Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces

7 pages. -- Figure S1. a) X-ray diffraction around STO(001). Finite size fringes indicate high-crystalline quality for all the LNMO films. Data for different films is shifted for increased visibility. b) Topography of a 5-uc-thick LNMO film. Step-and-terrace morphology is inherited by the TiO2-termi...

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Autores: Luca, Gabriele de, Spring, Jonathan, Kaviani, Moloud, Jöhr, Simon, Campanini, Marco, Zakharova, Anna, Guillemard, Charles, Herrero Martín, Javier, Erni, Rolf, Piamonteze, Cinthia, Rossell, Marta D., Aschauer, Ulrich, Gibert, Marta
Tipo de recurso: conjunto de datos
Fecha de publicación:2022
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/330593
Acceso en línea:http://hdl.handle.net/10261/330593
Access Level:acceso abierto
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dc.title.none.fl_str_mv Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
title Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
spellingShingle Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
Luca, Gabriele de
title_short Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
title_full Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
title_fullStr Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
title_full_unstemmed Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
title_sort Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide Interfaces
dc.creator.none.fl_str_mv Luca, Gabriele de
Spring, Jonathan
Kaviani, Moloud
Jöhr, Simon
Campanini, Marco
Zakharova, Anna
Guillemard, Charles
Herrero Martín, Javier
Erni, Rolf
Piamonteze, Cinthia
Rossell, Marta D.
Aschauer, Ulrich
Gibert, Marta
author Luca, Gabriele de
author_facet Luca, Gabriele de
Spring, Jonathan
Kaviani, Moloud
Jöhr, Simon
Campanini, Marco
Zakharova, Anna
Guillemard, Charles
Herrero Martín, Javier
Erni, Rolf
Piamonteze, Cinthia
Rossell, Marta D.
Aschauer, Ulrich
Gibert, Marta
author_role author
author2 Spring, Jonathan
Kaviani, Moloud
Jöhr, Simon
Campanini, Marco
Zakharova, Anna
Guillemard, Charles
Herrero Martín, Javier
Erni, Rolf
Piamonteze, Cinthia
Rossell, Marta D.
Aschauer, Ulrich
Gibert, Marta
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
description 7 pages. -- Figure S1. a) X-ray diffraction around STO(001). Finite size fringes indicate high-crystalline quality for all the LNMO films. Data for different films is shifted for increased visibility. b) Topography of a 5-uc-thick LNMO film. Step-and-terrace morphology is inherited by the TiO2-terminated STO substrate. c) Reciprocal space map around STO(103) indicates that a 90 uc (~ 35 nm) LNMO film is epitaxially strained to the substrate. -- Figure S2. a) Mn L3,2-edges XMCD spectra. b) Ni L3,2-edges XMCD spectra. -- Figure S3. a) XAS of Mn L3,2-edges for 5-uc-thick LNMO films subjected to different epitaxial strain conditions. The six different perovskite oxide substrates: LaAlO3 (LAO), NdGaO3 (NGO), LSAT, LaGaO3 (LGO), STO, and DyScO3 (DSO), exert a nominal strain of -2.1%, -0.5%, -0.2%, +0.4%, +0.7%, and +1.8% respectively. The LNMO heterostructure with the highest Mn3+ content is the one grown on STO, followed by the one on LSAT. Overall, the other heterostructures have similar spectra despite the very different strain conditions ranging from highly compressive to highly tensile. Still, signatures of Mn3+ can be observed in tensile-strained LNMO films grown on LGO and DSO. Data is collected at 300 K. b) Same data as in a) but spectra are vertically shifted for increased visibility. Reference lines for L3,2-edges maxima are also shown. c) Sketch of interfacial stacking sequence of LNMO//LSAT. The nominal ionic charge of each layer is indicated on the left. A polar discontinuity at the interface between film and substrate is present, albeit weaker when compared to LNMO//STO (Figure 2c). d) Sketch of interfacial stacking sequence of LNMO//LGO. -- Figure S4. Projected DOS for the Ni0.5Mn0.5O2 layer adjacent to the LNMO//STO (top) and LNMO//LGO (bottom) interface. -- Figure S5. Projected layer-resolved DOS for VO placed in the a) first, b) eleventh, c) twelfth and d) thirteenth layer from the surface of the LNMO//STO heterostructure. -- Figure S6. a) HAADF-STEM survey image of a 13 uc LNMO//STO film and corresponding atomic-resolution EDX elemental maps calculated from the EDX spectrum image using the Sr Kα, Ti Kα, La Lα, Mn Kα and Ni Kα lines. -- Figure S7. At neutral charge the rock-salt configuration (a) is the most stable while the row configuration (c) is the least stable. On the other hand, after adding an extra electron to the system, the column configuration (b) is the most stable. -- Figure S8. The DOS are shifted by the vacuum level determined from (001)pc surface calculations (the work functions for LNMO, LNO and LAO are 4.26, 4.71 and 5.49 eV respectively). -- Figure S9. a) XAS of Mn L3,2-edges for 5- and 10-uc-thick LNMO//STO shows different Mn3+ content as already evidenced in Figure 2a. LNO capping results in a Mn4+-like spectra while the LAO capping is characterized by the persistent presence of Mn3+. Data collected at 20 K. b) XAS of Mn L3,2-edges for 5- and 9-uc-thck LNMO//LSAT shows a larger Mn3+ content for reduced LNMO thickness, similar to what already observed at the LNMO//STO heterostructure. -- Figure S10. Normalized SQUID magnetization vs temperature of a LNO/LNMO(2uc)//STO heterostructure measured in a magnetic field of 0.5 T (gray line).
publishDate 2022
dc.date.none.fl_str_mv 2022
2023
2023
dc.type.none.fl_str_mv info:eu-repo/semantics/dataset
http://purl.org/coar/resource_type/c_ddb1
format dataset
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/330593
url http://hdl.handle.net/10261/330593
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Luca, Gabriele de; Spring, Jonathan; Kaviani, Moloud; Jöhr, Simon; Campanini, Marco; Zakharova, Anna; Guillemard, Charles; Herrero Martín, Javier ; Erni, Rolf; Piamonteze, Cinthia; Rossell, Marta D.; Aschauer, Ulrich; Gibert, Marta. Top-layer engineering reshapes charge transfer at polar oxide interfaces. https://doi.org/10.1002/adma.202203071. http://hdl.handle.net/10261/287662
https://doi.org/10.1002/adma.202203071
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Wiley-VCH
publisher.none.fl_str_mv Wiley-VCH
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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spelling Supporting Information for Adv. Mater., DOI: 10.1002/adma.202203071 Top-Layer Engineering Reshapes Charge Transfer at Polar Oxide InterfacesLuca, Gabriele deSpring, JonathanKaviani, MoloudJöhr, SimonCampanini, MarcoZakharova, AnnaGuillemard, CharlesHerrero Martín, JavierErni, RolfPiamonteze, CinthiaRossell, Marta D.Aschauer, UlrichGibert, Marta7 pages. -- Figure S1. a) X-ray diffraction around STO(001). Finite size fringes indicate high-crystalline quality for all the LNMO films. Data for different films is shifted for increased visibility. b) Topography of a 5-uc-thick LNMO film. Step-and-terrace morphology is inherited by the TiO2-terminated STO substrate. c) Reciprocal space map around STO(103) indicates that a 90 uc (~ 35 nm) LNMO film is epitaxially strained to the substrate. -- Figure S2. a) Mn L3,2-edges XMCD spectra. b) Ni L3,2-edges XMCD spectra. -- Figure S3. a) XAS of Mn L3,2-edges for 5-uc-thick LNMO films subjected to different epitaxial strain conditions. The six different perovskite oxide substrates: LaAlO3 (LAO), NdGaO3 (NGO), LSAT, LaGaO3 (LGO), STO, and DyScO3 (DSO), exert a nominal strain of -2.1%, -0.5%, -0.2%, +0.4%, +0.7%, and +1.8% respectively. The LNMO heterostructure with the highest Mn3+ content is the one grown on STO, followed by the one on LSAT. Overall, the other heterostructures have similar spectra despite the very different strain conditions ranging from highly compressive to highly tensile. Still, signatures of Mn3+ can be observed in tensile-strained LNMO films grown on LGO and DSO. Data is collected at 300 K. b) Same data as in a) but spectra are vertically shifted for increased visibility. Reference lines for L3,2-edges maxima are also shown. c) Sketch of interfacial stacking sequence of LNMO//LSAT. The nominal ionic charge of each layer is indicated on the left. A polar discontinuity at the interface between film and substrate is present, albeit weaker when compared to LNMO//STO (Figure 2c). d) Sketch of interfacial stacking sequence of LNMO//LGO. -- Figure S4. Projected DOS for the Ni0.5Mn0.5O2 layer adjacent to the LNMO//STO (top) and LNMO//LGO (bottom) interface. -- Figure S5. Projected layer-resolved DOS for VO placed in the a) first, b) eleventh, c) twelfth and d) thirteenth layer from the surface of the LNMO//STO heterostructure. -- Figure S6. a) HAADF-STEM survey image of a 13 uc LNMO//STO film and corresponding atomic-resolution EDX elemental maps calculated from the EDX spectrum image using the Sr Kα, Ti Kα, La Lα, Mn Kα and Ni Kα lines. -- Figure S7. At neutral charge the rock-salt configuration (a) is the most stable while the row configuration (c) is the least stable. On the other hand, after adding an extra electron to the system, the column configuration (b) is the most stable. -- Figure S8. The DOS are shifted by the vacuum level determined from (001)pc surface calculations (the work functions for LNMO, LNO and LAO are 4.26, 4.71 and 5.49 eV respectively). -- Figure S9. a) XAS of Mn L3,2-edges for 5- and 10-uc-thick LNMO//STO shows different Mn3+ content as already evidenced in Figure 2a. LNO capping results in a Mn4+-like spectra while the LAO capping is characterized by the persistent presence of Mn3+. Data collected at 20 K. b) XAS of Mn L3,2-edges for 5- and 9-uc-thck LNMO//LSAT shows a larger Mn3+ content for reduced LNMO thickness, similar to what already observed at the LNMO//STO heterostructure. -- Figure S10. Normalized SQUID magnetization vs temperature of a LNO/LNMO(2uc)//STO heterostructure measured in a magnetic field of 0.5 T (gray line).Peer reviewedWiley-VCHConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202320232022info:eu-repo/semantics/datasethttp://purl.org/coar/resource_type/c_ddb1application/pdfhttp://hdl.handle.net/10261/330593reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésLuca, Gabriele de; Spring, Jonathan; Kaviani, Moloud; Jöhr, Simon; Campanini, Marco; Zakharova, Anna; Guillemard, Charles; Herrero Martín, Javier ; Erni, Rolf; Piamonteze, Cinthia; Rossell, Marta D.; Aschauer, Ulrich; Gibert, Marta. Top-layer engineering reshapes charge transfer at polar oxide interfaces. https://doi.org/10.1002/adma.202203071. http://hdl.handle.net/10261/287662https://doi.org/10.1002/adma.202203071Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3305932026-05-22T06:33:51Z
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