Constructing oxide interfaces and heterostructures by atomic layer-by-layer laser molecular beam epitaxy
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Abstract
Abstract Advancements in nanoscale engineering of oxide interfaces and heterostructures have led to discoveries of emergent phenomena and new artificial materials. Combining the strengths of reactive molecular-beam epitaxy and pulsed-laser deposition, we show here, with examples of Sr1+x Ti1-x O3+δ, Ruddlesden–Popper phase La n+1Ni n O3n+1 (n = 4), and LaAl1+y O3(1+0.5y)/SrTiO3 interfaces, that atomic layer-by-layer laser molecular-beam epitaxy significantly advances the state of the art in constructing oxide materials with atomic layer precision and control over stoichiometry. With atomic layer-by-layer laser molecular-beam epitaxy we have produced conducting LaAlO3/SrTiO3 interfaces at high oxygen pressures that show no evidence of oxygen vacancies, a capability not accessible by existing techniques. The carrier density of the interfacial two-dimensional electron gas thus obtained agrees quantitatively with the electronic reconstruction mechanism.
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Research context
OpenAlex topics: Electronic and Structural Properties of Oxides · Magnetic and transport properties of perovskites and related materials · Semiconductor materials and devices
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (45)
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1. Hwang, H. Y. et al. Emergent phenomena at oxide interfaces. Nature Mater 11, 103–113 (2012).10.1038/nmat3223 ↗
2. Ohtomo, A. & Hwang, H. Y. A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface. Nature 427, 423–426 (2004).10.1038/nature02308 ↗
3. Lee, H. N., Christen, H. M., Chisholm, M. F., Rouleau, C. M. & Lowndes, D. H. Strong polarization enhancement in asymmetric three-component ferroelectric superlattices. Nature 433, 395–399 (2005).10.1038/nature03261 ↗
4. Warusawithana, M. P., Colla, E. V., Eckstein, J. N. & Weissman, M. B. Artificial dielectric superlattices with broken inversion symmetry. Phys. Rev. Lett. 90, 036802 (2003).10.1103/PhysRevLett.90.036802 ↗
5. Willmott, P. R. & Huber, J. R. Pulsed laser vaporization and deposition. Rev. Mod. Phys. 72, 315–328 (2000).10.1103/RevModPhys.72.315 ↗
6. Eckstein, J. N. & Bozovic, I. High-temperature superconducting multilayers and heterostructures grown by atomic layer-by-layer molecular beam epitaxy. Annu. Rev. Mater. Sci. 25, 679–709 (1995).10.1146/annurev.ms.25.080195.003335 ↗
7. Heani, J. H., Theis, C. D. & Schlom, D. G. RHEED intensity oscillations for the stoichiometric growth of SrTiO3 thin films by reactive molecular beam epitaxy. J Electroceram. 4, 385–391 (2000).10.1023/A:1009947517710 ↗
8. Brooks, C. M. et al. Growth of homoepitaxial SrTiO3 thin films by molecular-beam epitaxy. Appl. Phys. Lett. 94, 162905 (2009).10.1063/1.3117365 ↗
9. Ohnishi, T., Shibuya, K., Yamamoto, T. & Lippmaa, M. Defects and transport in complex oxide thin films. J. Appl. Phys. 103, 103703 (2008).10.1063/1.2921972 ↗
10. Liu, G. Z., Lei, Q. Y. & Xi, X. X. Stoichiometry of SrTiO3 films grown by pulsed laser deposition. Appl. Phys. Lett. 100, 202902 (2012).10.1063/1.4717984 ↗
11. Kanai, M., Kawai, T. & Kawai, S. Atomic layer and unit cell layer growth of (Ca,Sr)CuO2 thin film by laser molecular beam epitaxy. Appl. Phys. Lett. 58, 771–773 (1991).10.1063/1.104543 ↗
12. Herklotz, A. et al. Stoichiometry control of complex oxides by sequential pulsed-laser deposition from binary-oxide targets. Appl. Phys. Lett. 106, 131601 (2015).10.1063/1.4916948 ↗
13. Wood, C. E. C. RED intensity oscillations during MBE of GaAs. Surf. Sci. Lett 108, L441–L443 (1981).
14. Neave, J. H., Joyce, B. A., Dobson, P. J. & Norton, N. Dynamics of film growth of GaAs by MBE from rheed observations. Appl. Phys. A 31, 1–8 (1983).10.1007/BF00617180 ↗
15. Clarke, S. & Vvedensky, D. D. Origin of reflection high-energy electron-diffraction intensity oscillations during molecular-beam epitaxy: a computational modeling approach. Phys. Rev. Lett. 58, 2235–2238 (1987).10.1103/PhysRevLett.58.2235 ↗
16. Tenne, D. A. et al. Ferroelectricity in nonstoichiometric SrTiO3 films studied by ultraviolet Raman spectroscopy. Appl. Phys. Lett. 97, 142901 (2010).10.1063/1.3499273 ↗
17. Nilsen, W. G. & Skinner, J. G. Raman spectrum of strontium titanate. J. Chem. Phys. 48, 2240–2248 (1968).10.1063/1.1669418 ↗
18. Sreedhar, K. et al. Low-temperature electronic properties of the La n+1Ni n O3n+1 (n=2, 3, and ∞) system: evidence for a crossover from fluctuating-valence to Fermi-liquid-like behavior. J. Solid State Chem. 110, 208–215 (1994).10.1006/jssc.1994.1161 ↗
19. Nakagawa, N., Hwang, H. Y. & Muller, D. A. Why some interfaces cannot be sharp. Nature Mater 5, 204–209 (2006).10.1038/nmat1569 ↗
20. Kalabukhov, A. et al. Effect of oxygen vacancies in the SrTiO3 substrate on the electrical properties of the LaAlO3∕SrTiO3 interface. Phys. Rev. B. 75, 121404(R) (2007).10.1103/PhysRevB.75.121404 ↗
21. Siemons, W. et al. Origin of charge density at LaAlO3 on SrTiO3 heterointerfaces: possibility of intrinsic doping. Phys. Rev. Lett. 98, 196802 (2007).10.1103/PhysRevLett.98.196802 ↗
22. Yu, L. P. & Zunger, A. A polarity-induced defect mechanism for conductivity and magnetism at polar–nonpolar oxide interfaces. Nature Commun 5, 5118 (2014).10.1038/ncomms6118 ↗
23. Willmott, P. R. et al. Structural basis for the conducting interface between LaAlO3 and SrTiO3. Phys. Rev. Lett. 99, 155502 (2007).10.1103/PhysRevLett.99.155502 ↗
24. Chambers, S. A. et al. Instability, intermixing and electronic structure at the epitaxial LaAlO3/SrTiO3(001) heterojunction. Surf. Sci. Rep. 65, 317–352 (2010).10.1016/j.surfrep.2010.09.001 ↗
25. Joshua, A., Pecker, S., Ruhman, J., Altman, E. & Ilani, S. A universal critical density underlying the physics of electrons at the LaAlO3/SrTiO3 interface. Nat. Commun. 3, 1129 (2012).10.1038/ncomms2116 ↗
26. Xie, Y., Bell, C., Hikita, Y., Harashima, S. & Hwang, H. Y. Enhancing electron mobility at the LaAlO3/SrTiO3 interface by surface control. Adv. Mater. 25, 4735–4738 (2013).10.1002/adma.201301798 ↗
27. Kalabukhov, A. et al. Improved cationic stoichiometry and insulating behavior at the interface of LaAlO3/SrTiO3 formed at high oxygen pressure during pulsed-laser deposition. Europhys. Lett. 93, 37001 (2011).10.1209/0295-5075/93/37001 ↗
28. Sato, H. K., Bell, C., Hikita, Y. & Hwang, H. Y. Stoichiometry control of the electronic properties of the LaAlO3/SrTiO3 heterointerface. Appl. Phys. Lett. 102, 251602 (2013).10.1063/1.4812353 ↗
29. Ariando et al. Electronic phase separation at the LaAlO3/SrTiO3 interface. Nat. Commun. 2, 188 (2011).10.1038/ncomms1192 ↗
30. Reinle-Schmitt, M. L. et al. Tunable conductivity threshold at polar oxide interfaces. Nat. Commun. 3, 932 (2012).10.1038/ncomms1936 ↗
31. Cancellieri, C. et al. Electrostriction at the LaAlO3/SrTiO3 interface. Phys. Rev. Lett. 107, 056102 (2011).10.1103/PhysRevLett.107.056102 ↗
32. Salluzzo, M. et al. Orbital Reconstruction and the two-dimensional electron gas at the LaAlO3/SrTiO3 interface. Phys. Rev. Lett. 102, 166804 (2009).10.1103/PhysRevLett.102.166804 ↗
33. Salluzzo, M. et al. Origin of interface magnetism in BiMnO3/SrTiO3 and LaAlO3/SrTiO3 heterostructures. Phys. Rev. Lett. 111, 087204 (2013).10.1103/PhysRevLett.111.087204 ↗
34. Choi, W. S. et al. Atomic layer engineering of perovskite oxides for chemically sharp heterointerfaces. Adv. Mater. 24, 6423–6428 (2012).10.1002/adma.201202691 ↗
35. Warusawithana, M. P. et al. LaAlO3 stoichiometry is key to electron liquid formation at LaAlO3/SrTiO3 interfaces. Nat. Commun. 4, 2351 (2013).10.1038/ncomms3351 ↗
36. Breckenfeld, E., Bronn, N., Mason, N. & Martin, L. W. Tunability of conduction at the LaAlO3/SrTiO3 heterointerface: thickness and compositional studies. Appl. Phys. Lett. 105, 121610 (2014).10.1063/1.4896778 ↗
37. Brinkman, A. et al. Magnetic effects at the interface between nonmagnetic oxides. Nat. Mater. 6, 493–496 (2007).10.1038/nmat1931 ↗
38. Haviland, D. B., Liu, Y. & Goldman, A. M. Onset of superconductivity in the two-dimensional limit. Phys. Rev. Lett. 62, 2180–2183 (1989).10.1103/PhysRevLett.62.2180 ↗
39. Zhang, Z. Y. & Lagally, M. G. Atomistic processes in the early stages of thin-film growth. Science 276, 377–383 (1997).10.1126/science.276.5311.377 ↗
40. Müller, P. & Saúl, A. Elastic effects on surface physics. Surf. Sci. Rep. 54, 157–258 (2004).10.1016/j.surfrep.2004.05.001 ↗
41. Zinkevich, M. et al. Stability and thermodynamic functions of lanthanum nickelates. J. Alloys Compd. 438, 92–99 (2007).10.1016/j.jallcom.2006.08.047 ↗
42. Geohegan, D. B. Physics and diagnostics of laser ablation plume propagation for high-T c superconductor film growth. Thin Solid Films 220, 138–145 (1992).10.1016/0040-6090(92)90562-P ↗
43. Kawasaki, M. et al. Atomic control of the SrTiO3 crystal surface. Science 266, 1540–1542 (1994).10.1126/science.266.5190.1540 ↗
44. Ohnishi, T. et al. A-site layer terminated perovskite substrate: NdGaO3. Appl. Phys. Lett. 74, 2531–2533 (1999).10.1063/1.123888 ↗
45. Young, A. T. et al. A soft x-ray undulator beamline at the advanced light source with circular and variable linear polarization for the spectroscopy and microscopy of magnetic materials. Surf. Rev. Lett. 9, 549–554 (2002).10.1142/S0218625X02002622 ↗