NREUL: Rare-Earth Upconversion Contact-Quenching Sensing for Real-Time Molecular Detection in Complex Matrices
Year: 2026
Type: preprint
Abstract: NREUL: Rare‑Earth Upconversion Contact‑Quenching Sensing for Real‑Time Molecular Detection in Complex Matrices Abstract: Macroscopic critical behaviours and functional emergence within complex engineering, biological and material systems originate from conformation evolution, energy redistribution and interfacial hydration‑layer rearrangement driven by solid‑liquid interfacial molecular interactions. Investigations targeting critical dynamics of complex systems urgently demand in‑situ sensing tools that tolerate high‑turbidity real biological matrices and enable time‑resolved tracking of molecular‑recognition events. Conventional mainstream molecular‑interaction analytical techniques including Surface Plasmon Resonance (SPR), Bio‑Layer Interferometry (BLI), and FRET/LRET suffer intrinsic principle‑derived limitations. SPR/BLI deliver indirect readouts originating from interfacial mass change and cannot capture ligand‑conformational evolution or interfacial hydration‑microenvironment information. FRET/LRET sensing strictly requires donor‑acceptor spectral overlap, greatly restricting probe‑design flexibility. Critically, most above‑mentioned technologies require highly purified buffer environments and readily produce optical artefacts in whole‑blood or turbid bio‑fluids, distorting experimental outcomes. Based on proprietary granted and published Chinese patents CN119198650B, CN120741426A, CN121674053A together with two‑year closed‑loop experimental validation, this work reports NREUL (Nanoscale Rare‑Earth Upconversion Luminescence‑based contact‑quenching sensing), a novel sensing strategy, and elucidates the ligand‑mediated relay‑conformation‑modulated near‑field contact vibrational‑relaxation quenching mechanism. Distinct from dipole‑dipole energy transfer in FRET/LRET, rare‑earth upconversion nanocrystals are covalently anchored onto the end‑face of a quartz light‑guide rod to construct a solid‑state sensing interface. Sequential dipping of the light‑guide probe into individual wells of a 96‑well plate triggers step‑wise specific molecular recognition at the solid‑liquid interface. Molecular‑binding events induce conformational remodelling of interfacial‑anchored ligands together with reorganization of interfacial hydration‑layers, progressively establishing and expanding non‑radiative vibrational‑relaxation pathways and producing step‑wise specific luminescence‑intensity attenuation without requiring donor‑acceptor spectral overlap. Luminescence intensity ΔI is selected as the primary experimental observable. Mechanistic validation is accomplished via full‑process continuous‑gradient dipping assays, half‑process segmented‑control dipping assays, and multiple negative‑control experiments. Direct dipping measurements are performed using raw anticoagulated whole‑blood samples without any pre‑treatment. Combining signal intensity, kinetic time‑series profiles and negative‑control groups enables detection of molecular behaviours. Measured results demonstrate that interpretable time‑series sensing signals can be obtained by NREUL from raw whole‑blood samples without centrifugation, dilution or purification. Supporting both real‑time dynamic kinetic quantification and steady‑state end‑point quantification modes, NREUL can serve fundamental research on complex‑system critical dynamics and drug‑target interactions. It shows translational potential for IVD in‑vitro diagnostics and POCT point‑of‑care testing, and can be extended to cross‑disciplinary research scenarios such as agro‑biology and material‑interface science. Version statement: Version 1 (finalized experimental version), finalized after two‑year systematic replicate experiments. Synchronous luminescence‑lifetime validation experiments are not performed in V1 and will be implemented in iterative Version 2. Certain proprietary process parameters are omitted in this public preprint. Supplementary material files included in this upload: - SI‑1: Key Instrument Configurations and Detailed Experimental Workflows for Nanoparticle Synthesis - SI‑2: NREUL Technical Principles: Signal Origins and Signal Categories - SI‑3: Representative Raw‑Signal Datasets: Data Types, Signal Intervals, Sensing‑Graph Illustrations - SI‑4: Data‑Interpretation Workflows, Fitting‑Report Calculation‑Model Formulas For academic‑research reading only. Commercial use is prohibited without written permission from the copyright holder.
Authors: Teng, Lei, Wang, Shengjie, Teng, Che, Ding, YuXin
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7215700710
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