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Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy


External control of the conductivity of correlated oxides is one of the most promising schemes for realizing energy-efficient electronic devices. Vanadium dioxide (VO2), an archetypal correlated oxide compound, undergoes a temperature-driven metal–insulator transition near room temperature with a concomitant change in crystal symmetry. Here, we show that the metal–insulator transition temperature of thin VO2(001) films can be changed continuously from 285 to 345 K by varying the thickness of the RuO2 buffer layer (resulting in different epitaxial strains). Using strain-, polarization- and temperature-dependent X-ray absorption spectroscopy, in combination with X-ray diffraction and electronic transport measurements, we demonstrate that the transition temperature and the structural distortion across the transition depend on the orbital occupancy in the metallic state. Our findings open up the possibility of controlling the conductivity in atomically thin VO2 layers by manipulating the orbital occupancy by, for example, heterostructural engineering.

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Figure 1: Overview and strain-dependent MIT in VO2.
Figure 2: Polarization-dependent XAS.
Figure 3: Strain-dependent orbital-occupation changes.
Figure 4: Orbital–lattice correlation.

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The authors thank S. Yang, X. Jiang and A. Pushp for useful discussions and J. Jeong for help with VO2 deposition. Research at Stanford is supported by the US Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract DE-AC02-76SF00515. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, US Department of Energy under Contract No. DE-AC02-05CH11231. Part of this research was supported by the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the US Department of Energy, Office of Basic Energy Sciences.

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N.B.A., M.G.S. and S.S.P.P. designed the study. N.B.A. deposited VO2 films and L.G. deposited RuO2 films. X-ray diffraction and electrical transport measurements were performed and analysed by N.B.A., M.D. and M.C. with help from L.G. A.X.G., N.B.A., A.H.R., R.K. and H.O. carried out and analysed the X-ray absorption measurements, with assistance from C.A.J. and E.A. and under the supervision of H.A.D. M.G.S. helped with X-ray absorption data analysis and along with K.P.R. provided thin-film deposition expertise. N.B.A. and S.S.P.P. wrote the paper with contributions from A.X.G., H.A.D. and M.G.S. All authors discussed the results and commented on the manuscript.

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Correspondence to Nagaphani B. Aetukuri or Stuart S. P. Parkin.

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The authors declare no competing financial interests.

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Aetukuri, N., Gray, A., Drouard, M. et al. Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy. Nature Phys 9, 661–666 (2013).

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