Electrostatic charging and redox effects in oxide heterostructures
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1 Electrostatic charging and redox effects in oxide heterostructures Peter Littlewood 1,2,3 Nick Bristowe 3 & Emilio Artacho 3,6 Miguel Pruneda 4 and Massimiliano Stengel 5 1 Argonne National Laboratory 2 University of Chicago 3 University of Cambridge 4 Centre d'investigacion en Nanociencia i Nanotecnologia, Barcelona 5 Institut de Ciencia de Materials, Barcelona 6 CIC Nanogune, and DIPC, San Sebastian Bristowe et al., PRB 80, (2009); 83,20545 (2011); 85, (2012); JPCM 23, (2011); PRL 108, (2012) 9/16/2012 Impact
2 Why are heterostructure oxides interesting? Transition metal oxides are responsible for some interesting and useful physics and materials science: magnetism, superconductivity, ferroelectricity,... We use oxides to make batteries, capacitors, photovoltaics,... Physically, these are systems where the carriers are small (strongly correlated). Strong correlations means high energy density and therefore useful Control of doping by chemistry is the usual route, and it s challenging In semiconductors, we have learned to modulation dope, and this has been responsible for much modern semiconductor technology and essentially ALL of modern semiconductor physics 9/16/2012 Impact
3 Outline LaAlO 3 /SrTiO 3 (polar-insulator) Introduction: interface 2DEG, polar catastrophe argument Net interface charges formal argument Model test n-p superlattices Origin of 2DEG in reality surface redox? BaTiO 3 /La 0.7 Sr 0.3 MnO 3 (ferroelectric-half metal) Introduction: ferroelectric screening Redox calculations Magnetoelectric and tunneling electroresistance 9/16/2012 Impact
4 An example: LaAlO3 / SrTiO3 Interface between two band insulators is (sometimes) conducting Whence the carriers? Two (at least) points of view Ideal interface is charged (polar catastrophe) produces electrical potential attracts (mobile?) carriers Charged interfaces may destabilise growth produces (neutralising) charged defects also generates carriers A Ohtomo & H Hwang, Nature 427, 423 (2004) 9/16/2012 Impact
5 LaAlO 3 / SrTiO 3 Ohtomo and Hwang Nature 427, Sheet resistance of n-type SrTiO3/LaAlO3 interfaces. Temperature dependence. of the sheet resistance for SrTiO3/LaAlO3 conducting interfaces, grown at various partial oxygen pressures A. Brinkman et al Nat.Mater. 2007, 6, 493 9/16/2012 Impact
6 Surface polar adsorbates Carrier density and conductivity depends on details of growth and also (reversibly) on surface adsorbates AFM used to modulate buried interface layer conduction e.g. Cen et al. Nature Mater. 7, (2008). Carrier density at buried interface in LAO/STO is modulated by surface adsorption of polar molecules Xie et al Arxiv1105:3891 9/16/2012 Impact
7 Counting charge and polarisation How to count charge at an interface? Remember: dopants in a semiconductor, eg P (group V) in Si (group IV) P adds 5 valence electrons and +5 charge to core Compared with Si +1 impurity and 1 extra electron in this case weakly bound In compound semiconductors, it is possible to separate the charge from the impurity and capture it in a quantum well modulation doping Is this the correct picture in oxides? 9/16/2012 Impact
8 Modulation doping (a) Two semiconductors not in electrical contact (b) In electrical contact, chemical potentials balance (c) Donors added to wide gap material ionise and populate interfacial electron layer 9/16/2012 Impact
9 Capacitor Plate Model for STO/LAO σ c is the chemical charge density formal ionic charges 9/16/2012 Impact
10 12x 12 superlattice of LaAlO 3 / SrTiO 3 Bristowe et al PRB 80, (2009) 9/16/2012 Impact
11 Linear shift of potential with distance from interface Quantitative agreement of DFT results with capacitor plate model including lattice relaxation including a non-linear dielectric response P as function of electric field and strain NB contribution to P from ferroelectricity of strained SrTiO 3 But not with experiment... see later 9/16/2012 Impact
12 ... science fiction interlude... 9/16/2012 Impact
13 Self- modulation doping: Mobile charges in coupled valence and conduction bands Once E > E gap /d, mobile (?) carriers appear at the two interfaces. Beyond a critical spacing d c ~ 5 unit cells the charge transferred compensates the formal ionic charge The potential difference between the interfaces is pinned approximately at the gap (owing to large DoS). Carrier density grows with d but is generally quite small, for example n 12/12 = e/unit cell In LAO/STO strong screening -> large effective Bohr radius Potentially interesting Coulomb correlations Mott transition for excitons; superfluids and solids etc. e/cell 9/16/2012 Impact
14 Ultracapacitor / Photovoltaic Excitons: add electrons and holes in pairs Energy cost = Energy gap binding energy + interaction energy Tuned by external bias ~ 0 Capacitance is theoretically very large Store one exciton/bohr radius (Mott density) Intrinsic photovoltaic Enormous internal field ~ V/nm Energy per pair (in exciton Rydberg) as a function of density Zhu et al, PRB 54, (1996) 9/16/2012 Impact
15 ... back to reality... 9/16/2012 Impact
16 Not particularly consistent with experiments Problems: Strong dependence of carrier density on growth conditions (particularly oxygen pressure) more metallic when grown in lower oxygen pressures Model critical thickness (>6 u.c.) > observed ( <4 u.c.) No mobile holes seen at surface XPS measures no internal field HAXPS see electrons at interface before onset of conduction Resolution? Defects (bulk/surface) contribute to carriers... 9/16/2012 Impact
17 Resolution? Several suggested mechanisms: (Review: Schlom & Mannhart 2010) STO oxygen vacancies Ionic intermixing (La-Sr) La doping Hard to explain MIT of 4 u.c. consistently measured by several groups using various growth techniques None aid LAO screening Surface redox reactions stabilised under growth conditions by generating screening charge Bristowe et al, arxiv:1008:1951; Stephenson and Highland, arxiv: /16/2012 Impact
18 Surface redox reactions generated under growth conditions E.g. Oxygen vacancy creates (double) donor Electrons transfer to interface Thermodynamically stable for a thick enough layer transferred charges lower capacitive energy that grows with thickness Energy cost to create vacancy balanced against Coulomb 9/16/2012 Impact
19 Surface donor states stabilised by Coulomb? Free energy cost to create vacancy balanced against Coulomb Defect creation energy Defect interactions n = defect density d = film thickness Electrostatic energy Intrinsic charge density Reconstructed charge density Critical separation Field energy if interface partially screened 9/16/2012 Impact
20 Surface redox reactions and 2DEGs Bristowe et al. PRB 83, (2011) 9/16/2012 Impact
21 Outline LaAlO 3 /SrTiO 3 (polar-insulator) Introduction: interface 2DEG, polar catastrophe argument Net interface charges formal argument Model test n-p superlattices Origin of 2DEG in reality surface redox? BaTiO 3 /La 0.7 Sr 0.3 MnO 3 (ferroelectric-half metal) Introduction: ferroelectric screening Redox calculations Magnetoelectric and tunneling electroresistance 9/16/2012 Impact
22 Surprising stability of domains in thin BTO films 9/16/2012 Impact
23 Source of screening Conventional view : charged species and metallic screening - accidental charged species Redox reaction freeing charge to the interface? thermodynamic equilibrium established in writing/growth In context of ferroelectrics, see e.g. Stephenson and Highland, arxiv: /16/2012 Impact
24 Methods Bristowe et al PRB 85, (2012) 9/16/2012 Impact
25 Atomic displacements 9/16/2012 Impact
26 No polarisation in pristine film Bulk P (up/down) stabilised by compensating charges from (adatom/vacancy) [~1/2 per unit cell] Not surprising since it slightly overscreens the bulk polarization Needs further work to establish equilibrium density In addition Large magneto-electric effect Large tunnelling electroresistance See also Burton and Tsymbal Phys. Rev. B 82, (2010); Phys. Rev. Lett. 106, (2011) mechanism slightly different but principles the same 9/16/2012 Impact
27 Substantial magnetoelectric effect 9/16/2012 Impact
28 Electroresistance Perfect screening of surface redox Imperfect screening in LSMO Interface dipole shifts with polarisation state 9/16/2012 Impact
29 Tunnelling electroresistance There are other mechanisms for TER and ME effects involving changed magnetic ground states of the LSMO (Tsymbal 2010/2011) 9/16/2012 Impact
30 Electrochemistry? 9/16/2012 Impact
31 Spectroscopy of adatom/vacancy in manganites Bryant et al, Nat. Commun. 2:212 (2011) 9/16/2012 Impact
32 Bryant et al, Nat. Commun. 2:212 (2011) 9/16/2012 Impact
33 Electrochemical Strain Microscopy on LAO/STO 1V 30V Apply a tip bias, and measure both the topographic changes and the elastic response ramp up voltage in a sequence 9/16/2012 Impact
34 Conclusions Centrosymmetric materials can have a (non-switchable) polarization e.g. LAO The polarization is precisely half a quantum Heterostructures require polarization screening Either by internal charge transfer self modulation doping Or by charged defects Surface oxygen/vacancies plausible candidates? Can we control surface electrochemistry with nanoelectrodes? Is O vacancy a double donor? correlation effects? 9/16/2012 Impact
35 Collaborators: Nick Bristowe, Emilio Artacho, Miguel Pruneda, Massimiliano Stengel, Sergei Kalinin Discussions: Mineral Sciences group, G Catalan, J Scott, N Mathur, X Moya, V Garcia, M Bibes, J Junquera, J Iniguez, P Ordejon, H Hwang, W Pickett, D Vanderbilt, F Schoofs, T Fix, M Blamire Funding: 9/16/2012 Impact
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