupling of core-hole to spins Cu K-edge: indirect RIXS Cu L-edge: direct RIXS 4. Orbital RIXS on LaMnO 3
5 Typical RIXS spectra M.Z. Hasan et al. Science 288, 1811 (2000)
6 What happens in detail 4p empty initial intermediate final conduction valence 1s core U core U core
7 What happens in detail 4p empty initial intermediate Ultrashort Core-hole Lifetime (UCL): Integrate out intermediate states! final conduction valence 1s core U core U core
8 Theory Kramers-Heisenberg relation with Detuning from Inverse core-hole Intermediate states resonance lifetime
9 Theory - UCL expansion Scattering amplitude Using the Ultrashort Core-hole Lifetime gives
10 What does RIXS measure? We obtain Valence electrons Interaction of valence electrons with core-hole Intermediate state Hamiltonian Assume immobile core-hole, and local core-hole potential Arbitrary range hopping & Coulomb interactions At T = 0, approximate for both strong and weak potentials J. van den Brink & M. van Veenendaal, EPL 73, 121 (2006) L. Ament, F. Forte & J. van den Brink, PRB 75, (2007)
11 What does RIXS measure? Spinless fermions: with Charge density Fermions with spin: Resonant prefactor Charge density Longitudinal spin density J. van den Brink & M. van Veenendaal, EPL 73, 121 (2006) L. Ament, F. Forte & J. van den Brink, PRB 75, (2007)
12 What does RIXS measure? Conclusion: core-hole couples to charge. RIXS measures charge density and longitudinal spin density (= higher order charge density correlation function). Can we probe other excitations than charge ones? Data on Cu K-edge of La 2 CuO 4 below Mott gap (~ 2 ev) 500 mev peak! Phonons? d-d excitation? Magnons? Nd 2 CuO 4 : no shift J. van den Brink & M. van Veenendaal, EPL 73, 121 (2006) L. Ament, F. Forte J. Hill & J. et al., van arxiv: den Brink, PRB 75, (2007)
13 Magnetic RIXS on La 2 CuO 4 Perovskite layers of CuO 2 : Cu 3d e g holes at low energy: Single band Hubbard model Ground state is antiferromagnetically ordered Collective excitations: magnons
14 Magnetic RIXS on La 2 CuO 4 How does the core-hole couple to the spins? Go back to Hubbard model! K-edge: Hopping amplitude t Coulomb repulsion U Core-hole locally modifies superexchange! Coulomb repulsion U - U c
15 Magnetic RIXS on La 2 CuO 4 How does the core-hole couple to the spins? Indirect RIXS locally modifies superexchange! To first order in UCL: At T = 0, 2-magnon excitations are probed: 4-spin correlation function J. van den Brink, cond-mat/ F. Forte, L. Ament & J. van den Brink, arxiv:
16 Magnetic RIXS on La 2 CuO 4 Selection rule: vanishing intensity at q = (0,0) and q = (, ) J. Hill et al., arxiv: F. Forte, L. Ament & J. van den Brink, arxiv:
17 Magnetic RIXS on La 2 CuO 4 F. Forte, L. Ament & J. van den Brink, arxiv: Improve theory with longer range interactions: Theory J Theory + experimental resolution J. Hill et al., arxiv: Values from neutron scattering. Coldea et al., PRL 86, 5377 (2001)
18 Magnetic RIXS on La 2 CuO 4 F. Forte, L. Ament & J. van den Brink, arxiv: J. Hill et al., arxiv:
19 Magnetic RIXS on La 2 CuO 4 L-edge: direct RIXS - photoexcited electron in 3d-shell. G. Ghiringhelli et al. are measuring this right now! Sneak preview: 1. Dispersive feature similar to K-edge RIXS, becoming elastic in the low-q limit. 2. Another feature appearing at q = 0 around = 3 J. 3. This feature disappears off-resonance. What about the theory?
20 Magnetic RIXS on La 2 CuO 4 L-edge: direct RIXS - core-electron ends up in 3d-state Back to Hubbard model! The extra 3d-electron locally blocks superexchange The UCL results for the K-edge and L-edge are the same!
21 Magnetic RIXS on La 2 CuO 4 L-edge has more intensity than K-edge. Can we go beyond the UCL approximation? Reminder Off-resonance: bigger, and becomes more important! Currently, q = 0 is being measured by G. Ghiringhelli et al. To be continued!
22 Outlook - Orbital RIXS LaMnO 3 has a cubic structure: e g t 2g MnO 6 octahedron induces crystal field: 3d e g t 2g LaMnO 3 : A-type AFM order: spins align FM in each layer.
23 Orbital RIXS Kugel-Khomskii model without Hund s rule coupling: To first order, orbitals of different layers decouple! e g orbitals order antiferro-orbitally : e g t 2g Order by superexchange and/or Jahn-Teller distortion of octahedra Excitations: e g orbital waves (analogous to spin waves)
24 Orbital RIXS Initial Intermediate Final e g Looks like Heisenberg, but no conservation of pseudo- S z. This leads to single orbiton excitations. S. Ishihara & S. Maekawa, PRB 62, 2338 (2000) J. van den Brink, P. Horsch, F. Mack & A. M. Oles, PRB 59, 6795 (1999)
25 Orbital RIXS How does Initial the core-hole couple to the e g orbitals? Final 4p U =U+U c 4p 3d e g Intermediate 3d e g 1s Again, core-hole locally U =U-U c modifies superexchange! 1s
26 Orbital RIXS Orbital RIXS spectrum for LaMnO 3 Two-orbiton continuum J = 25 mev One-orbiton peak Experimental limitations: Resolution = 100 mev, inelastic peak
27 Conclusions Experimental progress is enormous Theoretical spectra can be easily obtained with the UCL expansion using e.g. a model Hamiltonian We now know which charge correlation functions we measure in indirect RIXS Both direct and indirect RIXS are a new probe for magnons (La 2 CuO 4 ) We can possibly detect orbitons in the manganites!
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