Rippled graphene pores as fluidic memristive devices with synaptic and neuromorphic functionalities
Pith reviewed 2026-05-10 02:40 UTC · model grok-4.3
The pith
A micrometer-sized pore wrapped by rippled graphene exhibits memory effects in ion transport.
A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.
Core claim
The central claim is that nanoscale morphology at the pore wall, specifically the rippled and stacked graphene rim, regulates ion transport to create memory even in micrometer-scale pores. Slow ion dynamics in the curved edges produce history-dependent conductance that persists over time, enabling neuromorphic functionalities such as reversible state modification and reliable performance in image identification and neural signal analysis when devices are integrated into circuits.
What carries the argument
Rippled and tightly stacked graphene edges wrapping the pore rim, which confine ions to produce slow dynamics and memory in conductance.
If this is right
- The memory is ion-selective and shows endurance comparable to synaptic protein lifetimes.
- Programmable voltage spikes can reversibly modify conductance states across various electrolytes.
- Integrated circuits can store and process information with high reliability, including identification of greyscale and color images.
- Real-time analysis of emulated neural signals becomes possible through the synaptic plasticity.
- The nanoconfinement requirement for ionic memory shifts from overall pore size to design of the rim structure.
Where Pith is reading between the lines
- If the rim-structure approach works, similar memory could be created in other curved two-dimensional material pores without shrinking the entire channel to nanoscale.
- Fabrication of large arrays becomes simpler because micrometer pores avoid the precision challenges of nanometer drilling.
- These devices might interface more readily with biological ionic environments since they use water-dissolved ions as carriers.
- Varying the degree of rippling or number of stacked layers could be tested to tune retention times for specific applications.
Load-bearing premise
The memory effect is caused specifically by slow ion dynamics in the rippled graphene edges rather than surface chemistry changes, contamination, or measurement artifacts.
What would settle it
If devices fabricated with rippled graphene rims show no hysteresis or memory when the graphene is smoothed to remove ripples while keeping all other conditions identical, the attribution to confined edge dynamics would be falsified.
Figures
read the original abstract
Nanofluidic memristive devices work with nanoscale pores and ions dissolved in water, which harness the ionic memory effect aiming to store and process information. These devices share the same charge carriers as biological systems and bring hope for better emulating the neural functions and developing ionic circuits for neuromorphic applications. Specially, theory and experiments suggest that nanoconfinement is essential for inducing a memory effect, which places limit on the pore size to nm-scale or smaller. Such devices are difficult to scale up with precision and operate with long-term stability. Here, we show that a micrometer size pore, generally expected to exhibit a linear ion transport, can display a pronounced memory effect, if its rim is wrapped by strongly curved and tightly stacked graphene. We attribute the observation to slow ion dynamics confined in the rippled graphene edges. The devices are easy to scale up and integrate into fluidic circuits. The memory effect is ion-selective and exhibits long endurance comparable to the lifetime of synaptic proteins, which enables reversible modification of the conductance states using programmable voltage spikes and various electrolytes over a long time, akin to biological synaptic plasticity. Thanks to this plasticity, our devices and their integrated circuits enable storing, transmitting and processing information with high reliability, fidelity and accuracy, as evidenced in the identification of both greyscale and color images, and in the real-time analysis of emulated neural signals. Our results highlight nanoscale morphology of the pore wall as an important parameter regulating ion transport and indicate that the stringent nanoconfinement for ionic memory can be lifted from restricting the pore size to designing its rim structure. The devices and their integrated circuits may find use in ionic neuromorphic applications.
Editorial analysis
A structured set of objections, weighed in public.
Referee Report
Summary. The manuscript experimentally demonstrates that micrometer-scale graphene pores with strongly curved and tightly stacked rippled rims exhibit ionic memory effects, ion selectivity, and long-term endurance, which the authors attribute to slow ion dynamics confined within the rippled edges; this enables synaptic plasticity, neuromorphic functionalities including image identification, and suggests that rim morphology can relax the conventional nanoconfinement requirement for fluidic memristors.
Significance. If the attribution to rim-confined ion dynamics is substantiated, the result would be significant for relaxing the pore-size limit in ionic neuromorphic devices, enabling easier fabrication and integration. The reported endurance comparable to synaptic proteins and demonstrations of programmable conductance states with various electrolytes and real-time neural signal analysis represent concrete strengths in experimental scope.
major comments (2)
- [Results (I-V characteristics and device performance)] Results section on I-V hysteresis and memory effect: The central attribution of the observed memory effect specifically to slow ion dynamics in the rippled graphene edges is not supported by comparative controls (e.g., flat-rim pores, cleaned surfaces, or electrolyte-specific tests) that would exclude alternatives such as surface chemistry variations or artifacts; this is load-bearing for the claim that rim structure lifts the nanoconfinement requirement.
- [Methods] Methods and data presentation: The reporting of quantitative metrics, error bars, statistical controls, and detailed fabrication/characterization protocols for the memory effect, endurance, and ion selectivity is insufficient to assess robustness, as the abstract provides no such data and the full methods do not appear to include them.
minor comments (2)
- [Figures] Figure captions and legends should explicitly label conditions (e.g., different electrolytes, spike protocols) and include scale bars or error indicators where data are plotted.
- [Abstract] The abstract could more precisely separate observed phenomena from mechanistic attribution to avoid implying the mechanism is directly measured.
Simulated Author's Rebuttal
We thank the referee for the positive evaluation of our work's significance and for the constructive major comments, which help clarify the presentation and strengthen the attribution of the observed effects. We address each point below and have revised the manuscript accordingly where appropriate.
read point-by-point responses
-
Referee: Results section on I-V hysteresis and memory effect: The central attribution of the observed memory effect specifically to slow ion dynamics in the rippled graphene edges is not supported by comparative controls (e.g., flat-rim pores, cleaned surfaces, or electrolyte-specific tests) that would exclude alternatives such as surface chemistry variations or artifacts; this is load-bearing for the claim that rim structure lifts the nanoconfinement requirement.
Authors: We acknowledge that direct side-by-side controls with flat-rim pores are not included in the current manuscript, which limits the strength of the attribution. The paper does report ion selectivity across multiple electrolytes and long-term endurance data that are consistent with confinement in the rippled rims rather than generic surface effects. To address this concern rigorously, we will add a new discussion subsection that explicitly considers alternative explanations (surface chemistry, contamination, or bulk electrolyte effects) and explains why the rim morphology is the most parsimonious interpretation based on the pore-size dependence and the stacked-ripple geometry. If additional control data become available from ongoing experiments, they will be incorporated; otherwise the discussion will note this limitation transparently. revision: partial
-
Referee: Methods and data presentation: The reporting of quantitative metrics, error bars, statistical controls, and detailed fabrication/characterization protocols for the memory effect, endurance, and ion selectivity is insufficient to assess robustness, as the abstract provides no such data and the full methods do not appear to include them.
Authors: We agree that the methods and results sections require expanded quantitative detail for reproducibility. In the revised manuscript we will (i) add error bars and statistical measures (standard deviation or SEM across multiple devices) to all I-V, endurance, and selectivity plots; (ii) include a dedicated methods subsection with step-by-step fabrication protocols, cleaning procedures, and characterization techniques (SEM, Raman, ionic current measurements); and (iii) report numerical values for key metrics such as on/off ratios, retention times, and endurance cycle counts. These additions will appear both in the main text and in an expanded supplementary information file. revision: yes
Circularity Check
No circularity: experimental observations independent of self-referential modeling or fitted predictions
full rationale
The manuscript is an experimental study reporting fabrication of micrometer-scale graphene pores with rippled rims, direct I-V measurements showing hysteresis and synaptic-like plasticity, and attribution of the effect to confined ion dynamics based on observed morphology. No derivation chain, equations, or first-principles predictions appear that reduce to inputs by construction. The central claim rests on comparative device behavior and endurance tests rather than any self-citation load-bearing uniqueness theorem, ansatz smuggling, or renaming of known results. Self-citations, if present in the full text, are not required to justify the core experimental attribution, satisfying the criteria for a self-contained observational result.
Axiom & Free-Parameter Ledger
axioms (1)
- domain assumption Standard principles of ion transport under nanoconfinement apply to rippled graphene edges
Reference graph
Works this paper leans on
-
[1]
Voglis, G. & Tavernarakis, N. The role of synaptic ion channels in synaptic plasticity. EMBO Rep. 7, 1104–1110 (2006)
work page 2006
-
[2]
Gerstner, W., Kistler, W. M., Naud, R. & Paninski, L. Neuronal dynamics: From single neurons to networks and models of cognition. (Cambridge University Press, West Nyack, 2014)
work page 2014
-
[3]
Memristor-the missing circuit element
Chua, L. Memristor-the missing circuit element. IEEE Trans. Circuit Theory 18, 507–519 (1971)
work page 1971
-
[4]
Chua, L., Sirakoulis, G. C. & Adamatzky, A. Handbook of memristor networks. (Springer, Cham, 2019)
work page 2019
-
[5]
Wang, Z. et al. Resistive switching materials for information processing. Nat. Rev. Mater. 5, 173–195 (2020)
work page 2020
-
[6]
Sebastian, A., Le Gallo, M., Khaddam-Aljameh, R. & Eleftheriou, E. Memory devices and applications for in-memory computing. Nat. Nanotechnol. 15, 529–544 (2020)
work page 2020
-
[7]
Lanza, M. et al. Memristive technologies for data storage, computation, encryption, and radio - frequency communication. Science 376, eabj9979 (2022)
work page 2022
-
[8]
Mayer, S. F. et al. Lumen charge governs gated ion transport in β-barrel nanopores. Nat. Nanotechnol. 21, 116–124 (2026)
work page 2026
-
[9]
Laughlin, S. B. de Ruyter van Steveninck, R. R. & Anderson, J. C. The metabolic cost of neural information. Nat. Neurosci. 1, 36–41 (1998)
work page 1998
-
[10]
Fu, S. et al. Constructing artificial neurons with functional parameters comprehensively matching biological values. Nat. Commun. 16, 8599 (2025)
work page 2025
-
[11]
Emmerich, T. et al. Nanofluidics. Nat. Rev. Methods Primers 4, 1–18 (2024)
work page 2024
- [12]
-
[13]
Bu, Y., Ahmed, Z. & Yobas, L. A nanofluidic memristor based on ion concentration polarization. Analyst 144, 7168–7172 (2019)
work page 2019
-
[14]
Zhang, P. et al. Nanochannel -based transport in an interfacial memristor can emulate the analog weight modulation of synapses. Nano Lett. 19, 4279–4286 (2019)
work page 2019
-
[15]
Robin, P., Kavokine, N. & Bocquet, L. Modeling of emergent memory and voltag e spiking in ionic transport through angstrom-scale slits. Science 373, 687–691 (2021)
work page 2021
-
[16]
Robin, P. et al. Long -term memory and synapse -like dynamics in two -dimensional nanofluidic channels. Science 379, 161–167 (2023)
work page 2023
-
[17]
Xiong, T. et al. Neuromorphic functions with a polyelectrolyte -confined fluidic memristor. Science 379, 156–161 (2023)
work page 2023
-
[18]
Emmerich, T. et al. Nanofluidic logic with mechano–ionic memristive switches. Nat. Electron. 7, 271– 278 (2024). 18
work page 2024
-
[19]
Kamsma, T. M. et al. Brain-inspired computing with fluidic iontronic nanochannels. Proc. Natl Acad. Sci. USA 121, e2320242121 (2024)
work page 2024
-
[20]
Ling, Y. et al. Single -pore nanofluidic logic memristor with reconfigurable synaptic functions and designable combinations. J. Am. Chem. Soc. 146, 14558–14565 (2024)
work page 2024
-
[21]
Yu, S.-Y. et al. Metal –organic framework nanofluidic synapse. J. Am. Chem. Soc. 146, 27022–27029 (2024)
work page 2024
-
[22]
Song, R. et al. Nanofluidic memristive transition and synaptic emulation in atomically thin pores. Nano Lett. 25, 5646–5655 (2025)
work page 2025
-
[23]
Programmable memristors with two-dimensional nanofluidic channels
Ismail, A., et al. Programmable memristors with two-dimensional nanofluidic channels. Nat. Commun. 16, 7008 (2025)
work page 2025
-
[24]
Cohen, L. D. & Ziv, N. E. Neuronal and synaptic protein lifetimes. Curr. Opin. Neurobiol. 57, 9–16 (2019)
work page 2019
-
[25]
Mohar, B. et al. DELTA: a metho d for brain-wide measurement of synaptic protein turnover reveals localized plasticity during learning. Nat. Neurosci. 28, 1089–1098 (2025)
work page 2025
-
[26]
Wahab, O. J. et al. Proton transport through nanoscale corrugations in two -dimensional crystals. Nature 620, 782–786 (2023)
work page 2023
-
[27]
Wu, Z. F. et al. Proton and molecular permeation through the basal plane of monolayer graphene oxide. Nat. Commun. 14, 7756 (2023)
work page 2023
-
[28]
Ji, Y. et al. High proton conductivity through angstrom-porous titania. Nat. Commun. 15, 10546 (2024)
work page 2024
-
[29]
Schnurr, B., Gittes, F. & MacKintosh, F. C. Metastable intermediates in the condensation of semiflexible polymers. Phys. Rev. E 65, 061904 (2002)
work page 2002
-
[30]
Xu, Z. P. & Buehler, M. J. Geometry controls conformation of graphene sheets: membranes, ribbons, and scrolls. ACS Nano 4, 3869–3876 (2010)
work page 2010
-
[31]
Zhao, Y. et al. Automated processing and transfer of two -dimensional materials with robotics. Nat. Chem. Eng. 2, 296–308 (2025)
work page 2025
-
[32]
Perram, J. W. & Stiles, P. J. On the nature of liquid junction and membrane potentials. Phys. Chem. Chem. Phys. 8, 4200 (2006)
work page 2006
-
[33]
Hall, J. E. Access resistance of a small circular pore. J. Gen. Physiol. 66, 531–532 (1975)
work page 1975
-
[34]
Zhang, W. C., Zhang, A., Zhou, W. Z., Ji, Y., Xu, Z. P. & Sun, P. Z. Revisiting ion transport through micropores: significant and non-negligible surface transport. Nanoscale Horiz. 11, 795–802 (2026)
work page 2026
-
[35]
LeCun, Y., Cortes, C. & Burges, C. J. C. The MNIST database of handwritten digits. http://yann.lecun.com/exdb/mnist/ (1998)
work page 1998
-
[36]
Krizhevsky, A., Hinton, G. et al. Learning multiple layers of features from tiny images. (University of Toronto, 2009)
work page 2009
-
[37]
Eshraghian, J. K. et al. Training spiking neural networks using lessons from deep learning. Proc. IEEE 111, 1016–1054 (2023)
work page 2023
-
[38]
Bean, B. P. The action potential in mammalian central neurons. Nat. Rev. Neurosci. 8, 451 (2007)
work page 2007
-
[39]
Brown, E. N., Kass, R. E. & Mitra, P. P. Multiple neural spike train data analysis: state of -the-art and future challenges. Nat. Neurosci. 7, 456–461 (2004)
work page 2004
-
[40]
Kruskal, Peter B., Jiang, Z., Gao, T. & Lieber, C. M. Beyond the patch clamp: nanotechnologies for intracellular recording. Neuron 86, 21–24 (2015)
work page 2015
-
[41]
Anumanchipalli, G. K., Chartier, J. & Chang, E. F. Speech synthesis from neural decoding of spoken sentences. Nature 568, 493–498 (2019)
work page 2019
-
[42]
Zhu, X., Wang, Q. & Lu, W. D. Memristor networks for real-time neural activity analysis. Nat. Commun. 11, 2439 (2020). Acknowledgements 19 P.Z.S. acknowledges support from the Natural Science Foundation of China (52322319), the Science and Technology Development Fund, Macao SAR (0002/2024/TFP, 0063/2023/RIA1, 0107/20 24/AMJ), UM research grant (MYRG -GRG2...
work page 2020
-
[43]
Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499, 419–425 (2013)
work page 2013
-
[44]
Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614– 617 (2013)
work page 2013
-
[45]
Cheng, L. J. & Guo, L. J. Rectified ion transport through concentration gradient in homogeneous silica nanochannels. Nano Lett. 7, 3165–3171 (2007)
work page 2007
-
[46]
Poggioli, A. R., Siria, A. & Bocquet, L. Beyond the tradeoff: dynamic selectivity in ionic transport and current rectification. J. Phys. Chem. B 123, 1171–1185 (2019)
work page 2019
-
[47]
Rollings, R. C., Kuan, A. T. & Golovchenko, J. A. Ion selectivity of graphene nanopores. Nat. Commun. 7, 11408 (2016)
work page 2016
-
[48]
Meyer, J. C., Girit, C. O., Crommie, M. F. & Zettl, A. Imaging and dynamics of light atoms and molecules on graphene. Nature 454, 319–322 (2008)
work page 2008
-
[49]
Sun, P. et al. Selective trans -membrane transport of alkali and alkaline earth cations through graphene oxide membranes based on cation-π interactions. ACS Nano 8, 850–859 (2014)
work page 2014
-
[50]
Chen, L. et al. Ion sieving in graphene oxide membranes via cationic co ntrol of interlayer spacing. Nature 550, 380–383 (2017)
work page 2017
-
[51]
Lin, K., Lin, C.-Y., Polster, J. W., Chen, Y. & Siwy, Z. S. Charge inversion and calcium gating in mixtures of ions in nanopores. J. Am. Chem. Soc. 142, 2925–2934 (2020)
work page 2020
-
[52]
Thermodynamics of solvation of ions
Marcus, Y. Thermodynamics of solvation of ions. Part 5.—Gibbs free energy of hydration at 298.15 K. J. Chem. Soc. Faraday Trans. 87, 2995–2999 (1991)
work page 1991
-
[53]
Sah, M. P. et al. A generic model of memristors with parasitic components. IEEE Trans. Circuits Syst. I: Regul. Pap. 62, 891–898 (2015). 34
work page 2015
-
[54]
Xiao, Y. et al. Neural functions enabled by a polarity-switchable nanofluidic memristor. Nano Lett. 24, 12515–12521 (2024)
work page 2024
-
[55]
Nagel, L. W. & Pederson, D. O. SPICE (Simulation Program with Integrated Circuit Emphasis). http://www2.eecs.berkeley.edu/Pubs/TechRpts/1973/22871.html (1973)
work page 1973
-
[56]
Xu, Z. Soft nanofluidic machinery. ACS Nano 18, 9765–9772 (2024)
work page 2024
-
[57]
Lee, C. et al. Large apparent electric size of solid -state nanopores due to spatially extended surface conduction. Nano Lett. 12, 4037–4044 (2012)
work page 2012
-
[58]
Logg, A., Mardal, K. A. & Wells, G. N. Automated Solution of Differential Equations by the Finite Element Method: The FEniCS Book (Springer Berlin Heidelberg, Heidelberg, 2012)
work page 2012
-
[59]
Fast parallel algorithms for short-range molecular dynamics
Plimpton, S. Fast parallel algorithms for short-range molecular dynamics. J. Comput. Phys. 117, 1–19 (1995)
work page 1995
-
[60]
Berendsen, H. J. C., Grigera, J. R. & Straatsma, T. P. The missing term in effective pair potentials. J. Phys. Chem. 91, 6269–6271 (1987)
work page 1987
-
[61]
Ryckaert, J.-P., Ciccotti, G. & Berendsen, H. J. Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes. J. Comput. Phys. 23, 327–341 (1977)
work page 1977
-
[62]
Jorgensen, W. L. & Tirado-Rives, J. The OPLS [optimized potentials for liquid simulations] potential functions for proteins, energy minimizations for crystals of cyclic peptides and crambin. J. Am. Chem. Soc. 110, 1657–1666 (1988)
work page 1988
-
[63]
Zhou, K. & Xu, Z. Deciphering the nature of ion-graphene interaction. Phys. Rev. Res. 2, 042034 (2020)
work page 2020
-
[64]
Hockney, R. W. & Eastwood, J. W. Computer Simulation Using Particles (CRC Press, 2021)
work page 2021
-
[65]
Luo, J. et al. Compression and aggregation-resistant particles of crumpled soft sheets. ACS Nano 5, 8943–8949 (2011)
work page 2011
-
[66]
Cranford, S. W. & Buehler, M. J. Packing efficiency and accessible surface area of crumpled graphene. Phys. Rev. B, 84, 205451 (2011)
work page 2011
- [67]
-
[68]
Zhou, K. & Xu, Z. Field -enhanced selectivity in nanoconfined ionic transport. Nanoscale 12, 6512– 6521 (2020)
work page 2020
-
[69]
Dočkal, J., Moučka, F. & Lísal, M. Molecular dynamics of graphene –electrolyte interface: Interfacial solution structure and molecular diffusion. J. Phys. Chem. C 123, 26379– 26396 (2019)
work page 2019
-
[70]
Gillespie, D. T. Exact stochastic simulation of coupled chemical rea ctions. J. Phys. Chem. 81, 2340– 2361 (1977)
work page 1977
- [71]
-
[72]
Paulo, G. et al. Hydrophobically gated memristive nanopores for neuromorphic applications. Nat. Commun. 14, 8390 (2023). 35 Supplementary figures and tables Figure S1. Additional electron micrographs. a, A representative TEM image of the rippled graphene edges. Dashed curve marks the position of SiNx aperture rim. Short yellow lines mark some of the paral...
work page 2023
discussion (0)
Sign in with ORCID, Apple, or X to comment. Anyone can read and Pith papers without signing in.