Excitations and Interactions

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Excitations and Interactions Magnon gases A7 A8 Spin physics A3 A5 A9 A10 A12 Quantum magnets A3 A8 B1 B2 B3 B4 B5 Synthesis B4 B6 B10 E Spectroscopy B11

Excitations and Interactions Charge-transfer induced changes in orbital occupation NEXAFS Real Systems B10 E B4 B2 Core-level shift at the charge-order transition HAXPES B6 B4 Many-body effects and density of states near E F STS B11 B6 Anisotropic strain in ferroelectric CT system CS

Excitations and Interactions B10 E B4 B2 CT Element-specific probe of unoccupied states pure donor hn 532 ev hn 399 ev Tuneable soft X-rays CT complex @ ANKA (Karlsruhe); MAXLAB (Lund) JACS 134, 4694 (2012)

NEXAFS on novel organic charge-transfer complexes Highlight: Novel CT-complexes based on pyrene derivatives or DTBDT with TCNQ CT-complex UHV-deposited and solution-grown crystallites Theory explains shifts of donor and acceptor orbitals Tetramethoxypyrene-TCNQ TTF-TCNQ: CDW instability JACS 134, 4694 (2012) Eur. Phys. J. B 88, 13 (2015) with J.-P. Pouget (Orsay) and E. Canadell (Barcelona) B10 E B2 B4 TCNQ DTBDT 0.3296 nm Extremely short interplanar C-C distances < 0.33 nm, very short S-S contacts ~ 0.34 nm

Charge-transfer state in DTBDT close to the Fermi level on PRB 89, 075435 (2014) STS B10 E B4 (3.2x1.8) nm 2 STM image Split HOMO state in DTBDT-F 4 TCNQ -compound indicates charge transfer

Excitations and Interactions Core-level shift at the CO transition Hard X-ray photoemission (HAXPES) hn = 6-10 kev B10 @ PETRA III B6 B4 B6 15-20 nm escape depth B11 B6 Bulk-sensitive photoemission

Layer-wise charging in HAXPES uncovered and solved 6 kev + + + + + + + + + + Highlight: HAXPES detecting chemical shift at charge-order transition in Fabre salt (TMTTF) 2 SbF 6 B 8 clarifying mechanism of anomalous charging detecting true chemical shift B 6 B11 Eur. Phys. J. B 87, 256 (2014) with J.-P. Pouget (Orsay)

HAXPES on Fabre salt (TMTTF) 2 SbF 6 5 nm Al all non-split at RT 225 K 110 K F 1s core level shift: fingerprint of displacement of anions at the CO transition. B 8 B 6 B11 Eur. Phys. J. B 87, 256 (2014) with J.-P. Pouget (Orsay)

Resumé on Electron & X-ray Spectroscopy NEXAFS: excitation in neutral complex HAXPES: Look through metal coating Radiation damage is an issue! 5 nm Al

Resumé on Electron & X-ray Spectroscopy NEXAFS: excitation in neutral complex HAXPES: Look through metal coating Radiation damage is an issue! Next: k-microscopy extremely low radiation dose 5 nm Al

Excitations and Interactions Charge-transfer induced changes in orbital occupation NEXAFS Core-level shift at the charge-order transition HAXPES Real Systems B10 E B4 B2 B6 B4 Many-body effects and density of states near E F Scanning Tunnelling Spectroscopy STS B6 Anisotropic strain in ferroelectric CT system Conductivity spectroscopy Excitations in magnonic systems Brillouin spectroscopy A7

Electron correlation in organic CT salts probed by STS B2 B6 B11 T. Sasaki et al., PRL 2010

Electron correlation in organic CT salts probed by STS - Study electronic properties of CT systems with lateral resolution - Many-body effects and density of states near Fermi energy - Investigate new charge transfer systems with electronic correlation B6 B11 STS BEDT-TTF b b Frankfurt / Kaiserslautern κ-(bedt-ttf) / Mainz 2 Cu[N(CN) 2 ]Br

Electron correlation in organic CT salts probed by STS arxiv:1410.5245. Anion layer: DOS = 0 at E F Energy gap of DOS Insulating behavior BEDT-TTF-layer: Finite DOS at E F V-shaped DOS B6 B11 Soft gap in Anderson localization

Electron correlation in organic CT salts probed by STS Highlight: Two gap superconducitivity in -Br arxiv: 1411.2813 B6 B11 Both gaps vanish at the same critical temperature strong interband coupling

Electron correlation in organic CT salts probed by STS Next: - Anderson localization for k-et2-x varied by rapid cooling X-ray irradiation - Bandwidth modulation by uniaxial pressure D8-H8 disorder - Study of novel CT salts B4 Courtesy of C.A. Jenkins, ALS

PRB 90, 095150 (2014)

Excitations and Interactions Charge-transfer induced changes in orbital occupation NEXAFS Core-level shift at the charge-order transition HAXPES Real Systems B10 E B4 B2 B6 B4 Many-body effects and density of states near E F Scanning Tunnelling Spectroscopy STS B6 Anisotropic strain in ferroelectric CT system Conductivity spectroscopy Excitations in magnonic systems Brillouin spectroscopy A7

Thin film investigations of ferroelectric organic CT systems Effects of anisotropic strain on ferroelectric state of mixed stack organic CTS TTF-QCl4 (neutral-ionic transition TNI) Degree of order-parameter coupling dimerization - charge transfer? Long-range order in dimerized spin-chain of donor-acceptor stacks? Highlights Mater. Res. Expr. 1, 046303 (2014); Appl. Phys. A 117, 1689 (2014) Thin film growth of TTF-QCl4 causes anisotropic strain Shift of TNI by 30% Non-invasive probing of ferroelectric transition by dielectric sensing in neighboring nano-granular metal layer (experiment & theory) Experiment Theory

Ferromagnetic nanodots embedded in TTF-QCl4 thin films Next: σi σi+1 Sn,Sn+1 First reference measurements Pt nanodots D 10nm d = 30nm Co nanodots (test) additional coupling to FM grains Completion strain-effect study Conductivity fluctuations ( B11) New heterostructures Exchange-bias-induced spin state pinning at TTF-QCl4/FM interface: ordered AFM state in dimerized spin chain? Influence of TTF-QCl4 polarization state on magnetic tunnel exchange coupling of FM nanodots?

Next: High-Resolution Photoelectron k-microscopy of Organic Charge-Transfer Salts at Variable Temperature 3D k-space object Mo(110) surf. res. k-microscope Ti-sapphire laser E DLD κ-br Planned: Sy radiation (BESSY, PETRA III, FLASH) Drift energy (ev) Ultramicroscopy, subm. (2014)