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Magnetism of amorphous and nanocrystalized dc-sputter-deposited MgO Thin Films
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Engineering Material Physics.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Engineering Material Physics.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Engineering Material Physics.
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2013 (English)In: NANOMATERIALS, ISSN 2079-4991, Vol. 3, no 3, 486-497 p.Article in journal (Refereed) Published
Abstract [en]

We report a systematic study of room-temperature ferromagnetism (RTFM) in pristine MgO thin films in their amorphous and nano-crystalline states. The as deposited dc-sputtered films of pristine MgO on Si substrates using a metallic Mg target in an O-2 containing working gas atmosphere of (N-2 + O-2) are found to be X-ray amorphous. All these films obtained with oxygen partial pressure (P-O2) similar to 10% to 80% while maintaining the same total pressure of the working gas are found to be ferromagnetic at room temperature. The room temperature saturation magnetization (MS) value of 2.68 emu/cm(3) obtained for the MgO film deposited in P-O2 of 10% increases to 9.62 emu/cm3 for film deposited at P-O2 of 40%. However, the MS values decrease steadily for further increase of oxygen partial pressure during deposition. On thermal annealing at temperatures in the range 600 to 800 degrees C, the films become nanocrystalline and as the crystallite size grows with longer annealing times and higher temperature, MS decreases. Our study clearly points out that it is possible to tailor the magnetic properties of thin films of MgO. The room temperature ferromagnetism in MgO films is attributed to the presence of Mg cation vacancies.

Place, publisher, year, edition, pages
2013. Vol. 3, no 3, 486-497 p.
Keyword [en]
room temperature ferromagnetism, Mg vacancy, magnetron sputtering, O-2 content; annealing
National Category
Metallurgy and Metallic Materials
Identifiers
URN: urn:nbn:se:kth:diva-122628DOI: 10.3390/nano3030486ISI: 000342201300009OAI: oai:DiVA.org:kth-122628DiVA: diva2:623077
Note

QC 20150626. Updated from manuscript to article in journal.

Available from: 2013-05-24 Created: 2013-05-24 Last updated: 2017-02-22Bibliographically approved
In thesis
1. Magnetism in Band Gap Engineered Sputtered MgxZn(1-x)O Thin Films
Open this publication in new window or tab >>Magnetism in Band Gap Engineered Sputtered MgxZn(1-x)O Thin Films
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This dissertation presents a comprehensive study of the intrinsic room temperature ferromagnetism, RTFM, in technologically important thin films of ZnO, MgO, Mg@ZnO, the so-called d0–magnets that do not contain any intrinsic magnetic elements. We also present the first report on magnetism in Mn doped MgO films fabricated by dc magnetron sputtering. We have just published (April 2013 ‘on-line’) a state of the art review entitled ‘p-type ZnO Theory, growth, properties, and devices’ in the prestigious journal ‘Progress in Materials Science’, summarizing the recent advances of the studies on p-type ZnO thin films and pointing out the major challenges that remain in the field. The experimental work then focuses on the magnetic properties of band gap engineered Mg@ZnO films exploiting the fact that by substitutional doping of Mg for Zn in ZnO it is possible to tailor new materials with bandgap energy in the range 3.3 eV to 7.2 eV, thus extending the possibilities for new magnetic and optical device applications. In addition, we show that by doping Mn in MgO its magnetic properties can be enhanced to saturation values as high as 38.5 emu/cm3 in a 92 nm thick film. These studies involve extensive characterization of the high quality films in the thickness range of nanometers, using SQUID magnetometer for magnetic properties, XRD for structural analysis, Dual beam HRSEM/FIB and AFM for accurate film cross-sectioning and surface morphology, EDXS for elemental analysis, UV-VIS NIR for measuring the band gap of MgxZn(1-x)O films, Mg K-edge NEXAFS experiment in order to understand electronic structure of specific cations present in the thin films The origin of the observed room temperature feerromaganetism is attributed to cation vacancies and its consequences on the polarization about these vacancies in the oxides...

ZnO films are promising materials for optoelectronic device applications, and the fabrications of high quality p-type ZnO and p–n junction are the key steps to realize these applications. However, reliable p-type doping of the material remains a major challenge because of the self-compensation from native donor defects (VO and Zni) and/or hydrogen incorporation. Considerable efforts to obtain p-type ZnO by doping different elements with various techniques have resulted in remarkable progress in the field both from theoretical and experimental point of view. In our paper, we discuss p-type ZnO materials: theory, growth, properties and devices, comprehensively. We first discuss the native defects in ZnO. Among the native defects in ZnO, VZn and Oi act as acceptors. We then present the theory of p-type doping in ZnO, and summarize the growth techniques for p-type ZnO and the properties of p-type ZnO materials. Experimentally, besides the intrinsic p-type ZnO grown at O-rich ambient, p-type ZnO (MgZnO) materials have been prepared by various techniques using Group-I, IV and V elements. We pay a special attention to the band gap of p-type ZnO by band gap engineering and room temperature ferro magnetism observed in p-type ZnO. Finally, we summarize the devices based on p-type ZnO materials.

In presenting the current studies, we first focus on the sputtering process in order to produce high quality films. From a comparative study of RTFM, in MgO films deposited by sputtering from 99.999% pure metallic Mg, Vs MgO targets respectively on glass/Si substrates under identical ambience during deposition it is found that the metallic targets give the best magnetic properties (e.g: with maximum Ms values of ~13.75 emu/g vs ~ 4.2 emu/g respectively on Si substrates.(supplement 2). Furthermore, the Ms values are strongly film thickness dependent with Mg target while it is weakly so for films from MgO target. Also, the as deposited MgO films using metallic Mg target are found to be amorphous, while it is nanocrystalline when the films are sputtered off MgO targets. The overall Ms values are found to be dependent on the oxygen content in the atmosphere during deposition, increasing to 2.69 emu/g at a oxygen partial pressure of 40% of the total working gas pressure. On annealing to nanocrystallize these films in the temperature range 600 to 8000C strong XRD peaks corresponding to (200) orientation are observed, and Ms values decrease proportionately. (supplement 3).

With the above information on studies for optimizing the effect of sputtering gas, film thickness, and oxygen partial pressure, PO2, comprehensive investigations on band gap engineering and magnetism in MgxZn(1-x)O co-sputtered thin films from Mg and Zn targets are then closely examined. The optical band gap calculated from absorption spectra shows that the band gaps of Mg-doped ZnO thin films increased linearly from 3.33 to 4.074 eV. Our studies indicate that both the magnetic properties and the band gap of the film can be tailored by tuning the film thickness and PO2 in the working gas.

In summary, RTFM ordering in the thin films originates from cation vacancies which couple ferromagnetically and establish long range magnetic order. The ferromagnetic ordering in these materials is shown to arise from defects situated at the cation sites. Electronic structure studies of some selected films disclose that the unoccupied O 2p states exist and this unoccupied state results from cation vacancy (VMg).

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2013. xii, 80 p.
Keyword
Magnetron co-sputtering, MgO, MgxZn(1-x)O, MnxMg(1-x)O, thin films, Room-temperature ferromagnetism, band gap engineering, and intrinsic defects
National Category
Materials Engineering Other Physics Topics
Identifiers
urn:nbn:se:kth:diva-122488 (URN)978-91-7501-807-2 (ISBN)
Public defence
2013-06-14, Sal F3, Lindstedtsvägen 26, KTH, Stockholm, 14:00
Opponent
Supervisors
Funder
EU, European Research Council
Note

QC 20130524

Available from: 2013-05-24 Created: 2013-05-22 Last updated: 2013-05-24Bibliographically approved

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