Piezo‐Acoustic Resistive Switching Behaviors in High‐Performance Organic–Inorganic Hybrid Perovskite Memristors

Abstract Memristors are regarded as promising candidates for breaking the problems including high off‐chip memory access delays and the hash rate cost of frequent data moving induced by algorithms for data‐intensive applications of existing computational systems. Recently, organic–inorganic halide perovskites (OIHPs) have been recognized as exceptionally favorable materials for memristors due to ease of preparation, excellent electrical conductivity, and structural flexibility. However, research on OIHP‐based memristors focuses on modulating resistive switching (RS) performance through electric fields, resulting in difficulties in moving away from complex external circuits and wire connections. Here, a multilayer memristor has been constructed with eutectic gallium and indium (EGaIn)/ MAPbI3/poly(3,4‐ethylenedioxythiophene): poly(4‐styrenesulphonate) (PEDOT: PSS)/indium tin oxide (ITO) structure, which exhibits reproducible and reliable bipolar RS with low SET/RESET voltages, stable endurance, ultrahigh average ON/OFF ratio, and excellent retention. Importantly, based on ion migration activated by sound‐driven piezoelectric effects, the device exhibits a stable acoustic response with an average ON/OFF ratio greater than 103, thus realizing non‐contact, multi‐signal, and far‐field control in RS modulation. This study provides a single‐structure multifunctional memristor as an integrated architecture for sensing, data storage, and computing.


Section 1. Schematic drawing of the memristors.
A schematic illustration of the MAPbI3-based memristors with a vertically aligned structure was displayed in Figure S1, which showed that the device was composed of the EGaIn top electrode, a MAPbI3 RS layer, a protective layer of PEDOT:PSS, and a bottom electrode of ITO on a glass substrate.

Section 3. Top-view SEM image of surface morphology
The top-view scanning electron microscopy (SEM) image (Figure S3) confirmed high surface coverage and reveals uniform perovskites film of MAPbI3 surface which was deposited by a one-step solution method under ambient condition.

Section 5. Raman spectroscopy of the MAPbI3 film
In addition, Raman spectroscopy with a range from 50 to 450 cm −1 provided a way to selectively study the structural dynamics of MA + .As illustrated in Figure S5, the modes located around 94 cm −1 originated from the bending or stretching motions of the octahedral PbI6 4− framework. [3,4]The experimentally measured Raman vibrations between 120 and 400 cm −1 can be attributable to stretching, wagging, and MA−MA asymmetrical stretching modes.
Interestingly, the peaks at 120 and 154 cm −1 were clear markers of vibrational modes of MA + , and those at 183, 200, 248, 299, and 398 cm −1 were purely associated with the torsional modes of the MA + . [5,6]Since MA + may be disordered around eight possible orientations in the octahedral PbI6 4− framework, there was an intrinsic dipole moment of MA + . [7]Therefore, the Raman spectrum confirmed that an intrinsic dipole MA + existed in our as-fabricated MAPbI3 perovskites, which may induce a structural distortion of the framework and generate crystal structure without inversion symmetry related to ferroelectric properties.

Figure
Figure S2 presented the atomic force microscopy (AFM) topography image of the MAPbI3

Figure S2 .
Figure S2.AFM image of the MAPbI3 film surface on a glass substrate.

Figure S3 .
Figure S3.Top-view SEM image of surface morphology of the MAPbI3 film on the

Figure S5 .
Figure S5.Raman spectroscopy of the MAPbI3 film on a glass substrate.

Figure S6 .
Figure S6.Absorption spectrum of the MAPbI3 film deposited on a glass substrate.

Figure S7 .
Figure S7.The PL spectrum of the MAPbI3 film deposited on a glass substrate.(excitation

Figure S9 .
Figure S9.The switching speed measurement result of the

Figure S10 .
Figure S10.Fitted logarithmic I-V behavior of negative voltage sweep.

Section 12 .
Figure S11.Cumulative probability plot of electrical endurance data.

Figure S12 .
Figure S12.The VTFL of the MAPbI3-memristors without the sound and with the sound at

Figure S15 .
Figure S15.Cumulative probability plot of acoustic-HRSs induced by different SPL.

Table S1 .
Statistical measures of endurance data.

Table S2 .
Summary of performance parameters of other memristors and this work.