PubMed İndeksli Yayınlar Koleksiyonu
Permanent URI for this collectionhttps://hdl.handle.net/20.500.12573/397
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Article Citation - Scopus: 1Labyrinthine Microstructures With a High Dipole Moment Boron Complex for Molecular Physically Unclonable Functions(American Chemical Society, 2025-10-29) Yıldız, T.A.; Kiremitler, N.B.; Kayacı, N.; Kalay, M.; Özcan, E.; Deneme, I.; Usta, H.The design and development of novel molecular-physically unclonable functions (PUFs) with advanced encoding characteristics and ease of fabrication have recently attracted attention in cryptography, secure authentication, and anticounterfeiting. Here, we report the development of a new high dipole-moment small molecule, InIm-BF<inf>2</inf>, a difluoroborate complex of an indolyl-imine ligand, and the fabrication of unique labyrinthine patterns through a facile two-step thin film process under ambient conditions. The new molecule has a dipolar, coplanar π-backbone and arranges in the solid state with antisymmetric cofacial π-stackings (3.86 Å). These properties, along with short C–H···π contacts (2.74–2.88 Å) and nonclassical C–H···F hydrogen bonds (2.47–2.51 Å) (23.4% and 11.5% of the Hirshfeld surfaces, respectively), drive the formation of amorphous molecular PUF patterns with disordered, short-range interactions. Spin-coating followed by thermal annealing at a moderate temperature produces nanoscopic molecular thin films with intricate labyrinthine patterns. These patterns, characterized by interconnected, irregularly shaped, micron-sized (≈50–100 μm) features, exhibit excellent PUF characteristics, verified through advanced image analysis and computational algorithms. Unlike randomly positioned isolated features in classical binarized keys, the interconnected labyrinthine patterns possess rich entropy and complex features, directly authenticated via deep-learning methodologies. Our work not only demonstrates a facile, promising approach to fabricating unique high-entropy PUF patterns but also provides critical insights into designing advanced molecular materials for next-generation security applications. © 2025 The Authors. Published by American Chemical SocietyArticle Citation - WoS: 1Citation - Scopus: 1Stochastic Orientational Encoding via Hydrogen Bonding Driven Assembly of Woven-Like Molecular Physically Unclonable Functions(Wiley-VCH Verlag GmbH, 2025-07-02) Kayaci, Nilgun; Kiremitler, Nuri Burak; Deneme, Ibrahim; Kalay, Mustafa; Ozbasaran, Aleyna; Zorlu, Yunus; Usta, HakanThe prevention of counterfeiting and the assurance of object authenticity require stochastic encoding schemes based on physically unclonable functions (PUFs). There is an urgent need for exceptionally large encoding capacities and multi-level responses within a molecularly defined, single-material system. Herein, a novel stochastic orientational encoding approach is demonstrated using a facile ambient-atmosphere solution processing of a molecular thin film based on the rod-shaped oligo(p-phenyleneethynylene) (OPE) pi-architecture. The nanoscopic film, derived from the small molecule 2EHO-CF3PyPE with donor, acceptor, and pi-spacer building units, is designed for energetically favorable uniaxial molecular assembly and crystal growth via directional multiple hydrogen-bonding motifs at the molecular termini and short C & horbar;H<middle dot><middle dot><middle dot>pi contacts at the center. A facile solvent vapor annealing induces concurrent dewetting and microscopic 1D random crystallization, yielding a woven-textured random features. Using convolutional neural networks, the rich variations in microcrystal domain properties and stochastic encoding of 1D crystal orientations generate artificial coloration, achieving an encoding capacity reaching (6.5 x 10(4))(2752 x 2208). The results demonstrate an effective strategy for achieving ultrahigh encoding capacities in a thin film composed of a single-material. This approach enables low-cost, solution-processed fabrication for mass production and broad adoption, while opening new opportunities to explore molecular-PUFs through structural design and engineering noncovalent interactions.