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Experimental Techniques and New Materials F. J. Himpsel
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Angle-resolved photoemission ( and inverse photoemission ) measure all quantum numbers of an electron in a solid “Smoking Gun” (P.W. Anderson) E, k x,y k z, point group, spin E kin, , , h, polarization, spin Electron Spectrometer Synchrotron Radiation Mott Detector
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E(k) from Angle-Resolved Photoemission States within k B T of the Fermi level E F determine transport, superconductivity, magnetism, electronic phase transitions… Ni 0.7 0.9 1.1 Å E k EFEF (eV) E, k multidetection: Energy bands on TV
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Spectrometer with E, x - Multidetection 50 x 50 = 2500 Spectra in One Scan !
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Lens focused to Energy Filter x - Multidetection The Next Generation: 3D, with E, , - Multidetection ( 2D + Time of Flight for E )
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Beyond quantum numbers: From peak positions to line shapes lifetimes, scattering lengths, … Self-energy: Spectral function: Im(G) Greens function G (e propagator in real space)
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Magnetic doping of Ni with Fe suppresses ℓ via large Im( ). Fe doped Im( ) : E = ħ/ , p = ħ/ℓ, = Lifetime, ℓ = Scattering Length Altmann et al., PRL 87, 137201 (2001)
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Spin-Dependent Lifetimes, Calculated from First Principles * Realistic solids are complicated ! No simple approximations. Zhukov et al., PRL 93, 096401 (2004)
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Perovskites (Cuprates, Ruthenates, Cobaltates …) Towards localized, correlated electrons Nanostructures (Nanocrystals, Nanowires, Surfaces, …) New physics in low dimensions Want Tunability Complex Materials Correlation U/W Magnetic Coupling J Dimensionality t 1D /t 2D /t 3D New Materials
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Atomic precision Achieved by self-assembly ( <10 nm ) Reconstructed surface as template Si(111)7x7 rearranges >100 atoms (to heal broken bonds) Steps produce 1D atom chains (the ultimate nanowires) Eliminate coupling to the bulk Electrons at E F de-coupled (in the gap) Atoms locked to the substrate (by covalent bonds) Self-Assembled Nanostructures at Si Surfaces
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Most stable silicon surface; >100 atoms are rearranged to minimize broken bonds. Si(111)7x7 Hexagonal fcc (diamond) (eclipsed)(staggered) Adatom (heals 3 broken bonds, adds 1 ) U Si/Si(111) 10 1 eV U Si/SiC(111) 10 0 eV
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Si(111)7x7 as 2DTemplate for Aluminum Clusters One of the two 7x7 triangles is more reactive. Jia et al., APL 80, 3186 (2002)
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Two-Dimensional Electrons at Surfaces Lattice planes Inversion Layer 10 11 e - /cm 2 10 17 e - /cm 3 Surface State 10 14 e - /cm 2 10 22 e - /cm 3 V(z) n(z) MOSFET Quantum Hall Effect ??? V(z)
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Metallic Surface States in 2D Doping by extra Ag atoms Fermi Surface Band Dispersion e - /atom: 0.0015 0.012 0.015 0.022 0.086 Crain et al., PRB 72, 045312 (2005)
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2D Superlattices of Dopants on Si(111) 1 monolayer Ag is semiconducting: 3x 3 Add 1/7 monolayer Au on top (dopant): 21x 21 (simplified)
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kxkx Si(111) 21x 21 1 ML Ag + 1/7 ML Au Fermi Surface of a Superlattice kyky Model using G 21x 21 Crain et al., PR B 66, 205302 (2002)
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Clean Triple step + 7x7 facet Atom Chains via Step Decoration" With Gold 1/5 monolayer Si chain Si dopant x-Derivative of the topography (illuminated from the left) One-Dimensional Electrons at Surfaces
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2D Fermi Surfaces from 2D to 1D 2D + super- lattice 1D
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t 1 /t 2 40 10 kxkx 1D/2D Coupling Ratio Tight Binding Model Fermi Surface Data t 1 /t 2 is variable from 10:1 to > 70:1 via the step spacing t2t2 t1t1
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Au Graphitic ribbon (honeycomb chain) drives the surface one-dimensional Tune chain coupling via chain spacing
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Total filling is fractional 8/3 e - per chain atom (spins paired) 5/3 e - per chain atom (spin split) Crain et al., PRL 90, 176805 (2003) Band Dispersion Fermi Surface Band Filling
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Fractional Charge at a 3x1 Phase Slip (End of a Chain Segment) Seen for 2x1 (polyacetylene): Su, Schrieffer, Heeger PR B 22, 2099 (1980) Predicted for 3x1: Su, Schrieffer PRL 46, 738 (1981) Suggested for Si(553)3x1-Au: Snijders et al. PRL 96, 076801 (2006)
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Physics in One Dimension Elegant and simple Lowest dimension with translational motion Electrons cannot avoid each other
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Hole Holon + Spinon FF Photo- electron 1D Only collective excitations Spin-charge separation Giamarchi, Quantum Physics in One Dimension 2D,3D Electrons avoid each other
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Delocalized e - Localized e - Tomonaga-Luttinger Model Hubbard, t-J Models Different velocities for spin and charge Holon and spinon bands cross at E F Two Views of Spin Charge Separation Holon Hole Spinon EFEF k E Holon
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Calculation of Spin - Charge Separation Zacher, Arrigoni, Hanke, Schrieffer, PRB 57, 6370 (1998) Spinon Holon E F = Crossing at E F Challenge: Calculate correlations for realistic solids ab initio v Spinon v F v Holon v F /g g<1 Needs energy scale
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Spin-Charge Separation in TTF-TCNQ (1D Organic) Localized, highly correlated electrons enhance spinon/holon splitting Claessen et al., PRL 88, 096402 (2002), PRB 68, 125111 (2003)
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Spin-Charge Separation in a Cuprate Insulator Kim et al., Nature Physics 2, 397 (2006)
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Is there Spin-Charge Separation in Semiconductors ? Bands remain split at E F Not Spinon + Holon Losio et al., PRL 86, 4632 (2001) Why two half-filled bands ? ~ two half-filled orbitals ~ two broken bonds EFEF Proposed by Segovia et al., Nature 402, 504 (1999) Si(557) - Au h = 34 eV E [eV]
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Sanchez-Portal et al. PRL 93, 146803 (2004) Calculation Predicts Spin Splitting No magnetic constituents ! Adatoms Step Edge Si-Au Antibonding E (eV) 0 ZB 1x1 Adatoms ZB 2x1 kxkx EFEF 0 Si-Au Bonding Spin-split band is similar to that in photoemission
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Si Adatoms Au Graphitic Honeycomb Chain Spin-Split Orbitals: Broken Au-Si Backbonds Si(557) - Au
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Is it Spin–Splitting ? Spin-orbit splitting: k Other splittings: E H Rashba ~ (e z x k) · k k,
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Evidence for Spin–Splitting E [eV] k x [Å −1 ] Avoided crossings located left / right for spin-orbit (Rashba) splitting. Would be top / bottom for non-magnetic, (anti-)ferromagnetic splittings. Barke et al., PRL 97, 226405 (2006) Si(553) - Au
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2D Au Chains on Si Au(111) Spin Split Fermi Surfaces 1D kyky kxkx
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Extra Level of Complexity: Nanoscale Phase Separation 1 Erwin, PRL 91, 206101 (2003) 2 McChesney et al., Phys. Rev. B 70, 195430 (2004) Si(111)5x2 - Au Doped and undoped segments ( 1D version of “stripes” ) gap ! metallic Competition between optimum doping 1 (5x8) and Fermi surface nesting 2 (5x4) Compromise: 50/50 filled/empty (5x4) sections
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On-going Developments
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Beyond Quantum Numbers: Electron-Phonon Coupling at the Si(111)7x7 Surface Analogy between Silicon and Hi-Tc Superconductors Kaminski et al, PRL 86, 1070 (2001) Specific mode at 70meV (from EELS) Electron and phonon both at the adatom Coupling strength as the only parameter 0.0 -0.5 Dressed Bare Barke et al., PRL 96, 216801 (2006)
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Rügheimer et al., PRB 75, 121401(R) (2007) Two-photon photoemission Filled Empty Static Dynamic
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Micro-Spectroscopy Gammon et al., Appl. Phys. Lett. 67, 2391 (1995) Overcoming the size distribution of quantum dots
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Fourier Transform from Real Space to k-Space Real space k- space Nanostructures demand high k-resolution (small BZ). Easier to work in real space via STS. dI/dV at E F Fermi surface | (r)| 2 | (k)| 2 Philip Hofmann (Bi surface) Seamus Davis (Cuprates)
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Are Photoemission and Scanning Tunneling Spectroscopy Measuring the Same Quantity ? Photoemission essentially measures the Greens function G. Fourier transform STS involves G and T, which describes back-reflection from a defect. Defects are needed to see standing waves. How does the Bardeen tunneling formula relate to photoemission ?
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Mugarza et al., PR B 67, 0814014(R) (2003) Phase from Iterated Fourier Transform with (r) confined From k to r : Reconstructing a Wavefunction from the Intensity Distribution in k-Space (r)(r)| (k)| 2
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Tunable solids Complex solids Need realistic calculations Is it possible to combine realistic calculations with strong correlations ? (Without adjustable parameters U, t, J, …) Challenges:
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