{"id":154919,"date":"2025-06-03T13:43:24","date_gmt":"2025-06-03T13:43:24","guid":{"rendered":"https:\/\/www.europesays.com\/uk\/154919\/"},"modified":"2025-06-03T13:43:24","modified_gmt":"2025-06-03T13:43:24","slug":"spectral-physical-unclonable-functions-downscaling-randomness-with-multi-resonant-hybrid-particles","status":"publish","type":"post","link":"https:\/\/www.europesays.com\/uk\/154919\/","title":{"rendered":"Spectral physical unclonable functions: downscaling randomness with multi-resonant hybrid particles"},"content":{"rendered":"<p>Au\/Si particles: laser fabrication and bright luminescence<\/p>\n<p>Hybrid metal-dielectric systems are recognized as versatile nanophotonic platforms, whose diverse combinations unlock extraordinary optical features<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Barreda, &#xC1;., Vitale, F., Minovich, A. E., Ronning, C. &amp; Staude, I. Applications of hybrid metal-dielectric nanostructures: state of the art. Adv. Photonics Res. 3, 2100286 (2022).\" href=\"#ref-CR31\" id=\"ref-link-section-d11611104e636\">31<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Linic, S., Chavez, S. &amp; Elias, R. Flow and extraction of energy and charge carriers in hybrid plasmonic nanostructures. Nat. Mater. 20, 916&#x2013;924 (2021).\" href=\"#ref-CR32\" id=\"ref-link-section-d11611104e636_1\">32<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Tan, C., Chen, J., Wu, X.-J. &amp; Zhang, H. Epitaxial growth of hybrid nanostructures. Nat. Rev. Mater. 3, 1&#x2013;13 (2018).\" href=\"#ref-CR33\" id=\"ref-link-section-d11611104e636_2\">33<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Renaut, C. et al. Reshaping the second-order polar response of hybrid metal&#x2013;dielectric nanodimers. Nano Lett. 19, 877&#x2013;884 (2019).\" href=\"#ref-CR34\" id=\"ref-link-section-d11611104e636_3\">34<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 35\" title=\"Shlesinger, I., Vandersmissen, J., Oksenberg, E., Verhagen, E. &amp; Koenderink, A. F. Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement. Sci. Adv. 9, eadj4637 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR35\" id=\"ref-link-section-d11611104e639\" target=\"_blank\" rel=\"noopener\">35<\/a>. To develop robust spectral PUFs, we chose the well-proven tandem of gold and silicon. This choice stems from their considerable environmental stability, leading to a potentially limitless lifetime under standard ambient conditions. Furthermore, hybrid Au\/Si structures (for example, nanoparticles) overcome the limitations of silicon in light emission by leveraging the superior light absorption of gold and its efficient hot carrier injection into the active material<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 36\" title=\"Cho, C.-H., Aspetti, C. O., Park, J. &amp; Agarwal, R. Silicon coupled with plasmon nanocavities generates bright visible hot luminescence. Nat. Photonics 7, 285&#x2013;289 (2013).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR36\" id=\"ref-link-section-d11611104e643\" target=\"_blank\" rel=\"noopener\">36<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 37\" title=\"Makarov, S. V. et al. Nanoscale generation of white light for ultrabroadband nanospectroscopy. Nano Lett. 18, 535&#x2013;539 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR37\" id=\"ref-link-section-d11611104e646\" target=\"_blank\" rel=\"noopener\">37<\/a>.<\/p>\n<p>To fabricate Au\/Si particles, we adopted the femtosecond (fs) laser-induced dewetting technique<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Makarov, S. V. et al. Controllable femtosecond laser-induced dewetting for plasmonic applications. Laser Photonics Rev. 10, 91&#x2013;99 (2016).\" href=\"#ref-CR38\" id=\"ref-link-section-d11611104e653\">38<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Oh, H. et al. Laser-induced dewetting of metal thin films for template-free plasmonic color printing. ACS Appl. Mater. Interfaces 10, 38368&#x2013;38375 (2018).\" href=\"#ref-CR39\" id=\"ref-link-section-d11611104e653_1\">39<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 40\" title=\"Zhou, X. et al. Color generation and polarization-sensitive encryption by laser writing on plasmonic reflector arrays. ACS Appl. Mater. Interfaces 16, 38404&#x2013;38413 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR40\" id=\"ref-link-section-d11611104e656\" target=\"_blank\" rel=\"noopener\">40<\/a>. In contrast to traditional ablation strategies<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Theerthagiri, J. et al. Fundamentals and comprehensive insights on pulsed laser synthesis of advanced materials for diverse photo- and electrocatalytic applications. Light Sci. Appl. 11, 1&#x2013;47 (2022).\" href=\"#ref-CR41\" id=\"ref-link-section-d11611104e660\">41<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Larin, A. O. et al. Plasmonic nanosponges filled with silicon for enhanced white light emission. Nanoscale 12, 1013&#x2013;1021 (2020).\" href=\"#ref-CR42\" id=\"ref-link-section-d11611104e660_1\">42<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Gurbatov, S. O. et al. Multigram-scale production of hybrid Au-Si nanomaterial by laser ablation in liquid (LAL) for temperature-feedback optical nanosensing, light-to-heat conversion, and anticounterfeit labeling. ACS Appl. Mater. Interfaces 15, 3336&#x2013;3347 (2023).\" href=\"#ref-CR43\" id=\"ref-link-section-d11611104e660_2\">43<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 44\" title=\"Gerasimova, E. N. et al. Single-step fabrication of resonant silicon&#x2013;gold hybrid nanoparticles for efficient optical heating and nanothermometry in cells. ACS Appl. Nano Mater. 6, 18848&#x2013;18857 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR44\" id=\"ref-link-section-d11611104e663\" target=\"_blank\" rel=\"noopener\">44<\/a>, our approach is more straightforward, providing ordered arrays of particle-based microstructures with high throughput. To achieve this, a tightly focused laser beam irradiates the surface of a thin bilayer gold-silicon film, cutting out micrometer-sized circles and simultaneously heating them (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig2\" target=\"_blank\" rel=\"noopener\">2<\/a>a, \u201cMethods\u201d section). As a result, patches of diatomic melt are formed that experience a sequence of non-equilibrium hydrodynamic perturbations<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 45\" title=\"Wang, X. W. et al. Laser-induced translative hydrodynamic mass snapshots: noninvasive characterization and predictive modeling via mapping at nanoscale. Phys. Rev. Appl. 8, 044016 (2017).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR45\" id=\"ref-link-section-d11611104e670\" target=\"_blank\" rel=\"noopener\">45<\/a>. Ultimately, the melt breaks up into randomly dispersed submicron droplets, governed by surface tension forces and Rayleigh-Plateau-like instabilities<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 46\" title=\"Kondic, L., Gonz&#xE1;lez, A. G., Diez, J. A., Fowlkes, J. D. &amp; Rack, P. Liquid-state dewetting of pulsed-laser-heated nanoscale metal films and other geometries. Annu. Rev. Fluid Mech. 52, 235&#x2013;262 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR46\" id=\"ref-link-section-d11611104e674\" target=\"_blank\" rel=\"noopener\">46<\/a>. The resulting particles represent an intricate intermixing of gold and silicon components, which is established during their solidification (Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">1<\/a>).<\/p>\n<p><b id=\"Fig2\" class=\"c-article-section__figure-caption\" data-test=\"figure-caption-text\">Fig. 2: Fabrication and optical characterization of printed particle-based Au\/Si microstructures.<\/b><a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-60121-9\/figures\/2\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig2\" src=\"https:\/\/www.europesays.com\/uk\/wp-content\/uploads\/2025\/06\/41467_2025_60121_Fig2_HTML.png\" alt=\"figure 2\" loading=\"lazy\" width=\"685\" height=\"345\"\/><\/a><\/p>\n<p><b>a<\/b> Schematic illustration of the experimental setup used to fabricate hybrid Au\/Si particles, and scanning electron microscopy (SEM) image of an array of created structures (scale bar: 5\u2009\u03bcm). The radius of the circles outlined by a femtosecond laser is 1.5\u2009\u03bcm. With a laser beam scanning speed of 50\u2009\u03bcm\/s, this fabrication method allows the creation of up to 200 structures per minute. The size distribution of particles in these structures is presented in Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">2<\/a>. <b>b<\/b> The PL spectrum measured from one of the obtained Au\/Si particles (red) vs. the spectrum from the initial bilayer film (gray). For PL excitation, we used a fs-laser system with a central wavelength of 1050\u2009nm (\u201cMethods\u201d section). A sharp peak at 525\u2009nm corresponds to the second harmonic generation (SHG). <b>c<\/b> Wavelength-dependent PL slopes (i.e., powers of nonlinear dependence of PL intensity on pump intensity at a given wavelength) from four randomly selected particles. Taking into account that 3PA in Au is more efficient than that in Si<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 37\" title=\"Makarov, S. V. et al. Nanoscale generation of white light for ultrabroadband nanospectroscopy. Nano Lett. 18, 535&#x2013;539 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR37\" id=\"ref-link-section-d11611104e705\" target=\"_blank\" rel=\"noopener\">37<\/a>, while 2PA is the most probable nonlinear process in Si<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 66\" title=\"Afinogenov, B. I. et al. Visible upconversion luminescence of doped bulk silicon for a multimodal wafer metrology. Opt. Lett. 46, 3071&#x2013;3074 (2021).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR66\" id=\"ref-link-section-d11611104e709\" target=\"_blank\" rel=\"noopener\">66<\/a>, one can assume that the overall white-light signal results from these two separate absorption processes, responsible for their parts of the spectrum. <b>d<\/b> Bright-Field (BF), Dark-Field (DF), and PL images of a printed pixel illustration of the Yin-Yang symbol. Scale bar: 20\u2009\u03bcm.<\/p>\n<p>The obtained Au\/Si structures exhibit an intensive ultra-broadband up-conversion PL signal, spanning from 450 to 900\u2009nm (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig2\" target=\"_blank\" rel=\"noopener\">2<\/a>b, \u201cMethods\u201d section). By analyzing luminescence slopes, we identified two- and three-photon absorption (2PA &amp; 3PA) processes as main contributors to the measured signal (Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">3<\/a>). Notably, the dependence of the slope on the emitted photon wavelength shows an interesting behavior: while PL in the near-infrared range is dominated mostly by 2PA, the blue component of the signal corresponds to 3PA (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig2\" target=\"_blank\" rel=\"noopener\">2<\/a>c).<\/p>\n<p>One of the key parameters of spectral PUFs is the signal acquisition time, which should be carefully optimized to avoid excessive readout duration<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 47\" title=\"Gu, Y. et al. Gap-enhanced Raman tags for physically unclonable anticounterfeiting labels. Nat. Commun. 11, 1&#x2013;13 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR47\" id=\"ref-link-section-d11611104e740\" target=\"_blank\" rel=\"noopener\">47<\/a>. This property directly depends on the fabricated structures\u2019 quantum efficiency (QE), which we estimated according to the method presented elsewhere<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"He, X., Liu, S., Li, S., Panmai, M. &amp; Lan, S. Si\/Au hybrid nanoparticles with highly efficient nonlinear optical emission: Implication for nanoscale white light sources. ACS Appl. Nano Mater. 5, 10676&#x2013;10685 (2022).\" href=\"#ref-CR48\" id=\"ref-link-section-d11611104e744\">48<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Xiang, J. et al. Crystalline silicon white light sources driven by optical resonances. Nano Lett. 21, 2397&#x2013;2405 (2021).\" href=\"#ref-CR49\" id=\"ref-link-section-d11611104e744_1\">49<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 50\" title=\"Zhang, C. et al. Lighting up silicon nanoparticles with Mie resonances. Nat. Commun. 9, 1&#x2013;7 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR50\" id=\"ref-link-section-d11611104e747\" target=\"_blank\" rel=\"noopener\">50<\/a> (see Supplementary Notes\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">1\u20133<\/a> and Supplementary Figs.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">4\u20137<\/a>). As an example, we demonstrate studies for three particles whose cross-sectional views and corresponding QEs are shown in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>a. We also measured the QE map from a particle-based microstructure (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>d). The obtained efficiencies (on the order of ~1\u22123.5%) are relatively high for silicon-based PL sources (Supplementary Table\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">1<\/a>). Accordingly, the typical signal acquisition time required to obtain low-noise PL spectra is quite short and ranges from 0.1 to several seconds, depending on the pump laser power (Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">8<\/a>).<\/p>\n<p><b id=\"Fig3\" class=\"c-article-section__figure-caption\" data-test=\"figure-caption-text\">Fig. 3: Investigation of the internal structure and multi-resonant nature of Au\/Si particles.<\/b><a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-60121-9\/figures\/3\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig3\" src=\"https:\/\/www.europesays.com\/uk\/wp-content\/uploads\/2025\/06\/41467_2025_60121_Fig3_HTML.png\" alt=\"figure 3\" loading=\"lazy\" width=\"685\" height=\"510\"\/><\/a><\/p>\n<p><b>a<\/b> HDAAF-STEM and BF-STEM imaging of cross-sections of three investigated hybrid Au\/Si particles and enlarged parts of BF-STEM maps. Scale bars: 150\u2009nm. Inscriptions indicate the measured mean Si grain size and QE values for each particle. Characteristic Fast Fourier Transforms of high-resolution TEM images of silicon grains reveal their poly-crystalline structure (Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">10<\/a>). <b>b<\/b> Gold-Silicon phase diagram. The arrows indicate the expected evolution of melt Au\/Si droplets during their solidification (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">4<\/a>). 1 \u2013 liquid cooling stage, 2 \u2013 undercooling, 3 \u2013 recalescence, 4 \u2013 quasi-equilibrium segregated solidification. After complete solidification, solid-state cooling returns the resulting particle to thermal equilibrium with the environment. <b>c<\/b> Grain size distribution of the particle #1 fitted according to the Kolmogorov\u2013Avrami\u2013Mehl\u2013Johnson (KAMJ) model described in ref. <a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 60\" title=\"Bergmann, R. B. &amp; Bill, A. On the origin of logarithmic-normal distributions: an analytical derivation, and its application to nucleation and growth processes. J. Cryst. Growth 310, 3135&#x2013;3138 (2008).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR60\" id=\"ref-link-section-d11611104e796\" target=\"_blank\" rel=\"noopener\">60<\/a>. Inscriptions indicate the estimated times of grain nucleation (tcI) and growth (tcv) during the solidification of this particle (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">5<\/a>). <b>d<\/b> SEM image of a laser-fabricated structure consisting of randomly dispersed hybrid particles and the corresponding measured QE map. <b>e<\/b> Cross section of a computer-generated model of our gold-silicon particle and a calculated normalized distribution of the electric field amplitude inside it when illuminated by a linearly polarized plane wave at a wavelength of 1050\u2009nm. <b>f<\/b> Numerical simulation results: dependence of the spectral width of the field enhancement factor (EF) range of the Au\/Si particle on the S-to-V value of its gold network. Straight lines indicate the general trend of dependence.<\/p>\n<p>To demonstrate the practical efficiency of Au\/Si microstructures and the scalability of our fabrication technique, we printed several pixel patterns (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig2\" target=\"_blank\" rel=\"noopener\">2<\/a>d). We performed their direct luminescence imaging under unfocused laser beam excitation with a standard digital camera (\u201cMethods\u201d section). The obtained bright photos once again confirm feasible, reliable, and quick measurement of PL from our microstructures, essential for potential applications. These intriguing results stem from the unique features of the Au\/Si particles\u2019 internal organization, which we consider further.<\/p>\n<p>Inner structure and multi-resonant nature of Au\/Si particles<\/p>\n<p>Next, we investigated the internal composition of the fabricated gold-silicon particles to determine how it affects their PL properties. For this, the cross-sections of three different particles with equivalent diameters of 600\u2009nm, 550\u2009nm, and 880\u2009nm were examined using scanning transmission electron microscopy (STEM). The results, shown in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>a, reveal their non-repeatable, intricate configuration with average sizes of silicon polycrystals of 20\u2009nm, 24\u2009nm, and 183\u2009nm, respectively. To understand such a well-developed Au-enriched network enveloping a system of percolated Si grains, we should consider the thermodynamics behind its formation.<\/p>\n<p>As described above, during laser-induced dewetting of Au\/Si bilayers, we create submicrodroplets of biatomic solution. Their solidification involves several successive steps<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 51\" title=\"Tiwari, A., Samanta, R. &amp; Chattopadhyay, H. Droplet solidification: physics and modelling. Appl. Therm. Eng. 228, 120515 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR51\" id=\"ref-link-section-d11611104e859\" target=\"_blank\" rel=\"noopener\">51<\/a>, beginning with rapid cooling and undercooling of the melt and culminating with spontaneous nucleation and growth of silicon grains (see Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>b and Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">4<\/a> for details). In this sequence, a key role is played by a truly stochastic phenomenon: thermal fluctuations. They dominate in the undercooled melt via dynamic formation and decomposition of short-range order, acting as a driving force for random nucleation<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 52\" title=\"Gottstein, G. Physical Foundations of Materials Science (Springer, Berlin, 2004).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR52\" id=\"ref-link-section-d11611104e869\" target=\"_blank\" rel=\"noopener\">52<\/a>. The random nature of atomic interactions is also strongly manifested during grain development, when chemical, thermal, and mechanical instabilities (associated with Au atom diffusion, free energy release, and volume reduction, respectively) govern the growth dynamics. By analyzing the grain size distribution, we estimated the duration of grain nucleation and growth to be of the order of several nanoseconds, which emphasizes the chaos of these processes (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>c; see also Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">5<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">9<\/a>). Therefore, the internal arrangement of our particles is formed stochastically and cannot be predetermined by any existing technology.<\/p>\n<p>Returning to optics, comparatively high QE values of Au\/Si particles can be attributed to special characteristics of their interior structure. Specifically, the gold-saturated internal network in these particles supports a high density of hot-spot modes and collective plasmon excitations<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 42\" title=\"Larin, A. O. et al. Plasmonic nanosponges filled with silicon for enhanced white light emission. Nanoscale 12, 1013&#x2013;1021 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR42\" id=\"ref-link-section-d11611104e886\" target=\"_blank\" rel=\"noopener\">42<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 53\" title=\"Zhong, J. et al. Strong spatial and spectral localization of surface plasmons in individual randomly disordered gold nanosponges. Nano Lett. 18, 4957&#x2013;4964 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR53\" id=\"ref-link-section-d11611104e889\" target=\"_blank\" rel=\"noopener\">53<\/a>, which enables strong field localization in a broad spectral range. This directly affects the recombination rates of hot carriers excited in or injected into silicon grains. The non-radiative lifetime is increased through the Auger effect, reinforced by large carrier densities, while the radiative one is shortened due to the Purcell phenomenon<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 50\" title=\"Zhang, C. et al. Lighting up silicon nanoparticles with Mie resonances. Nat. Commun. 9, 1&#x2013;7 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR50\" id=\"ref-link-section-d11611104e893\" target=\"_blank\" rel=\"noopener\">50<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 54\" title=\"Xiang, J. et al. Modifying Mie resonances and carrier dynamics of silicon nanoparticles by dense electron-hole plasmas. Phys. Rev. Appl. 13, 014003 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR54\" id=\"ref-link-section-d11611104e896\" target=\"_blank\" rel=\"noopener\">54<\/a>. Together, these mechanisms enhance the system\u2019s QE.<\/p>\n<p>Notably, as observed in experiments, the more complicated the gold network in a particle is (i.e., the lower the average grain size is), the higher QE this particle exhibits. Presumably, this behavior indicates a positive correlation between the surface-to-volume (S-to-V) ratio of the Au component and the efficiency of field localization inside silicon grains. To prove this hypothesis, we conducted a series of numerical simulations (\u201cMethods\u201d section). Namely, for a number of randomly generated Au\/Si particles, we calculated the spectral width of the enhancement factor range, which is one of the main criteria for improved PL intensities (Supplementary Figs.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">11<\/a> and <a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">12<\/a>). The obtained values were then plotted versus the S-to-V ratio of the particle\u2019s Au part (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>f) and illustrate the expected dependence: the higher the S-to-V values are, the more effectively the field is confined in the active material at different wavelengths; hence, the better QE it will demonstrate. The enhancement factor (i.e., localization efficiency) was assessed as an effective square (I2) and cube (I3) of the relative intensity inside silicon grains<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 50\" title=\"Zhang, C. et al. Lighting up silicon nanoparticles with Mie resonances. Nat. Commun. 9, 1&#x2013;7 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR50\" id=\"ref-link-section-d11611104e921\" target=\"_blank\" rel=\"noopener\">50<\/a>. Details of geometry generation and other aspects of solving this problem are available in \u201cMethods\u201d section.<\/p>\n<p>Ultimately, it is important to shed light on the following logical chain. Since the cooling rate is inversely proportional to the droplet radius<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 42\" title=\"Larin, A. O. et al. Plasmonic nanosponges filled with silicon for enhanced white light emission. Nanoscale 12, 1013&#x2013;1021 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR42\" id=\"ref-link-section-d11611104e929\" target=\"_blank\" rel=\"noopener\">42<\/a>, the larger the size of an Au\/Si melt is, the longer it takes to solidify (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">6<\/a>). Consequently, the characteristic time for Si grain growth increases, allowing small grains to coalesce into larger ones<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 55\" title=\"Kabalnov, A. Ostwald ripening and related phenomena. J. Dispersion Sci. Technol. 22, 1&#x2013;12 (2001).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR55\" id=\"ref-link-section-d11611104e936\" target=\"_blank\" rel=\"noopener\">55<\/a>. This, in turn, results in a less developed Au-enriched network with lower S-to-V values. Finally, according to our simulations, this indirectly results in a decline in the particle\u2019s QE. Therefore, there is a certain relationship between the size and QE of the fabricated hybrids, which is consistent with the results of QE mapping: larger particles possess poorer up-conversion characteristics (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig3\" target=\"_blank\" rel=\"noopener\">3<\/a>d). Nevertheless, it should be noted that the presented arguments make a number of assumptions and do not consider, for example, the formation of amorphous silicon, which becomes dominant with sufficiently small particle sizes and can negatively affect the PL generation (see Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">4<\/a>).<\/p>\n<p>Despite all the qualitative dependencies, the contribution of random variations in the internal structure of Au\/Si particles to the received PL signal is significant. The reason is, they directly affect the quantity and quality of hot spots and, accordingly, the field enhancement inside silicon grains. Together with the non-equilibrium effects accompanying the fabrication of the studied structures, this opens up great prospects for their use as spectral PUFs.<\/p>\n<p>Weak PUFs for anti-counterfeiting applications<\/p>\n<p>To effectively harness the potential of our fabrication approach, we designed three logically different strategies for its PUF-related security applications (see the scheme summarizing the Challenge, Response, Post-processing, Key, and Validation steps for each of these strategies in Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">13<\/a>). Our first concept employs the fact that every produced structure has a unique PL signal. Indeed, despite general similarities of Au\/Si luminescence spectra, they all have some inimitable features that may serve as unclonable keys. Extracting and encoding these features requires special attention. Using only the signal intensity significantly limits forgery-resistance (i.e., the ability to withstand attempts at forgery), while relying on purely cryptographic methods<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 56\" title=\"Ponkratova, E. et al. Coding of non-linear white-light luminescence from gold-silicon structures for physically unclonable security labels. Adv. Funct. Mater. 32, 2205859 (2022).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR56\" id=\"ref-link-section-d11611104e960\" target=\"_blank\" rel=\"noopener\">56<\/a> loses valuable physical insights embedded within the signal. Here, we build PL encryption based on the decomposition of each spectrum into a set of five separate parameters with different physical origins (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig4\" target=\"_blank\" rel=\"noopener\">4<\/a>b). Namely, we use integral PL intensity, percentage contributions of 2PA and 3PA to the overall PL signal, the full width at half maximum (FWHM) of PL, and the ratio of SHG intensity to PL one (see \u201cMethods\u201d section for their full description).<\/p>\n<p><b id=\"Fig4\" class=\"c-article-section__figure-caption\" data-test=\"figure-caption-text\">Fig. 4: Two strategies for the use of Au\/Si microstructures in PUF-based anti-counterfeiting.<\/b><a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-60121-9\/figures\/4\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig4\" src=\"https:\/\/www.europesays.com\/uk\/wp-content\/uploads\/2025\/06\/41467_2025_60121_Fig4_HTML.png\" alt=\"figure 4\" loading=\"lazy\" width=\"685\" height=\"691\"\/><\/a><\/p>\n<p><b>a<\/b> BF image of a QR code printed by the proposed fabrication technology (scale bar: 25\u2009\u03bcm). To enroll such a PUF label, its 10\u2009\u00d7\u200910 PL mapping is conducted, and the obtained map is encoded via application of the spectrum decomposition and clustering procedures<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 57\" title=\"Jenks, G. F. The data model concept in statistical mapping. Int. Yearbook Cartography 7, 186&#x2013;190 (1967).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR57\" id=\"ref-link-section-d11611104e981\" target=\"_blank\" rel=\"noopener\">57<\/a>. The resulting keys (each corresponding to one of the original PL features and representing a string of 100 0-to-4 numbers) are uploaded to a database, see \u201cMethods\u201d section. <b>b<\/b> Visual representation of the features used to decompose PL maps. <b>c<\/b> Pairwise matching map of 75 100-dimensional keys obtained from 15 different QR codes (the key dimension is defined by the mapping resolution). Hamming distance values close to 0 characterize similar keys. <b>d<\/b> Schematic illustration of the principle of comparing two PL images using computer vision for the second suggested PUF label model. The presence of similar patterns of bright areas (matches) in the pictures increases the likelihood of successful authentication<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 67\" title=\"Zhang, J. et al. An all-in-one nanoprinting approach for the synthesis of a nanofilm library for unclonable anti-counterfeiting applications. Nat. Nanotechnol. 18, 1027&#x2013;1035 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR67\" id=\"ref-link-section-d11611104e994\" target=\"_blank\" rel=\"noopener\">67<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 68\" title=\"Han, F. et al. Self-assembly of coordination polymers on plasmonic surfaces for computer vision decodable, unclonable and colorful security labels. J. Mater. Chem. C 7, 13040&#x2013;13046 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR68\" id=\"ref-link-section-d11611104e997\" target=\"_blank\" rel=\"noopener\">68<\/a>. <b>e<\/b> Distributions of the number of matches obtained during intra- and inter-comparison of approximately 60 captured images.<\/p>\n<p>As a proof-of-concept, we printed several QR codes with our hybrid structures as pixels (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig4\" target=\"_blank\" rel=\"noopener\">4<\/a>a). To enroll such PUF labels, we conducted their PL mapping and decomposed the obtained maps into five new ones, each describing one of the aforementioned spectrum features (\u201cMethods\u201d section). The resulting maps were then clustered using the Jenks optimization method<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 57\" title=\"Jenks, G. F. The data model concept in statistical mapping. Int. Yearbook Cartography 7, 186&#x2013;190 (1967).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR57\" id=\"ref-link-section-d11611104e1019\" target=\"_blank\" rel=\"noopener\">57<\/a> which allows storing only relative values, thus neglecting all the possible readout deviations (i.e., focus inaccuracy). The number of clusters was set to 5 (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">7<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">14<\/a>), and the unclonable keys obtained (five for each QR code with dimensions determined by the mapping resolution) were uploaded to a secure database. While more detailed measurements are also possible, choosing a mapping resolution of 10\u2009\u00d7\u200910 allows for easy and quick map reading (\u201cMethods\u201d section, Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">15<\/a>). To validate the authenticity of the QR code, a user needs to conduct its similar mapping and submit the result to the server. Then, five keys are extracted using the described protocol and compared with the ones stored in the database (\u201cMethods\u201d section). The label is considered genuine if the Hamming Distance (HD) calculated for all five pairs of keys does not exceed a specified number (0.55, see Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">7<\/a>). Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig4\" target=\"_blank\" rel=\"noopener\">4<\/a>c demonstrates a pairwise matching map characterizing our method\u2019s performance based on the analysis of 15 different QR codes. The values in the five 15\u2009\u00d7\u200915 blocks located on the diagonal of this map show the HD between the keys corresponding to the same PL characteristic, while other blocks mark the relation between vectors of different features. It is important to acknowledge that, despite the distinct physical origins of the five selected PL features, there exists a slight correlation among them. Additionally, the uneven distribution of pixels (structures) within the QR code results in observable non-random relationships when comparing different maps of the same feature. These correlations ultimately diminish the overall degrees of freedom in our PUF label, thereby reducing its true encoding capacity. Taking into account these inevitable but acceptable correlations and the HD gates set for authentication, we assessed the number of all the possible unique PUF labels distinguishable by our validation algorithm: ~1054 (more information can be found in \u201cMethods\u201d section). This value is enough for the successful use of the label<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 1\" title=\"Arppe, R. &amp; S&#xF8;rensen, T. J. Physical unclonable functions generated through chemical methods for anti-counterfeiting. Nat. Rev. Chem. 1, 1&#x2013;13 (2017).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR1\" id=\"ref-link-section-d11611104e1041\" target=\"_blank\" rel=\"noopener\">1<\/a>; if necessary, it can be boosted by increasing the mapping resolution.<\/p>\n<p>The second authentication concept is based on direct PL imaging using a digital camera with a standard 10\u00d7 objective, in which an unfocused laser beam illuminates the whole label area at once (\u201cMethods\u201d section). We revealed that photos captured this way display an unrepeatable spatial distribution of PL intensity for any of the laser-printed patterns. This is due to the large influence of microscale hydrodynamic instabilities associated with Au\/Si microstructures\u2019 creation. Thus, such PL images can be successfully used as unclonable keys. To prove this, we printed a number of visually identical Yin-Yang symbols and collected a database of their PL photos, each time changing the focus accuracy and shifting the position of the center of the pump laser beam. To correctly validate the obtained pictures, we developed an algorithm based on computer-vision techniques (see \u201cMethods\u201d section for more information). In short, when comparing two images, the number of their matches is calculated by analyzing the brightest areas (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig4\" target=\"_blank\" rel=\"noopener\">4<\/a>d). Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig4\" target=\"_blank\" rel=\"noopener\">4<\/a>e shows the distribution of the number of matches obtained during intra- and inter-comparison of 60 captured images. There is a considerable gap between these two sets of values, which allows us to determine a suitable threshold value, ensuring a wide range of accuracy, even for images captured in diverse conditions. Furthermore, the encoding capacity of this PUF model is estimated to be about 10141 (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">8<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">16<\/a>). However, this method is based mostly on microscale spatial randomness, using only PL intensity. Therefore, to fully realize the potential of our PUFs, we should encode their PL spectra individually, taking into account every piece of spectral information.<\/p>\n<p>Strong PUF for an all-optical OTP verification token<\/p>\n<p>Finally, we highlight that each created microstructure carries not one but several unique PL spectra due to its complex particle-based organization with characteristic sizes of ~500\u2212900\u2009nm. Indeed, the recorded spectra do vary depending on the position of the signal acquisition area and the excitation wave polarization (when using a high-aperture 100\u00d7 objective). Moreover, the number of such degrees of freedom can be roughly estimated as ~100 (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">9<\/a>). This indicates the potential for implementing a strong PUF, which, unlike the weak PUFs proposed above, can serve multiple security purposes. Building upon this concept, we present a model for an all-optical OTP verification token with a dynamic database, which could be used as a prototype for next-generation ultra-secure authentication protocols (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">10<\/a>).<\/p>\n<p>We describe the developed protocol by considering an array of printed Au\/Si microstructures (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig5\" target=\"_blank\" rel=\"noopener\">5<\/a>). Comparing the fabrication time of such a sample with the time required to measure all its possible spectra, we estimate their ratio as 1\u2013105 (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">11<\/a>). Therefore, with relatively fast manufacturing, the overall measurement of spectra is incredibly time-consuming. Moreover, as we show later, each individual spectrum can function as a unique key. During our token enrollment, N spectra are measured from random positions and uploaded to a database. Then, the user who wants to confirm ownership of the token measures PL from n points with server-provided coordinates. If most spectra are deemed as a match, the identification is confirmed, and these n spectra are removed from the database. In the next verification cycle, new spectra with coordinates that have not been disclosed yet will be used. If the token is transferred, its previous owner will no longer be able to pass verification, since new spectra will need to be measured for this. Moreover, if the token has a sufficient capacity, no party will have enough time to measure all its possible keys, which emphasizes the robustness of the proposed strategy. The number of verification cycles N\/n should be at least several hundred. Our example in Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">12<\/a> with N\u2009=\u20091200 and n\u2009=\u20095 demonstrates high verification accuracy, long service time, and ease-of-use of the token. To prevent database depletion, trusted users can upload new keys to it, but only over a secure communication line.<\/p>\n<p><b id=\"Fig5\" class=\"c-article-section__figure-caption\" data-test=\"figure-caption-text\">Fig. 5: Operating process of the developed all-optical OTP verification token.<\/b><a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-60121-9\/figures\/5\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig5\" src=\"https:\/\/www.europesays.com\/uk\/wp-content\/uploads\/2025\/06\/41467_2025_60121_Fig5_HTML.png\" alt=\"figure 5\" loading=\"lazy\" width=\"685\" height=\"247\"\/><\/a><\/p>\n<p><b>a<\/b> Token Enrollment. The token comprises a large array of laser-printed gold-silicon microstructures. All of them are effectively divided into 25 sections, each exhibiting a unique PL signal dependent on the pump laser beam\u2019s polarization (see Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">9<\/a> and Supplementary Figs.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">17<\/a> and <a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">18<\/a>). Consequently, the token functions as several arrays, each corresponding to a distinct laser polarization (0\u00b0, 45\u00b0, 90\u00b0, or 135\u00b0 relative to the y-axis). The orange frame highlights sections forming a single microstructure. During enrollment, N PL spectra are measured from randomly selected sections and stored in our dynamic database, along with their spatial coordinates (x, y) and the corresponding laser polarization (P). This database is then transferred to a secure cloud server, and the token is issued to the user. <b>b<\/b> Token Verification. First, on request, the server provides the coordinates (x, y, P) of n points from the database. Then, the user records the corresponding spectra and sends them as a response. Next, using our ML model, the server compares the user\u2019s spectra with the stored ones. In the event of a match, the user is verified, and the used spectra are removed from the database. Otherwise, verification fails. The whole verification process can be repeated cyclically until the database is depleted. The database size N is predetermined to accommodate a sufficient number of authentication cycles.<\/p>\n<p>For authentication purposes, we created a machine learning model, which is a conventional neural net with fully connected layers (\u201cMethods\u201d section). Taking a normalized PL spectrum together with a number of its features as input, the model produces a point in a multidimensional vector space. The distance between two points in this space determines the probability that the corresponding spectra are measured from the same coordinates. After a series of trainings, the distance threshold was set to maximize the model\u2019s true positive rate while maintaining low false positive values (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig6\" target=\"_blank\" rel=\"noopener\">6<\/a>b). The final single-spectrum authentication accuracy is 97% (at a cutoff threshold is 41.3), which is 15% higher than that achieved when classifying the original spectra (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#Fig6\" target=\"_blank\" rel=\"noopener\">6<\/a>c). A possible 3% mistake reflects an influence of noise on the measured data, which can be neglected with increasing signal acquisition time. Making verification decisions based on the results of comparing several spectra (instead of one) significantly increases the efficiency of our ML model (e.g., with n\u2009=\u20095, the accuracy is ~99.97%; Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">12<\/a>). To ensure the uniqueness and randomness of the generated embedding keys, we evaluated them using the NIST randomness test suite<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 58\" title=\"Bassham, L. et al. A statistical test suite for random and pseudorandom number generators for cryptographic applications &#010;                  https:\/\/tsapps.nist.gov\/publication\/get_pdf.cfm?pub_id=906762&#010;                  &#010;                 (2010).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR58\" id=\"ref-link-section-d11611104e1172\" target=\"_blank\" rel=\"noopener\">58<\/a>, yielding positive results (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">13<\/a> and Supplementary Table\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">2<\/a>). Furthermore, the computed information entropy values for each embedding coordinate indicate a high degree of unique information saturation, along with complete uniformity and unpredictability of the obtained keys (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">14<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">20<\/a>). Finally, the estimated encoding capacity of the embedding space is significant, reaching 10280 (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">15<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">21<\/a>). Thus, in contrast to electronic alternatives, which are often vulnerable to physical attacks<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 11\" title=\"Di Falco, A., Mazzone, V., Cruz, A. &amp; Fratalocchi, A. Perfect secrecy cryptography via mixing of chaotic waves in irreversible time-varying silicon chips. Nat. Commun. 10, 1&#x2013;10 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR11\" id=\"ref-link-section-d11611104e1198\" target=\"_blank\" rel=\"noopener\">11<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 12\" title=\"Horstmeyer, R., Judkewitz, B., Vellekoop, I. M., Assawaworrarit, S. &amp; Yang, C. Physical key-protected one-time pad. Sci. Rep. 3, 1&#x2013;6 (2013).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#ref-CR12\" id=\"ref-link-section-d11611104e1201\" target=\"_blank\" rel=\"noopener\">12<\/a>, our all-optical OTP system offers superior performance through the high entropy and enhanced security of stored keys.<\/p>\n<p><b id=\"Fig6\" class=\"c-article-section__figure-caption\" data-test=\"figure-caption-text\">Fig. 6: Comparative analysis of the performance of two spectrum comparison algorithms: with and without ML.<\/b><a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-60121-9\/figures\/6\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig6\" src=\"https:\/\/www.europesays.com\/uk\/wp-content\/uploads\/2025\/06\/41467_2025_60121_Fig6_HTML.png\" alt=\"figure 6\" loading=\"lazy\" width=\"685\" height=\"311\"\/><\/a><\/p>\n<p><b>a<\/b>\u2013<b>c<\/b> Basic comparison. This method directly compares two spectra by calculating the distance between their corresponding vectors. <b>d<\/b>\u2013<b>f<\/b> ML-driven comparison. Instead of raw spectra, this approach compares their embeddings generated by a trained ML model. Both methods rely on the notion of a cutoff distance for classification. Vectors located within this distance from each other are deemed a match, while those exceeding it are considered different. We evaluated both methods using a dataset of 2148 vectors describing spectra from both identical and distinct structures. The goal was to determine the optimal cutoff distance for accurate match predictions. <b>b<\/b>, <b>e<\/b> Density distributions of inter- and intra-device vector distances. <b>c<\/b>, <b>f<\/b> True positive, false positive, false negative, and true negative rates of the described spectrum classification vs. cutoff distance. The basic comparison achieved a maximum classification accuracy of 83%, while the ML-driven method significantly improved accuracy, reaching up to 97%. Notably, comparing not one but, for example, five spectra simultaneously boosts the accuracy up to 99.97% (Supplementary Note\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">12<\/a> and Supplementary Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-60121-9#MOESM1\" target=\"_blank\" rel=\"noopener\">19<\/a>). Also, preprocessing spectra with our model before storing them in the database will enhance token security against potential cyber-attacks.<\/p>\n","protected":false},"excerpt":{"rendered":"Au\/Si particles: laser fabrication and bright luminescence Hybrid metal-dielectric systems are recognized as versatile nanophotonic platforms, whose diverse&hellip;\n","protected":false},"author":2,"featured_media":154920,"comment_status":"","ping_status":"","sticky":false,"template":"","format":"standard","meta":{"footnotes":""},"categories":[3845],"tags":[65856,3965,29694,65857,3966,20454,4171,74,70,4172,16,15],"class_list":{"0":"post-154919","1":"post","2":"type-post","3":"status-publish","4":"format-standard","5":"has-post-thumbnail","7":"category-physics","8":"tag-ethical","9":"tag-humanities-and-social-sciences","10":"tag-information-storage","11":"tag-legal-and-other-societal-issues","12":"tag-multidisciplinary","13":"tag-nanophotonics-and-plasmonics","14":"tag-nonlinear-optics","15":"tag-physics","16":"tag-science","17":"tag-silicon-photonics","18":"tag-uk","19":"tag-united-kingdom"},"share_on_mastodon":{"url":"https:\/\/pubeurope.com\/@uk\/114619731857550262","error":""},"_links":{"self":[{"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/posts\/154919","targetHints":{"allow":["GET"]}}],"collection":[{"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/posts"}],"about":[{"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/types\/post"}],"author":[{"embeddable":true,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/users\/2"}],"replies":[{"embeddable":true,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/comments?post=154919"}],"version-history":[{"count":0,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/posts\/154919\/revisions"}],"wp:featuredmedia":[{"embeddable":true,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/media\/154920"}],"wp:attachment":[{"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/media?parent=154919"}],"wp:term":[{"taxonomy":"category","embeddable":true,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/categories?post=154919"},{"taxonomy":"post_tag","embeddable":true,"href":"https:\/\/www.europesays.com\/uk\/wp-json\/wp\/v2\/tags?post=154919"}],"curies":[{"name":"wp","href":"https:\/\/api.w.org\/{rel}","templated":true}]}}