X-ray non-resonant and resonant magnetic scattering Laurent C. Chapon, Diamond Light Source. European School on Magnetism L. C.

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X-ray non-resonant and resonant magnetic scattering Laurent C. Chapon, Diamond Light Source 1

The Diamond synchrotron 3 GeV, 300 ma

Lienard-Wiechert potentials n.b: Use S.I units throughout. rq : position of the charge r : position of the observer The retarded time tr: 3

Lienard-Wiechert potentials By changing variable: and considering the Jacobian, one finds: with The difficulty is in evaluating the vector fields at time t. This involves derivatives with a lot of chain rules. 4

Fields The far-field part of the electric field is: One can also prove that: These expressions are evaluated at the retarted time tr. 5

Dipole radiation and forward emitting cone with relativistic epoynting vector: 6

Brilliance and polarisation Bending Magnet Insertion Device Very small angular opening of the forward emittance cone (fraction of a mrad) Highly polarised radiation in the synchrotron orbit plane 7

Synchrotron brilliance versus transistor/inch 2 8

Conventions : Vertical geometry p k s 2q Q p k s s and p refer to linear polarisation of light perpendicular and parallel to the scattering plane 9

Conventions: Horizontal geometry s p s p k 2q Q k s and p refer to linear polarisation of light perpendicular and parallel to the scattering plane 10

Circular polarisation k k 11

Scattering X-ray kf dw F0 ki Transition rate, second order perturbation theory: 12

Maxwell's equations In the absences of charges and currents (free space), the solutions are plane-waves: 13

Quantizing the free electromagnetic field It is convenient to work in the Coulomb (radiation) Gauge, by setting: 14

Quantizing the free electromagnetic field The Gauge condition implies: transverse waves with two orthogonal polarization states. Electromagnetic energy: 15

Quantizing the free electromagnetic field 16

Electromagnetic field potential for a charge Lorentz force is not conservative (depends on speed) Using : 17

Hamiltonian of a charged particle in an EMF (no spin) Generalized momentum: 18

Zeeman & Spin-orbit coupling terms See Thomas factor for example in Jackson Classical Electromagnetism 19

Full Hamiltonian charge in an EMF Kinetic Zeeman SO coupling Coulomb EMF self-energy 20

Perturbing Hamiltonian Refers to Blume, 1985 Terms square in A contribute to the first order scattering term Terms linear in A contribute to the second order scattering term 21

First and second order terms Annihilate photon first Create photon first 22

Non-resonant contribution of second-order terms Using Need to evaluate 4 commutators, with the help of : 23

Magnetic contribution Here, lj and sj are given in units of 24

Separation of L and S p p 2q s s 25

Summary non-resonant magnetic X-ray scattering Rest mass of the electron =511 kev At 1 kev, scattering cross section 3.8 10-6 smaller than Thomson scattering. Only a few unpaired electrons contribute to the magnetic scattering vs. all electrons in the Thomson scattering. However, the flux available largely compensate for the weak scattering cross section. 26

Non-resonant magnetic scattering Cu 3Nb2O8 R. Johnson, Phys. Rev. Lett. (2011)

BiFeO3 : Non resonant micro-focused magnetic diffraction 1=( δ, δ, 0 ) P(c)

BiFeO3 : Non resonant micro-focused magnetic diffraction 50 mm resolution

BiFeO3 : Non resonant micro-focused magnetic diffraction L R p s q p' Q ki Experiment off resonance, 5.8 KeV R. D. Johnson,et al., Phys. Rev. Lett. 110, 217206 (2013) s' kf q h

BiFeO3 : Homochiral domains c c c k1=(d,d,0) P k2=(d,-2d,0) P k1=(d,d,0) P k3=(-2d,d,0) P k2=(d,-2d,0) P k3=(-2d,d,0) P

Resonant X-ray magnetic scattering Tune the energy of the X-ray beam to an absorption edge Photon is absorbed and the system re-emit a photon with the same energy Element specific information Combine the element specific information from spectroscopy techniques with Bragg scattering Polarization dependence effects Possibility to probe magnetic order but also other E/M-multipoles

Resonant X-ray magnetic scattering We need to evaluate the matrix elements: E1 E3 E2 M1 M2 M3 The power expansion is justified by the fact that the spatial extend of the core electron is relatively small (~0.1 A) We also use the following commutator, to switch to position representation 33

Resonant X-ray magnetic scattering : E1-E1 [1] J. P. Hill and D. F. McMorrow, X-ray resonant exchange scattering: polarization dependence and correlation functions, Acta Crystallogr., vol. A52, pp. 236 244, 1996. 34

Resonant X-ray magnetic scattering GdMn2O5 q=(1/2,0,0) Incommensurate q=(1/2+d,0,0.2) N. Lee, Phys. Rev. Lett. 110, 137203 (2013)

Resonant X-ray magnetic scattering GdMn2O5 E1-E1 LIII Gd Off-resonance Pb Pb b a N. Lee, Phys. Rev. Lett. 110, 137203 (2013)

Probing different multipolar orders [1] S. Di Matteo, Resonant x-ray diffraction: multipole interpretation, J. Phys. D. Appl. Phys., vol. 45, no. 16, p. 163001, 2012. 37

Note on link between cross section and absorption spectroscopy Optical theorem XMCD XMLD 38

Magnetic X-ray holography Thomas A. Duckworth, Feodor Ogrin, Sarnjeet S. Dhesi, Sean Langridge, Amy Whiteside, Thomas Moore, Guillaume Beutier, and Gerrit van der Laan, "Magnetic imaging by x-ray holography using extended references," Opt. Express 19, 16223-16228 (2011) 39

Ptychography [1] C. Donnelly et al., Three-dimensional magnetization structures revealed with X-ray vector nanotomography, Nature, vol. 547, no. 7663, pp. 328 331, 2017.

Neutrons and X-ray for magnetic scattering Neutron Born approximation valid Magnetic ~ nuclear scattering amplitude Very little beam heating low T Large penetration depth, bulky sample environments (magnets, dilution.) Manipulate polarization and analysis but costly (flux) Large divergence, relatively poor Q-resolution Lack of spatial resolution Flux typically up to 1010 n.cm-2.s-1 (scattering volume) No direct L/S separation (only by fitting form factor) X-ray Off resonance can get quantitative M but scaling to charge scattering not always easy (use of attenuators for charge scattering...) Magnetic Xs much smaller but compensated by flux. Beam heating can be a problem not straightforward to go to dilution T Not easy to do k=0 work Manipulate polarization and analysis Highly collimated, excellent Q-resolution Spatial resolution down to 20nm High brilliance and flux Direct L/S separation Resonant element specific Resonant probe tensor beyond magnetic dipole 41