A universal all-dry microfabrication method for sensitive electronic materials via an inorganic molecular lithographic mediator

Domain: neuroscience
Published: 2026-01-28
Editorial outcome: minor_revision

Abstract
Lithography is pivotal in fabricating micro/nanoscale patterns and processing materials for electronic microdevices. However, conventional organic polymeric resists inevitably entail the use of various chemical solutions or solvents, which especially compromise fragile electronic materials featuring atomic-level surfaces. Here, we introduce inorganic selenium molecules as a lithographic mediator for sensitive electronic material processing without direct exposure to solutions or solvents. Specifically, the inorganic selenium molecular film functions as both a lithographic mediator for direct patterning due to its weak intermolecular van der Waals interactions and as a protective encapsulation layer for atomic electronic materials without compromising structural and electronic characteristics. Wafer-scale arrays of sensitive materials with high-quality, sharp edges are facilely achieved by a non-destructive mechanical peeling of the selenium layer. This approach provides a solvent-free lithographic route for microfabricating sensitive materials and high-performance electronic devices.

Introduction
Lithography underpins modern semiconductor manufacturing1,2, widely used in electronics systems3, integrated circuits4,5, and flexible electronic devices6,7, which allows micro/nanopatterning through a series of physical-chemical reactions between photons or electrons interacting with sensitive resist8–13. The commercial organic resist is a critical-formulated polymer composite of phenolic resin, photo-sensitizer, solvent14. The processes based on the conventional organic resists use kinds of solutions and solvents, including developer, remover, and cleaner. Such solutions or solvent residuals are inevitably adsorbed on the sample’s surface or substrate, potentially scattering the local concentration of charge carriers and disrupting charge transportation15–17, especially in modern two-dimensional electronic devices and atomic-scale monolayer materials with large specific surface areas. In addition, for high-sensitive electronic materials such as perovskite, black phosphorus (BP), and halides18–21, such solutions or solvents can even induce chemical reactions or doping, critically degrading the structural integrity of the functional materials22,23. For example, phosphorus atoms are prone to irreversible oxidation while black phosphorus contacts with solvents due to the easy transfer of the lone pair electrons24. Applying a chemically stable protective layer (such as graphene or boron nitride) over the surface of sensitive materials allows for minimized corrosion and contamination from solvents25,26. Unfortunately, the approaches introduce added complexity to the device construction and make it challenging to be compatible with the staple semiconductor industry integration processes. The conventional organic resist does not accommodate microfabrication of solvent-sensitive electronic materials with considerable potential.

Here, we explore the inorganic selenium molecules as a microlithographic mediator for sensitive electronic materials. Selenium molecules directly pattern with a localized photothermal sublimation sequentially under irradiation, due to weak van der Waals forces between the molecule units. In addition, adhesion discrepancy between the selenium layer and substrate is introduced to easily mechanically peel the selenium film at wafer scale for object patterns, ensuring a high-clean contact interface. Based on the inorganic molecular processing, a non-destructive micropatterning for highly sensitive materials, halides, and perovskites, was successfully realized. The process is compatible with large-area array device preparation of sensitive electronic materials, and the prepared field effect transistors exhibit a high electronic transport. In addition, the inorganic selenium molecular medium is simple in composition, controllable in thickness, and inexpensive compared to conventional organic photoresists. The inorganic molecular strategy realizes the solvent-free micropatterning of solvent-sensitive electronic materials, which is vital for the large-scale integration of novel two-dimensional electronic materials and high-performance microelectronic devices.

Results
Inorganic selenium molecular microlithographic mediator
Conventional micro/nanofabrication processes based on inorganic polymer mediators routinely employ chemical reagents such as photoresists, developing agents, and cleaning solutions, which inherently contain organic solvents, aqueous components, and even corrosive alkaline solutions. Upon interfacial contact between these chemical agents and sensitive materials, they readily induce interfacial damage, including dissolution of functional constituents, surface defects, and contaminant residue, especially to sensitive materials (Fig. 1a). Elementary selenium, known as an inorganic molecular material, is used as the lithographic mediator for the protective processing of sensitive materials in this work. A uniform wafer-scale film can be easily obtained by simple thermal vapor deposition from commercial selenium powder at a low temperature (150 °C) (Fig. 1b and Supplementary Fig. 1). The deposited selenium films exhibit close contact with the substrate, a dense and smooth surface, and a uniform and adjustable thickness (Fig. 1c and Supplementary Figs. 2–4). Essentially, the amorphous selenium film was constructed by isolated selenium species such as small molecular rings and chain fragments linked by weak van der Waals interaction (Supplementary Fig. 5)27–29. When exposed to irradiation, the weak intermolecular van der Waals interactions are easily broken up by the absorbed outside energy30. Thus, the irradiated partial region of the selenium film would be exposed by the localized thermal sublimation of small molecular fragments, forming a designed pattern (Fig. 1d). This robust stability significantly bolsters the case for the applicability in real manufacturing environments. A series of consecutive Raman spectra were collected to monitor selenium molecular structure during laser irradiation (Supplementary Fig. 6). Specifically, the irradiated point on the selenium surface immediately hole formation, as selenium molecular volatilization, exposed the substrate under the sensitive wavelength laser irradiation. Micropatterns with different shapes and feature sizes are directly obtained by laser writing in the selenium film, with no need of the development step in conventional lithography. Straight line patterns can be easily achieved for micro-scale features with 1 μm trenches and 2 μm lines (Fig. 1e and Supplementary Fig. 7). The statistics of trenches and lines show that the patterns are of high quality in width uniformity. With different thicknesses, selenium films are still patterned with clear boundaries (Supplementary Fig. 8). The resolution of the line micropatterns can be adjusted and optimized by laser beam parameters, such as output powers, Laser wavelength, and scanning speeds (Supplementary Figs. 9–11). For instance, the 532 nm laser produces a finer resolution of approximately 1.1 μm than the 633 nm. This is attributed to the higher photon energy and potentially tighter focal spot achievable with the shorter wavelength, leading to more confined photothermal energy and thus finer feature definition. As for the etched trench precision, three-dimensional AFM topographic images suggest that the patterns obtained are sharp edges in the unexposed area (Supplementary Fig. 11). The irradiated areas exhibits similarly minimal height variations (−0.3 nm ~ 0.4 nm) and nearly identical image roughness values (Ra: 0.42 nm ~ 0.45 nm), which indicate the presence of discrete nanoparticles and support a residue-free patterning process (Supplementary Fig. 12). Large area XPS detections consistently find no Se characteristic signs in the substrate, suggesting that the proposed method enables the complete removal of selenium molecules (Supplementary Fig. 13). Additionally, complementary distributions of Se and substrate (Si) signal strength in elemental mapping demonstrate that selenium molecules in the unexposed area are not affected during laser irradiation (Supplementary Fig. 14). Precisely spatial control of laser beam movement enables to obtain various delicate micropatterns, such as array patterns, line patterns, curvilinear patterns, character patterns, and numeric patterns (Supplementary Fig. 15). Complex patterns with various sharp angles and curves can also be obtained by direct writing (Fig. 1f). The direct lithography excludes contamination with chemical organic solvent or solution, showing more simple processing for structures and materials.

Inorganic molecular mediator towards sensitive materials
The inorganic selenium molecular microlithography is particularly suited to processing sensitive materials. The direct sublimation lithographic etching and drying removal processes avoid solvent-induced damage, preserving the structural and electronic characteristics of the functional materials. As proof of the feasibility, we chose different kinds of representative sensitive materials to compare the inorganic selenium lithography with standard organic polymer lithography (Fig. 2a, b). Typical solvent-sensitive samples, such as halide [PbBr2], perovskite [(MP)PbI4], and alkali metal compound [LiInP2S6], phosphorus sulfide [MgPS3], black phosphorus [BP] (Fig. 2c–g and Supplementary Fig. 16), are covered with selenium molecular layer and organic polymer photoresist layer, respectively. In the exposed windows, these sensitive materials can maintain the original morphology through selenium microlithography (Fig. 2h–l). Furthermore, these solvents can induce chemical reactions or doping, degrading the structural integrity of the functional materials, especially for halide [PbBr2] and perovskite [(MP)PbI4] (Fig. 2m–q). The organic polymer resist induces structural defects and damage to BP atomic surface, and residues in the substrate, which would cause charge carriers scattering (Fig. 2q and Supplementary Fig. 17). The disappearance or shift of Photoluminescence (PL) and Raman signals indicates that the crystal structures have been seriously damaged during the organic resist lithography process (Fig. 2r–t). Whereas, the detected optical signs remain completely consistent during the selenium lithography process, demonstrating that the non-destructive superiority of the inorganic selenium process is more pronounced in the non-destructive processing of solvent-sensitive materials (Fig. 2r–t and Supplementary Figs. 18 and 19).

Wafer-scale micropatterns by physical lift-off process
Thin-film deposition and patterning are the fundamental steps to integrate any novel material into a miniaturized device. The proposed inorganic molecular microlithography involves coating an inorganic molecular lithographic mediator layer on substrate, laser/plasma exposure to patterning, object material preparation, and removing a lithographic mediator (Fig. 3a). In conventional organic lithography, solvents such as acetone and ethanol are used to remove residual photoresist during the lift-off process, potentially damaging the functional objective samples especially for those sensitive to solvents. To avoid this issue, we develop an effective physical approach for drying removal of the selenium mediator layer by virtue of polydimethylsiloxane (PDMS) adhesion (Fig. 3b). Specially, PDMS, as an elastomer with low modulus and low surface energy, easily establishes a closely conformal contact with object sample lamination, via van der Waals interaction adhesion31,32. Qualitatively comparison by mechanically separating the layers in different stacking orders found that the adhesion at different contact interfaces between adjacent layers possesses radical discrepancy (Supplementary Fig. 20). Among them, the interfacial adhesion between the selenium film and the substrate (F2) is much weaker than that of the object layer and substrate (F1), which is the key to enabling the successful physical removal of the selenium mediator layer (Supplementary Fig. 21 and Supplementary Movie 1). Nano-scratching measurement was used to further quantitative test the adhesive force between the different contact interfaces (Supplementary Fig. 22). Consequently, the average adhesive force represented as critical load parameter is 1.35 mN for the selenium/substrate interface (F2), lower than that of the object/substrate (F1, 7.34 mN) (Fig. 3c and Supplementary Fig. 23). The weak interfacial adhesion allows to easily remove the redundant selenium mediator by physically peeling off from the substrate, without the assistance for any chemical solutions.

To verify the peeling function above, we fabricate the different object micropatterns by the inorganic selenium lithography (Fig. 3d). Before the object patterning, large-area redundant Se/object layer can be completely separated from substrate (Fig. 3e). For example, metal Au pattern and arrays can be easily fabricated by the drying lift-off process (Supplementary Fig. 24–26). The van der Waals interactions of PDMS with the object layer are the crucial characteristics during lift-off process (Supplementary Fig. 27). Except for the interfacial contact, the boundary contact between the selenium molecular layer and the metal layer is another critical factor in determining the final quantity of the patterns. Object patterns with straight boundary and curved boundary were investigated, respectively. After PDMS removal, the resulting edge of metal layer is completely complementary to the straight edge of the original selenium film (Supplementary Fig. 28a). The complementarity is highly matching even in extremely curved boundary (Supplementary Fig. 28b). The proposed microlithography approach based on interfacial adhesion discrepancy enables to preparation of high-quality metal electrode patterns.

Further, large-area sensitive material arrays are also prepared by this mechanical peeling method, as exemplified by electronic halide lead bromide (PbBr2) materials (Fig. 3f, Supplementary Fig. 29 and Supplementary Movie 2). Different density arrays can be presented simultaneously after one-step mechanical peeling. Wafer surface cleanliness after processing is a vital index sign in evaluating lift-off effect. AFM topographic image of SiO2/Si substrate after lift-off process shows that the surface undulation is consistent with the fresh silicon surface in the range from −1 nm to 1 nm (Fig. 3g). It indicates that the silicon surface is quite clean with no remnant selenium particles or metal particles after the physical peeling processes. In contrast, organic polymer mediator leave a large amount of residues on the substrate, which will directly affect the performance of electronic materials (Supplementary Fig. 30). In a word, the selenium microlithographic process can achieve a high cleanness with the auxiliary PDMS. It is worth noting that one physical peeling step can simultaneously achieve different array patterns of varying densities in one wafer. Figure 3h shows six pattern arrays obtained in the same wafer after lift-off by peeling. All of the small 30 patterns ran chosen from array I to array VI show uniform size and height (Supplementary Fig. 31). Statistical half violins of pattern roughness (average 0.85 nm), pattern-substrate vertical angle (average 92°, containing probe moving error in step), and substrate roughness (average 0.35 nm) demonstrate the flat pattern surface, sharp edge, and clear substrate (Fig. 3i). The wafer-scale fabrication of the high-quality halide lead iodide PbI2 patten arrays strongly confirms the solid accessibility and reliability of the selenium molecular microlithography for sensitive materials (Supplementary Fig. 32), Importantly, the simplified selenium microlithography does not involve any chemical solvent or solution contact to sensitive materials, comparison with the standard organic resist lithography (Supplementary Fig. 33 and Supplementary Movie 3). In addition, compared with other dry fabrication strategies, including shadow mask techniques and mechanical transfer methods, the organic selenium-mediated method uniquely combines: high resolution and freedom pattern design on a single substrate without custom masks, and less surface contamination without transfer polymers. This low-contamination and non-destructive method provides a reliable foundation for the preparation of high-performance electronic devices.

Microlithography for 2D material electronic device
To verify the applications of such the drying microlithography process in electronic device fabrication, we further fabricate two-dimensional material field-effect transistors (FET) by selenium molecular lithographic technology (Fig. 4a). The channel material used is the typical sensitive BP and monolayer MoS2. BP is highly sensitive to solvent, surface absorption, and contamination, which usually needs extra special protection measurements when served in electronic devices24,33,34. The exfoliated BP flake on the substrate is contacted with metal Au as drain and source electrodes, and the doped Si covered by SiO2 layer (300 nm) is used as the back gate and gate dielectric. During our fabrication process, the surface atoms of the BP layer are covered by the selenium molecular mediator, which avoids contact erosion toward BP from solution/solvent/air. Figure 4b illustrates the optical microscopy images of a single BP FET device before and after metal electrode construction. The transfer characteristics (Ids–Vgs) of the transistor show a typical P-type behavior (Fig. 4c). The achieved on/off ratio is competitive with, and in some cases superior to, that of reported for BP devices (Supplementary Fig. 34 and Supplementary Table 1). The linear output curves (Ids–Vds) in Fig. 4d suggest nearly ideal ohmic contact behavior. The inorganic selenium molecular mediator allows a high-cleanness surface for efficient carrier transport.

The inorganic selenium molecules integrated microlithography enables the large-area microelectronic fabrication of field-effect transistor arrays (Supplementary Fig. 35). Figure 4e shows the fabricated FETs based on monolayer molybdenum disulfide (MoS2) device with a channel length (Lch) of 25 μm and channel width (Wch) of 10 μm. MoS2 is considered to be a potential channel electronic material due to its adjustable bandgap and high mobility35–37. The Ids–Vds transfer curves with drain-source voltage at 0.5 V show typical n-type transistor characteristics. Histogram statistical analyses in Fig. 4f confirm the spatially uniform n-type transistor operation with reliable electrical performance in parameters on-current Ion and on-off ratio with Gaussian distribution. The average and best on-off ratios are about 107 and 109, respectively. For comparison, two MoS2 FET arrays with the same channel length and width (Lch/Wch = 12/5 μm) are fabricated by inorganic selenium molecular lithography and traditional organic resist lithography, respectively (Supplementary Fig. 36). The FET devices by the inorganic microlithography exhibits a higher on/off ratio (108–109) and much improved electronic uniformity than that of organic resist (Fig. 4g), suggesting the atomic structure of sensitive materials can be greatly maintained during the selenium microlithographic fabrication. The devices achieve an average on/off ratio that is significantly higher than those of other reported back-gated MoS2 FETs with SiO2 dielectric fabricated by the organic resist lithography, by over an order of magnitude against most references and about fivefold against the highest benchmark17,37–48 (Fig. 4h and Supplementary Table 2). Electronic transport property is susceptible to the atomic crystal structure of two-dimensional materials. The combined electrical results above confirm that the inorganic selenium molecular mediator greatly maintains the atomic structure stability of sensitive materials during the fabrication of electronic devices, which profoundly improves the intrinsic carrier conductivity in electronic devices. The great electronic transport property and high-consistent electrical signals demonstrate that the inorganic selenium microlithography is highly compatible with the current industry CMOS (complementary metal oxide semiconductor) manufacturing processes for scalable integration.

Methods
Inorganic selenium molecular microlithography process
(1) Selenium molecule deposition. Selenium molecules were deposited on the substrate via thermal evaporation under vacuum conditions (1–5 Pa). The sublimation process was initiated at 150–200 °C with a sample plate rotation speed of 50–100 rpm, enabling uniform film formation. (2) Laser/plasma exposure. The laser was directly exposed on the selenium film to form patterns. 532 nm and 633 nm laser beams were focused on the surface of the selenium film through an objective lens. The exposed local area of the selenium film can be precisely controlled by tuning the laser beam intensity, scanning speed, and scanning position. (3) Object material deposition. Functional halide layer (PbBr2, PbI2) and metal layers (Au, Sn, Cu) were deposited on patterned selenium films using magnetron sputtering or electron-beam evaporation. To enhance interfacial adhesion, a 5 nm Cr or Bi interlayer was introduced prior to Au deposition. (4) Selenium layer removal. Two solvent-free methods were employed. Mechanical peeling: A polydimethylsiloxane (PDMS) stamp was conformally attached to the selenium film (bubble-free interface verified by optical microscopy) and mechanically peeled in seconds, simultaneously removing excess selenium and overlying object layers. Thermal evaporation: Residual selenium was sublimated through vacuum annealing at 150 °C for 3 h, preserving substrate-bound patterns with atomic-leveled edge definition.

Standard resist photolithography
Standard photolithography used resist (AZ5214) and tetramethylammonium hydroxide (TMAH, 2.38%) developer (ZX-238). The resist was spin-coasted on the silicon substrate and heated at 95 °C for 90 s. After light focusing and irradiation, resist then dissolved in developer and exposed to the designed window patterns.

Materials synthesis
Halide PbBr2 crystal flakes were obtained by chemical vapor deposition (CVD) growth in a one-inch horizontal quartz tube furnace under ambient pressure49. Atomic vapor was gradually deposited on fresh-cleaved mica substrates.

Alkali metal compound LiInP2S6 single crystals were prepared by the chemical vapor transport (CVT) process50. First, raw LiInP2S6 powder and I2 transporting agent were sealed in a quartz tube. The tube was placed in a two-zone furnace and heated to 660 °C (source zone) and 560 °C (sink zone), held for one week, and then cooled to ambient temperature. The LiInP2S6 crystals were obtained on the sink side and mechanically exfoliated by tape to crystal nanoflakes. The exfoliated crystal flakes were transferred to the substrate for photolithography.

Organo-inorganic hybrid perovskite (MP)PbI4 single crystals were prepared by solution cooling crystallization. Under stirring, 1 mmol of lead oxide (0.223 g) was first dissolved in a mixture of 3.5 mL of hydroiodic acid and 1.5 mL of hypophosphate solution, and then 1 mmol (155 μL) of MeOPEA was added to the solution. After stirring at 65 °C for 30 min, the solution was slowly cooled to room temperature at a cooling rate of 1 °C h−1. Finally, orange perovskite (MP)PbI4 crystals were obtained and then mechanically exfoliated by tape. The exfoliated crystal flakes were transferred to a silicon substrate for photolithography.

Phosphorus sulfide MgPS3 was synthesized by chemical vapor transport. Use Mg pellets, red phosphorus, and sulfur powder as raw materials. A total of 2 g of the raw materials was weighed according to the stoichiometric ratio. The mixed powder was loaded into a quartz tube, which was then evacuated to a vacuum of 10−2 Pa and sealed. The sealed tube was placed in a dual-zone muffle furnace and subjected to the following program: heating to 650 °C (source zone) and 500 °C (deposition zone) over 20 h, maintaining for 100 h, cooling to 250 °C, and finally cooling naturally to room temperature. Colorless transparent sheet-like crystals were obtained from the quartz tube.

Black phosphorus crystals were purchased from Nanjing MK NANOTech. Co., Ltd. Black phosphorus flakes were obtained by mechanically exfoliating the black phosphorus crystals.

Materials characterizations
The morphology images of Se film and patterns were obtained by an optical microscope (Olympus BX51). The thickness and roughness were determined by an atomic force microscope (AFM, Bruker Dimension Icon). The X-ray diffraction (XRD) patterns were collected with a Bruker D8 Advance by Cu-Kα radiation at 30 kV and 10 mA with a scan step width of 0.02°. Scanning electron microscope (SEM, FEI Quanta 650) was used to identify the morphology and elements. Raman spectrum and mapping (WITec Alpha300 Raman) were performed on a confocal microscope spectrometer with × 100 microscope objective. All Raman spectra were calibrated as a reference of silicon characteristic peak 520 cm−1.

Film adhesion forces
The film adhesion force was investigated on the scratching module of a nanomechanical testing system (Agilent Nano Indenter, G200). Interfacial adhesions between three films and silicon substrate was measured. Standard output load gradually increased from 0 mN to 30 mN with a scratching distance of about 300 μm.

Electronic device fabrication and measurement
Mechanically exfoliated 2D materials were transferred on a cleaned SiO2/Si substrate. SiO2 and Si were used as the back-gate insulator and electrode, respectively. For electronic device fabrication, metal Au layers as drain and source electrodes were performed to pattern by the selenium microlithography process. When the material on the substrate has a strong binding force with the selenium layer, the selenium film is removed by heating evaporation at 200 °C before PDMS mechanical stripping. The electronic current-voltage measurements were performed using a semiconductor device analyzer (Agilent B1500A) in a probe station (Lake Shore CRX-6.5 K) at room temperature (~300 K).

Peer review rounds
[{"round": 1, "reviewer_comments": {"reviewer_1": "General comments: This manuscript reports an innovative microlithographic fabrication strategy utilizing inorganic selenium molecules as a mediator for patterning sensitive electronic materials. The new approach successfully circumvents solvent-/solution-induced damage to critical electronic components—a persistent limitation in traditional organic polymer-based processes. The presented results demonstrate high promises for advancing electronic device manufacturing methodologies. This well-executed study represents a significant contribution to the field and is recommended for publication in Nature Communications after clarification the following points:\nComment 1. The paper describes laser-based removal of selenium molecules from the material surface. Could the authors comment on the resulting surface condition of the treated material surface? In addition, this paper demonstrates the feasibility of 532 nm and 633 nm laser sources. Then, can ultraviolet laser source, which is often used in laser direct writing equipment, and even the electron radiation in electron beam lithography be used here?\nComment 2. The authors' one-step mechanical stripping technique enables wafer-scale patterning of solvent-sensitive materials without chemical reagents (Figure 3), offering distinct advantages. Given the broad applicability of metal arrays in electronics, could the authors discuss the feasibility and potential adaptations required to extend this physical method to metallic systems?\nComment 3. While the work effectively demonstrates patterning across several sensitive materials (Halide PbBr₂, Perovskite (MP)₂PbI₄, Alkali metal LiInP₂S₆), information regarding other synthesized materials, such as phosphorus sulfide [MgPS₃] and black phosphorus [BP], is absent. Suggest providing relevant discussion or justification.\nComment 4. The study presents mechanical stripping and physical vapor transport as methods for selenium removal. Given the well-known solubility of selenium in carbon disulfide (CS₂), could the use of CS₂ solution as an alternative solvent-based removal method be explored for patterning applications?\nComment 5. One of the important parameters of lithography technology is the resolution limit. The author has already presented the results at the micrometer scale here. So, have you attempted to go even further with nanoscale patterns?\nComment 6. The fabrication of a single black phosphorus (BP) field-effect transistor (FET) convincingly validates the method’s feasibility (Figure 5). Could the authors elaborate on the specific rationale for selecting molybdenum disulfide (MoS₂) rather than BP for the subsequent FET array demonstration?\nComment 7. As shown in step 3 of Supplementary Fig.33, during the process of removing the Se layer by argon plasma, it is inevitable that the MoS2 material in the source-drain region will be damaged or etched away. How can the performance uniformity and yield of the transistor device be guaranteed in this case?\nComment 8. There are some textual details in the article that need to be corrected, such as incorrect citation of pictures (from lines 115 to 159, Figure 3 was wrongly written as Figure 2); The image reference is missing on line 145.", "reviewer_2": "The manuscript introduces solvent-free microlithographic flow using an amorphous selenium (Se) mediator and PDMS-assisted lift-off. The idea is highly relevant for solvent-sensitive materials and is supported by substantial characterization. However, several key aspects—residue verification at scale, metrology choices, dose/feature-size dependence, perovskite device-level validation, and substrate-dependent variations—require further evidence or clarification before acceptance.\nMajor comment\n1.The main theme of this research is a lithography method for chemically sensitive materials. While the authors have quantitatively demonstrated good performance for MoS₂, the data for black phosphorus (BP) appears to be limited to a qualitative comparison. It seems that to truly validate the method's utility, obtaining quantitative performance data for a genuinely chemically unstable material would be more compelling. We would be interested to hear the authors' perspective on this matter.\n2.The authors claim a clean surface after the Se lift-off process, supported by AFM and Raman analysis. However, two points require clarification. First, according to Supplementary Data 33, a final vacuum annealing step is performed after the lift-off. The rationale for this step is unclear if the lift-off process itself is sufficient to produce a clean surface. Second, the use of Raman spectroscopy to confirm the absence of residual Se is questionable. It is known that the laser excitation used in Raman can induce the sublimation of Se. Therefore, this measurement may not be a reliable indicator of residual Se on the as-processed surface requires further verification.\n3.The manuscript would be strengthened by an analysis of residual Se particles over a larger area. This is essential to evaluate the uniformity and scalability of the proposed method. As a suggestion, the authors could perform a surface-sensitive analysis, such as XPS, on a test substrate where the entire Se film has been sublimated by the laser. This would provide more robust and quantitative evidence regarding the presence or absence of any non-volatile residues across a wider region.\n4.I would expect a significant amount of residual Se to remain in the finer patterns, as they likely receive an insufficient laser dose for complete sublimation. Could the authors provide direct evidence, such as high-magnification SEM images, to prove that this is not the case?\n5.A potential issue may arise from the differing adhesion coefficients of Se on the substrate versus on the target material (e.g., a perovskite flake). This could lead to non-uniformity in the deposited Se thickness, which in turn could negatively impact the resolution and fidelity of the laser patterning process. This could become a potential issue when fabricating fine and complex patterns on such heterogeneous surfaces. What is the authors' perspective on this matter? Furthermore, could they provide direct experimental evidence, such as AFM line scans across flake edges, to quantify the Se thickness uniformity?\nMinor comments\n6.Color/legend in Supplementary Fig. 6 (panels c,d)\nThe normalized Se-(250 cm⁻¹) and Si-(520 cm⁻¹) trends for 633 nm vs. 532 nm (panels c,d) use similar colors/markers and may confuse readers. Please revise palette/legend for immediate discrimination.\n7.Typo on p.9 (main text), line ~21\nThe phrase “one-step mechanical peeling ( )” contains empty parentheses—please correct.", "reviewer_3": "This manuscript presents an all-dry microfabrication strategy using inorganic selenium molecules as a lithographic mediator for processing solvent-sensitive electronic materials. The selenium film is patterned with a localized photothermal sublimation sequentially under light irradiation. Large-scale patterns and devices have been fabricated with this method. The strategy developed in this manuscript is potentially interesting, but several critical issues need clarification and revision to support the claims:\n1. Several all-dry microfabrication strategies for solvent-sensitive materials (e.g., perovskites) have already been developed, including shadow mask techniques (Nature Protocols, 20, 1915–1929, 2025; Advanced Materials Technologies, 4, 1900519, 2019) and mechanical transfer methods (Nat. Nanotechnol. 17, 1206–1213, 2022). The manuscript does not clearly articulate how the selenium-mediated approach outperforms these alternatives—for example, in resolution, scalability, material compatibility, or device performance. A direct comparative analysis is necessary to highlight its unique value.\n2. The reported device performance such as on/off ratios for MoS₂ FETs (average ~10⁷, best ~10⁹; Fig. 4f) is less compelling when compared to recent works using device fabrication processes based on organic polymeric resists, which demonstrates average on/off ratios of ~10⁸ for devices on SiO₂ or high-κ oxide substrates (Nature Electronics 8, 571–577, 2025; Nature Electronics 6, 146–153, 2023; Nature Electronics 8, 135–146, 2025). This challenges the value of adopting the method described in the manuscript.\n3. The manuscript attributes selenium’s photothermal sublimation to weak intermolecular van der Waals forces but lacks critical details on how laser parameters (wavelength, power density, scanning speed) influence patterning precision. Specifically: How do different laser wavelengths affect trench resolution? Does varying laser power lead to residual selenium on the substrate, and if so, how is this quantified? Without such data, the reproducibility and controllability of the patterning process remain uncertain.\n4. Information on the stability of selenium films during storage or device fabrication is absent. For instance: Does prolonged exposure to air (e.g., oxygen, humidity) induce oxidation or degradation of the selenium layer? How does such exposure affect the film’s adhesion to the substrate or its ability to be patterned via laser sublimation?\nThese factors are critical for assessing the practical utility of the method in large-scale manufacturing.\n5. The claim that “patterns obtained are sharp edges in the unexposed area and no small particle residues in the irradiated region” is insufficiently supported. The AFM height scale in the provided images is too large (~300 nm) to resolve nanoscale residues (a few nanometers or smaller), which could still impact device performance and uniformity.\n6. Numerous typos and inconsistencies in figure numbering undermine readability. For example, references to “Fig. 2c, 2d, 2e, 2f” appear to correspond to “Fig. 3c, 3d, 3e, 3f” in the manuscript. A thorough proofread is required to correct these issues and ensure clarity."}, "author_response": "Response to the reviewers’comments\nReviewer #1:\nGeneral comments: This manuscript reports an innovative microlithographic fabrication strategy\nutilizing inorganic selenium molecules as a mediator for patterning sensitive electronic materials.\nThe new approach successfully circumvents solvent-/solution-induced damage to critical electronic\ncomponents—a persistent limitation in traditional organic polymer-based processes. The presented\nresults demonstrate high promises for advancing electronic device manufacturing methodologies.\nThis well-executed study represents a significant contribution to the field and is recommended for\npublicationinNatureCommunications after clarificationthefollowing points:\nResponse: We appreciate your positive comments and insightful suggestions. We have addressed all\ntheissues point-by-point in our response below.Weadded some experimental dataaccording to these\nsuggestions. We hope that our revised manuscript has addressed your concerns. The detailed\nresponses toall comments of theReviewer are provided below:\nComment 1. The paper describes laser-based removal of selenium molecules from the material\nsurface. Could the authors comment on the resulting surface condition of the treated material\nsurface? In addition, this paper demonstrates the feasibility of 532 nm and 633 nm laser sources.\nThen, can ultraviolet laser source, which is isoften used inlaser direct writing equipment, andeventhe\nelectron radiationin electronbeam lithographybeused here?\nResponse: We employed direct laser irradiation to remove the selenium molecules from the material\nsurface. To systematically evaluate the surface condition after processing, we examined the surface\nmorphology of five different types of sensitive electronic materials (Fig. 2). Optical microscopy\nimages revealed that the laser-treated materials remained structurally intact and exhibited a clean\nsurface. For more detailed surface characterization, we performed additional atomic force\nmicroscopy (AFM) experiments to compare the surface topography of mechanically exfoliated MoS₂\nflakes before selenium coating and after laser removal (Figure R1). The AFM results clearly\ndemonstrate that both the flake surface and the surrounding substrate remain highly clean, with no\nsignificant change in roughness in the scanned regions. These findings collectively indicate that the\nlaser treatment and selenium removal process effectively preserve the original surface state of the\nsensitiveelectronic materials.\nremovingseleniummolecules.a,Schematicdiagramsoftheexfoliatedflakeonthesubstrateandthentreatedby\nlaserremovalofseleniummolecules.b,AFMimagesofthefreshexfoliatedflakeandthetreatedflake,Raisthe\nimageroughnessofthescanningarea.\nWe share your interest in whether other types of lithographic sources can be applied to etch\nselenium molecules. In addition to 532 nm and 633 nm lasers, we have also experimented with a 405\nnm ultraviolet laser for etching the selenium layer. The results indicate that selenium molecules\nwithin a certain thickness range can be effectively removed, and increasing the laser power further\nenhances the etching depth. Moreover, we evaluated the feasibility of electron beam lithography, but\nfound no significant removal of selenium molecules by the electron beam—only minor irradiation\ndamage to surface atoms was observed (Figure R2). This may be attributed to the relatively low\nthermal effect of the electron beam, which appears insufficient to support substantial volatilization of\ntheselenium molecules.\nFigureR2.SEMimagesoftheseleniumlayerexposedbyelectronradiation.a,b,Seleniumsurfacebeforeand\nafterelectronradiationinelectronbeamlithography(EBL).\nsolvent-sensitive materials without chemical reagents (Figure 3), offering distinct advantages. Given\nthe broad applicability of metal arrays in electronics, could the authors discuss the feasibility and\npotentialadaptationsrequired toextend this physical method tometallicsystems?\nResponse: We thank you for recognizing the advantages of our one-step mechanical stripping\ntechnique for solvent-sensitive materials and for raising this valuable question regarding its\napplicability tometallic systems.\nWe are pleased to confirm that the proposed dry patterning approach is indeed fully applicable to\nthefabrication ofmetal arrays.As illustrated in Figure R3, the process for metal patterning involves:\n(1) laser etching of the pre-deposited selenium layer to define the desired patterns, (2) deposition of\nthe metal (e.g., Au) by physical vapor deposition, and (3) one-step mechanical stripping to remove\nthe excess selenium together with the overlying metal film, leaving behind well-defined electrode\npatterns. By simply adjusting the laser-written patterns in the selenium layer, this method allows\nflexiblefabrication of electrode structures with varying geometries andnumbers.\nFurthermore, this process is readily scalable, enabling the production of large-area, uniform metal\narrays without the use of solvents or wet chemicals. The method preserves the advantages of being a\ndry, reagent-free process, thus maintaining compatibility with solvent-sensitive materials while\nextendingits utilityto versatile metal patterning forabroad range ofelectronic applications.\nFigureR3.MetalAuelectrodefabricatedbytheinorganicSemicrolithography.Opticalimagesoffabricating\ntwometalelectrodes(a)andfourmetalelectrodes(b).TheprocessincludesthelaseretchingonSefilm,Auatom\ndeposition,andmechanicalpeelingremovalforthemetalelectrode.\n(Halide PbBr , Perovskite (MP) PbI , Alkali metal LiInP S ), information regarding other\nsynthesized materials, such as phosphorus sulfide [MgPS ] and black phosphorus [BP], is absent.\n₂ ₂ ₄ ₂₆\nSuggest providing relevant discussion orjustification.\n₃\nResponse: Thanks to your suggestion, we have added information about sensitive materials as\nfollows.\nPhosphorus sulfide MgPS was synthesized by chemical vapor transport. Use Mg pellets, red\n3\nphosphorus, and sulfur powder as raw materials. A total of 2 g of the raw materials was weighed\naccording to the stoichiometric ratio. The mixed powder was loaded into a quartz tube, which was\nthen evacuated to a vacuum of 10-2 Pa and sealed. The sealed tube was placed in a dual-zone muffle\nfurnace and subjected to the following program: heating to 650 °C (source zone) and 500 °C\n(deposition zone) over 20 hours, maintaining for 100 hours, cooling to 250 °C, and finally cooling\nnaturally to room temperature. Colorless transparent sheet-like crystals were obtained from the\nquartz tube.\nBlack phosphorus crystals were purchased from Nanjing MKNANO Tech. Co., Ltd. Black\nphosphorus flakes were obtained bymechanically exfoliating theblack phosphorus crystals.\nWe subjected the obtained crystalline material to XRD tests, as shown in Figure R4. The\nmeasured XRD peaks are well matched with the simulated patterns and have a small full width at\nhalf-maximum (FWHM). This proves that the obtained sample is highly crystalline single-crystal\nmaterials.Theabove information has been added to theMethods andSupplementary Fig. 17.\nFigureR4.XRDofthesensitivecrystalmaterials.a,PhosphorussulfideMgPS₃.b,Blackphosphorus[BP].The\nbluelinesareexperimentaldata,andthegraylinesaresimulateddiffractionpatternsfromcrystalstructures.The\ncorrespondingcrystalstructuresareindicatedbesidetheXRDpatterns.\nselenium removal. Given the well-known solubility of selenium in carbon disulfide (CS ), could the\nuse of CS solution as an alternative solvent-based removal method be explored for patterning\n₂\napplications?\n₂\nResponse: We thank you for the insightful suggestion regarding the use of carbon disulfide (CS ) as\n2\na solvent-based approach for selenium removal. To evaluate this possibility, we explored CS as an\n2\nalternative method for selectively dissolving excess selenium in patterning applications. In the\nsolvent-based removal process (Figure R5a), the selenium layer gradually dissolves in CS , leading\n2\nto the automatic detachment of the overlying target film from the substrate. After complete removal\noftheselenium layer,thepre-designed patterns remain intact onthesubstrate.\nAs shown in Figure R5b, the initially transparent CS solution turns yellow following selenium\n2\ndissolution, with fragmented metal film suspended in the solvent. With the dissolution of the\nselenium interlayer, the upper metal film cleanly separates from the substrate, leaving well-defined\nelectrode patterns behind. By this method, we successfully fabricated metal patterns, such as Au\nelectrodeand Cu circuit pattern (Figures R5c,R5d).\nThese results collectively demonstrate that the CS -based dissolution method can successfully be\n2\napplied for patterned fabrication. We believe that CS -based removal offers a universal and\n2\nalternativemethod to pattern delicate electronic materials.\nFigureR5.CS₂solventremovalmethod.a,SchematicofCS₂solventremovalprocess,includingobjectmetal\ndeposition,seleniummoleculardissolution,andmetalpattern.b,PhotoimageofCS solutionbeforeandafter\n2\nremovingSe.c,OpticalimageoftheAuelectrode.d,OpticalimageofmetalCucircuitpattern.\nComment 5. One of the important parameters of lithography technology is the resolution limit. The\nauthor has already presented the results at the micrometer scale here. So, have you attempted to go\nevenfurther withnanoscalepatterns?\nattempts to push the patterning resolution toward the nanoscale. The achievable resolution is indeed\ninfluenced by several key factors, including laser wavelength, spot size, power density, and the\nmaterial properties of the selenium layer. In our current changing the power density using 532 nm\nand 633 nm lasers (Figure R6), we have achieved a minimum feature size of ~1 μm, which\napproaches thepractical diffraction-limited resolutionfor these wavelengths.\nFigureR6.LaserwavelengtheffectontrenchresolutionofSefilmpatterns.OpticalimagesofSepattern\netchedby532nm(a)and633nm(b)lasersunderlaserpower0.1mW,1.0mW,2.0mW,4.0mW,6.0mW,8.0\nmW,and10.0mW.c,Statisticalchartoftheetchedtrenchwidthsusing533nmand633nmlasersatdifferentpower\nlevels.\nWe have conducted preliminary experiments with shorter wavelengths (325 nm and 405 nm) to\nexplore nanoscale patterning. However, due to insufficient power output from our available UV laser\nsources, we were unable to consistently achieve complete selenium sublimation and form\nwell-defined nanoscale patterns under routine conditions. This limitation is primarily constrained by\nourcurrent laboratory hardware.\nWe firmly believe that achieving nanoscale patterning is fundamentally feasible with optimized\nparameters, including shorter-wavelength lasers with adequate power density, reduced spot size, and\nprecise process control. Pushing the resolution toward the nanoscale represents a key and active\ndirection ofour ongoing and future research efforts.\nconvincingly validates the method’s feasibility (Figure 5). Could the authors elaborate on the\nspecific rationale for selecting molybdenum disulfide (MoS ) rather than BP for the subsequent FET\narraydemonstration? 2\nResponse: As highlighted by the reviewer, the fabrication of a single black phosphorus (BP)\nfield-effect transistor successfully validated the feasibility and effectiveness of our inorganic\nselenium-based lithography process for sensitive electronic materials. We had initially planned to\nutilize BP for the fabrication of integrated FET arrays as a logical extension of this work. A\nlarge-area crystalline film with sufficient quality and uniformity is required for array fabrication.\nHowever, the synthesis of large-area, few-layer BP remains a significant challenge in the field, as\nconfirmed by recent literature (Nat. Mater. 2025, 24, 1375; Nat. Mater. 2023, 22, 717). This material\nconstraint led us to select monolayer atomic molybdenum disulfide (MoS ) for the array\n2\ndemonstration. Monolayer MoS was chosen as it represents a widely available, structurally uniform\n2\ntwo-dimensional semiconductor withmature synthesis methods.\nWebelieve that the successful demonstration of a functional MoS FET array, in combination with\n2\nthe initial BP device, strongly supports the versatility and broad applicability of our lithographic\napproach in atomically sensitivematerial processing.\nComment 7.As shownin step 3of Supplementary Fig.33, duringthe process of removing theSe layer\nby argon plasma, it is inevitable that the MoS material in the c will be damaged or etched away.\nResponse: We agree that ensuring the integrity of the underlying material during the Se removal\nprocess isparamount for device performance and yield.\nIn our preliminary experiments, we systematically evaluated the plasma etching behavior of both\nmaterials. We found that MoS exhibits its high sensitivity to O or SF -based plasmas, significantly\n2 2 6\nlower susceptibility to Ar plasma compared to amorphous selenium. This selectivity is achievable\ndue to the significant difference in physical properties between the volatile Se and the MoS .\noptimizing key parameters—including low plasma power, operating pressure, and particularly\nexposure time—we can precisely control the etching depth to desorb and volatilize the Se molecules\nbut not to etch or introduce detectable damage into the MoS . We conducted the following\n2\ncharacterizationand analysis:\n2\nthewhitedashedboxisetchedbyargonplasmaforthesourceanddrain.Thelong-shapedMoS nanosheet\n2\nmaintaineditssurfacemorphologyintactbothbeforeandafteretching.b,Peaklocationsandintensitiesofthe\ntypicalMoS Ramanlocatedat385cm−1(E 1)and403cm−1(A )shownomeasurablechangebeforeandafter\n2 2g 1g\netchingtheSelayer.\nMaterial Characterization: Optical images and Raman spectroscopy performed on the MoS in the\n2\nsource/drain region before and after plasma treatment show no measurable change in surface\ntopography or degradation in crystal quality (Figure R7), confirming that the structural integrity of\nMoS ispreserved.\n2 2\neffecttransistorsdrivenbydrain-sourcevoltageat0.5V.b,Correspondinghistogramstatisticalanalysesfor\non-currentI ,on–offratio,subthresholdswing,andmobilitywithnormaldistributioncurves.\nmax\nElectrical Performance Uniformity: The electrical characteristics of the fabricated FET arrays\nserve as the most direct evidence. As presented in Figure R8, the devices exhibit spatial uniformity\n8\nin key electrical performance metrics such as on-current I , on–off ratio, subthreshold swing, and\nmax\nmobility. The high yield of functional devices across the arrays indicates that the MoS channel\n2\nremains intact and undamaged during theplasmaprocess.\nTherefore, we conclude that with our carefully optimized plasma parameters, the removal of the\nSe layer is achieved selectively, guaranteeing the performance uniformity and yield of the transistor\ndevices.\nComment 8. There are some textual details in the article that need to be corrected, such as incorrect\ncitation of pictures (from lines 115 to 159, Figure 3 was wrongly written as Figure 2); The image\nreferenceis missingonline145.\nResponse:Thanks forthis kind reminder.Thetextual errors mentioned abovehave been revised.The\nempty bracket on line 145 is unnecessary and has been removed in the revised manuscript. We\ncarefully checked all text in the whole manuscript again, and the changes made in the revised\nmanuscript are indicated in red.\nThe manuscript introduces solvent-free microlithographic flow using an amorphous selenium (Se)\nmediator and PDMS-assisted lift-off. The idea is highly relevant for solvent-sensitive materials and\nis supported by substantial characterization. However, several key aspects—residue verification at\nscale, metrology choices, dose/feature-size dependence, perovskite device-level validation, and\nsubstrate-dependent variations—requirefurther evidence or clarification beforeacceptance.\nMajor comment\n1.The main theme of this research is a lithography method for chemically sensitive materials. While\nthe authors have quantitatively demonstrated good performance for MoS , the data for black phosphorus (BP) appears to be limited to a qualitative comparison. It seems that to trulyvalidate the\n₂\nmethod's utility, obtaining for a genuinely chemically unstable material would be more compelling.\nWewould beinterested tohear theauthors'perspective onthis matter.\nResponse: We thank you for this insightful comment regarding the validation of our method using\nchemically unstable materials. We agree that demonstrating the utility of our lithography approach\nfor highly sensitive materials is crucial. In our past study, we deliberately compared our\nselenium-based lithography with conventional polymer-based processing for black phosphorus (BP)\ndevices. Mechanically exfoliated few-layer BP flakes are extremely susceptible to degradation upon\nair exposure and contact with organic photoresists, developers, and cleaning agents (Figure R9),\noften resulting in the fabrication failure of functional electronic devices altogether. As a common\nalternative, thicker multilayer BP flakes are sometimes used in conventional processes to mitigate\nthisdegradation; however,this comes at thecost ofcompromised electrical performance.\nFigureR9.Degradationprocessoffew-layerBPflakeexposedinairandflakeincontactwithorganic\nphotoresists.(Ourteampreviousresearch,Adv.Mater.2022,34,2106041)\nthe conventional method using multilayer BP show high current but suffer from poor gate\nmodulation, resulting in a low on/off ratio (Figure R10a). In contrast, devices fabricated using our\nselenium-mediated lithography successfully preserved few-layer BP flakes. These devices\ndemonstrate clear gate modulation and a significantly improved on/off ratio (Figure R10b,c).\nFurthermore, the achieved on/off ratio is competitive with, and in some cases superior to, values\nreported in literature for BP devices (Figure R10d), as detailed in the performance comparison\nprovided as SupplementaryTable1and Fig. 36intherevised Supplementary Information.\nFigureR10.ComparisonoftheelectricalperformanceofBPdevice.OutputcharacteristiccurvesofBPfield\neffecttransistorfabricatedbyorganicpolymerlithography(a)andinorganicseleniumlithography(b).c,Transfer\ncharacteristiccurvesofBPfieldeffecttransistorunderdrain-sourcevoltagesat0.5V,1.0V,and2.0V.d,\nComparisonoftheaverageon/offratioofBPtransistorfabricatedinthisworkandliterature-reportedBPFETs.\nThis direct comparison strongly validates the protective capability and practical advantage of the\nselenium-based lithography for processing genuinely sensitivematerials.\n2.The authors claim a clean surface after the Se lift-off process, supported by AFM and Raman\nanalysis. However, two points require clarification. First, according to Supplementary Data 33, a\nfinal vacuum annealing step is performed after the lift-off. The rationale for this step is unclear if the\n11\nlift-off process itself is sufficient to produce a clean surface. Second, the use of Raman spectroscopy\nto confirm the absence of residual Se is questionable. It is known that the laser excitation used in\nRamancan induce the sublimation of Se. Therefore, this measurementmay not bea reliableindicator\nofresidual Seon theas-processed surfacerequires further verification.\nResponse: We thank you for these insightful questions regarding the surface cleaning validation and\nthespecific process flow,which help us clarify important methodological details.\nClarificationon thevacuumannealing andlift-offstep\nWe further clarify the rationale for the fabrication process of large-area transistor arrays (Previous\nSupplementary Fig. 33). To clearly explain the process flow, we added the schematic Figure R11.\nThe initial lift-off step (Step 5) is performed to remove the patterned organic mask layer along with\nthe excess deposited metal. It is crucial to emphasize that the selenium layer itself remains entirely\nintact on the substrate after this step. The subsequent vacuum annealing step (Step 6) is then\nexplicitly employed to remove this remaining selenium layer by leveraging its relatively low\nsublimation temperature (as detailed in the Methods). This final thermal desorption cleanly exposes\ntheunderlying active material channels and contact regions, completing thedevice fabrication.\nFigureR11.SchematicdiagramoftransistorarraysfabricationbySe-assistedmicrolithography.\nRe-evaluationofRaman spectroscopy forSeresiduedetection\nThe 633 nm laser we used is indeed suitable for characterizing bulk Se films or powder.As for the\nselenium residues on the substrate surface, especially selenium nanoparticles, the Raman laser may\ncause the selenium molecules already sublimated while detecting them. Upon careful consideration\nof the comment that the Raman laser excitation itself may induce sublimation of trace Se, we agree\nthat this makes Raman spectroscopy an unreliable method for verifying the Se residue on the\nas-processed surface. In light of this consideration, we have removed the Raman data about Se\nresidue previously presented in Supplementary Fig. 29 from the manuscript. More surface-specific\ntechniques (AFM or XPS)would be provided for better detection ofresidual Se.\n12\n3.The manuscript would be strengthened by an analysis of residual Se particles over a larger area.\nThis is essential to evaluate the uniformity and scalability of the proposed method. As a suggestion,\nthe authors could perform a surface-sensitive analysis, such as XPS, on a test substrate where the\nentire Se film has been sublimated by the laser. This would provide more robust and quantitative\nevidence regardingthepresence or absence of anynon-volatileresidues acrossawider region.\nResponse: Thanks to you for this valuable suggestion to further strengthen the evidence regarding\nsurface cleanliness and the scalability of our method. According to your suggestion, we have\nperformed wide-area surface-sensitiveanalysis usingX-ray photoelectron spectroscopy (XPS).\nAs shown in the newly added Figure R12, XPS spectra were collected in 1 cm×1 cm substrate\nfrom six randomly selected locations (Area 1–Area 6) across a SiO /Si substrate where the selenium\n2\nfilm had been removed by the laser sublimation process. The results consistently show no detectable\nSe characteristic peaks across all measured points, with only the intrinsic signals from the substrate\nbeing observed. the Se atomic ratio at the six substrate positions is extremely small, only ranging\nfrom (0.13%–0.22%), compared with that of the Se film on SiO /Si substrate (35.98%). This\n2\nquantitative data provides robust evidence that our process enables the clean and complete removal\nof selenium over large areas, thereby strongly supporting the uniformity and scalability of the\nproposed method. we have added XPS data as Supplementary Fig. 14 in the revised Supplementary\nInformation.\nFigureR12.XPSspectraofthesubstratesurfaceafterremovingSe.a,XPSspectraofsixrandomlyselected\nlocations(Area1–Area6)acrossaSiO /SisubstrateafterremovingSe,andSefilmXPSspectrum.b,Seatomic\n2\nratioofthesixsubstratelocationsandSefilm.TheatomicdataareobtainedfromXPSmeasurement,includingthe\nC1s,O1s,andSe3d.\n13\n4.I would expect a significant amount of residual Se to remain in the finer patterns, as they likely\nreceive an insufficient laser dose for complete sublimation. Could the authors provide direct\nevidence, suchas high-magnificationSEMimages, to prove thatthis is notthe case?\nResponse:This is an important point regarding potential residual Se in finer features. Toaddress this\nconcern directly,we haveperformed high-resolution characterization ofthepatterned channels.\nFigureR13.SEMandAFMimagesofthefineSepatterns.\nAs shown in Figure R13, high-magnification SEM images reveal clean and well-defined edges\nwithin the fine-pitched patterns, with no observable particulate residues in the channel regions.\nAdditionally, we employed dark-field optical microscopy, a technique highly sensitive to the\ndetection of micro- and nanoparticles that may not be readily visible in standard bright-field mode\n(Figure R14a). The dark-field image of the fine patterns (Figure R14b) shows no scattered bright\nspots, which would be characteristic of residual Se particles. This observation provides further\ncorroborating evidence for the absence of Se residue. The absence of morphological anomalies or\nresidual particles provides direct evidence that the laser process, under our optimized parameters,\nachieves completeSesublimation even withinfiner patterns.\nFigureR14.Light-fieldanddark-fieldopticalimages.a,thesubstratewithmicro-nanoparticles.Thebright\nspots(arrowindicator)inthedark-fieldimagesaremicro-nanoparticles.b,thepatternswithacleansurface.\n14\n5.Apotential issue may arise from the differing adhesion coefficients of Se on the substrate versus on\nthe target material (e.g., a perovskite flake). This could lead to non-uniformity in the deposited Se\nthickness, which in turn could negatively impact the resolution and fidelity of the laser patterning\nprocess. This could become a potential issue when fabricating fine and complex patterns on such\nheterogeneous surfaces. What is the authors' perspective on this matter? Furthermore, could they\nprovide direct experimental evidence, such as AFM line scans across flake edges, to quantify the Se\nthickness uniformity?\nResponse: In our process, the selenium is deposited via physical vapor deposition, which is a highly\ndirectional and conformal deposition technique. While a certain degree of thickness variation at the\nimmediate edge of the flakes is inevitable, our optimized deposition parameters ensure a consistent\nand sufficiently uniform Se film across both the substrate and the top surface of the target materials\nwithin the central regions of the features. The height difference at the edge depends on the relative\nvalues between the selenium film thickness and the target material thickness. Furthermore, the laser\npatterning process operates in an ablation regime with a clear threshold. As long as the local Se\nthickness exceeds this ablation threshold across the patterned area, the removal is complete.\nTherefore, ourmethod possesses an inherent tolerance to minorthickness variations.\nAs shown in the new Figure R15, we observe the Se thickness uniformity on the heterogeneous\nsurfaces of the target MoS material. In AFM line scans across the edge, the height profiles\n2\ndemonstrate that the Se film conforms well to the underlying topography. The measured thickness\nvariation on the target material and the adjacent Se layer is nearly identical, with a variation of less\nthan 1% of the nominal thickness, which falls well within the process window for uniform laser\npatterning.\nFigureR15.TheSefilmandtargetmaterialedge.(a),OpticalimageoftheSe/MoS heterogeneoussurfaces.b,\nWe agree that this is an important consideration, and it is also a key future direction for us to\nenhancethe resolution and fidelityof ourmethod in dealing with heterogeneous surfaces.\n6.Color/legend in Supplementary Fig. 6(panels c,d)\nThe normalized Se-(250 cm ¹) and Si-(520 cm ¹) trends for 633 nm vs. 532 nm (panels c,d)\nuse similar colors/markers and may confuse readers. Please revise palette/legend for immediate\n⁻ ⁻\ndiscrimination.\nResponse: Thanks for this kind reminder. We're sorry for the confusion over the colours! We added\nthe clear legend in Supplementary Fig. 6 for immediate discrimination. The figure is updated as\nSupplementary Fig. 7inthe revised Supplementary Information.\nSupplementaryFig.7Laserwavelengthdependenceofirradiationoninorganicseleniummolecularfilm.\n7.Typoonp.9(main text),line~21\nThephrase “one-step mechanical peeling ()”contains emptyparentheses—please correct.\nResponse: The empty parentheses on line 21 are unnecessary and have been removed in the revised\nmanuscript. We carefully checked all text in the whole manuscript again, and the changes made in\ntherevised manuscript are indicated inred.Thanks again for thiskind reminder.\nThis manuscript presents an all-dry microfabrication strategy using inorganic selenium molecules as\na lithographic mediator for processing solvent-sensitive electronic materials. The selenium film is\npatterned with a localized photothermal sublimation sequentially under light irradiation.\nLarge-scale patterns and devices have been fabricated with this method. The strategy developed in\nthis manuscript is potentially interesting, but several critical issues need clarification and revision to\nsupporttheclaims:\n1. Several all-dry microfabrication strategies for solvent-sensitive materials (e.g., perovskites) have\nalready been developed, including shadow mask techniques (Nature Protocols, 20, 1915–1929,\n2025; Advanced Materials Technologies, 4, 1900519, 2019) and mechanical transfer methods (Nat.\nNanotechnol. 17, 1206 –1213, 2022). The manuscript does not clearly articulate how the\nselenium-mediated approach outperforms these alternatives—for example, in resolution, scalability,\nmaterial compatibility, or device performance. A direct comparative analysis is necessary to\nhighlightitsuniquevalue.\nResponse: We thank you for this critical comment, which allows us to better articulate the unique\nvalue and positioning of our selenium-mediated lithography within the ecosystem of all-dry\nfabrication methods. We fully agree that shadow masking and mechanical transfer are established\nand valuable techniques for solvent-sensitive materials. The key advantage of our approach lies in its\nability to bridge the gap between design flexibility and resolution in a substrate-general manner,\nwhich we willelucidate through adirect comparative analysis below.\nFabrication Typical DesignFlexibility/\nKeyLimitation OurMethod'sDistinction\nMethod Resolution Scalability\nLow:Newphysicalmask\nLimitedresolutionandpattern Photolithographicflexibility:Laserwriting\nShadow requiredforeachdesign\n~10-50μm complexity;poorscalabilityfor enablesdirectpatterningwithoutcustommasks,\nMask change;Patternedge\nmulti-layerdevices. achieving~1μmresolution.\nextensionchallenges.\nMedium:Re-patternneeds; Difficulttoachievecomplex, Materialandcircuitintegration:patterned\nreliesonorganicploymer interconnectedcircuitsona mediatoranddepositedelectrodesonthetarget\nMechanical\n~1-2μm layers(e.g.,PMMA,PVA); singlesubstrate;potentialfor materialandsubstrate,enablingthefabricationof\nTransfer\nlimitedto2Dmaterial transferdefectsandelectrical contacted,interconnectedFETarraysand\narrays. shortcircuits.\nminimalinterfacecontamination.\nHigh:Anydefinedpattern\nThis Work canbewrittenbylaser; Requireslaserpatterningstep\n~1μm Combinesmaterialandprocessingcompatibility.\n(SeMediator) suitableformulti-layer andpatterningefficiency.\nprocessing.\nuniquely combines:\nHigh Resolution (~1 μm) and Freedom Pattern Design on a single substrate, surpassing shadow\nmasks.\nLess surface contaminationand goodelectrical contact comparableto mechanical transfer.\nBroad Material Compatibility, as successfully demonstrated with sensitive materials like BP,\nhalide,andperovskite without solvent damage.\nTherefore, we posit that our method does not replace existing techniques but provides a\nsupplementary versatile and powerful alternative. We have now incorporated this comparative\ndiscussion into the discussion section of the revised manuscript to better frame our unique value\n(page 11), highlighted in red.\n2. The reported device performance such as on/off ratios for MoS FETs (average ~10 , best ~10 ;\nFig. 4f) is less compelling when compared to recent works using device fabrication processes based\n₂ ⁷ ⁹\non organic polymeric resists, which demonstrates average on/off ratios of ~10 for devices on SiO\nor high-κoxide substrates (NatureElectronics 8, 571–577, 2025; NatureElectronics 6, 146–153,\n⁸ ₂\n2023; Nature Electronics 8, 135–146, 2025). This challenges the value of adopting the method\ndescribed inthemanuscript.\nResponse: Thank you for this important comment regarding the performance comparison of the\nMoS FETs. We would like to emphasize a critical factor in device performance: the dielectric layer.\npredominantly utilize high-κ oxide dielectrics (e.g., HfO ). It is well-established that the use of\n2\nhigh-κ dielectrics significantly enhances the gate-field coupling, leading to higher on-state currents,\nand consequently, dramatically improved on/off ratios compared to devices employing a SiO\n2\nback-gate (e.g., Nat. Electron. 2020, 3, 473-478; Nat. Mater. 2023, 22, 1078-1084; Nat. Mater. 2025,\n24, 197-204). To ensure a fair and direct assessment of the device value, we have therefore focused\nthe performance comparison on a unified basic device architecture: MoS FETs using a standard\n2\ndielectrics and isolates theimpact ofthe fabrication process itself.\nFollowing the reviewer's suggestion, we have thoroughly updated the performance comparison\n(Figure R16). We have added the provided references and other recent key works using the same\nSiO back-gate structure to Fig. 4h and Supplementary Table 2 in the revised manuscript. The\n2\n18\nupdated data clearly show that the on/off ratios achieved by our devices are highly competitive with,\nand in many cases superior to, those reported in recent literature for MoS FETs on SiO fabricated\n2 2\nwith conventional polymer-based resists. This comparison demonstrates that our selenium-mediated,\nall-dry lithography process does not compromise the electrical performance of the sensitive channel\nmaterial.\nWefirmly believe that integrating our method with high-κ dielectrics in a top-gate geometry could\nfurther significantly enhance device performance. The competitive results achieved on SiO\n2\nsubstrates strongly attest to the non-damaging nature of our process. This promising potential\nmotivates our ongoing work to further develop the selenium-mediated technique for use with\nadvanced dielectric materials in futurework.\nFigureR16.Comparison ofthe average on/offratio ofback-gated MoS FETs with SiO dielectric.\n2 2\n3. The manuscript attributes selenium’s photothermal sublimation to weak intermolecular van der\nWaals forces but lacks critical details on how laser parameters (wavelength, power density, scanning\nspeed) influence patterning precision. Specifically: How do different laser wavelengths affect trench\nresolution? Does varying laser power lead to residual selenium on the substrate, and if so, how is\nthis quantified? Without such data, the reproducibility and controllability of the patterning process\nremain uncertain.\nResponse:These are insightful questions regarding the critical relationship between laser parameters\nand patterning precision. We agree that a quantitative understanding is essential for demonstrating\nthe controllability and reproducibility of our process. We have added a systematic series of\nexperimentsto address these pointsdirectly.\n(1)Influenceof LaserWavelength andPoweronTrench Resolution\nTo investigate the effect of wavelength, we patterned line trenches into the selenium layer using\n19\nboth 532 nm and 633 nm lasers at a constant scanning speed. As shown in the optical micrographs\n(Figure R17a, b), a clear difference in process efficiency and resolution is observed. For the 532 nm\nlaser, clean and well-defined trenches exposing the underlying silicon substrate (purple color) were\nachieved across a wide power range, from 0.1 mW to 10.0 mW. In contrast, with the 633 nm laser,\npowers from 0.1 mW to 4.0 mW only resulted in partial removal of the selenium layer, failing to\nclear the film completely. Complete removal and exposure of the substrate required a higher\nthreshold power of6.0mW.\nFigureR17.LaserwavelengtheffectontrenchresolutionofSefilmpatterns.OpticalimagesofSepattern\netchedby532nm(a)and633nm(b)lasersunderlaserpower0.1mW,1.0mW,2.0mW,4.0mW,6.0mW,8.0\nmW,and10.0mW.c,Statisticalchartoftheetchedtrenchwidthsusing533nmand633nmlasersatdifferentpower\nlevels.\nThe AFM profiles were used to precisely extract the trench widths, allowing us to plot resolution\nas a function of laser power for both wavelengths (Figure R17c). The data conclusively show that\nthe 532 nm laser produces finer resolution than the 633 nm. For instance, at its lowest effective\npower (0.1 mW), the 532 nm laser achieved a resolution of approximately 1.1 μm, whereas the 633\nnm laser, at its threshold power (6.0 mW), yielded a resolution of about 1.8 μm. This is attributed to\nthe higher photon energy and potentially tighter focal spot achievable with the shorter wavelength,\nleading to more confined photothermal energy and thus finer feature definition. We have added the\nfigure as Supplementary Fig. 11in therevised Supplementary Information.\n20\n(2)Influenceof LaserPowerand Quantification ofResidue\nThe experiments directly address how varying laser power affects patterning completeness. We\nidentified a distinct threshold power for complete sublimation, which is wavelength-dependent. For\nthe 633 nm laser, operation below 6.0 mW led to incomplete removal, leaving residual selenium, as\nvisually evident in the optical micrographs. To rigorously prove the absence of residues at and above\nthe threshold power, we performed the roughness analysis across five randomly selected locations in\ndifferent power etching (Area 1 - Area 6) (Figure R18). The surface roughness measured inside\nthese trenches is consistently below 0.4-0.7 nm. These approximate values are statistically close to\nthe roughness of a fresh SiO /Si substrate and are characteristic of the native atomic-scale roughness\n2\nofthesubstrate itself.\nFigureR18.Statisticalsurfaceroughnessofthelaser-irradiatedregionunderdifferentpowers.Roughness\\oftheSepatterntrenchesetchedbya532nmlaserunderlaserpowersof0.1mW,1.0mW,2.0mW,4.0mW,6.0\nmW,8.0mW,and10.0mW.\nIn summary, the provided data establishes a clear correlation between laser parameters and\npatterning outcomes. This systematic analysis robustly demonstrates the controllability and\nreproducibilityofour selenium-based lithography process.\n4. Information on the stability of selenium films during storage or device fabrication is absent. For\ninstance: Does prolonged exposuretoair (e.g., oxygen, humidity) induce oxidation or degradation of\ntheselenium layer? How does such exposureaffect the film’s adhesion to thesubstrate or its ability\nto be patterned via laser sublimation? These factors are critical for assessing the practical utility of\nthemethod in large-scale manufacturing.\nResponse: The environmental stability of the selenium films is indeed vital for assessing the\npractical utility and scalability of our method. We have conducted a systematic study on the\nevolutionof theselenium layer uponprolonged exposuretoambient air and room temperature.\n21\n(1)Chemical StabilityAgainstOxidationand Degradation\nWe firstly detected the chemical state of the selenium films over an extended period of\napproximately 0 months, 18 months, 24 months, and 42 months using X-ray diffraction (XRD) and\nX-ray photoelectron spectroscopy (XPS).\nFigureR19.XRDandXPSspectraoftheSefilmsdepositedonSiO /Sisubstrateafterdifferentperiodsof\n2\nstorageinair.a,XRDspectraofSefilmsagedapproximately0months,18months,24months,and42months.\nThescanningdegreeisonlyintherangeof10-32toavoidtheextremelystrongdiffractionpeaksofthesilicon\nsubstrate.High-resolutionSe3d(b)andO1s(c)XPSspectra.\nThe XRD patterns of the Se films, even after prolonged air exposure, show only the characteristic\nbroad halo of amorphous selenium (Figure R19a). No detectable crystalline peaks corresponding to\nselenium oxides were observed, indicating the absence of long-range crystalline oxidation products.\nThe high-resolution Se 3d and O 1s XPS spectra provide more surface-sensitive information (Figure\nR19b,c). The spectra for freshly deposited films are dominated by the elemental Se 3d doublet.\nCritically, the binding energy position of the Se 3d peak shows no chemical shift even after 42\nmonths of air exposure, indicating the absence of significant chemical transformation in the bulk of\nthe film. While the peak position remains stable, we observe a slight attenuation of the Se 3d peak\nintensity over time. Correspondingly, the O 1s signal intensity remains largely unchanged for\nsamples stored up to 42 months. It seems that no formation of a superficial native oxide layer (SeO )\n2\nonthefilm surfaceover an exceptionally long duration.\nfor 2 years. This robust stability significantly bolsters the case for the applicability in real\nmanufacturing environments.The figure about filmstability isadded as Supplementary Fig.11.\n(2)Impact onAdhesionandPatterning Performance\nToevaluate the functional impact of aging onthe lithographic process, we performed two key tests\nonsamples exposed toair for different durations.\n Mechanical Lift-off Test: The adhesion of the aged selenium films to the substrates was\nevaluated. We found that the films maintained excellent adhesion and could still be completely\nremoved,even after storage for 42months,viaPDMSmechanical peeling process (FigureR20).\nFigureR20.MechanicalpeelingofSefilmsafterdifferentperiodsofstorageinair.PDMSlayerislaminated\\onthesurfaceoftheSefilmpre-depositedonSiO /Sisubstrate,andthenispeeledoffthesubstratebytweezer.\n2\n Laser Patterning: Most importantly, we tested the laser-induced sublimation patterning on aged\nfilms (Figure R21). The results confirm that the aged films, despite the partial phase transition,\nremain highly susceptible to photothermal sublimation. We successfully patterned features with\ncomparable resolution and edge definition to those fabricated on fresh films. The laser power\nrequired forcomplete removal didnot showastatistically significant increase.\nFigureR21.Laserdirectwritingonseleniumfilmsafterdifferentperiodsofstorageinair.Opticalimages\noftheline-patterningSefilmswiththedifferentthicknessesafter532nmlaserdirectwritingwith1.0mW.\nselenium film remains chemically stable and, critically, its core lithographic functions—both in\nmechanical lift-off and laser patterning—are fully preserved. This robustness against ambient\ndegradation significantly bolsters the case for the practical applicability of our method in a standard\nlaboratory orpilot-scalemanufacturing environment.\n5. The claim that “patterns obtained are sharp edges in the unexposed area and no small particle\nresidues in the irradiated region” is insufficiently supported. TheAFM height scale in the provided\nimages is too large (~300 nm) to resolve nanoscale residues (a few nanometers or smaller), which\ncould stillimpact device performanceanduniformity.\nResponse: We agree that the initial AFM height scale was indeed too coarse to definitively rule out\nthe presence of nanometer-scale particles. In direct response, we have performed new, nanoscale\nAFM measurements toquantitatively address thisconcern.\nThe revised analysis features high-resolution (1 μm × 1 μm) AFM scans of the laser-irradiated\nregion on a SiO /Si substrate, acquired with a greatly reduced Z-scale. We provide three key\n2\nquantitativemetrics to rigorously assess surface cleanliness:\n Line Profile Analysis: The average line profile across the scanned area shows a surface height\nvariation in the range of -0.34 nm to +0.42 nm. This fluctuation is on the atomic scale of the\nSiO /Sisurface itself.\n2\n Surface Roughness: The calculated image roughness of the irradiated region is 0.432 nm, which\nisexceptionally low.\n Statistical Height Distribution: The distribution of all height data points (comprising 200 points\nper line profile) follows a near-perfect Gaussian distribution. Critically, there are no statistical\noutliersor \"tails\" in thedistributionthat would indicatethe presenceof discrete nanoparticles.\nTo confirm uniformity, we repeated this analysis across six randomly selected locations (Area 1 -\nArea 6)within thelaser-treated region (FigureR22).All six areas exhibited similarly minimal height\nvariations and nearly identical image roughness values, which were statistically indistinguishable\nfrom thosemeasured ona pristine, fresh SiO /Si substrate.\nlaser-irradiated region is free of nanoscale Se residues. The observed topography is consistent with\nthe intrinsic roughness of the underlying substrate, thereby fully supporting our claim of a clean,\nresidue-freepattern.Thenew nanoscaleAFM images are nowincluded as Supplementary Fig. 13.\nwithinrandomlyselectedlocations(Area1-Area6).Surfaceheightcurves,imageroughness(Ra),andstatistical\nheightdistributionarerespectivelymarkedinsixfigures.\n6. Numerous typos and inconsistencies in figure numbering undermine readability. For example,\nreferences to“Fig. 2c, 2d,2e, 2f”appear to correspond to“Fig. 3c, 3d,3f”inthe manuscript.\nAthorough proofread isrequired to correct these issuesandensureclarity.\nResponse: Thanks for this kind reminder. The figure numbering issues mentioned above have been\nrevised. We carefully checked all text in the whole manuscript again, and the changes made in the\nrevised manuscript are indicated inred.\n-Ending-\n25"}, {"round": 2, "reviewer_comments": {"reviewer_1": "The authors well addressed the comments and i suggested its acceptance for publication in Nature Communications", "reviewer_2": "Dear Authors,\nI have reviewed the revised manuscript and the authors' response. The authors have fully addressed my previous concerns.\nThe clarifications and added data have significantly improved the clarity and quality of the paper. I have no further\nreservations and recommend acceptance.", "reviewer_3": "In the revised manuscript, the authors have performed additional experiments and analyses. The paper has been\nsignificantly improved. In general, I am satisfied with the revision and responses. If the authors clarify the following points,\nthe manuscript will be further improved:\n(1) What is the sample size of devices with Lch/Wch = 12/5 μm statistically analyzed in Fig. 4h?\n(2) Why is the average on/off ratio of MoS₂ devices with Lch/Wch = 12/5 μm more than one order of magnitude higher than\nthat of MoS₂ devices with Lch/Wch = 25/10 μm?\n(3) In the revised manuscript, the authors claim that the on/off ratio of their devices is one order of magnitude higher than that\nof other works on silica substrates. However, considering that their average on/off ratio data in Fig. 4h is only 5-fold higher\nthan that of other reported works, this claim appears to be overstated, and the authors are advised to revise it to align with\nthe experimental results."}, "author_response": "Response to the reviewer’ comments\nReviewer #3:\nIn the revised manuscript, the authors have performed additional experiments and analyses. The paper\nhas been significantly improved. In general, I am satisfied with the revision and responses. If the\nauthors clarify the following points, the manuscript will be further improved:\nComment 1. What is the sample size of devices with Lch/Wch = 12/5 μm statistically analyzed in Fig.\n4h?\nResponse: The statistical analysis of the on/off ratio presented in Fig. 4h is based on a sample size of\nsix individual FET devices with Lch/Wch = 12/5 μm. These six devices exhibit uniform on/off ratios.\nThe average on/off ratio was calculated from the electrical measurements of these six devices. The\noptical microscopy images and the corresponding electrical results for all six devices are provided in\nSupplementary Fig. 38 for verification.\nComment 2. Why is the average on/off ratio of MoS₂ devices with L /W = 12/5 μm more than one\nch ch\norder of magnitude higher than that of MoS₂ devices with L /W = 25/10 μm?\nch ch\nResponse: Thank you for this important question. The higher on/off ratio observed in devices with\nL /W = 12/5 µm compared to those with 25/10 µm is a key finding, primarily resulting from the\nch ch\nimpact of channel resistance and electrostatic control at these channel lengths.\nIn the longer-channel devices (25 µm), the total resistance is dominated by the high channel\nresistance, which limits the on-state current (I ). Furthermore, the extended channel is more\non\nsusceptible to leakage paths caused by material inhomogeneities and less uniform gate control, leading\nto a relatively higher off-state current (I ). Conversely, in the shorter-channel devices (12 µm), the\noff\nchannel resistance is significantly lower. This provides a higher Ion. More critically, the shorter gate\nlength enables superior and more uniform electrostatic control across the entire channel, ensuring more\ncomplete carrier depletion in the off state and thus a lower I . The combination of a higher I and a\noff on\nlower I directly explains the order-of-magnitude improvement in the on/off ratio.\noff\nThis trend aligns with same reported studies, such as the work by Shen et al. (Nat. Commun. 2021,\n12, 693), which highlights the channel length (Figure R1). We appreciate the opportunity to discuss\nthis point, which underscores the importance of channel geometry in 2D electronics.\n2\n(Ref. Nat. Commun. 2021, 12, 693)\nComment 3. In the revised manuscript, the authors claim that the on/off ratio of their devices is one\norder of magnitude higher than that of other works on silica substrates. However, considering that\ntheir average on/off ratio data in Fig. 4h is only 5-fold higher than that of other reported works, this\nclaim appears to be overstated, and the authors are advised to revise it to align with the experimental\nresults.\nResponse: We thank you for this precise comment regarding the performance comparison. We\nappreciate the opportunity to clarify this point. Our initial statement that the on/off ratio is \"one order\nof magnitude higher\" was intended to reflect the comparison with the majority of the reported data\npoints in Figure 4h.\nWe agree that for more accuracy and to align perfectly with the presented data, the claim should be\nspecifically tempered when comparing against the top-performing referenced data point. Following\nyour advice, we have revised the relevant statement in the manuscript to more precisely reflect that the\ndevices achieve an average on/off ratio that is significantly higher than those of other reported back-\ngated MoS FETs with SiO dielectric fabricated by the organic resist lithography, by over an order of\n2 2\nmagnitude against most references and about fivefold against the highest benchmark.\nWe believe this revision provides a perfectly accurate and transparent description of our\nperformance results.\n-Ending-"}]

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