Optoelectronic Devices Research Articles

Near-Infrared Absorbing Aza-BODIPY Dyes for Optoelectronic Applications.

Organic dyes that absorb light in the visible to near-infrared region have garnered significant interest, owing to their extensive utility in organic photovoltaics and various biomedical applications. Aza-boron-dipyrromethene (Aza-BODIPY) dyes are a class of chromophores with impressive photophysical properties such as tunable absorption from the visible region towards near infrared (NIR) region, high molar absorptivity, and fluorescence quantum yield. In this review, we discuss the developments in the aza-BODIPYs, related to their synthetic routes, photophysical properties and their applications. Their design strategies, modifications in chemical structures, mode/position of attachment, and their impact on photo-physical properties are reviewed. The potential applications of aza-BODIPY derivatives such as organic solar cells, photodynamic therapy, boron-neutron capture therapy, fluorescence sensors, photo-redox catalysis, photoacoustic probes and optoelectronic devices are explained.

Doctor Blade Casting of Thin Films Containing Different Concentrated Endemic Plant Extracts: Determination of Structure and Optical Properties

This study provides a thorough properties of the optical analysis of the thin films which produced from Astragalus tokatensis Fisch., Helichrysum noeanum Boiss. and Stachys huber-morathii R. Bhattacharjee extracts. Methanol extracts of plants were obtained via Soxhlet extractor. The highest extract yield (10.10%) was determined in H. noeanum. Doctor blade coating method is used to make thin film layer on glass substrate. The optical behavior of the deposited films is tested by means of he UV-vis-near IR absorbance and transmittance characterization. It is found that the maximum transmittance spectra reaches nearly to a value of 90 % for A. tokatensis sample. Significantly, all the samples display same optical absorbace spectra behavior. Energy band gaps of the films are presented based on Tauc relation and were found to be in the range between 3.68-3.81 eV. Besides, the analysis of functional groups available in the materials is broadly studied by Fourier transform infrared (FT-IR) spectroscopy. FT-IR measurement also confirms that all produced films have carbohydrate pattern. These findings demonstrate a cost-efficient approach for the production of thin films with plant extraction, and open a new perspective on the potential applications of optoelectronic devices.

Modification of PEDOT:PSS thin film properties using pyridine-based solid additive for optoelectronic applications

Poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) is one of the most promising hole transport layers that is widely used in high-performance optoelectronic devices. However, the hygroscopic nature and acidity of PEDOT:PSS is known to cause degradation in devices and decrease their performance. In this study, a new pyridine solid additive, 2,3-dihydropyridine (2,3-DHP) was incorporated into the PEDOT:PSS solution to improve its characteristics. A low-temperature solution-based spin-coating device was utilized to produce the thin films. From the results, the PEDOT:PSS@2,3-DHP (1 wt%) exhibited excellent optical characteristics. It also provided informative and controlled morphology when it was annealed at 100 °C, suggesting that PEDOT:PSS@2,3-DHP has a potential advantage in photovoltaic (PV) devices. Moreover, in the photodetection experiment utilizing LED of 380 nm, PEDOT:PSS@2,3-DHP showed a higher photocurrent response when compared with pristine PEDOT:PSS. It also significantly reduced sheet resistance and achieved superior electrical conductivity. Interaction between the 2,3-DHP, PEDOT, and PSS chains altered the mechanical properties of the PEDOT:PSS, leading to the modification in structural and electrical characteristics. Overall, these findings highlight the importance and applicability of PEDOT:PSS@2,3-DHP in a wide range of optoelectronic devices.

Arylazopyrazole-modulated stable dual-mode phototransistors.

High-performance organic devices with dynamic and stable modulation are essential for building devices adaptable to the environment. However, the existing reported devices incorporating light-activated units exhibit either limited device stability or subpar optoelectronic properties. Here, we synthesize a new optically tunable polymer dielectric functionalized with photochromic arylazopyrazole units with a cis-isomer half-life of as long as 90 days. On this basis, stable dual-mode organic transistors that can be reversibly modulated are successfully fabricated. The trans-state devices exhibit high carrier mobility reaching 7.4 square centimeters per volt per second and excellent optical figures of merit, whereas the cis-state devices demonstrate stable but starkly different optoelectronic performance. Furthermore, optical image sensors are prepared with regulatable nonvolatile memories from 36 hours (cis state) to 108 hours (trans state). The achievement of dynamic light modulation shows remarkable prospects for the intelligent application of organic optoelectronic devices.

Screening of Functional Small Molecules via Modified Machine Learning Strategy toward Efficient All-Inorganic Perovskite Solar Cells.

Organic small molecules are proven to be capable of passivating the bulk/interfacial defects in inorganic perovskite solar cells. Considering the burdensome situation to screen the functional small molecules, we employ a modified machine learning (ML) strategy to guide screening suitable small molecules toward efficient solar cells through three modified ML algorithms to construct the prediction model: (i) random forest algorithm (RF), (ii) support vector machine algorithm (SVR), and (iii) XGBoost. Among them, the XGBoost algorithm displays a better overall predictive performance, whereby the R2 index reaches 0.939. Accordingly, eight small molecules are selected to modify the interface of perovskite films, and both the theoretical and experimental results certify that the difluorobenzylamine with additional fluorine atoms has a better interface modification effect among the small molecules containing functional groups, e.g., the benzene ring and amino group. The high accuracy of the modified machine learning model enables us to simplify the small-molecule screening process and form an important step for ongoing developments in perovskite solar cells and other optoelectronic devices.

Ultranarrow Deep-Blue Luminescence of Perovskite Nanocrystals by A-Site Cation Control.

Metal-halide perovskite nanocrystals (NCs) are one of the most promising emitters for the application of display and nanolight sources. The full width at half-maximum (FWHM) of photoluminescence (PL) emission is essential for color purity, which however remains a difficulty to further reduce the FWHM of the perovskite NCs at room temperature. Here, we show the quasi-sphere perovskite NCs with narrow PL emission at a deep-blue wavelength of ∼430 nm; its PL FWHM reaches ∼11 nm at room temperature, owing to the monodispersion in size distribution as well as the symmetric quasi-sphere morphology of NCs releasing the fine structure splitting-induced inhomogeneous broadening. Through regulating A cations with respect to the ratio of FA (or MA)-to-Cs and Cs-to-Pb, the PL emission of the NCs could be tuned from ∼505 to ∼430 nm combined with varied morphologies from large cube to small quasi-sphere. Such spectroscopic and morphological discrepancies are supposed to be attributed to the different crystalline kinetics that is strongly dependent on the synthetic condition. To be specific, in the case of increasing FA (or MA)-to-Cs, the growth rate of CsPbBr3 and FAPbBr3 (or MAPbBr3) perovskites is determined by the reactivity of transient species, while in the case of decreasing the Cs-to-Pb ratio, the growth rate of perovskites is slowed down by the serious reduction of Cs+ in the precursor. This study provides an effective strategy to adjust the emission across from green to deep-blue color and promotes the perovskite NCs with a narrow FWHM, and tunable PL emission facilitates in application of optoelectronic devices.

Dual-Adaptive Heterojunction Synaptic Transistors for Efficient Machine Vision in Harsh Lighting Conditions.

Photoadaptive synaptic devices enable in-sensor processing of complex illumination scenes, while second-order adaptive synaptic plasticity improves learning efficiency by modifying the learning rate in a given environment. The integration of above adaptations in one phototransistor device will provide opportunities for developing high-efficient machine vision system. Here, a dually adaptable organic heterojunction transistor as a working unit in the system, which facilitates precise contrast enhancement and improves convergence rate under harsh lighting conditions, is reported. The photoadaptive threshold sliding originates from the bidirectional photoconductivity caused by the light intensity-dependent photogating effect. Metaplasticity is successfully implemented owing to the combination of ambipolar behavior and charge trapping effect. By utilizing the transistor array in a machine vision system, the details and edges can be highlighted in the 0.4% low-contrast images, and a high recognition accuracy of 93.8% with a significantly promoted convergence rate by about 5 times are also achieved. These results open a strategy to fully implement metaplasticity in optoelectronic devices and suggest their vision processing applications in complex lighting scenes.

Highly Stable Silver Nanowire Plasmonic Electrodes for Flexible Polymer Light-Emitting Devices.

Silver nanowire (AgNW) transparent electrodes are considered as a promising candidate for applications in flexible optoelectronic devices. However, it remains a great challenge to obtain flexible AgNW electrodes with excellent optoelectrical properties and mechanical flexibility. Here, highly stable Ag nanoparticle (AgNP)-enhanced plasmonic AgNW electrodes are demonstrated via the controllable in situ growth of AgNPs at the AgNW junctions and introduction of an l-histidine (l-His) wrapping layer. The flexible transparent electrodes of AgNW-AgNP/l-His possess a low sheet resistance (Rsh) of ∼17.5 Ω sq-1, a high transmittance of ∼92.5% (550 nm), and a robust mechanical stability (100,000 bending cycles). Benefiting from plasmon-coupling effects, flexible polymer light-emitting devices (FPLEDs) with AgNW-AgNP/l-His electrodes present a current efficiency (CE) of ∼14.8 cd A-1 and an external quantum efficiency (EQE) of ∼5.6%, constituting ∼80% and ∼75% increases compared to those of the reference devices with AgNW electrodes, respectively. Additionally, the laminated flexible transparent PLEDs (FT-PLEDs) are demonstrated by integrating polydimethylsiloxane/AgNW-AgNP anodes by a soft lamination process. The FT-PLEDs present a CE of ∼7.1 cd A-1 (cathode side: ∼3.9 cd A-1; anode side: ∼3.2 cd A-1) and an EQE of ∼2.7% (cathode side: ∼1.5%; anode side: ∼1.2%). Furthermore, the FPLEDs and FT-PLEDs exhibit robust mechanical durability, maintaining ∼89% and ∼86% of their initial luminance after 1000 bending cycles at a bending radius of 2 mm, respectively. This work opens up a new avenue for the development of high performance and stable flexible optoelectronic devices.

New-Style Logic Operation and Neuromorphic Computing Enabled by Optoelectronic Artificial Synapses in an MXene/Y:HfO2 Ferroelectric Memristor.

Today's computing systems, to meet the enormous demands of information processing, have driven the development of brain-inspired neuromorphic systems. However, there are relatively few optoelectronic devices in most brain-inspired neuromorphic systems that can simultaneously regulate the conductivity through both optical and electrical signals. In this work, the Au/MXene/Y:HfO2/FTO ferroelectric memristor as an optoelectronic artificial synaptic device exhibited both digital and analog resistance switching (RS) behaviors under different voltages with a good switching ratio (>103). Under optoelectronic conditions, optimal weight update parameters and an enhanced algorithm achieved 97.1% recognition accuracy in convolutional neural networks. A new logic gate circuit specifically designed for optoelectronic inputs was established. Furthermore, the device integrates the impact of relative humidity to develop an innovative three-person voting mechanism with a veto power. These results provide a feasible approach for integrating optoelectronic artificial synapses with logic-based computing devices.

Optical and dielectric features of PVC/ZnCo2O4/MWCNTs/TBAI polymers for optoelectronic and energy storage applications

Zinc cobalt oxide is considered a highly desirable substance for use in a wide range of applications, particularly supercapacitors. In this study, polyvinyl chloride/zinc cobalt oxide/multi-walled carbon nanotubes/x wt % tetrabutylammonium iodide (PVC/ZnCo2O4/MWCNTs/x wt % TBAI) composite polymers were fabricated using casting and hydrothermal approaches. The resulting composites were then analyzed to determine their structure, optical properties, and dielectric characteristics. The structure of ZnCo2O4 and PVC/ZnCo2O4/MWCNTs/x wt.% TBAI were studied using the X-ray diffraction technique. The morphologies of doped polymer were investigated using SEM technique. The impact of ZnCo2O4/MWCNTs/x wt.% TBAI filler samples on the linear and nonlinear optical properties of PVC polymer has been analyzed through UV diffused reflectance measurements. The doped samples could serve as effective shields against ultraviolet radiation across different wavelengths (UVA, UVB, UVC) and a highly effective material for absorbing solar energy in solar cells. The lowest optical energy gap values are attained (3.77, 3.03) and (3.32, 2.55) eV for the direct and indirect optical band gaps in PVC/ZnCo2O4/MWCNTs/3 wt% TBAI polymer, respectively. The largest refractive index value at 600 nm was observed in the doped polymer with 6 wt% TBAI. The fluorescence emission spectra and dielectric properties of the PVC/ZnCo2O4/MWCNTs/x wt.% TBAI polymers are also studied. The highest electrical dielectric constant was achieved in the ZnCo2O4/MWCNTs/9 wt% TBAI polymer. It follows that the PVC/ZnCo2O4/MWCNTs/x wt % TBAI has the ability to open up new possibilities for use in optoelectronic devices.

Modulating the Structure and Optoelectronic Properties of Solution-Processed Bismuth-Based Nanocrystals.

Bismuth-based chalcogenides have emerged as promising candidates for next-generation, solution-processable semiconductors, mainly benefiting from their facile fabrication, low cost, excellent stability, and tunable optoelectronic properties. Particularly, the recently developed AgBiS2 solar cells have shown striking power conversion efficiencies. High performance bismuth-based photodetectors have also been extensively studied in the past few years. However, the fundamental properties of these Bi-based semiconductors have not been sufficiently investigated, which is crucial for further improving the device performance. Here, we introduce multiple time-resolved and steady-state techniques to fully characterize the charge carrier dynamics and charge transport of solution-processed Bi-based nanocrystals. It was found that the Ag-Bi ratio plays a critical role in charge transport. For Ag-deficient samples, silver bismuth sulfide thin films behave as localized state induced hopping charge transport, and the Ag-excess samples present band-like charge transport. This finding is crucial for developing more efficient Bi-based semiconductors and optoelectronic devices.

Enhancement of electrical properties by CuS–PVP nanocomposite on the ZnO/polymer heterojunction

AbstractA nanocomposite matrix of covellite–polyvinylpyrrolidone (CuS–PVP) was synthesized through a solution processing method and applied via spin coating onto hydrothermally grown zinc oxide (ZnO) nanorods. Characterization techniques, including X‐ray powder diffraction and scanning electron microscopy, confirmed the successful decoration of chain‐like CuS–PVP polymer composites onto hexagonal ZnO nanorods. The UV‐vis spectroscopy revealed an absorption peak at 372 nm, indicating excitonic absorption of ZnO, and a reduction in the band gap from 3.11 to 2.59 eV upon CuS–PVP polymer decoration, enhancing light harvesting efficiency. Photoluminescence spectra demonstrated the lowest charge carrier recombination rate in the ZnO/CuS–PVP sample, promoting efficient charge separation and transportation, supported by Fourier‐transform infrared analysis indicating chemical bonding. Subsequently, the impact of CuS–PVP as an insertion layer in the ZnO/poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) inorganic–organic heterojunction was investigated. Favorable band alignment between ZnO, CuS–PVP, and PEDOT:PSS improved conduction, increasing current from 0.3394 to 1.14 mA for D2 (poly‐ethyleneterephthalate/Indium tin oxide/ZnO/PEDOT:PSS/Al) and D1 (poly‐ethyleneterephthalate/Indium tin oxide/ZnO/CuS–PVP/PEDOT:PSS/Al) at a +2 V bias. Transient photo‐responses (J–t) at 0 V bias revealed decreased rise and fall times from 0.382 and 1.154 s to 0.301 and 0.229 s for D2 and D1 devices, respectively. This novel approach provides control over charge carrier transport characteristics at the interface, potentially benefiting self‐powered photo‐detection in optoelectronic devices.

High‐Efficiency Luminescent Solar Concentrators Based on Carbon Dots with Simultaneously Ultrabright Solid‐State and Liquid‐State Luminescence

AbstractCarbon dots (CDs) are ideal fluorophores for optoelectronic devices. However, it is still a great challenge to obtain CDs with high solid‐state photoluminescence quantum yields (PLQYs). In this work, it is first reported that the barium‐doped CDs (Ba‐CDs), which can be simply synthesized on a large scale via a direct one‐step heating approach using an open vessel. The as‐synthesized Ba‐CDs exhibit ultrabright luminescence both in liquid and solid states. The as‐synthesized Ba‐CDs with a scale of 8.6 g per batch show a Stokes shift of ≈0.68 eV and high PLQYs of 80.8% and 66.8% in liquid and solid state, respectively. Interestingly, an efficient fluorescence enhancement phenomenon occurs when Ba‐CDs are mixed with polyvinylpyrrolidone (PVP), which reveals the critical issue of compatibility between CDs and polymer matrix can be well resolved. As a proof‐of‐concept, the Ba‐CDs are employed as fluorophores for high‐efficiency luminescent solar concentrator (LSC) fabrication. The Ba‐CDs@PVP‐based LSC has a PLQY of 88.78%, showing a breakthrough optical conversion efficiency of 7.16% and power conversion efficiency of 6.87% under natural light irradiation (40 mW cm−2). The results demonstrate the potential application of the ultrabright Ba‐CDs in efficient photovoltaic devices.

Insight into Interfacial Heat Transfer of β-Ga2O3/Diamond Heterostructures via the Machine Learning Potential.

β-Ga2O3 is an ultrawide-band gap semiconductor with excellent potential for high-power and ultraviolet optoelectronic device applications. Low thermal conductivity is one of the major obstacles to enable the full performance of β-Ga2O3-based devices. A promising solution for this problem is to integrate β-Ga2O3 with a diamond heat sink. However, the thermal properties of the β-Ga2O3/diamond heterostructures after the interfacial bonding have not been studied extensively, which are influenced by the crystal orientations and interfacial atoms for the β-Ga2O3 and diamond interfaces. In this work, molecular dynamics simulations based on machine learning potential have been adopted to investigate the crystal-orientation-dependent and interfacial-atom-dependent thermal boundary resistance (TBR) of the β-Ga2O3/diamond heterostructure after interfacial bonding. The differences in TBR at different interfaces are explained in detail through the explorations of thermal conductivity value, thermal conductivity spectra, vibration density of states, and interfacial structures. Based on the above explorations, a further understanding of the influence of different crystal orientations and interfacial atoms on the β-Ga2O3/diamond heterostructure was achieved. Finally, insightful optimization strategies have been proposed in the study, which could pave the way for better thermal design and management of β-Ga2O3/diamond heterostructures according to guidance in the selection of the crystal orientations and interfacial atoms of the β-Ga2O3 and diamond interfaces.

Raman scattering owing to magneto-polaron states in monolayer transition metal dichalcogenides

Magneto-optical measurements are fundamental research tools that allow for studying the hitherto unexplored optical transitions and the related applications of topological two-dimensional (2D) transition metal dichalcogenides (TMDs). A theoretical model is developed for the first-order magneto-resonant Raman scattering in a monolayer of TMD. A significant number of avoided crossing points involving optical phonons in the magneto-polaron (MP) spectrum, a superposition of the electron and hole states in the excitation branches, and their manifestations in optical transitions at various light scattering configurations are unique features for these 2D structures. The Raman intensity reveals three resonant splittings of double avoided-crossing levels. The three excitation branches are present in the MP spectrum provoked by the coupling of the Landau levels in the conduction and valence bands via an out-of-plane A1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$A_1$$\\end{document}-optical phonon mode. The energy gaps at the anticrossing points in the MP scattering spectrum are revealed as a function of the electron and hole optical deformation potential constants. The resonant MP Raman scattering efficiency profile allows for quantifying the relative contribution of the conduction and valence bands in the formation of MPs. The results obtained are a guideline for controlling MP effects on the magneto-optical properties of TMD semiconductors, which open pathways to novel optoelectronic devices based on 2D TMDs.

Stretchable OLEDs based on a hidden active area for high fill factor and resolution compensation

Stretchable organic light-emitting diodes (OLEDs) have emerged as promising optoelectronic devices with exceptional degree of freedom in form factors. However, stretching OLEDs often results in a reduction in the geometrical fill factor (FF), that is the ratio of an active area to the total area, thereby limiting their potential for a broad range of applications. To overcome these challenges, we propose a three-dimensional (3D) architecture adopting a hidden active area that serves a dual role as both an emitting area and an interconnector. For this purpose, an ultrathin OLED is first attached to a 3D rigid island array structure through quadaxial stretching for precise, deformation-free alignment. A portion of the ultrathin OLED is concealed by letting it ‘fold in’ between the adjacent islands in the initial, non-stretched condition and gradually surfaces to the top upon stretching. This design enables the proposed stretchable OLEDs to exhibit a relatively high FF not only in the initial state but also after substantial deformation corresponding to a 30% biaxial system strain. Moreover, passive-matrix OLED displays that utilize this architecture are shown to be configurable for compensation of post-stretch resolution loss, demonstrating the efficacy of the proposed approach in realizing the full potential of stretchable OLEDs.

Structural and electronic properties of AlGaN nanowires modulated by Al component and sectional size: A first principles study with DFT+U method

AlGaN nanowires have plenty of applications in optoelectronic functional devices. However, the electronic characteristics and stability of AlGaN nanowires are rarely explored, especially for an actual prediction of bandgaps with varying Al components. In this work, we utilize first principles calculation with DFT + U method to study the stability, charge redistribution, band structures, density of states of AlxGa1-xN alloy nanowires with x spanning from 0 to 1. The results indicate that the stability of the nanowire is enhanced with increasing nanowire diameter and Al component. The bond length in the outermost layer, vertical to the specified direction, is stretched as the Al component increases. The bandgap of nanowire is larger than that of bulk phase and the bowing parameter of nanowire is relatively low. According to the analysis of density of states (DOS), the migration of band structures is attributed to N-p states at VBM and Ga-s and Al-p states at CBM. The calculation of Crystal Orbital Hamilton Population (COHP) reveals the variation of bandgap with changing Al component and diameter. According to the analysis of electron density difference and charge transfer, Al atom has a stronger electron negativity and the electron density surrounding Ga is more delocalized compared Al atom. The results obtained in this study is expected to give some guidance for the preparation of optoelectronic devices based on AlGaN nanowires.

Ion-Exchange Polymer Network Enhanced Interfacial Compatibility for Stable and Efficient Inverted Perovskite Solar Cells.

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as a low-cost and water-processable hole transport material has been widely used in various optoelectronic devices. Although the incorporation of anionic polyelectrolyte PSS in PEDOT contributes to superior water solubility, the trade-off between efficiency and stability remains a challenging issue, limiting its reliable application in perovskite solar cells (PSCs). Herein, we proposed an ion-exchange (IE) strategy to effectively control the doping degree, interfacial charge dynamics, and reliability of PEDOT:PSS in PSCs. This IE approach based on hard cation-soft anion rules enabled effective anion exchange between PEDOT:PSS and lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), which favored enhancing the film conductivity, regulating the perovskite crystallization, and reducing the carrier losses at the interfaces. Consequently, a notable increase of the open-circuit voltage from 0.88 to 1.02 V was realized, resulting in a champion efficiency of 18.7% compared to the control (15.4%) in inverted PSCs. More encouragingly, this IE strategy significantly promoted the thermal and environmental stability of unsealed devices by maintaining over 80% of initial efficiencies after 2000 h. This work provides an effective way to regulate the doping state of the PEDOT-based hole transport material and guides the development of robust polymeric conducting materials for efficient perovskite photovoltaics.

Electronic and optical properties of COFs/graphene and COF/hBN heterostructures

Covalent organic frameworks (COFs) are a class of intriguing materials with tunable electronic and optical properties. In this work, we investigate the electronic and optical properties of COFs embedded with hBN and graphene. Our results demonstrate that graphene integration enhances the ultraviolet and visible light absorption of C6N6 and B6O6 monolayers, while charge transfer in all COF/graphene heterostructures leads to the formation of a built-in electric field. Furthermore, we show that incorporating hBN into B6O6 and C6N6 heterostructures enables control of their bandgap through an applied electric field, resulting in a semiconductor-to-metal transition under moderate electric field strengths. Additionally, B6O6/hBN exhibits suitable band edge alignment for photocatalytic water splitting. These findings provide valuable insights into the electronic and optical properties of COF heterostructures and their potential applications in electronic and optoelectronic devices. Our study contributes to ongoing efforts in the design and development of novel COF and 2D material heterostructures for future electronic and photonic applications.

Enhancing the Quality of MOF Thin Films for Device Integration Through Machine Learning: A Case Study on HKUST‐1 SURMOF Optimization

AbstractMetal–organic Frameworks (MOFs), especially as thin films, are increasingly recognized for their potential in device integration, notably in sensors and photo detectors. A critical factor in the performance of many MOF‐based devices is the quality of the MOF interfaces. Achieving MOF thin films with smooth surfaces and low defect densities is essential. Given the extensive parameter space governing MOF thin film deposition, the use of machine learning (ML) methods to optimize deposition conditions is highly beneficial. Combined with robotic fabrication, ML can more effectively explore this space than traditional methods, simultaneously varying multiple parameters to improve optimization efficiency. Importantly, ML can provide deeper insights into the synthesis of MOF thin films, an essential area of research. This study focuses on refining an HKUST‐1 SURMOF (surface‐mounted MOF) to achieve minimal surface roughness and high crystallinity, including a quantitative analysis of the importance of the various synthesis parameters. Using the SyCoFinder ML technique, thin film surface quality is markedly enhanced in just three generations created by a genetic algorithm, covering 30 distinct parameter sets. This method greatly reduces the need for extensive experimentation. Moreover, the results enhance the understanding of the vast synthesis parameter space in HKUST‐1 SURMOF growth and broaden the applications of MOF thin films in electronic and optoelectronic devices.