Supporting Information - Dual-mode 0D/2D Spatial Asymmetry Optoelectronic Device Enabled by in situ Microzone Femtosecond Laser Deposition

Aug 31, 2026

Supporting information elaborates fabrication and evaluation details for dual-mode 0D/2D optoelectronic devices enabled by in situ microzone femtosecond laser deposition. Comparative scoring is provided across spin/drop coating, PVD, and CVD versus microzone FLD, using criteria including temperature, atmosphere, spatial resolution, in-situ programmability, material generality, and cleanliness. Additional sections document MoS2 adsorption spectrum testing, dry transfer fabrication, and statistical performance summaries. Morphology and distribution analyses for black phosphorus films and nanoparticles are supported by SEM/TEM preprocessing, particle diameter estimation, and laser-fluence-dependent ablation behavior, complemented by Raman spectroscopy and explanation of detection limits in mapping.

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Supporting materials

Comparison of dual-mode devices

Evaluation of fabrication process for 0D/2D heterostructure

Light adsorption spectrum testing for MoS2

Fabrication process of dry transfer method

Statistical of dual-mode optoelectronic devices

Morphology and distribution criteria of BP film and nanoparticles

Analysis of Raman spectra

Supporting Information for Dual-mode 0D/2D Spatial Asymmetry Optoelectronic Device Enabled by in situ Microzone Femtosecond Laser Deposition Zehua Li 1,2, Guisheng Zou1,2, Jinpeng Huo1,2,*, Jin Peng1,2, Tianming Sun1,2, Yu Xiao3, Jiali Huo4, Bin Feng1,2, Lei Liu1,2,* 1 State Key Laboratory of Clean and Efficient Turbomachinery Power Equipment, Department of Mechanical Engineering, Tsinghua University, Beijing, 100084, China 2 Key Laboratory for Advanced Materials Processing Technology, Ministry of Education, Beijing 100084, China 3 School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Center of Hydrogen Science, Shanghai Key Lab of Electrical Insulation & Thermal Aging, Shanghai Jiao Tong University, Shanghai 200240, China 4 Department of Electrical and Computer Engineering, National University of Singapore, 4 Engineering Drive 3, Singapore 117583, Singapore. * Correspondence: Lei Liu: liulei@tsinghua.edu.cn, +86 18610814123. Jinpeng Huo: huojp@tsinghua.edu.cn, +86 18800101565. 1 State Key Laboratory of Clean and Efficient Turbomachinery Power Equipment, Department of Mechanical Engineering, Tsinghua University, Beijing, 100084, China 2 Key Laboratory for Advanced Materials Processing Technology, Ministry of Education, Beijing 100084, China Supporting materials Comparation of dual-mode devices Tab. S1. Statistics of dual-mode conversion of photodetector and optoelectronic synapse Evaluation of fabrication process for 0D/2D heterostructure The fabrication processes are evaluated based on temperature, atmosphere, spatial resolution, in-situ programmability, material generality, and cleanliness. The scoring rules and scores for different process are as shown in Tab. S1 and Tab. S2, respectively. The reasons for the score are as follows: Spin-coating/drop-coating (SC/DC): room temperature in air; macroscale patterns (≥100 µm), limited by fluid spreading; not pixel-addressable, global coating; very broad with colloids/inks; solvent/binder/surfactant residues are typical unless aggressively removed. Physical Vapor Deposition (PVD): typically, RT–400 ℃ depending on film density/crystallinity; requires high vacuum; µm-scale via hard masks/shadow masks; not reconfigurable on finished devices without additional lithography; broad for elemental/compound films, but limited by vacuum hardware/material volatility. Generally clean without organic. Chemical Vapor Deposition (CVD): Temperature: Often ≥400 ℃ (lower with PECVD, but still elevated for many materials). low-pressure or atmospheric with reactive gases/precursors. mask-/template-assisted; typical feature sizes in the 1–100 µm range. process-level growth, not suited to post-fabrication pixel-wise rewriting. depends on specific gaseous precursors/chemistries (material-selective). good film purity. Microzone Femtosecond Laser Deposition (M-FLD): room temperature in air; no vacuum required; h-BN Mask-confined micro-zones with ~µm-scale edge acuity; no chemical precursors; dry process with solvent-free. Tab. S2 Scoring criteria of defferent feature. Tab. S3 Scoring results for different preparation processes. Light adbsorption spectrum testing for MoS2 Fig. S1 Adsorption spectrum of MoS2. Fabrication process of dry transfer method Fig. S2 Transfer method of device. Statistical of dual-mode optoelectronic devices Fig. S3 Statistical graph of the performance of the dual-mode optoelectronic devices Morphology and distribution criteria of BP film and nanoparticles Fig. S4 High-resolution TEM (HGTEM) of BP. Fig. S5 SEM image of BP after M-PLD under the frequency of 124 mJ cm-2. (a) and 213 mJ cm-2 (b). Fig. S6 Preprocessing of BP NPs SEM images. (a) SEM image of BP NPs. (b) Binarization of SEM image. The equivalent diameter can be calculated as follows: 𝐷e=𝑆𝜋∙2#𝐸𝑞𝑢. 𝑆3 where S is the area of the particles. Fig. S7 Effect of laser fluence on the ablation morphology of black phosphorus in a single scanning lin

FAQs

Why are black phosphorus nanoparticles difficult to detect well in Raman spectroscopy mapping?

When BP NPs are relatively small and sparse, the weak Raman signal can be “ignored” by the detection laser, leading to barely detectable distribution in mapping except at larger particles.

Aug 31, 2026

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