Optoelectronic Performance Research Articles

All-solution preparation of perovskite light-emitting diodes in ambient air through film-forming regulation of light-emitting layers based on dual-additive doping and oxygen plasma treatment

Organic-inorganic hybrid perovskites are promising for optoelectronics owing to their high color purity, tunable bandgaps, and low nonradiative recombination rates. However, challenges such as rough surfaces and poor film-forming properties constrain the optoelectronic performance of light-emitting devices. Herein, the PEDOT:PSS film treated by oxygen plasma serves as the hole transport layer, while the formation of perovskite films is optimized by dual-additive doping of PEO and TPBi in ambient air. The results show that the PEDOT:PSS films with PSSH-rich after oxygen plasma treatment provide more nucleation sites, favoring the formation of the perovskite film. Meanwhile, the dual-additive prompts to form a dense and uniform film as well. The intrinsic mechanisms involve PEO as a binder to fill grain gaps and improve water-oxygen stability in the perovskite film, while TPBi acts as a passivator to stimulate uniform nucleation and dense crystallization, improving the grain coverage of the light-emitting layer. Under atmospheric conditions, all-solution processed perovskite devices reach a maximum luminance of 810.4 cd m−2 and a maximum current efficiency of 0.437 cd A−1. This work highlights the significance of using oxygen plasma treatment and additives to improve the performance of perovskite films and achieve superior PeLEDs.

Effect of partial cation substitution on optoelectronic properties and ion diffusion behavior of inorganic lead halide perovskite: A theoretical investigation

Cation substitution is a widely utilized approach for tailoring the properties of lead halide perovskites. A comprehensive understanding of the impact of various cation substitutions on optoelectronic properties and ion diffusion behavior is crucial for enhancing the performance of halide perovskite materials. In this study, we constructed various double halide perovskites by cation substitution and investigated their optoelectronic properties and ion diffusion behavior through first-principles calculations. Our findings reveal that the A-site substitution with alkali cation Rb does not significantly influence the optoelectronic properties of lead halide perovskites. However, it will boost the halide migration due to the enlarged migration bottleneck. The B-site substitution with alkali earth element Sr significantly suppresses the halide migration; while the material will be no longer suitable for visible light absorption due to the enlarged bandgap. The substitution of Pb with d-orbital fulfilled Zn can also suppress the halide migration, but it will give rise to an indirect bandgap and hence affect the optoelectronic performance. The substitution of Pb with Sn can enhance both the thermostability and optoelectronic performance owing to the smaller ionic radius and similar ns2-containing electronic configuration. The increased migration barrier indicates that ion diffusion is also inhibited in double perovskite Cs2SnPbI6. Our results imply that the optoelectronic properties can be further optimized by tuning the ratio of Sn/Pb or the thickness of the perovskite layer in photovoltaic device. These results would be useful guide for the development of novel lead-less optoelectronic perovskite materials.

Tuning of optoelectronic performance of SrTiO3 by surface termination and thickness

The outstanding optical and electrical properties make ternary oxides highly suitable for advanced optoelectronic applications comparing to the traditional silicon-based materials and heterostructures. SrTiO3 (STO), a pivotal perovskite oxide with a direct energy band gap of 3.2 eV, exhibits significant promise in ultraviolet (UV) photodetection. However, the photovoltaic performance of homoepitaxial STO has long been neglected. In this study, we investigated the optoelectronic characteristics of STO by manipulating the crucial factors of surface termination and thickness using oxide molecular beam epitaxy (oxide MBE). We achieved an exceptional charge carrier mobility of 56.5975 cm2 V-1s−1, along with an impressive ON/OFF ratio of 6000 % and a specific detectivity (D*) of 2.95 × 109 Jones (cm Hz1/2 W−1) under near-UV irradiation at room temperature. We observed a thickness-dependent semiconductor-to-metal transition with a critical thickness of 3.5 u.c. STO. The metallic STO displayed an extremely high mobility exceeding 105 cm2 V−1 s−1, accompanied by a substantial MR value exceeding 1000 % at 3 K. Furthermore, the thickness-dependent Hall effect and photoluminescence (PL) indicated that oxygen defects may govern the semiconducting/metallic behavior of STO. This study illustrates the optoelectrical capabilities of homoepitaxial STO, paving the way for advanced and high-performance photodetection in intricate optical materials and devices through homoepitaxy.

Colloidal Quantum Dot‐Based Near and Shortwave Infrared Light Emitters: Recent Developments and Application Prospects

AbstractSolution‐processed quantum dot‐based near and short‐wave infrared light emitters have witnessed substantial developments in recent years. A variety of colloidal quantum dots (CQDs)‐based light emitters, including light‐emitting diodes, optical down‐converters, and emitters showing amplified spontaneous emission, lasing in the near and short‐wave infrared region, are demonstrated over the years. The progress in chemical synthesis of CQDs, development of novel CQDs, better understanding of the surface properties, chemical treatments to improve the optoelectronic properties, and suitable device engineering led to tremendous advances in the light emission performance in the near and short‐wave infrared region. A broad investigation is done into various CQD materials to achieve efficient near‐infrared light emitters. This review gives a detailed account of the advancement of the CQD‐based near and short‐wave infrared light emitters, strategies to improve the optoelectronic performance, controlling optical properties, demonstrated applications, the challenges that need to be tackled for further development, and future research direction.

Unraveling lead-free Fr-based perovskites FrQCl3 (Q = Ca, Sr) and their pressure induced physical properties: DFT analysis for advancing optoelectronic performance

A comprehensive study of structural, electronic, elastic, and optical properties of the cubic FrQCl3 (Q = Ca, Sr) perovskite under pressure 0 − 105 GPa has been considered. Interestingly, FrCaCl3 experiences a shift from an indirect to a direct bandgap material at 12 GPa, while FrSrCl3 undergoes the same shift at 10 GPa, rendering these materials more advantageous for application in optoelectronic devices. As pressure rises, the electronic density of states increases near the Fermi level by shifting valence band electrons upward. This leads to a reduction in the bandgap and a shift of the bandgap from the ultraviolet to the visible region. The examination of mechanical properties indicates that FrQCl3 (Q = Ca, Sr) perovskite exhibits significant potential for uses requiring a combination of anisotropic, and ductile behavior. Optical property analysis reveals that with an increase in hydrostatic pressure, dielectric constant's peak of both material shift towards lower photon energy area.

Rational synthesis of core/shell heterostructured quantum dots for improved self-powered photodetection performance enabled by energy band engineering

Colloidal quantum dots (CQDs), especially core-shell QDs, have attracted dramatic interests as emerging materials in optoelectronic devices due to their size tuneable band-gap, high absorption coefficient, facile and low-cost synthesis routing, etc. However, the precise design of core/shell band engineering along with charge carrier transfer efficiency are still challenging, inevitably impacting the performance of optoelectronic devices. Herein, three different types of CdSe/CdS core-shell heterostructured QDs have been obtained via a proposed synthesis strategy of adjusting the core size but fixing the shell thickness. The performance of the core-shell QDs based self-powered photodetectors can be efficiently regulated by the optimization of synthesis strategy with the design of energy band alignment. Compared to the quasi type-II and the type-I QDs devices, the Ilight/Idark ratio of type-II heterostructure based photodetector is increased by ∼2 and ∼5 orders of magnitude, respectively. The champion device exhibits extraordinary optoelectronic performance in terms of ultrahigh light-to-dark current ratio of 105, photoresponsivity of 10.64 mA/W, at bias of 0 V, respectively. The charge carrier dynamics and transfer mechanisms of the QDs were further investigated, revealing the improved carrier separation and transportation efficiency induced by a strong build-in electric field in type-II CdSe/CdS core-shell heterostructure. This work provides a new strategy for the next-generation self-powered QDs optoelectronics enabled by the proposed synthesis approach along with the design of energy band alignment.

Quantification of Two-Dimensional Interfaces: Quality of Heterostructures and What Is Inside a Nanobubble.

Trapped materials at the interfaces of two-dimensional heterostructures (HS) lead to reduced coupling between the layers, resulting in degraded optoelectronic performance and device variability. Further, nanobubbles can form at the interface during transfer or after annealing. The question of what is inside a nanobubble, i.e., the trapped material, remains unanswered, limiting the studies and applications of these nanobubble systems. In this work, we report two key advances. First, we quantify the interface quality using RAW format optical imaging (unprocessed image data) and distinguish between ideal and non-ideal interfaces. The HS/substrate ratio value is calculated using a transfer matrix model and is able to detect the presence of trapped layers. The second key advance is the identification of water as the trapped material inside a nanobubble. To the best of our knowledge, this is the first study to show that optical imaging alone can quantify interface quality and find the type of trapped material inside spontaneously formed nanobubbles. We also define a quality index parameter to quantify the interface quality of HS. Quantitative measurement of the interface will help answer the question whether annealing is necessary during HS preparation and will enable creation of complex HS with small twist angles. Identification of the trapped materials will pave the way toward using nanobubbles for optical and engineering applications.

Organic-Inorganic Rubrene/WS2 Heterostructure for Broadband Detection and Polarization Imaging.

Organic single crystals exhibit improved carrier mobility, longer exciton diffusion length, anisotropic charge transport, and unique linear dichroism, while its high exciton binding energy seriously limits the free-carrier generation and photoelectric conversion efficiency. Layered van der Waals heterostructures, which integrate organic crystals with high mobility two-dimensional (2D) inorganic semiconductors, are promising for promoting exciton dissociation and boosting sensitivity by utilizing the interfacial potential and photogating effect. In this work, organic single-crystal rubrene is integrated with a few-layer WS2 to design the high-performance photodetector. The device exhibits an excellent responsivity of 1000 A W-1, and a fast speed of 180 μs, which is far superior to the individual WS2 device. Equally importantly, this device provides excellent polarization detection performance by virtue of the anisotropic properties of rubrene, and the dichroic ratios are 1.56, 1.5, and 1.7 for 375, 405, and 658 nm irradiation, respectively. Finally, several high-resolution single-pixel broadband polarization imaging was demonstrated. Our work shows that organic-inorganic heterostructure is an essential candidate for improving optoelectronics performance and has potential for polarization imaging.

Optoelectronic performance of Jatropha oil-derived poly(ethyl carbamate) gel polymer electrolyte as quasi-solid-state solution for photoelectrochemical cells

Optoelectronic performance of Jatropha oil-derived poly(ethyl carbamate) gel polymer electrolyte as quasi-solid-state solution for photoelectrochemical cells

Extending the Charge Carrier Recombination Lifetime by Octahedral Rotations in Ruddlesden-Popper Ba3Zr2S7 Perovskites.

Intentional distortions of [BX6] octahedra within perovskite structures have been recognized as a potent strategy for precise band gap adjustments and optimization of their photovoltaic properties, yet information regarding charge carrier dynamics linked to octahedral distortion under ambient conditions for chalcogenide perovskites remains limited. In this study, we utilize ab initio nonadiabatic molecular dynamics to explore the dynamics of photogenerated carriers in a representative two-dimensional Ba3Zr2S7 material in the Ruddlesden-Popper phase. The theoretical results highlight the influence of octahedral rotation on the materials' stability and carrier recombination lifetime of the system. Specifically, the octahedrally rotating P42/mnm phase exhibits a prolonged nonradiative carrier recombination lifetime attributed to the stabilized electron-phonon coupling. These findings offer valuable insights into the fundamental physical characteristics of imposed octahedral distortion and its potential for optimizing the optoelectronic performance of 2D Ruddlesden-Popper Ba-Zr-S chalcogenide materials.

Concentric hollow multi-hexagonal platelets from a small molecule

The creation of well-defined hollow two-dimensional structures from small organic molecules, particularly those with controlled widths and numbers of segments, remains a formidable challenge. Here we report the fabrication of the well-defined concentric hollow two-dimensional platelets with programmable widths and numbers of segments through constructing a concentric multiblock two-dimensional precursor followed by post-processing. The fabrication of concentric multi-hexagons two-dimensional platelets is realized by the alternative heteroepitaxial growth of two donor-acceptor molecules. Upon ultraviolet irradiation, one of the two donor-acceptor molecules can be selectively oxidized by singlet oxygen generated during the process, and the oxidized product becomes more soluble due to increased polarity. This allows for selective removal of the oxidized segments simply by solvent dissolution, yielding hollow multiblock two-dimensional structures. The hollow two-dimensional platelets can be utilized as templates to lithograph complex electrodes with precisely controlled gap sizes, thereby offering a platform for examining the optoelectronic performance of functional materials.

Tin doping modulates electron-hole recombination in Dion-Jacobson phase 2D hybrid perovskite

To obtain less-toxic and optimal-band-gap perovskite materials, tin (Sn)-lead (Pb) hybrid technology comes into the sight of researchers. The Sn–Pb ratio primarily affects the electronic band structure, conductivity, and carrier transport, which are essential for optoelectronic performance. While most reports are about 3D materials, there has been little coverage of 2D Sn–Pb perovskites which exhibiting improved stability. In this paper, the e-h recombination dynamics in Dion-Jacobson Phase 2D Sn–Pb perovskites are studied using time-dependent ab initio nonadiabatic molecular dynamics (NAMD) simulation. It is found that Sn doping plays a significant role in narrowing the band-gap of 2D perovskites and localizing the charge distribution. Only a small amount of Sn doping can minimize NA coupling and shorten decoherence time of frontier orbitals simultaneously, then leading to longer charge recombination time. NAMD simulations reveal the optimal Sn ratio (25 mol%) and provide an effective way to design high-performance 2D perovskite materials.

Piezotronically tuned photosensitivity in ZnO varistor-type interface devices

The study of piezotronic and piezo-phototronic features in semiconducting piezoelectrics has gained considerable attention for optimizing electronic and optoelectronic device performance. In this study, we explore the photocurrent response within a ZnO varistor-type interface device and examine its UV photosensitivity enhancement through piezo-phototronic modulation of the potential barriers at grain boundaries. Doped ZnO bicrystals were synthesized using the epitaxial solid-state transformation method with polarization vectors perpendicular to the interface. The vectors can be directed both into and out of the interfaces depending on the crystallographic orientation of the crystals designated as (0001̅)|(0001̅) and (0001)|(0001) interfaces, respectively. These varistor-type boundaries demonstrate an exceptional photoelectric response to UV photons. Furthermore, our results indicate that the photoresponsivity of bicrystals with (0001)|0001 crystallographic orientation can be further enhanced under piezo-phototronic influence. Application of compressive stress of 100 MPa not only increased photocurrent formation by 1000 % but also boosted photosensitivity by 1400 %, attributed to the elevated double Schottky barrier (DSB) height at the interface resulting from mechanical loading on the bicrystal. Our findings highlight the significant role of piezoelectrically tuned potential barriers at grain boundaries in enhancing the separation and extraction of photogenerated excitons for photocurrent formation. This study introduces the engineered varistor-type interface as a promising candidate for future optoelectronic devices and contributes to our understanding of the piezo-phototronic concept in semiconductor-semiconductor interface devices.

Noise equivalent temperature difference study of type-II superlattice MWIR focal plane arrays for high operating temperature performance.

Achieving high operating temperature (HOT) plays a crucial role in miniaturizing type-II superlattice (T2SL) mid-wavelength infrared (MWIR) focal plane arrays (FPAs). However, their full potential has yet to be realized due to a lack of complete understanding of their operation from the perspective of detection principles. Here, by investigating the photon transmission path and optoelectronic performance of the simulated devices, a detailed noise equivalent temperature difference (NETD) model of the T2SL MWIR FPAs was established. The NETD limitations in the optics-limited and detector-limited modes were revealed by studying the effects of the source, optical system, and FPA-related parameters. Although NETD exhibits sensitivity to dark currents, improvements in the quantum efficiency and well capacity can further boost its performance. When the defects and carrier lifetimes are well controlled to completely suppress the dark current, the NETD of an MWIR system with optimized integration times, which operates between 150 K and 200 K, is predicted to be below 10 mK when detecting room-temperature targets. The results provide new insights into the model and sources contributing to the NETD and demonstrate the possibility of high-temperature operation of T2SLs MWIR FPAs.

X‐ray‐ultraviolet–visible‐near‐infrared photoresponses realized in a lead‐free hybrid perovskite ferroelectric through light‐induced ferro‐pyro‐phototronic effect

AbstractDue to the built‐in electric field induced by spontaneous polarization in hybrid perovskite (HP) ferroelectrics, the devices based on them exhibit excellent performance in self‐powered photodetection. However, most of the self‐powered photodetector are made of lead‐based HP ferroelectrics and have a relatively narrow photoresponse waveband. Although lead‐free HPs solve the problem of lead toxicity, their optoelectronic performance is inferior to that of lead‐based HPs and photoresponse waveband is limited by its optical band gap, which hinders their further application. To solve this problem, herein, a lead‐free HP ferroelectric (HDA)BiI5 (HDA is hexane‐1,6‐diammonium) with large spontaneous polarization shows an enhanced photocurrent and achieves x‐ray‐ultraviolet–visible‐near‐infrared (x‐ray‐UV–Vis–NIR) photoresponse through the ferro‐pyro‐phototronic (FPP) effect. The ferroelectric, pyroelectric, and photovoltaic characteristics coupled together in a single‐phase (HDA)BiI5 ferroelectric is an effective way to improve the performance of the devices. What is particularly attractive is that the FPP effect not only improves the optoelectronic performance of (HDA)BiI5, but also achieves broadband photoresponses beyond its optical absorption range. Especially, the current boosting with an exceptional contrast of ~1100% and 2400% under 520 and 637 nm, respectively, which is associated with FPP effect. Meanwhile, single crystal self‐powered photodetector based on (HDA)BiI5 also exhibit significant FPP effects even under high‐energy x‐ray, which owns an outstanding sensitivity of 170.7 μC Gy−1 cm−2 and a lower detection limit of 266 nGy s−1 at 0 V bias. Therefore, it is of great significance to study the coupling of multiple physical effects and improve device performance based on lead‐free HP ferroelectrics.image

Modulate the work function of MXene in MXene/InGaN heterojunction for visible light photodetector

MXene/InGaN heterojunction photodetectors with simple structure and superior optoelectronic performance are considered a viable option for optical communication. However, the integration of MXene with InGaN faces the problem of a relatively low Schottky barrier, leading to electron backflow, which hinders the separation of carriers and limits the photoresponse of photodetectors. Herein, high-performance MXene/InGaN heterojunction photodetectors were fabricated, and the work function of Ti3C2TX was modulated to explore its effect on the performance of the photodetectors. The ascorbic acid treatment increased the work function of MXene from 4.20 to 4.34 eV, enhancing the Schottky barrier height of the heterojunction from 0.56 to 0.70 eV. The devices exhibit excellent photoresponse performances, such as a responsivity of 0.133 A W−1 and a specific detectivity of 2.81 × 1011 Jones at −1 V bias, as well as a short rise/decay time of 37.49/110 μs at 0 V bias. Additionally, the photodetectors achieve high stability that can maintain over 95% of the initial value after 3 months. This work indicates the potential for utilizing tunable MXene work function to construct high-performance optoelectronic devices for visible light applications.

Tailoring Interface Energies via Phosphonic Acids to Grow and Stabilize Cubic FAPbI3 Deposited by Thermal Evaporation.

Coevaporation of formamidinium lead iodide (FAPbI3) is a promising route for the fabrication of highly efficient and scalable optoelectronic devices, such as perovskite solar cells. However, it poses experimental challenges in achieving stoichiometric FAPbI3 films with a cubic structure (α-FAPbI3). In this work, we show that undesired hexagonal phases of both PbI2 and FAPbI3 form during thermal evaporation, including the well-known 2H-FAPbI3, which are detrimental for optoelectronic performance. We demonstrate the growth of α-FAPbI3 at room temperature via thermal evaporation by depositing phosphonic acids (PAc) on substrates and subsequently coevaporating PbI2 and formamidinium iodide. We use density-functional theory to develop a theoretical model to understand the relative growth energetics of the α and 2H phases of FAPbI3 for different molecular interactions. Experiments and theory show that the presence of PAc molecules stabilizes the formation of α-FAPbI3 in thin films when excess molecules are available to migrate during growth. This migration of molecules facilitates the continued presence of adsorbed organic precursors at the free surface throughout the evaporation, which lowers the growth energy of the α-FAPbI3 phase. Our theoretical analyses of PAc molecule-molecule interactions show that ligands can form hydrogen bonding to reduce the migration rate of the molecules through the deposited film, limiting the effects on the crystal structure stabilization. Our results also show that the phase stabilization with molecules that migrate is long-lasting and resistant to moist air. These findings enable reliable formation and processing of α-FAPbI3 films via vapor deposition.

Ultrahigh Bipolar Photoresponse in a Self-Powered Ultraviolet Photodetector Based on GaN and In/Sn-Doped Ga2O3 Nanowires pn junction.

Self-powered ultraviolet photodetectors with bipolar photoresponse have great potential in the fields of ultraviolet optical communication, all-optical controlled artificial synapses, high-resolution ultraviolet imaging equipment, and multiband photoelectric detection. However, the current low optoelectronic performance limits the development of such polar switching devices. Here, we construct a self-powered ultraviolet photodetector based on GaN and In/Sn-doped Ga2O3 (IGTO) nanowires (NWs) pn junction structure. This unique nanowire/thin film structure allows GaN and IGTO to dominate the absorption of light at different wavelengths, resulting in a highly bipolar photoresponse. The device has a responsivity of 2.04 A/W and a normalized detectivity of 7.18 × 1013 Jones at 254 nm and a responsivity of -2.09 A/W and a normalized detectivity of -7 × 1013 Jones at 365 nm, both at zero bias. In addition, it has an extremely high Ilight/Idark ratio of 1.05 × 105 and ultrafast response times of 2.4/1.9 ms (at 254 nm) and 5.7/5.2 ms (at 365 nm). These excellent properties are attributed to the high specific surface area of the one-dimensional nanowire structure and the abundant voids generated by the nanowire network to enhance the absorption of light, and the p-n junction structure enables the rapid separation and transfer of photogenerated electron-hole pairs. Our findings provide a feasible strategy for high-performance wavelength-controlled polarity switching devices.

A new strategy for fabricating low haze p-type CuI film

As an intrinsic p-type transparent conductor with a wide band gap of 3.1 eV, γ-CuI full of potential has gradually attracted the attention of researchers. However, γ-CuI films deposited by various techniques generally exhibit high haze with a frosted glass-like appearance, which significantly affects the device performance. Herein, a new strategy is proposed in which true p-type CuI thin films with low haze have been successfully synthesised at room temperature. The specular transmittance of the CuI film over 85% in the visible region (400–800 nm) can be achieved. The haze of the as-prepared γ-CuI films can be as low as 0.7%. Meanwhile, the as-prepared CuI film has an FOM as high as 230 MΩ−1. This ideal stable p-type optoelectronic performance was significant among various typical p-type transparent conductive films.

High‐sensitive and fast MXene/silicon photodetector for single‐pixel X‐ray imaging

AbstractThe demand for high‐performance X‐ray detectors leads to material innovation for efficient photoelectric conversion and carrier transfer. However, current X‐ray detectors are often susceptible to chemical and irradiation instability, complex fabrication processes, hazardous components, and difficult compatibility. Here, we investigate a two‐dimensional (2D) material with a relatively low atomic number, Ti3C2Tx MXenes, and single crystal silicon for X‐ray detection and single‐pixel imaging (SPI). We fabricate a Ti3C2Tx MXene/Si X‐ray detector demonstrating remarkable optoelectronic performance. This detector exhibits a sensitivity of 1.2 × 107 μC Gyair−1 cm−2, a fast response speed with a rise time of 31 μs, and an incredibly low detection limit of 2.85 nGyair s−1. These superior performances are attributed to the unique charge coupling behavior under X‐ray irradiation via intrinsic polaron formation. The device remains stable even after 50 continuous hours of high‐dose X‐ray irradiation. Our device fabrication process is compatible with silicon‐based semiconductor technology. Our work suggests new directions for eco‐friendly X‐ray detectors and low‐radiation imaging system.image