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Multifunctional molybdenum disulfide flash memory using a PEDOT:PSS floating gate


Two-dimensional transition metal dichalcogenide materials (TMDs), such as molybdenum disulfide (MoS2), have been considered promising candidates for future electronic applications owing to their electrical, mechanical, and optical properties. Here, we present a new concept for multifunctional MoS2 flash memory by combining a MoS2 channel with a PEDOT:PSS floating layer. The proposed MoS2 memory devices exhibit a switching ratio as high as 2.3 × 107, a large memory window (54.6 ± 7.80 V), and high endurance (>1,000 cycles). As the PEDOT:PSS film enables a low-temperature solution-coating process and mechanical flexibility, the proposed P-memory can be embedded on a polyimide substrate over a rigid silicon substrate, offering high mechanical endurance (over 1,000 cycle bending test). Furthermore, both MoS2 and PEDOT:PSS have a bandgap that is desirable in optoelectronic memory operation, where charge carriers are stored differently in the floating gate depending on light illumination. As a new application that combines photodiodes and memory functions, we demonstrate multilevel memory programming based on light intensity and color.


With the advent of the fourth industrial revolution, consumer electronics are in dire need of versatility beyond conventional electronic functions1,2,3,4. For example, conventional memory technology requires high-performance memory characteristics, such as fast switching, long-term retention, and high endurance5,6,7,8. On the other hand, current electronics demand the development of multifunctional memory devices with characteristics such as mechanical flexibility9,10,11, multilevel storage12,13, neuromorphic functions14,15, and tunable memory operation16, along with the conventional expectation of excellent memory features. However, existing silicon-based memory processes and structures have limitations in developing new features when the multifunctional memory deviates from the conventional complementary metal–oxide–semiconductor process frame. Therefore, with the development of new materials, the development of new electronic device concepts is crucial.

Meanwhile, as emerging semiconductor materials, transition metal dichalcogenides (TMDs) have attracted considerable attention17,18,19,20,21. TMDs have the potential to provide multifunctional material platforms due to a variety of physical properties, including their atomically thin nature22, van der Waals interface23, and controllable energy band structure24,25,26. Moreover, TMDs have shown the possibility of new electronic device features such as gate-tunable memristic behavior16,27, neuromorphic functions28, and optoelectronic properties29,30.

Here, we present multifunctional nonvolatile memory using a molybdenum disulfide (MoS2) semiconductor and a poly(3,4-ethylenedioxythinophene):poly(styrene sulfonate) (PEDOT:PSS)31 floating gate (P-memory). The combination of the MoS2 semiconductor and PEDOT:PSS floating gate provides a switching current ratio as high as 2.3 × 107, a large memory window up to 62 V, excellent endurance (>1000 cycles), and a long retention time (>2000 s). We also investigate device-to-device variation by examining 30 P-memory devices fabricated with the same fabrication process. This process results in uniform memory operation properties with average Ierase/Iprogram of 2.18 × 106 ± 4.77 × 106, memory window of 54.3 V ± 7.80 V, threshold voltage under the programmed state VTH, programmed of 16.40 ± 8.25 V, and threshold voltage under the erased state VTH, erased of −40.53 ± 5.87 V. Furthermore, the proposed P-memory has photoprogrammable memory behavior, as photoinduced charge carriers contribute to programming and erasing operations in P-memory. As a result, we demonstrate photosensing with nonvolatile memory behavior to distinguish illumination light intensity and color. This information is stored directly inside the floating gate. Finally, we implement P-memory embedded onto a flexible polyimide (PI) substrate, as both MoS2 and PEDOT:PSS can be simply deposited regardless of the substrate type. The fabricated P-memory on the PI substrate exhibits excellent memory operation (Ierase/Iprogram= 1.07 × 106) with a high mechanical endurance (over 1000 cycle bending test). This result suggests that the multifunctional characteristics of a flash memory device can be obtained from a new material combination of layered MoS2 and PEDOT:PSS polymer in a floating-gate transistor structure.

Materials and methods

Device fabrication

The device fabrication process is schematically shown in Fig. S1. A Si/SiO2 substrate was treated with O2 plasma for 5 min. A synthesized highly resistive PEDOT:PSS solution was spin-coated on the substrate at 8000 rpm for 60 s through a 0.45 µm syringe filter. The thin film was then thermally annealed on a hot plate at 150 °C for 10 min. After floating-gate formation on the Si/SiO2 substrate, Al2O3 of 80 nm thickness as the tunneling dielectric layer (TDL) was deposited on the PEDOT:PSS floating-gate layer using ALD. To utilize MoS2 flakes as the channel, mechanically exfoliated MoS2 flakes were transferred onto the TDL by peeling them from a bulk crystal using Scotch tape. To complete the P-memory device fabrication, Ti/Au (20 nm/100 nm) source/drain electrodes, respectively, were patterned by photolithography using AZ GXR-601 photoresist, followed by E-beam evaporation and an etching process. Next, a 20 nm-thick Al2O3 passivation layer (PL) was deposited on the P-memory device by using ALD. For flexible memories, a flexible substrate was prepared by spin coating solution-based PI on a cleaned SiO2/Si substrate (3000 rpm for 30 s). Then, the flexible device was fabricated following the same process as shown in Scheme 1. As the last step, the flexible memory was peeled off by carefully separating the edges of the flexible memory and rigid substate with tweezers, which completed the flexible memory fabrication process.

Scheme 1

Fabrication process for flexible MoS2 flash memory using a PEDOT:PSS floating gate and solution-coated polyimide (PI) as a flexible substrate.

Synthesis of the highly resistive PEDOT:PSS solution

Poly(4-styrene sulfonate) (PSS) was used as a dispersant and dopant for PEDOT. The weight ratio of PEDOT:PSS was controlled to be 1:7.5. To synthesize the PEDOT:PSS dispersion, PSS (18.75 g) was added to distilled water (1000 g), and the mixture was stirred for 30 min. Then, nitrogen gas (99.999%) was bubbled through the solution for 60 min at a rate of 3 L min−1 to prevent oxidation by the dissolved oxygen in the water. To this solution, the EDOT monomer (2.50 g, 1.76 × 10−2 mol) was added and stirred with a mechanical stirrer for 30 min. The synthesis of the PEDOT:PSS dispersion was carried out using an Fe3+-catalyzed oxidative polymerization process. The oxidizing agents iron(III) sulfate (0.035 g, 8.79 × 10–5 mol) and sodium persulfate (5.02 g, 2.1 × 10–2 mol) were dissolved in 100 mL of distilled water by sonication and added to the reaction solution. Polymerization was performed for 40 h at 25 °C with bubbling nitrogen gas. After polymerization of the PEDOT:PSS dispersion, the product was mixed with 500 mL of a mixture of cation and anion ion exchange resin for 1 h and filtered with a 30 μm mesh filter. Table 1 shows previous reports about solvent exchange processes for water-based PEDOT:PSS solutions.

Table 1 Previously reported solvent exchange processes for water-based PEDOT:PSS solutions.

Device characterization

The memory operation characteristics of MoS2 flash memory devices were determined with a Keithley 4200-SCS semiconductor characterization system equipped with a probe station in the dark under ambient atmosphere. For determining the photoinduced memory operation properties, illumination sources of 638 nm and 405 nm (MCLS1, Thorlabs) and 532 nm (MGL-FN-532, CNI) were used. The incident power densities of the illumination light were measured by a laser power meter (PM100A, Thorlabs). To perform a cyclic bending test, the flexible MoS2 flash memory was loaded onto a multimodal bending tester, which repeated the sequence of a tensile stress (1 s)/flat (1 s) cycle 1000 times. The surface morphology and thickness profile of MoS2 were measured using atomic force microscopy (XE7, Park Systems).

Results and discussion

Flash memory structure based on MoS2 and PEDOT:PSS

First, we fabricated the P-memory on a rigid SiO2/Si substrate. The memory device is composed of multilayer MoS2 (thickness of 94.09 nm) as the channel; PEDOT:PSS of 80 nm thickness as the floating gate; 80 nm- and 40 nm-thick Al2O3 as a TDL and a PL, respectively; Ti/Au (20 nm/100 nm) as source/drain electrodes, respectively; and a 300 nm SiO2/Si substrate as a blocking dielectric layer (BDL) and a control gate (CG) (Fig. 1a). Further details of the fabrication process are provided in Fig. S1, and thickness scans are shown in Fig. S2.

Fig. 1: MoS2 flash memory using a PEDOT:PSS floating gate.

a Three-dimensional schematic illustration of MoS2 flash memory using a PEDOT:PSS floating gate. b Molecular structure of PEDOT:PSS. c Optical microscope image of fabricated MoS2 flash memory. Scale bar is 20 μm. d Transfer characteristics showing negligible hysteresis of the MoS2 transistor without the PEDOT:PSS floating gate under forward and reverse gate bias sweeps at VD = 1 V. e Transfer characteristics of MoS2 flash memory with a PEDOT:PSS floating gate. f Endurance of MoS2 flash memory. ID plot under the programmed state (red dot) and erased state (blue dot) for 1000 consecutive sweep cycles. One cycle consists of a program and erase voltage sweep from −60 V to 60 V and from 60 V to −60 V at VD = 1 V. Endurance of the ID switching ratio (Ierase/Iprogram) as a function of 1000 consecutive sweep cycles (bottom). Energy band diagram of the MoS2 memory device with a PEDOT:PSS floating gate for g programming and h erasing operation. i Retention characteristics of the MoS2 memory device with a PEDOT:PSS floating gate under programmed and erased states. The memory device was programmed at VC = 30 V and erased at VC = − 30 V. j Retention characteristics of the extrapolated line on a double logarithmic scale.

We spin-coated a PEDOT:PSS layer on top of a BDL SiO2 layer, and thereby, the PEDOT:PSS acted as a charge trapping layer for data storage operation (Fig. 1b, c). To understand the effects of the floating-gate layer, we characterized the MoS2 transistor depending on the existence of the PEDOT:PSS floating gate using the same device structure and fabrication conditions. The MoS2 transistor without the PEDOT:PSS floating gate exhibited transfer characteristics without I-V hysteresis (Fig. 1d). On the other hand, the P-memory with the PEDOT:PSS floating gate exhibited transfer characteristic with a large memory window of 54.6 V ± 7.80 V, indicating that the PEDOT:PSS floating gate between the TDL and BDL layers acts as a charge storage layer (Fig. 1e and Fig. S3), showing a switching ratio as high as 2.3 × 107.

Electrical characteristics of the P-memory

To investigate the endurance of the P-memory, we performed 1000 consecutive sweeps of programming and erasing operations (Vprogram = 60 V and Verase = −60 V) (Fig. 1f). The measured endurance of the P-memory exhibited stable programming and erasing operations with average Ierase of 1.4 ± 0.25 µA, Iprogram of 9.46 ± 11.7 pA, and Ierase/Iprogram of 1.07 × 106 under 1000 consecutive sweep cycles. We also evaluated the dynamic behavior of the P-memory (Fig. S4). Stable switching behavior between the programmed and erased states was obtained depending on the applied voltage pulses, with a programming pulse of 45 V at 400 ms and an erasing pulse of −45 V at 400 ms for a fixed VD = 1 V. Figure 1g, h shows simplified energy band diagrams of the P-memory under programming and erasing operations considering an energy bandgap of MoS2 of 5.15–5.39 eV26,32. Electron carriers enter the PEDOT:PSS floating gate through the TDL Al2O3 layer by the mechanisms of Fowler-Nordheim tunneling33 and trap-assisted tunneling (TAT)34, resulting in a positive shift of VTH. Under a negative applied VG (i.e., VG < − 20 V), the trapped electrons pass through the energy barrier inside the floating gate, causing a negative shift of VTH. By enlarging the applied CG voltage VCG bias in the P-memory, the degree of VTH shift was controlled (Fig. S5). With greater applied VG and thus energy band bending to inject more electron carriers into the floating gate, a larger shift of VTH can be obtained.

To investigate the reproducibility and uniformity of the P-memory, we fabricated and characterized 30 devices. Figure 2a, b shows the statistical variation of the Iprogram/Ierase ratio (average value = 2.18 × 106 ± 4.77 × 106) and the memory window (average value = 54.6 V ± 7.80), respectively, in the 30 devices. The distribution shows that the devices with an Iprogram/Ierase ratio ≥105 comprise ~75% of the 30 devices. In addition, 17 devices have a memory window ranging from 50 V to 60 V, ~50% of the total. Figure 2c, d presents the VTH distribution in the programmed state (Vprogram = 60 V) and erased state (Verase = −60 V), respectively. The obtained average VTH is 16.40 ± 8.25 V in the programmed state and −40.53 ± 5.87 V in the erased state. Details of the 30 P-memory device characteristics are given in Figs. S6 and S7.

Fig. 2: Statistical analysis of the properties of 30 distinct MoS2 flash memories.

Histogram showing the statistical distribution of a Ierase/Iprogram, b the memory window, (c) the threshold voltage at Vprogram = 60 V, and d the threshold voltage at Verase = −60 V.

Photoactivation effect on the P-memory

In the P-memory, the illumination light wavelength and intensity information can be stored as multilayered MoS2- and PEDOT:PSS-polymer-generated photoactivated excess carriers (Fig. 3a, b). To study the photoactivation effect on the operation of the P-memory, we illuminated it with light (excitation wavelength λex = 405 nm and incident optical power densities Pinc = 1 and 5 mW/cm2) during programming and erasing operations (i.e., photoinduced programming and photoinduced erasing, respectively). After the respective photoinduced programming and erasing operations, we performed a DC sweep of the P-memory to observe how light illumination influences the charge programming and erasing behavior (Fig. 3d, e). When programming in the dark state was activated, VTH shifted to the positive side, showing VTH = 7.18 V, whereas when the programming was operated under a light illumination of Pinc = 1 mW/cm2, a smaller VTH shift to VTH = 4.23 V was observed. The observed phenomenon is attributable to the charge screening effect of the photogenerated excess carriers, preventing tunneling of electron carriers into the floating PEDOT:PSS layer (Fig. 3c). As a result, a smaller VTH shift is induced by the programming under light illumination.

Fig. 3: Photoinduced memory operation.

a Schematic of MoS2 flash memory with a PEDOT:PSS floating gate under light illumination. b Three-dimensional cross-sectional schematic image of MoS2 flash memory under light illumination. c Energy band diagram of MoS2 flash memory under light illumination. d Transfer curves of MoS2 flash memory depending on various photoinduced programming operations. e Transfer curves of MoS2 flash memory after various photoinduced erasing operations. The excitation wavelength (λex) of the laser is 405 nm, and the incident optical power densities (Pinc) are 1 and 5 mW/cm2.

It was observed that a higher Pinc = 5 mW/cm2 resulted in more photogenerated excess carriers that contributed to the screening effect, and thus, less of a VTH shift (VTH = 3.75 V) was observed compared to that of the programmed state under Pinc = 1 mW/cm2 (Fig. 4a). We also investigated the light illumination effects during the erasing operation. Different from the photoinduced programming behavior, there was no VTH change under the photoinduced erasing operation. Rather than a change in the VTH shift, the photoinduced erasing operation resulted in an increase in the on-current in the switching-on region (VG > 10 V). The observed increase in the on-current resulted from the slow decay of the generated photocurrent in the multilayered MoS2, which supports previously reported phenomena in several studies35,36,37. The photoinduced programming and erasing behaviors under other light illumination (λex = 532 and 638 nm) are shown in Figs. S811.

Fig. 4: Parameters extracted from photoinduced memory operation characteristics.

Variation of the a threshold voltage (VTH), b transconductance (gm), c on-current, and d off-current of MoS2 flash memory after various photoinduced programming/erasing operations. Red circles: erasing operation. Blue squares: programming operation.

Photosensing memory operation

The photoinduced programming behavior with a change in VTH shift allowed us to demonstrate multilevel photomemory applications that combine photodiodes with memory functions. During the programming operation, the P-memory is programmed differently depending on the presence or absence of light illumination and its light intensity, and thus, the degree of light exposure can be directly stored in the device. We illuminated blue light (λex = 405 nm) onto the P-memory during the programming operation at VP = 30 V, and we sequentially measured the read current at VR = 0 V as a function of the photosensing retention time (Fig. 5a). The programming operation at VP = 30 V in the dark resulted in the P-memory exhibiting VTH = 7.18 V, which produced a current of 1–2 pA (IR) at VR = 0 V across the entire range of the photosensing retention time. On the other hand, the programming operation at VP = 30 V under light illumination enabled the P-memory to provide a more than thousandfold higher IR than that in the programmed state in the dark. The increased IR with photoactivated programming was unchanged over the entire range of the photosensing retention time test (>400 s) (Fig. 5b). A higher light intensity resulted in a higher IR with a lower resistance state of the P-memory (Fig. 5c). Under red and green light illumination (λex = 532 and 638 nm), we also observed similar IR increases. As expected, light with a lower wavelength enabled the P-memory to have a greater IR increase with a lower resistance state, which potentially provides a classification operation according to the wavelength of light (Fig. 5d, Figs. S12 and S13).

Fig. 5: Multilevel data storage characteristics of MoS2 flash memory under various photoinduced programming conditions.

a Schematic diagram of measurement conditions depending on various light illumination under programming operation. b Multilevel retention characteristics of blue photoinduced programming with different light intensities at VD = 0.1 V. c Average resistance in the retention measurement until 400 s at VD = 0.1 V as a function of the incident power density (Pinc). d Average resistance in red, green, and blue retention measurements until 400 s at VD = 0.1 V as a function of the excitation wavelength (λex).

Mechanically flexible device manufacturing of the P-memory

As the MoS2 and PEDOT:PSS layers can be manufactured on top of flexible substrates owing to their excellent thermal budget (<200 °C), we next implemented flexible P-memory. A solution-based PI film was coated on a Si/SiO2 substrate, and flexible P-memory was fabricated with the same process as for the rigid memory (Scheme 1). For the BDL and the TDL, we deposited 100 nm- and 80 nm-thick Al2O3, respectively. By delaminating the P-memory with the PI film from the substrate, we obtained flexible P-memory (Fig. 6a, b). Further details of the flexible P-memory fabrication are given in the Experimental Section. The flexible P-memory exhibited a large memory window, ΔV = 60 V, obtained by programming/erasing the charges in the PEDOT:PSS floating layer, as we described in the P-memory operation part (Fig. 6c). The amount of VTH shift can be controlled by the applied VCG bias, in which a higher VCG bias results in a larger VTH shift toward the negative or positive side depending on Verase and Vprogram, respectively.

Fig. 6: Flexible MoS2 flash memory.

a Three-dimensional schematic device structure of flexible MoS2 flash memory on a PI substrate. b Photograph and OM image of fabricated flexible MoS2 flash memory. Scale bars are 1 cm and 10 μm, respectively. c Transfer characteristics of flexible MoS2 flash memory. The obtained memory window is ~60 V. d Extracted threshold voltage VTH under different Vprogram and Verase at VD = 1 V.

To evaluate the mechanical durability of the flexible P-memory, we measured its I-V transfer characteristics before and after 1000 bending cycles at a bending radius of curvature r = 5 mm (Fig. 7a, Supporting Video 1). Details of the bending test are given in the Experimental Section. The flexible P-memory exhibited the same I-V transfer characteristics without any degradation or current change compared to those before the 1000 bending cycles. The observed excellent mechanical durability resulted from the layered structure of MoS2 and the high flexibility of the PEDOT:PSS layer. To further investigate whether the flexible P-memory operated effectively after 1000 bending cycles, we performed a memory retention test (Fig. 7c). The current ratio of the programmed and erased states was above hundred for 8000 s of the retention measurement time.

Fig. 7: Bending test and photoinduced operation of flexible MoS2 flash memory.

a Photograph of MoS2 flash memory bent in the bending tester. The bending radius and scale bar are 5 mm and 2 cm, respectively. b Comparison of transfer characteristics of MoS2 flash memory before and after 1000 bending cycles with a 5 mm bending radius. c Schematic diagram of the retention measurement conditions and obtained retention characteristics of MoS2 flash memory under a control gate pulse of ±35 V at VD = 0.1 V for 8000 s after 1000 bending cycles with a 5 mm bending radius. d Multilevel retention characteristics of red, green, and blue photoinduced programming (638 nm, 532 nm, and 405 nm, respectively).

Photosensing memory operation of the flexible P-memory

We also tested the photosensing retention time of the flexible P-memory after 1000 bending cycles (Fig. 7d). As expected, lower wavelength light illumination under the programming operation (Vprogram = 35 V) allowed the device to exhibit a higher IR, so the flexible P-memory provided distinguishable resistance states depending on the light exposure properties. The abovementioned comprehensive memory tests confirmed that flexible P-memory exhibited no abnormality in the memory or photoactivated memory operations even after 1000 bending cycles.


In summary, we proposed P-memory that combines a layered MoS2 thin-film transistor structure with a PEDOT:PSS floating gate. Owing to the virtues of the MoS2 and PEDOT:PSS combined structure, the P-memory exhibited high performance, including a high switching current ratio >107, a large memory window >50 V, excellent endurance >1000 cycles, and a long retention time >2000 s. These were confirmed by multiple device fabrication and characterization to evaluate the reproducibility and uniformity (>30 devices). We also achieved a photoactivated memory operation that combines photodiode and memory functions. Depending on whether light was illuminated, the P-memory provided a different degree of programming, and thus, the degree of light exposure could be stored directly in the device. Furthermore, we demonstrated flexible P-memory by manufacturing the device on a flexible PI substrate. The results indicated that the device maintained its multifunctional memory behavior even after 1000 bending cycles. Through comprehensive experiments, this study showed not only the memory characteristics of conventional floating-gate-based flash memory but also new versatility such as mechanical flexibility and photoactivated memory behavior. These reported results are expected to be useful guidelines in the development of new electronic device features using new nanomaterials.


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This research was supported by the National Research Foundation of Korea (2018R1A2B2003558) and the Basic Science Research Program through the National Research Foundation of Korea (NRF), which is funded by the Ministry of Education (2020R1I1A1A01070907 and 2020R1I1A1A01073884). H.Y. acknowledges funding support from the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. NRF-2020M3A9E4104385 and 2020R1A2C1101647).

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Hong, S., Park, J., Lee, J.J. et al. Multifunctional molybdenum disulfide flash memory using a PEDOT:PSS floating gate. NPG Asia Mater 13, 38 (2021).

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