Circular polarization sensitive opto-neuromorphic operation at plasmonic hot electron transistor using chiral gold nanoparticles.

Opto-neuromorphic operation is critical for biological system to recognize the visual objects and mimicking such operation is important for artificial prosthesis as well as machine vision system for industrial applications. To sophisticatedly mimic biological system, regulation of learning and memorizing efficiency is needed, however engineered synthetic platform has been lack of controllability, which makes huge gap between biological system and synthetic platform. Here we demonstrated controllable learning and memorizing opto-neuromorphic operation at plasmonic hot electron transistor. Especially, circularly polarized light (CPL) sensitive synaptic characteristics and learning experience capability are enabled by incorporating chiral plasmonic nanoparticle. Furthermore, gate voltage gives rise to controllable neuromorphic operation due to hot electron injection and trapping effect, resulting in high remaining synaptic weight of ∼70% at negative gate voltage under CPL excitation. We believe that this discovery makes significant leap toward on-demand in-sensor computing as well as toward bio-realistic device.

Neural-Network-Enabled Design of a Chiral Plasmonic Nanodimer for Target-Specific Chirality Sensing.

Quantitative analysis of chiral molecules in various solvents is essential. However, there are still many challenges to enhancing the sensitivity in precisely determining both concentration and chirality. Here, we built an algorithmic methodology to predict and optimally design the chiroptical response of chiral plasmonic sensors for a specific target chiral analyte with the aid of deep learning. Based upon the analytic and intuitive understanding of the Born-Kuhn type plasmonic nanodimer, we designed and trained the neural networks that can successfully predict the chiroptical properties and further inversely design the plasmonic structure to achieve the intended circular dichroism. The developed algorithm could identify the optimum structure exhibiting the maximum sensitivity for the given specific analytes. Surprisingly, we discovered that sensitivity strongly depends on the various conditions of analytes and can be finely tuned with the structural parameters of plasmonic nanodimers. We envision that this study can provide a general platform to develop ultrasensitive chiral plasmonic sensors whose structure and sensitivity have been evolved algorithmically for adoption in specific applications.

Magnetic Control of the Plasmonic Chirality in Gold Helicoids.

Chiral plasmonic nanostructures have facilitated a promising method for manipulating the polarization state of light. While a precise structural modification at the nanometer-scale-level could offer chiroptic responses at various wavelength ranges, a system that allows fast response control of a given structure has been required. In this study, we constructed uniformly arranged chiral gold helicoids with cobalt thin-film deposition that exhibited a strong chiroptic response with magnetic controllability. Tunable circular dichroism (CD) values from 0.9° to 1.5° at 550 nm wavelength were achieved by reversing the magnetic field direction. In addition, a magnetic circular dichroism (MCD) study revealed that the gap structure and size-related surface plasmon resonance induced MCD peaks. We demonstrated the transmitted color modulation, where the color dynamically changed from green-to-red, by controlling the field strength and polarizer axis. We believe current work broadens our understanding of magnetoplasmonic nanostructure and expands its potential applicability in optoelectronics or optical-communications.

Circularly polarized light-sensitive, hot electron transistor with chiral plasmonic nanoparticles.

The quantitative detection of circularly polarized light (CPL) is necessary in next-generation optical communication carrying high-density information and in phase-controlled displays exhibiting volumetric imaging. In the current technology, multiple pixels of different wavelengths and polarizers are required, inevitably resulting in high loss and low detection efficiency. Here, we demonstrate a highly efficient CPL-detecting transistor composed of chiral plasmonic nanoparticles with a high Khun's dissymmetry (g-factor) of 0.2 and a high mobility conducting oxide of InGaZnO. The device successfully distinguished the circular polarization state and displayed an unprecedented photoresponsivity of over 1 A/W under visible CPL excitation. This observation is mainly attributed to the hot electron generation in chiral plasmonic nanoparticles and to the effective collection of hot electrons in the oxide semiconducting transistor. Such characteristics further contribute to opto-neuromorphic operation and the artificial nervous system based on the device successfully performs image classification work. We anticipate that our strategy will aid in the rational design and fabrication of a high-performance CPL detector and opto-neuromorphic operation with a chiral plasmonic structure depending on the wavelength and circular polarization state.

Adenine oligomer directed synthesis of chiral gold nanoparticles.

Precise control of morphology and optical response of 3-dimensional chiral nanoparticles remain as a significant challenge. This work demonstrates chiral gold nanoparticle synthesis using single-stranded oligonucleotide as a chiral shape modifier. The homo-oligonucleotide composed of Adenine nucleobase specifically show a distinct chirality development with a dissymmetric factor up to g ~ 0.04 at visible wavelength, whereas other nucleobases show no development of chirality. The synthesized nanoparticle shows a counter-clockwise rotation of generated chiral arms with approximately 200 nm edge length. The molecular dynamics and density functional theory simulations reveal that Adenine shows the highest enantioselective interaction with Au(321)R/S facet in terms of binding orientation and affinity. This is attributed to the formation of sequence-specific intra-strand hydrogen bonding between nucleobases. We also found that different sequence programming of Adenine-and Cytosine-based oligomers result in chiral gold nanoparticles' morphological and optical change. These results extend our understanding of the biomolecule-directed synthesis of chiral gold nanoparticles to sequence programmable deoxyribonucleic acid and provides a foundation for programmable synthesis of chiral gold nanoparticles.

Ultrasensitive Near-Infrared Circularly Polarized Light Detection Using 3D Perovskite Embedded with Chiral Plasmonic Nanoparticles.

Chiral organic ligand-incorporated low-dimensional metal-halide perovskites have received increasing attention for next-generation photodetectors because of the direct detection capability of circularly polarized light (CPL), which overcomes the requirement for subsidiary optical components in conventional CPL photodetectors. However, most chiral perovskites have been based on low-dimensional structures that confine chiroptical responses to the ultraviolet (UV) or short-wavelength visible region and limit photocurrent due to their wide bandgap and poor charge transport. Here, chiroptical properties of 3D Cs0.05 FA0.5 MA0.45 Pb0.5 Sn0.5 I3 polycrystalline films are achieved by incorporating chiral plasmonic gold nanoparticles (AuNPs) into the mixed PbSn perovskite, without sacrificing its original optoelectronic properties. CPL detectors fabricated using chiral AuNP-embedded perovskite films can operate without external power input; they exhibit remarkable chirality in the near-infrared (NIR) region with a high anisotropy factor of responsivity (gres ) of 0.55, via giant plasmon resonance shift of chiral plasmonic AuNPs. In addition, a CPL detector array fabricated on a plastic substrate demonstrates highly sensitive self-powered NIR detection with superior flexibility and durability.

Revealing Structural Disorder in Hydrogenated Amorphous Silicon for a Low-Loss Photonic Platform at Visible Frequencies.

The high refractive index of hydrogenated amorphous silicon (a-Si:H) at optical frequencies is an essential property for the efficient modulation of the phase and amplitude of light. However, substantial optical loss represented by its high extinction coefficient prevents it from being utilized widely. Here, the bonding configurations of a-Si:H are investigated, in order to manipulate the extinction coefficient and produce a material that is competitive with conventional transparent materials, such as titanium dioxide and gallium nitride. This is achieved by controlling the hydrogenation and silicon disorder by adjusting the chemical deposition conditions. The extinction coefficient of the low-loss a-Si:H reaches a minimum of 0.082 at the wavelength of 450 nm, which is lower than that of crystalline silicon (0.13). Beam-steering metasurfaces are demonstrated to validate the low-loss optical properties, reaching measured efficiencies of 42%, 62%, and 75% at the wavelengths of 450, 532, and 635 nm, respectively. Considering its compatibility with mature complementary metal-oxide-semiconductor processes, the low-loss a-Si:H will provide a platform for efficient photonic operating in the full visible regime.

Tyrosyltyrosylcysteine-Directed Synthesis of Chiral Cobalt Oxide Nanoparticles and Peptide Conformation Analysis.

Chiral inorganic nanomaterials have revealed opportunities in various fields owing to their strong light-matter interactions. In particular, chiral metal oxide nanomaterials that can control light and biochemical reactions have been highlighted due to their catalytic activity and biocompatibility. In this study, we present the synthesis of chiral cobalt oxide nanoparticles with a g-factor of 0.01 in the UV-visible region using l- and d-Tyr-Tyr-Cys ligands. The conformation of the Tyr-Tyr-Cys peptide on the nanoparticle surfaces was identified by 2D NMR spectroscopy analysis. In addition, the sequence effect of Tyr-Tyr-Cys developing chiral nanoparticles was analyzed. The revealed peptide structure, along with the experimental results, demonstrate the important role of the thiol group and carboxyl group of the Tyr-Tyr-Cys ligand in chirality evolution. Importantly, due to the magnetic properties of chiral cobalt oxide nanoparticles and their strong absorption in the UV region, the circular dichroism (CD) responses can be dramatically modulated under an external magnetic field.

Synaptic transistors based on a tyrosine-rich peptide for neuromorphic computing.

In this article, we propose an artificial synaptic device based on a proton-conducting peptide material. By using the redox-active property of tyrosine, the Tyr-Tyr-Ala-Cys-Ala-Tyr-Tyr peptide film was utilized as a gate insulator that shows synaptic plasticity owing to the formation of proton electric double layers. The ion gating effects on the transfer characteristics and temporal current responses are shown. Further, timing-dependent responses, including paired-pulse facilitation, synaptic potentiation, and transition from short-term plasticity to long-term plasticity, have been demonstrated for the electrical emulation of biological synapses in the human brain. Herein, we provide a novel material platform that is bio-inspired and biocompatible for use in brain-mimetic electronic devices.

Proton-enabled activation of peptide materials for biological bimodal memory.

The process of memory and learning in biological systems is multimodal, as several kinds of input signals cooperatively determine the weight of information transfer and storage. This study describes a peptide-based platform of materials and devices that can control the coupled conduction of protons and electrons and thus create distinct regions of synapse-like performance depending on the proton activity. We utilized tyrosine-rich peptide-based films and generalized our principles by demonstrating both memristor and synaptic devices. Interestingly, even memristive behavior can be controlled by both voltage and humidity inputs, learning and forgetting process in the device can be initiated and terminated by protons alone in peptide films. We believe that this work can help to understand the mechanism of biological memory and lay a foundation to realize a brain-like device based on ions and electrons.

Quantitative analysis of the coupling between proton and electron transport in peptide/manganese oxide hybrid films.

Understanding how electrons and protons move in a coupled manner and affect one another is important to the design of proton-electron conductors and achieving biological transport in synthetic materials. In this study, a new methodology is proposed that allows for the quantification of the degree of coupling between electrons and protons in tyrosine-rich peptides and metal oxide hybrid films at room temperature under a voltage bias. This approach is developed according to the Onsager principle, which has been thoroughly established for the investigation of mixed ion-electron conductors with electron and oxide ion vacancies as carriers at high temperatures. Herein, a new device platform using electron-blocking electrodes provides a new strategy to investigate the coupling of protons and electrons in bulk materials beyond the molecular level investigation of coupled proton and electron transfer. Two Onsager transport parameters, αi* and σe', are obtained from the device, and the results of these transport parameters demonstrate that the coupled transport of electrons and protons inside the hybrid film plays an important role in the macroscopic-scale conduction. The results suggest that an average of one electron is dragged by one proton in the absence of a direct driving force for electron movement ∇ηe.

Optical properties of the crumpled pattern of selectively layered MoS2.

Crumple-structured two-dimensional MoS2 was evaluated as an essential element for future optoelectronic and stretchable devices owing to its interesting optical properties. This Letter reports the characteristics of the crumpled structure of MoS2 directly layered on a MoS2 sheet by chemical vapor deposition. The crumpling structure is presented as a method for selectively layering MoS2 with crumpled layered patterning and tunable optical properties as a crumpled structure on a single substrate. Optical analysis by the fast Fourier transform revealed the distribution characteristics of the crumple structure, and a Raman, photoluminescence, and optical absorption analysis confirmed the change in peak shift and intensity according to the degree of the crumpled structure. This material has potential future optoelectronic applications.

Physically Transient Field-Effect Transistors Based on Black Phosphorus.

Black phosphorus (BP) has shown great potential as a semiconductor material beyond graphene and MoS2 because of its intrinsic band gap and high mobility. Moreover, the biocompatibility of the final biodegradation products of BP has led to extensive research on biomedical applications. Herein, physically transient field-effect transistors (FETs) based on black phosphorus have been demonstrated using peptide insulator as a gate dielectric layer. The fabricated devices show high hole mobility up to 468 cm2 V-1 s-1 and on-off current ratio over 103. The combined use of black phosphorus, peptide, and molybdenum provides rapid disappearance of the devices within 36 h. Dissolution kinetics and cytotoxicity of black phosphorus are assessed to clarify its availability to be applied in transient electronics. This work provides transient FETs with high degradability and high performance based on biocompatible black phosphorus.

Effects of proton conduction on dielectric properties of peptides.

Peptides have been overlooked for their use in the field of electronics, even though they are one of the most commonly found bio-induced materials, and are not only easy to mass-produce but also exhibit a high dielectric constant. Additionally, unlike proteins, which are gaining considerable interest with materials researchers, peptides are much simpler, rendering their original characteristics easier to maintain without significant alteration of their structure. On the other hand, proteins tend to deform due to their susceptibility to environmental changes. Combining such superb dielectric properties with their relatively stable nature, peptides could be utilized as a component of electronic devices ranging from basic capacitors to more complex thin-film transistors. In this paper, a peptide chain (YYACAYY) composed of tyrosine, alanine, and cysteine was extensively studied using an impedance analyzer to determine its innate charge movement mechanism in order to extend our understanding of the electric properties of peptides. The movement of mobile protons inside the peptide insulator was found to be the source of the high relative permittivity of the peptide insulator, and the dielectric constant of the peptide insulator was found to be over 17 in humid conditions. By widening the understanding of the dielectric properties of the peptide insulator, it is expected that the peptide can be further utilized as an insulator in various electronic devices.

Influence of post-annealing on the off current of MoS2 field-effect transistors.

Two-dimensional materials have recently been spotlighted, due to their unique properties in comparison with conventional bulk and thin-film materials. Among those materials, MoS2 is one of the promising candidates for the active layer of electronic devices because it shows high electron mobility and pristine band gap. In this paper, we focus on the evolution of the electrical property of the MoS2 field-effect transistor (FET) as a function of post-annealing temperature. The results indicate that the off current drastically decreased at 200°C and increased at 400°C while other factors, such as the mobility and threshold voltage, show little variation. We consider that the decreasing off current comes from the rearrangement of the MoS2 film and the elimination of the surface residue. Then, the increasing off current was caused by the change of the material's composition and adsorption of H2O and O2.