X-ray Scattering: Liquid Metal/Vapor Interfaces P.S. Pershan SEAS & Dept of Physics, Harvard Univ., Cambridge, MA, US I: Liquid Metal/Vapor Interfaces.

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X-ray Scattering: Liquid Metal/Vapor Interfaces P.S. Pershan SEAS & Dept of Physics, Harvard Univ., Cambridge, MA, US I: Liquid Metal/Vapor Interfaces II: Examples from experiments done by our group and others. III: Open questions on surface freezing of liquid metals (Mechler) Pershan/LAMXIV

Our Group. Colleagues (~20 years) Pershan/LAMXIV Balagurusamy, V. S. K. Berman, E. √√Deutsch, M. DiMasi, E. Fukuto, M. Gebhardt, J. Gog, T. Graber, T. Grigoriev, A. Huber, P. Kawamoto, E. H. Kuzmenko, I. Lin, B. H. Magnussen, O. M. √√Mechler, S. Meron, M. Ocko, B. M. Pontoni, D. Regan, M. J. Sellner, S. Shpyrko, O. G. Steimer, C. Stoltz, S. Streitel, R. Tostmann, H. √√Yahel, E Harvard, Non-Harvard, Beam Line √√ Speakers at LAMXIV

Fresnel X-ray Reflectivity Pershan/LAMXIV : Diffuse scattering:

Grazing Incidence Diffraction (GID) Pershan/LAMXIV Diffuse Scattering at Larger 2D Bragg Peaks

Real Liquid Surfaces Pershan/LAMXIV Surface Structur e Thermal capillary waves Reflectivity Diffuse Scattering

Hg In Ga Hg: Magnussen et al. (1995). Ga: Regan et al.(1995) In: Tostmann et al.(1999) Type I: Elemental Liquid Layer Response of Bulk Susceptibility Pershan/LAMXIV Metallic Liquids (D’Evelyn & Rice ‘83)

Type II: Surface Adsorption(Ga-Bi alloy) Bulk Phase Coexistence Pershan/LAMXIV Nattland &Freyland, ’94 Chatain & Wynblatt, ‘96 P. Huber,’03  Surface Tension Gibbs: < 1900 Butler: ’35 Egry: ‘05 Electron Density ξ d  Influence Parameter: d vs T  Calphad Initiative(data)  Gibbs free energy density:

TypeIIIa: Surface Phase Transition 2 Phase Binary Solution Pershan/LAMXIV Bilayer Monolayer Liquid Shpyrko et al. Science 313, 77 (2006) vol. 313 (5783) Mechler et al. LAMXIV (2010) 2D Au-Si Crystals +Layer Au-Si Eutectic Is this Gibbs? Yang et al. PRB. 62, (2000) Gibbs Adsorption Pb-monolayer on Ga 2D Crystal. GID Scattering

Type IIIb: Phase Transition (Insoluble Monolayer ) Pershan/LAMXIV Kraack et al. The Structure and Phase Diagram of Langmuir Films of Alcohols on Mercury. Langmuir 20, 5386 (2004) GID

Structure Factor &Thermal Effects Debye-Waller  Capillary Waves Pershan/LAMXIV 2D Debye-Waller Diffuse Scat: In ~0.01Å -1

Debye-Waller Demonstration Pershan/LAMXIV Ga vs. T GaGa In Hg In Ga GaGa In

Distorted Crystal Layer Model Pershan/ESRF DCM (Magnussen ’95) Only 3 Adjustable Parameters n=

Elemental Liquid Metals Studied Pershan/ESRF KGaInSnBiHg DCM +1 ?  ☐  ☐ Why are 1 st Layers for Bi and Sn different from K, Ga and In? Sn Mol. Dynamic. Simulations Calderín et al. PRB,80, (2009) No Bump  Bump Bi is like Sn! Why is Hg so different?

Eutectic Alloys Pershan/ESRF J. W. Gibbs  B Surface is Rich in “B”. A x B 1-x  A)/  B) Δ H * (mixing) Concentration of Surface Layers 1st2 nd 34d Ga x Bi 1-x 718/378=1.90+4Liquid-Liquid Phase Sep. Ga 83.5 In /556= %In In 78 Bi /378=1.4735%Bi Sn 57 Bi /378= %Bi25%Bi53%Bi Au 71 Sn /560= %Sn<1%Sn24%Sn Au 72 Ge /621= No Gibbs Adsorption Au 82 Si /865= layers, 2DXtal (AuSi 2 ) Pd 81 Ge /621= ~40 Å wetting layer (No Measureable Gibbs Adsorption)

9th Int. Conf on Surf. X-ray and Neutron Scan (Taiwan, Jul.’06). 15 Gibbs Surface Adsorption(BiSn)  Bi =378,  Sn =560, Alloy: Bi and Sn  (Bi) ≈ 398  (Sn)≈ 567 dyne/cm Energy Dispersion: Bi:L3 f(E) Adsorption Scat. Ampl.

Surface Freezing Au 82 Si 18 Eutectic Pershan/LAMXIV SiAu T/γ~0.8 Bragg Peaks LT: Bilayer Xtal HT: Monolayer LL: Liquid Mechler (LAMXIV) Gallium T/γ~0.56 2D-Crystal  Rigidity Rigidity Reduces Debye-Waller

AuGe Eutectic(Should be Similar to Au-Si) Pershan/ESRF  (Au)/γ  Si or Ge) ΔH Au 72 Ge /621= Au 82 Si /865= Au-Si Au-Ge Au-Ge is Different from Au-Si No Surface Freezing Why? Au-Si Surface Frozen Ge≤6.5 atm% 2D GID Scans Pasturel et al. Structure- Liquid Au-Si - molecular dynamics. PRB (2010) Upmanyu et al. (in preparation): NE Sub surface Si enrichment! Si (Surface) (Au-Si) (bonding)

Surface Freezing of Au 82 Si 18 and Glass Forming!(Mechler) Pershan/LAMXIV Glass Former Au-Si Not A Glass Former Au-Ge Glass Former Pd-Si Pd-Ge

Summary Elemental metals  Surface induced layering. Simplest Distorted Crystal Model (Ga,In, K) Debye-Waller Effects of Thermal Capillary Waves Near surface deviations from DCM (Sn, Bi). Other Metal/Vapor Interfaces 2 Phase Binary Alloys (Ga-Bi, Ga-Pb, Ga-Tl)  Gibbs Adsorption, Wetting, 2D Crystals Langmuir Monolayers on Hg (Deutsch) Unexplained behavior of Au 82 Si 18 (Mechler) Eutectic 2D Surface phase transitions for Au-Si New Results I: Au-Cu-Si: (Mechler: LAMXIV) New Results II: Liquid Ge: No Layering (Private Discussion: Mechler and Yahel) New Results from Others:Liquid Metal/Solid: (Deutsch: LAMXIV) Pershan/ESRF