Modulation-doping a correlated electron insulator

Mondal, Debasish; Mahapatra, Smruti Rekha; Derrico, Abigail M.; Rai, Rajeev Kumar; Paudel, Jay R.; Schlueter, Christoph; Gloskovskii, Andrei; Banerjee, Rajdeep; Hariki, Atsushi; DeGroot, Frank M. F.; Sarma, D. D.; Narayan, Awadhesh; Nukala, Pavan; Gray, Alexander X.; Aetukuri, Naga Phani B.

doi:10.1038/s41467-023-41816-3

Title: Modulation-doping a correlated electron insulator

Journal Article · 04 October 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-41816-3 · OSTI ID:2007681

; Mahapatra, Smruti Rekha; Derrico, Abigail M.;

; Paudel, Jay R.; Schlueter, Christoph; Gloskovskii, Andrei; Banerjee, Rajdeep; Hariki, Atsushi;

;

; Narayan, Awadhesh;

;

Abstract Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO ₂ ) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO ₂ —especially without inducing structural changes—has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO ₂ -based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard X-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5 × 10 ²¹ cm ⁻³ without inducing any measurable structural changes. We find that the MIT temperature (T _MIT ) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e ⁻ /vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions.

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Research Organization:: Temple Univ., Philadelphia, PA (United States); Temple University, Philadelphia, PA (United States)

Sponsoring Organization:: Army Research Office DURIP; Indian Institute of Science; JSPS KAKENHI; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0019297

OSTI ID:: 2007681

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (58)

Modulation-Doped In ₂ O ₃ /ZnO Heterojunction Transistors Processed from Solution Khim, Dongyoon; Lin, Yen-Hung; Nam, Sungho Advanced Materials, Vol. 29, Issue 19 https://doi.org/10.1002/adma.201605837	journal	March 2017
Nonvolatile Control of Metal–Insulator Transition in VO ₂ by Ferroelectric Gating Lee, Yoon Jung; Hong, Kootak; Na, Kyeongho Advanced Materials, Vol. 34, Issue 32 https://doi.org/10.1002/adma.202203097	journal	July 2022
Band Alignment at Heteroepitaxial Perovskite Oxide Interfaces. Experiments, Methods, and Perspectives Giampietri, Alessio; Drera, Giovanni; Sangaletti, Luigi Advanced Materials Interfaces, Vol. 4, Issue 11 https://doi.org/10.1002/admi.201700144	journal	May 2017
Observation of the Pinch‐Off Effect during Electrostatically Gating the Metal‐Insulator Transition Yajima, Takeaki; Toriumi, Akira Advanced Electronic Materials, Vol. 8, Issue 2 https://doi.org/10.1002/aelm.202100842	journal	November 2021
Nb‐Doped VO₂ Thin Films Prepared by Aerosol‐Assisted Chemical Vapour Deposition Piccirillo, Clara; Binions, Russell; Parkin, Ivan P. European Journal of Inorganic Chemistry, Vol. 2007, Issue 25 https://doi.org/10.1002/ejic.200700284	journal	August 2007
Phase Diagram of V1-xAlxO2 Brückner, W.; Gerlach, U.; Thuss, B. Physica Status Solidi (a), Vol. 40, Issue 2 https://doi.org/10.1002/pssa.2210400248	journal	April 1977
Identifying the Collective Length in VO₂ Metal–Insulator Transitions Yajima, Takeaki; Nishimura, Tomonori; Toriumi, Akira Small, Vol. 13, Issue 12 https://doi.org/10.1002/smll.201603113	journal	January 2017
Experimental study of the electronic and lattice contributions to the VO2 transition Pintchovski, F.; Glaunsinger, W. S.; Navrotsky, A. Journal of Physics and Chemistry of Solids, Vol. 39, Issue 9 https://doi.org/10.1016/0022-3697(78)90108-7	journal	January 1978
The two components of the crystallographic transition in VO2 Goodenough, John B. Journal of Solid State Chemistry, Vol. 3, Issue 4 https://doi.org/10.1016/0022-4596(71)90091-0	journal	November 1971
Metallization of Epitaxial VO ₂ Films by Ionic Liquid Gating through Initially Insulating TiO ₂ Layers Passarello, Donata; Altendorf, Simone G.; Jeong, Jaewoo Nano Letters, Vol. 16, Issue 9 https://doi.org/10.1021/acs.nanolett.6b01882	journal	August 2016
Modulation of the Electrical Properties of VO ₂ Nanobeams Using an Ionic Liquid as a Gating Medium Ji, Heng; Wei, Jiang; Natelson, Douglas Nano Letters, Vol. 12, Issue 6 https://doi.org/10.1021/nl300741h	journal	May 2012
Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial Liu, Mengkun; Hwang, Harold Y.; Tao, Hu Nature, Vol. 487, Issue 7407 https://doi.org/10.1038/nature11231	journal	July 2012
Collective bulk carrier delocalization driven by electrostatic surface charge accumulation Nakano, M.; Shibuya, K.; Okuyama, D. Nature, Vol. 487, Issue 7408 https://doi.org/10.1038/nature11296	journal	July 2012
Positive-bias gate-controlled metal–insulator transition in ultrathin VO2 channels with TiO2 gate dielectrics Yajima, Takeaki; Nishimura, Tomonori; Toriumi, Akira Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms10104	journal	December 2015
Band alignment of rutile and anatase TiO2 Scanlon, David O.; Dunnill, Charles W.; Buckeridge, John Nature Materials, Vol. 12, Issue 9 https://doi.org/10.1038/nmat3697	journal	July 2013
Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping Chen, Y. Z.; Trier, F.; Wijnands, T. Nature Materials, Vol. 14, Issue 8 https://doi.org/10.1038/nmat4303	journal	June 2015
Hydrogen stabilization of metallic vanadium dioxide in single-crystal nanobeams Wei, Jiang; Ji, Heng; Guo, Wenhua Nature Nanotechnology, Vol. 7, Issue 6 https://doi.org/10.1038/nnano.2012.70	journal	May 2012
Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy Aetukuri, Nagaphani B.; Gray, Alexander X.; Drouard, Marc Nature Physics, Vol. 9, Issue 10 https://doi.org/10.1038/nphys2733	journal	September 2013
Directional ionic transport across the oxide interface enables low-temperature epitaxy of rutile TiO2 Park, Yunkyu; Sim, Hyeji; Jo, Minguk Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15142-x	journal	March 2020
Metal–insulator transition tuned by oxygen vacancy migration across TiO2/VO2 interface Lu, Qiyang; Sohn, Changhee; Hu, Guoxiang Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-75695-1	journal	October 2020
Mott transition field effect transistor Newns, D. M.; Misewich, J. A.; Tsuei, C. C. Applied Physics Letters, Vol. 73, Issue 6 https://doi.org/10.1063/1.121999	journal	August 1998
Metal-insulator transition in epitaxial V1−xWxO2(0≤x≤0.33) thin films Shibuya, Keisuke; Kawasaki, Masashi; Tokura, Yoshinori Applied Physics Letters, Vol. 96, Issue 2 https://doi.org/10.1063/1.3291053	journal	January 2010
Field-effect modulation of conductance in VO ₂ nanobeam transistors with HfO ₂ as the gate dielectric Sengupta, Shamashis; Wang, Kevin; Liu, Kai Applied Physics Letters, Vol. 99, Issue 6 https://doi.org/10.1063/1.3624896	journal	August 2011
A heterojunction modulation-doped Mott transistor Son, Junwoo; Rajan, Siddharth; Stemmer, Susanne Journal of Applied Physics, Vol. 110, Issue 8 https://doi.org/10.1063/1.3651612	journal	October 2011
Probing the metal-insulator transition of NdNiO ₃ by electrostatic doping Son, Junwoo; Jalan, Bharat; Kajdos, Adam P. Applied Physics Letters, Vol. 99, Issue 19 https://doi.org/10.1063/1.3659310	journal	November 2011
Two-dimensional electron gas in a modulation-doped SrTiO ₃ /Sr(Ti, Zr)O ₃ heterostructure Kajdos, Adam P.; Ouellette, Daniel G.; Cain, Tyler A. Applied Physics Letters, Vol. 103, Issue 8 https://doi.org/10.1063/1.4819203	journal	August 2013
Modulation of over 10 ¹⁴ cm ⁻² electrons in SrTiO ₃ /GdTiO ₃ heterostructures Boucherit, M.; Shoron, O.; Jackson, C. A. Applied Physics Letters, Vol. 104, Issue 18 https://doi.org/10.1063/1.4875796	journal	May 2014
The new dedicated HAXPES beamline P22 at PETRAIII Schlueter, C.; Gloskovskii, A.; Ederer, K. PROCEEDINGS OF THE 13TH INTERNATIONAL CONFERENCE ON SYNCHROTRON RADIATION INSTRUMENTATION – SRI2018, AIP Conference Proceedings https://doi.org/10.1063/1.5084611	conference	January 2019
Atomically-smooth single-crystalline VO ₂ (101) thin films with sharp metal-insulator transition Mondal, Debasish; Mahapatra, Smruti Rekha; Ahmed, Tanweer Journal of Applied Physics, Vol. 126, Issue 21 https://doi.org/10.1063/1.5124106	journal	December 2019
Oxygen vacancies: The (in)visible friend of oxide electronics Gunkel, F.; Christensen, D. V.; Chen, Y. Z. Applied Physics Letters, Vol. 116, Issue 12 https://doi.org/10.1063/1.5143309	journal	March 2020
Electron mobilities in modulation‐doped semiconductor heterojunction superlattices Dingle, R.; Störmer, H. L.; Gossard, A. C. Applied Physics Letters, Vol. 33, Issue 7 https://doi.org/10.1063/1.90457	journal	October 1978
Doping-driven resistive collapse of the Mott insulator in a minimal model for VO2 Fratino, L.; Bag, S.; Camjayi, A. Physical Review B, Vol. 105, Issue 12 https://doi.org/10.1103/PhysRevB.105.125140	journal	March 2022
Metal-insulator transition in vanadium dioxide Zylbersztejn, A.; Mott, N. F. Physical Review B, Vol. 11, Issue 11, p. 4383-4395 https://doi.org/10.1103/PhysRevB.11.4383	journal	June 1975
Structural Aspects of the Metal-Insulator Transitions in Cr-Doped V O 2 Marezio, M.; McWhan, D. B.; Remeika, J. P. Physical Review B, Vol. 5, Issue 7 https://doi.org/10.1103/PhysRevB.5.2541	journal	April 1972
Evidence for a structurally-driven insulator-to-metal transition in VO 2 : A view from the ultrafast timescale Cavalleri, A.; Dekorsy, Th.; Chong, H. H. W. Physical Review B, Vol. 70, Issue 16 https://doi.org/10.1103/PhysRevB.70.161102	journal	October 2004
Modulation doping near Mott-insulator heterojunctions Lee, Wei-Cheng; MacDonald, A. H. Physical Review B, Vol. 74, Issue 7 https://doi.org/10.1103/PhysRevB.74.075106	journal	August 2006
Photoemission evidence for a Mott-Hubbard metal-insulator transition in VO 2 Eguchi, R.; Taguchi, M.; Matsunami, M. Physical Review B, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevB.78.075115	journal	August 2008
Insulator to correlated metal transition in V 1 − x Mo x O 2 Holman, K. L.; McQueen, T. M.; Williams, A. J. Physical Review B, Vol. 79, Issue 24 https://doi.org/10.1103/PhysRevB.79.245114	journal	June 2009
Metal-insulator transitions in TiO 2 / VO 2 superlattices Shibuya, Keisuke; Kawasaki, Masashi; Tokura, Yoshinori Physical Review B, Vol. 82, Issue 20 https://doi.org/10.1103/PhysRevB.82.205118	journal	November 2010
Filling-controlled Mott transition in W-doped VO2 Takami, Hidefumi; Kanki, Teruo; Ueda, Shigenori Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/PhysRevB.85.205111	journal	May 2012
Emergent Topological Phenomena in Thin Films of Pyrochlore Iridates Yang, Bohm-Jung; Nagaosa, Naoto Physical Review Letters, Vol. 112, Issue 24 https://doi.org/10.1103/PhysRevLett.112.246402	journal	June 2014
Effects of Low-Energy Excitations on Spectral Properties at Higher Binding Energy: The Metal-Insulator Transition of VO 2 Gatti, Matteo; Panaccione, Giancarlo; Reining, Lucia Physical Review Letters, Vol. 114, Issue 11 https://doi.org/10.1103/PhysRevLett.114.116402	journal	March 2015
Field Effect and Strongly Localized Carriers in the Metal-Insulator Transition Material VO 2 Martens, K.; Jeong, J. W.; Aetukuri, N. Physical Review Letters, Vol. 115, Issue 19 https://doi.org/10.1103/PhysRevLett.115.196401	journal	November 2015
Correlation-Driven Insulator-Metal Transition in Near-Ideal Vanadium Dioxide Films Gray, A. X.; Jeong, J.; Aetukuri, N. P. Physical Review Letters, Vol. 116, Issue 11 https://doi.org/10.1103/PhysRevLett.116.116403	journal	March 2016
Simultaneous Structural and Electronic Transitions in Epitaxial VO 2 / Ti O 2 ( 001 ) Paez, Galo J.; Singh, Christopher N.; Wahila, Matthew J. Physical Review Letters, Vol. 124, Issue 19 https://doi.org/10.1103/PhysRevLett.124.196402	journal	May 2020
Oxides Which Show a Metal-to-Insulator Transition at the Neel Temperature Morin, F. J. Physical Review Letters, Vol. 3, Issue 1 https://doi.org/10.1103/PhysRevLett.3.34	journal	July 1959
VO 2 : Peierls or Mott-Hubbard? A view from band theory Wentzcovitch, Renata M.; Schulz, Werner W.; Allen, Philip B. Physical Review Letters, Vol. 72, Issue 21 https://doi.org/10.1103/PhysRevLett.72.3389	journal	May 1994
Dynamical Singlets and Correlation-Assisted Peierls Transition in V O 2 Biermann, S.; Poteryaev, A.; Lichtenstein, A. I. Physical Review Letters, Vol. 94, Issue 2 https://doi.org/10.1103/PhysRevLett.94.026404	journal	January 2005
Oxygen transport in single-crystal LaAlO3 substrates Schwab, Christian; Schraknepper, Henning; De Souza, Roger A. Physical Review Materials, Vol. 5, Issue 10 https://doi.org/10.1103/PhysRevMaterials.5.105001	journal	October 2021
Local electronic structure of rutile RuO2 Occhialini, Connor A.; Bisogni, Valentina; You, Hoydoo Physical Review Research, Vol. 3, Issue 3 https://doi.org/10.1103/PhysRevResearch.3.033214	journal	September 2021
Metal-insulator transitions Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263 https://doi.org/10.1103/RevModPhys.70.1039	journal	October 1998
Modulation-doped GaAs/AlGaAs heterojunction field-effect transistors (MODFET's), ultrahigh-speed device for supercomputers Solomon, P. M.; Morkoc, H. IEEE Transactions on Electron Devices, Vol. 31, Issue 8 https://doi.org/10.1109/T-ED.1984.21654	journal	August 1984
Suppression of Metal-Insulator Transition in VO2 by Electric Field-Induced Oxygen Vacancy Formation Jeong, J.; Aetukuri, N.; Graf, T. Science, Vol. 339, Issue 6126 https://doi.org/10.1126/science.1230512	journal	March 2013
Functional Ion Defects in Transition Metal Oxides Kalinin, S. V.; Spaldin, N. A. Science, Vol. 341, Issue 6148 https://doi.org/10.1126/science.1243098	journal	August 2013
Molecular Beam Epitaxial Growth of Al-doped ZnMgO Alloy Films for Modulation-doped ZnO/ZnMgO Heterostructures Koike, Kazuto; Hama, Kenji; Nakashima, Ippei Japanese Journal of Applied Physics, Vol. 44, Issue 6R https://doi.org/10.1143/JJAP.44.3822	journal	June 2005
Conducting Transition Metal Oxides: Possibilities for RuO[sub 2] in VLSI Metallization Krusin-Elbaum, L. Journal of The Electrochemical Society, Vol. 135, Issue 10 https://doi.org/10.1149/1.2095391	journal	January 1988
Strongly Correlated Electronic Materials: Present and Future Dagotto, E.; Tokura, Y. MRS Bulletin, Vol. 33, Issue 11 https://doi.org/10.1557/mrs2008.223	journal	November 2008
X-Ray Spectroscopy of Ultra-Thin Oxide/Oxide Heteroepitaxial Films: A Case Study of Single-Nanometer VO2/TiO2 Quackenbush, Nicholas; Paik, Hanjong; Woicik, Joseph Materials, Vol. 8, Issue 8 https://doi.org/10.3390/ma8085255	journal	August 2015

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