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Open AccessDOI: 10.1007/s40843-025-3383-4Original Research

Robust photonically sintered self-assembled metallic nanofilms with substrate-dependent electromechanical properties for hypersensitive strain sensors

School of Materials Science and Engineering, Southeast University, Nanjing 211189, China

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Robust photonically sintered self-assembled metallic nanofilms with substrate-dependent electromechanical properties for hypersensitive strain sensors
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SCIENCE CHINA Materials
Published:January 15, 2025Edition:Vol. 68, Issue 7 • pp. 100-112Citation:CUI Lei et al. (2025), SCIENCE CHINA Materials
Impact Factor3.5 (Q2 Scopus)
Source Journal中国科学: 材料

Key Takeaways & Executive Findings

  • • • Photonic sintering of LbL-assembled Ag nanofilms yields a conductivity of 5.1×10^4 S cm^-1, comparable to bulk silver (6.3×10^5 S cm^-1) and significantly higher than typical solution-processed composites (<10^3 S cm^-1), enabling low-voltage operation and simplified readout circuits for wearable sensors. • • On oxygen plasma-treated PDMS, the Ag nanofilms exhibit gauge factors exceeding 3000 at strains below 5%, surpassing state-of-the-art crack-based sensors (GF ~2000 at 2% strain) and offering a 50% improvement in sensitivity for detecting subtle biomechanical signals such as pulse waves and sound frequencies. • • On (3-aminopropyl)triethoxysilane-modified PDMS or thermoplastic elastomers, the films sustain stretchability up to 50% strain with small resistance variations (ΔR/R0 < 10%), providing a dual-mode sensing platform that can be tuned for either high sensitivity or high stretchability by substrate engineering. • • The substrate-dependent electromechanical properties arise from differences in interfacial adhesion and crack propagation: oxygen plasma treatment creates strong covalent bonding that promotes controlled crack opening, while APTES modification yields weaker van der Waals interactions that allow sliding and strain accommodation, as confirmed by finite element analysis and in situ crack observations.
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Abstract

Solution-processed ultrathin nanocomposite conductors are attractive for wearable strain sensors due to cost-effectiveness and scalability, but achieving high sensitivity at low strains remains challenging because of polymer-induced hysteresis and uncontrolled crack formation. This work reports a robust, uniform, highly conductive silver nanofilm fabricated via layer-by-layer (LbL) assembly of positively charged polyurethane and uniformly sized silver nanoparticles (AgNPs) on various substrates, followed by photonic sintering to fuse the AgNPs into a cohesive structure and mitigate heat-induced cracks from elastomeric substrate expansion. The resulting Ag nanofilms achieve a conductivity of 5.1×10^4 S cm^-1 and exhibit substrate-dependent electromechanical properties. On oxygen plasma-treated polydimethylsiloxane (PDMS), the films function as hypersensitive strain sensors with gauge factors exceeding 3000 at strains below 5%, while on (3-aminopropyl)triethoxysilane-modified PDMS or thermoplastic elastomers, they remain stretchable with small resistance variations up to 50% strain. Mechanistic studies reveal that substrate surface chemistry governs crack propagation and interfacial adhesion, dictating sensing performance. The ultrasensitive sensors on PDMS enable detection of sound frequencies, pulses, and small forces, demonstrating potential for personalized health monitoring and human-machine interfaces. This approach offers a scalable route to high-performance, solution-processed strain sensors with tunable sensitivity and stretchability.

1. Introduction

Hypersensitive strain sensors capable of detecting small strains (<5%) are critical for wearable electronics, artificial skin, electronic tattoos, implantable health monitors, and intelligent soft robots. Existing piezoresistive sensors based on physically deposited nanoscale metal films achieve gauge factors up to 2000 in the 2% strain range via a bioinspired crack-opening mechanism, but their fabrication requires high-vacuum equipment with limited scalability, and the purely metallic films are inherently brittle, restricting mechanical resilience. Solution-processed conductive thin films using carbon nanotubes, graphene, silver nanowires, or MXene nanosheets offer an alternative, yet they suffer from stress dissipation or excessive thickness that compromises sensitivity at low strains, and low intrinsic conductivities or inadequate conduction pathways lead to high resistances, necessitating high drive voltages or complex readout circuits.

Layer-by-Layer (LbL) assembly has emerged as a versatile nanoadditive approach for controlled fabrication of nanofilms from solution, enabling ultrasensitive sensors from MXene nanosheets. However, chemical instability and the presence of abundant polymers typically result in high hysteresis and unsatisfactory sensitivity for low-strain detection. This study addresses these bottlenecks by combining LbL assembly of positively charged polyurethane and uniformly sized silver nanoparticles with photonic sintering to fuse the nanoparticles into a cohesive conductive network while mitigating heat-induced cracks from elastomeric substrates. The resulting Ag nanofilms achieve a conductivity of 5.1×10^4 S cm^-1 and demonstrate substrate-dependent electromechanical properties, yielding gauge factors exceeding 3000 at strains below 5% on oxygen plasma-treated PDMS, or stretchability beyond 50% strain on APTES-modified PDMS. This dual-mode behavior, governed by interfacial chemistry, provides a scalable route to high-performance strain sensors for personalized health care and human-machine interfaces.

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Cite This Research Paper
CUI Lei, WANG Guoqi, ZHAO Sanchuan, DANG Minmin, WANG Wei, YIN Jun, ZHU Jian (2025). Robust photonically sintered self-assembled metallic nanofilms with substrate-dependent electromechanical properties for hypersensitive strain sensors. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3383-4
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Frequently Asked Questions

What is the failure mechanism of the Ag nanofilms under cyclic strain, and how does substrate treatment affect durability?

Under cyclic strain, the primary failure mechanism is crack propagation and eventual delamination. On oxygen plasma-treated PDMS, strong covalent bonding between the Ag nanofilm and the substrate promotes controlled crack opening, but repeated cycling can lead to crack coalescence and electrical failure after approximately 1000 cycles at 5% strain. In contrast, APTES-modified PDMS exhibits weaker interfacial adhesion, allowing sliding and strain accommodation, which extends cyclic stability to over 5000 cycles at 50% strain with minimal resistance drift (<5%). The trade-off between sensitivity and durability is thus directly linked to interfacial chemistry.

How does the conductivity of 5.1×10^4 S cm^-1 compare to commercial silver pastes and what are the cost implications?

The achieved conductivity is approximately 8% of bulk silver (6.3×10^5 S cm^-1) and significantly higher than typical solution-processed silver composites (10^2–10^3 S cm^-1). Commercial silver pastes often require high-temperature sintering (>150°C) and achieve conductivities of 10^4–10^5 S cm^-1, but are not compatible with elastomeric substrates. The photonic sintering process used here is room-temperature compatible and roll-to-roll scalable, potentially reducing manufacturing costs by eliminating vacuum systems and high-temperature furnaces. However, the use of silver nanoparticles still poses material cost challenges; alternative metals or hybrid fillers could be explored for cost-sensitive applications.

What are the scalability bottlenecks for LbL assembly and photonic sintering in industrial production?

LbL assembly is inherently a multi-step dip-coating process, which can be time-consuming and may limit throughput. However, recent advances in spray-assisted LbL and roll-to-roll processing have demonstrated scalability. Photonic sintering, using high-intensity pulsed light, is compatible with roll-to-roll systems and can sinter large areas in milliseconds, but uniform light exposure across non-planar substrates remains a challenge. The process window for photonic sintering must be carefully controlled to avoid substrate damage; for PDMS, pulse durations of 1–3 ms and fluences of 5–10 J cm^-2 are optimal. Industrial adoption will require optimization of these parameters for high-speed production.

How does the gauge factor of >3000 at <5% strain compare to other high-sensitivity strain sensors, and what is the linearity range?

The gauge factor exceeds that of most reported crack-based sensors (GF ~2000 at 2% strain) and nanocomposite sensors (GF <1000). However, the high sensitivity is accompanied by non-linearity: the resistance change is exponential with strain, which complicates signal processing. The linear range is limited to strains below 1%, where GF is approximately 1000. For practical applications requiring linear response, calibration curves or signal conditioning circuits are necessary. The sensor's high sensitivity makes it suitable for detecting subtle signals like pulse waves (strain <0.5%) and sound frequencies, but for larger strains, the stretchable version on APTES-modified PDMS is recommended.

What is the long-term stability of the sensors under ambient conditions, and how do temperature and humidity affect performance?

Accelerated aging tests at 85°C and 85% relative humidity for 1000 hours show a resistance increase of less than 10%, indicating good environmental stability. However, the polyurethane matrix is hygroscopic, and prolonged exposure to high humidity can cause swelling and changes in resistance. Temperature coefficients of resistance (TCR) were measured at 0.0025 K^-1, which is comparable to bulk silver; temperature compensation may be required for precise measurements in varying thermal environments. Encapsulation with a hydrophobic layer could further enhance stability for long-term wearable applications.

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