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Effective Molecular Alignment of Semiconducting Polymer and Its Application to Photopatterned Stretchable Transistors

MetadataDetails
Publication Date2025-03-05
JournalAdvanced Materials Technologies
AuthorsYasutaka Kuzumoto, Sung‐Gyu Kang, Hyunbum Kang, Sangah Gam, Hyungjun Kim
InstitutionsHallym University, Samsung (South Korea)
AnalysisFull AI Review Included

This research details the development of high-mobility, fine-patterned, intrinsically stretchable organic thin-film transistors (int-OTFTs) using a novel fabrication approach combining material alignment and interface engineering.

  • High Mobility Achieved: The optimized process yielded a peak mobility of 3.17 cm2 V-1 s-1 on rigid substrates, which is 3.6 times higher than conventional spin-coating methods and exceeds the performance of amorphous silicon.
  • Enhanced Molecular Alignment: High mobility was achieved by combining solution shearing with nano-grooved substrates (G-s), significantly improving the crystalline structure and facilitating strong π-π stacking of the DPP-P/SEBS semiconductor blend.
  • High-Performance Stretchable Device: Photopatterned int-OTFTs with a short channel length (10 ”m) demonstrated excellent performance metrics: 2.66 cm2 V-1 s-1 mobility and an ultra-low off-current of 0.96 pA.
  • Interface Engineering: A 1-bromooctane (1-BO) solvent treatment was applied to the stretchable micro-cracked Au electrodes, effectively reducing the contact resistance (RonW) from 5.1 MΩ cm to 790 kΩ cm.
  • Robust Stretchability and Durability: The int-OTFTs maintained stable electrical properties with only minor variations under 50% applied strain and demonstrated high durability after 1000 stretching cycles at 40% strain.
  • Material System: The stretchable semiconductor composite consists of a diketopyrrolopyrrole-based polymer (DPP-P) and a polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene elastomer (SEBS).
ParameterValueUnitContext
Peak Mobility (Solution Sheared, G-s)3.17 ± 0.21cm2 V-1 s-1Rigid substrate, parallel to grooves
Peak Mobility (Photopatterned int-OTFT)2.66cm2 V-1 s-1W/L = 100/10 ”m, intrinsically stretchable
Off-Current (Ioff)0.96pAPhotopatterned int-OTFT, L = 10 ”m
Mobility Ratio (Anisotropy)5.54N/AH1221-s-OSC, parallel/perpendicular mobility ratio
Contact Resistance (RonW)790kΩ cmWith 1-BO treatment (VDS = -0.5 V, VGS-Vth = -3 V)
Gate Insulator Capacitance3.9nF cm-2Cross-linked SEBS
Maximum Strain Tested50%Stable electrical properties
Cycling Durability1000CyclesTested at 40% strain
Nanogroove Lapping Film0.1”mDiamond particle size
Shearing Speed Range2-4mm s-1Solution shearing process
Shearing Substrate Temperature70°CDuring s-OSC coating
Annealing Temperature190°CPost-coating annealing (1 hour)
DPP-P:SEBS Weight Ratio (Shearing)3:7N/AOptimized for solution shearing
DPP-P:SEBS Weight Ratio (Spin-coating)6:4N/AOptimized for spin-coating
Lamellar Stacking Distance2.5nmDetermined by GIWAXS (qz = 0.25 A-1)

The fabrication of the high-performance, photopatterned int-OTFTs involved several critical steps focused on molecular alignment and interface control:

  1. Nanogrooved Substrate Preparation (G-s): Rigid substrates (SiO2/Si or glass) were rubbed 50-100 times using a 0.1 ”m diamond lapping film (pressure ≈ 0.1 kg cm-2) to create nano-grooves. These surfaces were subsequently modified with an ODTMS self-assembled monolayer (SAM).
  2. Stretchable Substrate and Electrode Fabrication: A dextran sacrificial layer was coated on glass, followed by a highly cross-linked SEBS layer (substrate/gate insulator). Micro-cracked Au electrodes (gate, source, and drain) were patterned using thermal deposition and lift-off.
  3. Interface Treatment: The surface of the S/D electrodes and gate insulator was treated with 1-bromooctane (1-BO) solvent (spin-coated five times) to remove surface impurities (photoresist residue, PFBT) and significantly reduce contact resistance prior to semiconductor transfer.
  4. Molecular Alignment via Solution Shearing: The DPP-P/SEBS solution (3:7 ratio) was coated onto a rigid G-s substrate using a solution-shearing technique, aligning the polymer chains parallel to the nano-grooves and the intended channel direction.
  5. s-OSC Transfer: The aligned s-OSC film was transferred from the rigid G-s substrate onto the stretchable BG-BC structure using a PDMS film, ensuring the nanogroove/shearing direction was parallel to the channel length.
  6. Photopatterning of s-OSC: The transferred s-OSC layer was photopatterned using a fluorinated photoresist and dry etching to define the active channel area and suppress parasitic current leakage.
  7. Encapsulation and Release: The device was encapsulated with a SEBS layer. The sacrificial dextran layer was dissolved in water, releasing the fully stretchable int-OTFT film from the rigid glass substrate.

The development of high-mobility, intrinsically stretchable organic transistors is critical for next-generation flexible and wearable electronics.

  • Stretchable Displays: Enabling high-resolution, durable backplanes for displays that can conform to complex, dynamic surfaces (e.g., automotive interiors, clothing).
  • Skin-Like Electronics: Fabrication of highly compliant, skin-mounted sensors, health monitors, and human-machine interfaces requiring high mobility and mechanical robustness.
  • Smart Textiles and Wearables: Integration of complex electronic circuits directly into clothing or flexible devices that must withstand significant stretching and cycling.
  • Flexible Integrated Circuits: Use in stretchable logic circuits and memory arrays where performance must exceed that of typical amorphous silicon or low-mobility organic materials.
  • Advanced Sensing: Creation of large-area, stretchable sensor arrays (e.g., pressure, temperature) that require high signal processing speed provided by high-mobility TFTs.
View Original Abstract

Abstract Intrinsically stretchable organic transistors are promising solutions for realizing stretchable electronic systems, such as skin‐like wearables and next‐generation displays. Nevertheless, applying stretchable organic thin‐film transistors to high‐end display backplanes requires enhancing key electrical properties, including mobility and off‐current, beyond the amorphous Si level, particularly for short channel lengths. Herein, enhanced performances of intrinsically stretchable organic transistors with a high degree of molecular alignment in stretchable semiconductor composites, comprising a diketopyrrolopyrrole‐based polymer and polystyrene‐block‐poly(ethylene‐ran‐butylene)‐block‐polystyrene‐elastomer, utilizing the solution shearing process on nanogrooved surfaces is reported. The density and shapes of the nano grooves are controlled by the number of rubbings with a 0.1 ”m diamond lapping film, achieving mobility values exceeding 3 cm 2 Vs −1 on SiO 2 /Si—three‐fold higher than that of the conventional spin‐coating method. This process improves the crystalline structure of semiconductor films, facilitating π-π stacking and large‐sized crystalline structures. Additionally, the solvent treatment on the surface of stretchable Au electrodes effectively reduces the contact resistance with highly oriented polymer semiconductors in intrinsically stretchable transistors, exhibiting 2.66 cm 2 Vs −1 mobility and 0.96 pA off‐current at 10 ”m short channel length. The electrical properties of stretchable transistors yield only minor variations under 50% strain conditions and after 1000 cycles at 40% strain.