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It has been a challenge to achieve deoxyribonucleic acid (DNA) metallization and mass production with a high quality. The main aim of this study was to develop a large-scale production method of metal-ion-coated DNA hybrid fibers, which can be useful for the development of physical devices and sensors. Cetyltrimethylammonium-chloride-modified DNA molecules (CDNA) coated with metal ions through self-metallization exhibit enhanced optical and magnetic properties and thermal stability. In this paper, we present a simple synthesis route for Cu2+-coated CDNA hybrid fibers through ion exchange followed by self-metallization and analyze their structural and chemical composition (by X-ray diffraction (XRD), high-resolution field emission transmission electron microscopy (FETEM), and energy-dispersive X-ray spectroscopy (EDS)) and optical (by ultraviolet (UV)–visible absorption, Fourier transform infrared (FTIR), and X-ray photoelectron spectroscopies (XPS)), magnetic (by vibrating-sample magnetometry), and thermal (by a thermogravimetric analysis) characteristics. The XRD patterns, high-resolution FETEM images, and selected-area electron diffraction patterns confirmed the triclinic structure of Cu2+ in CDNA. The EDS results revealed the formation of Cu2+-coated CDNA fibers with a homogeneous distribution of Cu2+. The UV–vis, FTIR, and XPS spectra showed the electronic transition, interaction, and energy transfer between CDNA and Cu2+, respectively. The Cu2+-coated CDNA fibers exhibited a ferromagnetic nature owing to the presence of Cu2+. The magnetization of the Cu2+-coated CDNA fibers increased with the concentration of Cu2+ and decreased with the increase in temperature. Endothermic (absorbed heat) and exothermic (released heat) peaks in the differential thermal analysis curve were observed owing to the interaction of Cu2+ with the phosphate backbone.

Researchers have begun to use DNA molecules as an efficient template for arrangement of multiple functionalized nanomaterials for specific target applications. In this research, we demonstrated a simple process to co-dope synthetic DNA nanostructures (by a substrate-assisted growth method) and natural salmon DNA thin films (by a drop-casting method) with divalent metal ions (M2+, e.g., Co2+ and Cu2+) and trivalent lanthanide ions (Ln3+, e.g., Tb3+ and Eu3+). To identify the relationship among the DNA and dopant ions, DNA nanostructures were constructed while varying the Ln3+ concentration ([Ln3+]) at a fixed [M2+] with ion combinations of Co2+–Tb3+, Co2+–Eu3+, Cu2+–Tb3+, and Cu2+–Eu3+. Accordingly, we were able to estimate the critical [Ln3+] (named the optimum [Ln3+], [Ln3+]O) at a given [M2+] in the DNA nanostructures that corresponds to the phase change of the DNA nanostructures from crystalline to amorphous. The phase of the DNA nanostructures stayed crystalline up to [Tb3+]O ≡ 0.4 mM and [Eu3+]O ≡ 0.4 mM for Co2+ ([Tb3+]O ≡ 0.6 mM and [Eu3+]O ≡ 0.6 mM for Cu2+) and then changed to amorphous above 0.4 mM (0.6 mM). Consequently, phase diagrams of the four combinations of dopant ion pairs were created by analyzing the DNA lattice phases at given [M2+] and [Ln3+]. Interestingly, we observed extrema values of the measured physical quantities of DNA thin films near [Ln3+]O, where the maximum current, photoluminescence peak intensity, and minimum absorbance were obtained. M2+- and Ln3+-multidoped DNA nanostructures and DNA thin films may be utilized in the development of useful optoelectronic devices or sensors because of enhancement and contribution of multiple functionalities provided by M2+ and Ln3+.