Optoelectrical and mechanical properties of multiwall carbon nanotube-integrated DNA thin films.

Thin films made of deoxyribonucleic acid (DNA), dissolved in an aqueous solution, and cetyltrimethyl-ammonium-modified DNA (CDNA), dissolved in an organic solvent, utilising multiwall carbon nanotubes (MWCNTs) are not yet well-understood for use in optoelectronic device and sensor applications. In this study, we fabricate MWCNT-integrated DNA and CDNA thin films using the drop-casting method. We also characterise the optical properties (i.e. absorption spectra, Fourier-transform infrared spectra, Raman spectra, photoluminescence, and time-of-flight secondary ion mass spectrometry) to study spectral absorption, interaction, functional group, chirality, and compositional moiety and its distribution of MWCNTs in DNA and CDNA thin films. The electrical property for conductance and the mechanical characterisations of hardness, modulus and elasticity for stability are also discussed. Lastly, to show the feasibility of directional alignment of MWCNTs in DNA thin films, we perform an alignment experiment with MWCNTs in DNA via brushing and shearing methods, and we evaluate the results using polarised optical microscopy. Our simple methodology to align ingredients in DNA and CDNA thin films leveraging various optical, electrical and mechanical properties, provides great potential for the development of efficient devices and sensors.

The observation of resistive switching characteristics using transparent and biocompatible Cu2+-doped salmon DNA composite thin film.

For the potential switching bio-memory device application using DNA composite thin film, we fabricated and characterized the transparent and biocompatible resistive switching random access memory (RRAM) device within the structure stacking of Pt/Cu2+ doped salmon DNA/FTO, where Cu2+ doping into salmon DNA was solution-processed. The device shows good bipolar switching characteristics with SET and RESET processes at negative and positive sweeps, respectively, with switching memory window greater than 103 ratios. The device was observed to be in low resistance state as its pristine state and an initial RESET state was necessary to achieve programmable SET and RESET cycles. Based on the electrical characteristics of the Cu2+-doped salmon DNA-based RRAM device we propose a switching mechanism with the formation and rupture of conductive filaments due to the migration of Cu2+ during the electrical stress. Our understanding could contribute to the engineering of biomaterial memory switching medium for the environmentally benign, biocompatible and biodegradable memory storage devices.

Band gap, dielectric constant, and susceptibility of DNA layers as controlled by vanadium ion concentration.

Deoxyribonucleic acid (DNA) doped with transition metal ions shows great versatility for molecular-based biosensors and bioelectronics. Methodologies for developing DNA lattices (formed by synthetic double-crossover tiles) and DNA layers (used by natural salmon) doped with vanadium ions (V3+), as well as an understanding of the physical characteristics of V3+-doped DNA nanostructures, are essential in practical applications in interdisciplinary research fields. Here, DNA lattices and layers doped with V3+ are constructed through substrate-assisted growth and drop-casting methods. In addition, enhanced physical characteristics such as the band gap energy, work function, dielectric constant, and susceptibility of V3+-doped DNA nanostructures with varying V3+ concentration ([V 3+ ]) are investigated. The critical concentration ([V 3+ ]C ) at a given amount of DNA was predicted based on an analysis of the phase transition of DNA lattices from crystalline to amorphous with specific [V 3+ ]. Generally, the [V 3+ ]C provided crucial information on the structural stability and extremum physical characteristics of V3+-doped DNA nanostructures due to the optimum incorporation of V3+ into DNA. We obtained the optical absorption spectra for energy band gap estimation; Raman spectra for identifying the preferential coordination sites of V3+ in DNA; x-ray photoelectron spectra to examine the chemical state, chemical composition, and functional groups; and ultraviolet photoelectron spectra to estimate the work function. In addition, we addressed the electrical properties (i.e. current, capacitance, dielectric constant, and storage energy) and magnetic properties (magnetic field-dependent and temperature-dependent magnetizations and susceptibility) of DNA layers in the presence of V3+. The development of biocompatible materials with specific optical, electrical, and magnetic properties is required for future applications because they must have designated functionality, high efficiency, and affordability.

Magneto-optical and thermal characteristics of magnetite nanoparticle-embedded DNA and CTMA-DNA thin films.

Recently, DNA molecules embedded with magnetite (Fe3O4) nanoparticles (MNPs) drew much attention for their wide range of potential usage. With specific intrinsic properties such as low optical loss, high transparency, large band gap, high dielectric constant, potential for molecular recognition, and their biodegradable nature, the DNA molecule can serve as an effective template or scaffold for various functionalized nanomaterials. With the aid of cetyltrimethylammonium (CTMA) surfactant, DNA can be used in organic-based applications as well as water-based ones. Here, DNA and CTMA-DNA thin films with various concentrations of MNPs fabricated by the drop-casting method have been characterized by optical absorption, refractive index, Raman, and cathodoluminescence measurements to understand the binding, dispersion, chemical identification/functional modes, and energy transfer mechanisms, respectively. In addition, magnetization was measured as a function of either applied magnetic field or temperature in field cooling and zero field cooling. Saturation magnetization and blocking temperature demonstrate the importance of MNPs in DNA and CTMA-DNA thin films. Finally, we examine the thermal stabilities of MNP-embedded DNA and CTMA-DNA thin films through thermogravimetric analysis, derivative thermogravimetry, and differential thermal analysis. The unique optical, magnetic, and thermal characteristics of MNP-embedded DNA and CTMA-DNA thin films will prove important to fields such as spintronics, biomedicine, and function-embedded sensors and devices.

Charge Transport in 2D DNA Tunnel Junction Diodes.

Recently, deoxyribonucleic acid (DNA) is studied for electronics due to its intrinsic benefits such as its natural plenitude, biodegradability, biofunctionality, and low-cost. However, its applications are limited to passive components because of inherent insulating properties. In this report, a metal-insulator-metal tunnel diode with Au/DNA/NiOx junctions is presented. Through the self-aligning process of DNA molecules, a 2D DNA nanosheet is synthesized and used as a tunneling barrier, and semitransparent conducting oxide (NiOx ) is applied as a top electrode for resolving metal penetration issues. This molecular device successfully operates as a nonresonant tunneling diode, and temperature-variable current-voltage analysis proves that Fowler-Nordheim tunneling is a dominant conduction mechanism at the junctions. DNA-based tunneling devices appear to be promising prototypes for nanoelectronics using biomolecules.

Preparation of Eu3+ ions activated Ca2La8(SiO4)6O2 oxyapatite nanophosphors through two-step surfactant-free method and their optical and electrical properties.

Eu3+ ions activated Ca2La8(SiO4)6O2 (CLSO):Eu3+ nanophosphor samples were synthesized by a mixed solvothermal and hydrothermal method. The samples were carefully studied using various characterization techniques. The XRD patterns of CLSO:Eu3+ and CLSO confirmed that the samples were crystallized in hexagonal phase with a space group of P63/m (176). The morphology of the nanoparticles was studied by varying the reaction parameters such as growth, temperature and time. The photoluminescence (PL) excitation and PL emission spectra exhibited the typical Eu3+ bands in the wavelength range of 200-550 nm and 400-750 nm, respectively. The intensity of the [Formula: see text] electric dipole (ED) transition peak was strong in the PL emission spectrum which imparts the red color when observed under ultraviolet light. The ED transition peak intensity increased when the sample was calcined at an elevated temperature of 700 °C, indicating improved asymmetry ratio and good chromaticity coordinates. The electrical properties of the prepared materials were studied by spin-coating the powder dispersed solutions on the silica substrate. The output current values were also measured for the CLSO nanoparticles prepared under different growth conditions. These results showed the advantages of CLSO nanoparticles for their application in optics and feasibility in nanoelectronic and energy harvesting devices.

Electromagnetic and optical characteristics of Nb5+-doped double-crossover and salmon DNA thin films.

We report the fabrication and physical characteristics of niobium ion (Nb5+)-doped double-crossover DNA (DX-DNA) and salmon DNA (SDNA) thin films. Different concentrations of Nb5+ ([Nb5+]) are coordinated into the DNA molecules, and the thin films are fabricated via substrate-assisted growth (DX-DNA) and drop-casting (SDNA) on oxygen plasma treated substrates. We conducted atomic force microscopy to estimate the optimum concentration of Nb5+ ([Nb5+]O = 0.08 mM) in Nb5+-doped DX-DNA thin films, up to which the DX-DNA lattices maintain their structures without deformation. X-ray photoelectron spectroscopy (XPS) was performed to probe the chemical nature of the intercalated Nb5+ in the SDNA thin films. The change in peak intensities and the shift in binding energy were witnessed in XPS spectra to explicate the binding and charge transfer mechanisms between Nb5+ and SDNA molecules. UV-visible, Raman, and photoluminescence (PL) spectra were measured to determine the optical properties and thus investigate the binding modes, Nb5+ coordination sites in Nb5+-doped SDNA thin films, and energy transfer mechanisms, respectively. As [Nb5+] increases, the absorbance peak intensities monotonically increase until ∼[Nb5+]O and then decrease. However, from the Raman measurements, the peak intensities gradually decrease with an increase in [Nb5+] to reveal the binding mechanism and binding sites of metal ions in the SDNA molecules. From the PL, we observe the emission intensities to reduce them at up to ∼[Nb5+]O and then increase after that, expecting the energy transfer between the Nb5+ and SDNA molecules. The current-voltage measurement shows a significant increase in the current observed as [Nb5+] increases in the SDNA thin films when compared to that of pristine SDNA thin films. Finally, we investigate the temperature dependent magnetization in which the Nb5+-doped SDNA thin films reveal weak ferromagnetism due to the existence of tiny magnetic dipoles in the Nb5+-doped SDNA complex.

Phase, current, absorbance, and photoluminescence of double and triple metal ion-doped synthetic and salmon DNA thin films.

We fabricated synthetic double-crossover (DX) DNA lattices and natural salmon DNA (SDNA) thin films, doped with 3 combinations of double divalent metal ions (M2+)-doped groups (Co2+-Ni2+, Cu2+-Co2+, and Cu2+-Ni2+) and single combination of a triple M2+-doped group (Cu2+-Ni2+-Co2+) at various concentrations of M2+ ([M2+]). We evaluated the optimum concentration of M2+ ([M2+]O) (the phase of M2+-doped DX DNA lattices changed from crystalline (up to ([M2+]O) to amorphous (above [M2+]O)) and measured the current, absorbance, and photoluminescent characteristics of multiple M2+-doped SDNA thin films. Phase transitions (visualized in phase diagrams theoretically as well as experimentally) from crystalline to amorphous for double (Co2+-Ni2+, Cu2+-Co2+, and Cu2+-Ni2+) and triple (Cu2+-Ni2+-Co2+) dopings occurred between 0.8 mM and 1.0 mM of Ni2+ at a fixed 0.5 mM of Co2+, between 0.6 mM and 0.8 mM of Co2+ at a fixed 3.0 mM of Cu2+, between 0.6 mM and 0.8 mM of Ni2+ at a fixed 3.0 mM of Cu2+, and between 0.6 mM and 0.8 mM of Co2+ at fixed 2.0 mM of Cu2+ and 0.8 mM of Ni2+, respectively. The overall behavior of the current and photoluminescence showed increments as increasing [M2+] up to [M2+]O, then decrements with further increasing [M2+]. On the other hand, absorbance at 260 nm showed the opposite behavior. Multiple M2+-doped DNA thin films can be used in specific devices and sensors with enhanced optoelectric characteristics and tunable multi-functionalities.

Growth and Detachment of 5 Helix DNA Ribbons.

We report on the concentration-dependent surface-assisted growth and time-temperature-dependent detachment of one-dimensional 5 helix DNA ribbons (5HR) on a mica substrate. The growth coverage ratio was determined by varying the concentration of the 5HR strands in a test tube, and the detachment rate of 5HR on mica was determined by varying the incubation time at a fixed temperature on a heat block. The topological changes in the concentration-dependent attachment and the time-temperature-dependent detachment for 5HR on mica were observed via atomic force microscopy. The observations indicate that 5HR started to grow on mica at ~10 nM and provided full coverage at ~50 nM. In contrast, 5HR at 65 °C started to detach from mica after 5 min and was completely removed after 10 min. The growth and detachment coverage show a sinusoidal variation in the growth ratio and a linear variation with a rate of detachment of 20%/min, respectively. The physical parameters that control the stability of the DNA structures on a given substrate should be studied to successfully integrate DNA structures for physical and chemical applications.

Broadband supercontinuum generation using a hollow optical fiber filled with copper-ion-modified DNA.

We experimentally demonstrated supercontinuum generation through a hollow core photonic bandgap fiber (HC-PBGF) filled with DNA nanocrystals modified by copper ions in a solution. Both double-crossover nano DNA structure and copper-ion-modified structure provided a sufficiently high optical nonlinearity within a short length of hollow optical fiber. Adding a higher concentration of copper ion into the DNA nanocrystals, the bandwidth of supercontinuum output was monotonically increased. Finally, we achieved the bandwidth expansion of about 1000 nm to be sufficient for broadband multi-spectrum applications.

Construction and characterization of Cu²âº, Ni²âº, Zn²âº, and Co²âº modified-DNA crystals.

We studied the physical characteristics of modified-DNA (M-DNA) double crossover crystals fabricated via substrate-assisted growth with various concentrations of four different divalent metallic ions, Cu(2+), Ni(2+), Zn(2+), and Co(2+). Atomic force microscopy (AFM) was used to test the stability of the M-DNA crystals with different metal ion concentrations. The AFM images show that M-DNA crystals formed without deformation at up to the critical concentrations of 6 mM of [Cu(2+)], 1.5 mM of [Ni(2+)], 1 mM of [Zn(2+)], and 1 mM of [Co(2+)]. Above these critical concentrations, the M-DNA crystals exhibited deformed, amorphous structures. Raman spectroscopy was then used to identify the preference of the metal ion coordinate sites. The intensities of the Raman bands gradually decreased as the concentration of the metal ions increased, and when the metal ion concentrations increased beyond the critical values, the Raman band of the amorphous M-DNA was significantly suppressed. The metal ions had a preferential binding order in the DNA molecules with G-C and A-T base pairs followed by the phosphate backbone. A two-probe station was used to measure the electrical current-voltage properties of the crystals which indicated that the maximum currents of the M-DNA complexes could be achieved at around the critical concentration of each ion. We expect that the functionalized ion-doped M-DNA crystals will allow for efficient devices and sensors to be fabricated in the near future.

Ternary and senary representations using DNA double-crossover tiles.

The information capacity of DNA double-crossover (DX) tiles was successfully increased beyond a binary representation to higher base representations. By controlling the length and the position of DNA hairpins on the DX tile, ternary and senary (base-3 and base-6) digit representations were realized and verified by atomic force microscopy. Also, normal mode analysis was carried out to study the mechanical characteristics of each structure.

White light emission produced by CTMA-DNA nanolayers embedded with a mixture of organic light-emitting molecules.

Researchers have started to recognize that biomaterial-based devices and sensors can be used in the development of high-performing environmentally-friendly technologies. In this regard, DNA can be utilized as a competent scaffold for hosting functional nanomaterials to develop a designated platform in the field of bionanotechnology. Here, we introduce a novel methodology to construct CTMA-modified DNA nanolayers (CDNA NLs) embedded with single (e.g., red, green, and blue), double (violet, yellow, and orange), and triple (white) iridium-based organic light-emitting materials (OLEMs, including Ir(piq)2(acac) for red, Ir(ppy)2(acac) for green, FIrpic for blue) that can serve as active light-emitting layers. The OLEM-embedded CDNA NLs were fabricated using simple solution processes, and their spectral properties were investigated via Fourier-transform infrared (FTIR), X-ray photoelectron (XPS), UV-Vis, and photoluminescence (PL) spectroscopies. FTIR analysis of OLEM-embedded CDNA NLs suggested that the complexes are stable and chemically inert. XPS revealed the various modes of interaction between OLEMs and CDNA. The evidence of interactions between blue OLEM and CDNA was demonstrated by peak shifts. The wide band gap characteristics (∼4.76 eV) and relatively high optical quality (no absorption in the visible region) of OLEM-embedded CDNA NLs were observed in UV-Vis absorption measurements. We observed PL emission in OLEM-embedded CDNA NLs, which was caused by the energy transfer from CDNA to OLEMs (ligand-centered and metal to ligand charge transfer). Lastly, a white light-emitting OLEM-embedded CDNA thin film was constructed using a combination of appropriate concentrations of red, green, and blue OLEMs. Its characteristic was demonstrated through spectral measurements. In addition, colour coordinates were plotted in the International Commission on Illumination (CIE) colour space, which confirmed the colour identity for the developed colours (including white). Consequently, the OLEM-embedded CDNA NLs can likely be used as a functional material in bio-imaging and bio-photonics.

DNA Multilayers with Mono-, Hetero-, and Mixed-Type Plasmonic Nanoparticles for Broadband Absorption and Energy Storage.

DNA incorporated with functional materials has led to development of hybrids with different functionalities. Among the functional materials, metal nanoparticles such as Au, Ag, and Cu (also known as plasmonic nanoparticles [PNPs]), which can exhibit surface plasmon resonance, are good candidates to fabricate useful optoelectronic devices and sensors. Here, we constructed PNP-assorted DNA (PNP-DNA) layers with mono-, hetero-, and mixed-type PNPs formed by successive spin-coating to obtain the required number of layers. Further, structural analysis of PNP-DNA was performed by scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The optical evaluation was carried out by Raman, UV-visible, and photoluminescence (PL) spectroscopies followed by measurement of capacitance. Cross-sectional SEM images of DNA single, DNA triple, and PNP-DNA triple layers indicated their thicknesses (i.e., 90, 280, and 395 nm, respectively), while the base pair distance of double helixes (∼0.4 nm) for the PNP-DNA multilayers was measured by XRD. The presence of Ag, Au, and Cu PNPs was confirmed by existence of spin-orbit coupling in the corresponding XPS spectra. The addition of PNPs in DNA multilayers caused significant enhancement in the intensities of Raman bands (especially in the range of 1200-1850 cm-1) due to Raman resonance. UV-vis absorption and PL demonstrated stacking-order-dependent and layer-dependent light absorption and energy transfer (observed as quenching of fluorescence between PNPs and DNA), respectively. We observed n-type semiconducting behavior with a relatively higher dielectric constant for a PNP-assorted DNA single layer at a low frequency of 5 kHz. The dielectric constants of all samples decreased exponentially with increased frequency. Upon addition of PNPs, enhancement in the dielectric constant as well as capacitance was noted. Consequently, the simple fabrication method used in this study can be adopted to construct various nanomaterial-assorted DNA multilayers whose specific functionalities may be controlled with high efficiency.

Large-Scale Fabrication of Copper-Ion-Coated Deoxyribonucleic Acid Hybrid Fibers by Ion Exchange and Self-Metallization.

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.

Metal and Lanthanide Ion-Co-doped Synthetic and Salmon DNA Thin Films.

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+.

DNA nanostructures doped with lanthanide ions for highly sensitive UV photodetectors.

Deoxyribonucleic acid (DNA) and lanthanide ions (Ln3+) exhibit exceptional optical properties that are applicable to the development of nanoscale devices and sensors. Although DNA nanostructures and Ln3+ ions have been investigated for use in the current state of technology for more than a few decades, researchers have yet to develop DNA and Ln3+ based ultra-violet (UV) photodetectors. Here, we fabricate Ln3+ (such as holmium (Ho3+), praseodymium (Pr3+), and ytterbium (Yb3+))‒doped double crossover (DX)‒DNA lattices through substrate-assisted growth and salmon DNA (SDNA) thin films via a simple drop-casting method on oxygen (O2) plasma-treated substrates for high performance UV photodetectors. Topological (AFM), optical (UV-vis absorption and FTIR), spectroscopic (XPS), and electrical (I‒V and photovoltage) measurements of the DX‒DNA and SDNA thin films doped with various concentrations of Ln3+ ([Ln3+]) are explored. From the AFM analysis, the optimum concentrations of various Ln3+ ([Ln3+]O) are estimated (where the phase transition of Ln3+‒doped DX‒DNA lattices takes place from crystalline to amorphous) as 1.2 mM for Ho3+, 1.5 mM for Pr3+, and 1.5 mM for Yb3+. The binding modes and chemical states are evaluated through optical and spectroscopic analysis. From UV-vis absorption studies, we found that as the [Ln3+] was increased, the absorption intensity decreased up to [Ln3+]O, and increased above [Ln3+]O. The variation in FTIR peak intensities in the nucleobase and phosphate regions, and the changes in XPS peak intensities and peak positions detected in the N 1 s and P 2p core spectra of Ln3+‒doped SDNA thin films clearly indicate that the Ln3+ ions are properly bound between the bases (through chemical intercalation) and to the phosphate backbone (through electrostatic interactions) of the DNA molecules. Finally, the I‒V characteristics and time-dependent photovoltage of Ln3+‒doped SDNA thin films are measured both in the dark and under UV LED illuminations (λLED = 382 nm) at various illumination powers. The photocurrent and photovoltage of Ln3+‒doped SDNA thin films are enhanced up to the [Ln3+]O compared to pristine SDNA due to the charge carriers generated from both SDNA and Ln3+ ions upon the absorption of light. From our observations, the photovoltages as function of illumination power suggest higher responsivities, and the photovoltages as function of time are almost constant which indicates the stability and retention characteristics of the Ln3+‒doped SDNA thin films. Hence, our method which provides an efficient doping of Ln3+ into the SDNA with a simple fabrication process might be useful in the development of high-performance optoelectronic devices and sensors.

High performance UV photodetectors using Nd3+ and Er3+ single- and co-doped DNA thin films.

Even though lanthanide ion (Ln3+)-doped DNA nanostructures have been utilized in various applications, they are rarely employed for photovoltage generating devices because of difficulties in designing DNA-based devices that generate voltages under light illumination. Here, we constructed DNA lattices made of synthetic strands and DNA thin films extracted from salmon (SDNA) with single-doping of Nd3+ or Er3+ and co-doping of Nd3+/Er3+ for high performance UV detection. The topological change of the DNA double-crossover (DX) lattices during the course of annealing was estimated from atomic force microscope (AFM) images to find the optimum concentration of Ln3+ ([Ln3+]O). No topological disturbance in DNA DX lattices were observed up to [Ln3+]O, and significant enhancement in the physical properties was obtained at [Ln3+]O. The interactions between Ln3+ and SDNA were examined using spectroscopic methods of UV-visible, Raman, and X-ray photoelectron spectroscopy (XPS). Current and photovoltage measurements for Ln3+-doped SDNA thin films under UV illumination with varying power intensities were conducted. Under UV illumination, the photocurrent and photovoltage of Ln3+-doped SDNA thin films increased with increasing applied external voltages and input power intensities, respectively. In addition, we observed considerable increases in photovoltage responses, i.e., 5-fold increase for Nd3+, 10-fold for Er3+, and 13-fold for Nd3+/ Er3+, compared to the pristine SDNA due to the additional charge carriers generated in Ln3+-doped SDNA thin films. Device performance was measured in terms of photovoltage responsivity and retention characteristics. These phenomena indicate the high stability and substantial endurance characteristics of Ln3+-doped SDNA thin films.

A Neuromorphic Device Implemented on a Salmon-DNA Electrolyte and its Application to Artificial Neural Networks.

A bioinspired neuromorphic device operating as synapse and neuron simultaneously, which is fabricated on an electrolyte based on Cu2+-doped salmon deoxyribonucleic acid (S-DNA) is reported. Owing to the slow Cu2+ diffusion through the base pairing sites in the S-DNA electrolyte, the synaptic operation of the S-DNA device features special long-term plasticity with negative and positive nonlinearity values for potentiation and depression (αp and αd), respectively, which consequently improves the learning/recognition efficiency of S-DNA-based neural networks. Furthermore, the representative neuronal operation, "integrate-and-fire," is successfully emulated in this device by adjusting the duration time of the input voltage stimulus. In particular, by applying a Cu2+ doping technique to the S-DNA neuromorphic device, the characteristics for synaptic weight updating are enhanced (|αp|: 31→20, |αd|: 11→18, weight update margin: 33→287 nS) and also the threshold conditions for neuronal firing (amplitude and number of stimulus pulses) are modulated. The improved synaptic characteristics consequently increase the Modified National Institute of Standards and Technology (MNIST) pattern recognition rate from 38% to 44% (single-layer perceptron model) and from 89.42% to 91.61% (multilayer perceptron model). This neuromorphic device technology based on S-DNA is expected to contribute to the successful implementation of a future neuromorphic system that simultaneously satisfies high integration density and remarkable recognition accuracy.

Topological, chemical and electro-optical characteristics of riboflavin-doped artificial and natural DNA thin films.

DNA is considered as a useful building bio-material, and it serves as an efficient template to align functionalized nanomaterials. Riboflavin (RF)-doped synthetic double-crossover DNA (DX-DNA) lattices and natural salmon DNA (SDNA) thin films were constructed using substrate-assisted growth and drop-casting methods, respectively, and their topological, chemical and electro-optical characteristics were evaluated. The critical doping concentrations of RF ([RF]C, approx. 5 mM) at given concentrations of DX-DNA and SDNA were obtained by observing the phase transition (from crystalline to amorphous structures) of DX-DNA and precipitation of SDNA in solution above [RF]C. [RF]C are verified by analysing the atomic force microscopy images for DX-DNA and current, absorbance and photoluminescence (PL) for SDNA. We study the physical characteristics of RF-embedded SDNA thin films, using the Fourier transform infrared spectrum to understand the interaction between the RF and DNA molecules, current to evaluate the conductance, absorption to understand the RF binding to the DNA and PL to analyse the energy transfer between the RF and DNA. The current and UV absorption band of SDNA thin films decrease up to [RF]C followed by an increase above [RF]C. By contrast, the PL intensity illustrates the reverse trend, as compared to the current and UV absorption behaviour as a function of the varying [RF]. Owing to the intense PL characteristic of RF, the DNA lattices and thin films with RF might offer immense potential to develop efficient bio-sensors and useful bio-photonic devices.