Lateral flow assays (LFAs) are widely favored for on-site analysis due to their simplicity and cost-effectiveness. However, their limited quantitative capabilities constrain them to qualitative testing. In contrast, etalon sensors offer high sensitivity and enable quantitative detection. They operate by producing interference-based optical signals through multiple reflections of light within a cavity formed by two parallel reflective surfaces. This requires a stable optical path length, traditionally limiting their use to smooth substrates.

This study presents an integrated separation-sensing microfluidic platform (EtLFA). By fabricating etalons on commercial membranes and evaluating sensor's sensitivity and surface roughness, we determined that membrane surface roughness must meet two criteria — Sa < 0.5 μm and Smr > 90% — to support functional etalons. Capillary and permeability remain intact after etalon integration, ensuring membrane's purification performance. We further functionalized the etalon to respond specifically to glucose, to demonstrate the quantitative detection of glucose levels in a mimic blood sample. A glucose-responsive etalon@nylon served as the sensor module, while regenerated cellulose membrane enabled separation. This dual-module configuration filtered PDMS particles mimicking red blood cells and produced a 25 nm shift for 100 mg/dL glucose, enabling linear quantification via portable spectrometry. By incorporating etalon sensor onto rough membrane substrates, our platform transforms conventional LFAs into a quantitative analytical tool, offering novel avenues for enhancing analytical capabilities and broadening the applications of lateral flow assays. ... Read more

Food and medicines are two of the most essential categories of goods for human beings, providing vital nourishment and healthcare. However, as these products are commercialized and distributed on a global scale, consumers face the threat of counterfeit and deteriorated products. In response, this dissertation presents four prototypes consisting of On-Dose-Authentication (ODA) binarycodes and battery-less indicators based on smart hydrogel that are edible and reader-friendly to address these issues. First, a microfluidic platform for continuous synthesis of hydrogel microparticles with superparamagnetic colloids (SPCs) embedded at prescribed positions has been established. The shape of the cross-linked microparticle is independently controlled by stop-flow lithography, whereas the position of trapped SPCs is dictated by virtual magnetic molds made of 2D nickel patches facilitating magnetic trapping. The spatial positions of trapped SPCs collectively function as a binary code matrix for product authentication. The proposed magnetic microparticles will contribute to the development of soft matter-inspired product quality control, tracking, and anti-counterfeiting technologies. (Chapter 2) Second, a Physical Unclonable Functions (PUF) algorithm was developed to enhance the ODA binary codes' safety level. This algorithm exploits the diameter and coordinates of spheres as input, abandoning color and intensity as inputs, enabling imaging using common illumination and low-magnification microscopy hence lifting the reading constraints to advanced labs that are usually found in other current graphical PUF systems. Two sets of Poly(ethylene glycol) diacrylate ODA-PUF tags that can be read out via this algorithm were fabricated. The sets are single-diameter PUF leveraging random distributed superparamagnetic colloids of identical diameters and multiple-diameter PUF utilizing vortexed sunflower oil drops of various diameters, respectively. The performance of the single-diameter system was investigated. It passed NIST Statistical tests, demonstrating sufficient randomness, ideal bit uniformity, Hamming distance, and device uniqueness. The encoding capacity of the single-diameter system was found to be $9.2 imes10^{18}$, which can satisfy labeling the annual output of Aspirin. (Chapter 3) Third, a humidity indicator has been created that mechanically bends and rolls itself irreversibly upon exposure to high humidity conditions. The indicator is made of two food-grade polymer films with distinct ratios of a milk protein, casein, and a plasticizer, glycerol, that are physically attached to each other. Based on the thermogravimetric analysis and microstructural characterization, the bending mechanism is a result of hygroscopic swelling and consequent counter diffusion of water and glycerol. Guided by this mechanism, the rolling behavior, including response time and final curvature, can be tuned by the geometric dimensions of the indicator. As the proposed indicator is made of food-grade ingredients, it can be placed directly in contact with perishable products to report exposure to undesirable humidity inside the package, without the risk of contaminating the product or causing oral toxicity in case of accidental ingestion - features that commercial inedible electronic and chemo-chromatic sensors cannot provide presently. (Chapter 4) Finally, an alginate TTI bead that encapsulates betacyanin, a natural colorant extracted from purple pitaya, is proposed to continuously monitor and reflect the temperature history of the perishable products to diagnose the storage conditions. The instability of betacyanin is exploited to demonstrate undesirable temperature abuse through visual color changes. The thermochromic change of the purple pitaya extract and the pitaya-extract-encapsulated bead was investigated under various temperatures, pH, and gaseous atmosphere conditions. Experimental results show that the proposed TTI exhibits an irreversible thermochromic change under a wide operation temperature range up to at least 100 extdegree C with negligible disturbance from the gaseous composition. (Chapter 5) ... Read more

On-dose authentication (ODA) enhances security by incorporating customized molecular or micro-tags into each pill, preventing counterfeit products in genuine packages. ODA's security relies on tag non-replication and non-reverse engineering. Combining ODA with graphical Physical Unclonable Functions (PUF) promises maximum security. PUF uses intrinsic micro or nanoscale randomness as a unique ‘fingerprint’. However, current graphical PUFs have limitations like specific illumination requirements and the use of toxic materials, restricting their use in pharmaceuticals. In this study, we propose a novel approach called on-dose PUF. This method involves embedding microspheres randomly within micro biocompatible hydrogel particles. We showcase two distinct types of such on-dose PUFs. The first type utilizes randomly distributed superparamagnetic colloids (SPC) of identical diameters, while the second type utilizes vortexed sunflower oil drops of various diameters. The diameter and coordinates of the microspheres serve as input for generating cryptographic keys. A universal circle identification and binning program is used for extracting this information. One advantage of this approach is that it enables imaging using white light illumination and low-magnification microscopy, as color and signal intensity information are not crucial. This method enables patients to verify their medication by using their mobile phones from home. To assess the performance of the proposed on-dose PUF, we conducted canonical investigations on the single-diameter system. This system can only generate one layer of cryptographic keys, making it potentially more vulnerable than the multiple-diameter system. However, the single-diameter system successfully passed NIST Statistical tests and exhibited sufficient randomness, ideal bit uniformity, Hamming distance, and device uniqueness. Furthermore, we found that the encoding capacity of the single-diameter system was 9.2×10¹⁸, providing ample labeling potential. ... Read more

Elevated humidity levels in medical, food, and pharmaceutical products may reduce the products' shelf life, trigger bacterial growth, and even lead to complete spoilage. In this study, we report a humidity indicator that mechanically bends and rolls itself irreversibly upon exposure to high humidity conditions. The indicator is made of two food-grade polymer films with distinct ratios of a milk protein, casein, and a plasticizer, glycerol, that are physically attached to each other. Based on the thermogravimetric analysis and microstructural characterization, we hypothesize that the bending mechanism is a result of hygroscopic swelling and consequent counter diffusion of water and glycerol. Guided by this mechanism, we demonstrate that the rolling behavior, including response time and final curvature, can be tuned by the geometric dimensions of the indicator. As the proposed indicator is made of food-grade ingredients, it can be placed directly in contact with perishable products to report exposure to undesirable humidity inside the package, without the risk of contaminating the product or causing oral toxicity in case of accidental digestion, features that commercial inedible electronic and chemo-chromatic sensors cannot provide presently. ... Read more

A microfluidic platform for continuous synthesis of hydrogel microparticles with superparamagnetic colloids (SPCs) embedded at prescribed positions is described. The shape of the cross-linked microparticle is independently controlled by stop–flow lithography, whereas the position of trapped SPCs are dictated by virtual magnetic moulds made of 2D nickel patches facilitating magnetic trapping. The spatial positions of trapped SPCs collectively function as a binary code matrix for product authentication. Analytical and finite element methods are combined to optimize the trapping efficiency of SPCs by systematically investigating magnetic field microgradients produced by nickel patches. It is envisioned that the proposed magnetic microparticles will contribute to the development of soft matter inspired product quality control, tracking and anti-counterfeiting technologies. ... Read more