Flexible Unipolar IGZO Transistor-Based Integrate and Fire Neurons for Spiking Neuromorphic Applications.

In this article, three different implementations of an Axon-Hillock circuit are presented, one of the basic building blocks of spiking neural networks. In this work, we explored the design of such circuits using a unipolar thin-film transistor technology based on amorphous InGaZnO, often used for large-area electronics. All the designed circuits are fabricated by direct material deposition and patterning on top of a flexible polyimide substrate. Axon-Hillock circuits presented in this article consistently show great adaptability of the basic properties of a spiking neuron such as output spike frequency adaptation and output spike width adaptation. Additional degrees of adaptability are demonstrated with each of the Axon-Hillock circuit varieties: neuron circuit threshold voltage adaptation, differentiation between input signal importance, and refractory period modulation. The proposed neuron can change its firing frequency up to three orders of magnitude by varying a single voltage brought to a circuit terminal. This allows the neuron to function, and potentially learn, at vastly different timescales that coincide with the biologically meaningful timescales, going from milliseconds to seconds, relevant for circuits meant for interaction with the environment. Thanks to careful design choices, the average measured power consumption is kept in the nW range, realistically allowing upscaling towards the spiking neural networks in the future. The spiking neuron with refractory period modulation presented in this work has an area of 607.3 µm × 492.2 µm, it experimentally demonstrated firing rates as low as 11.926 mHz, and its energy consumption per spike is ≈ 700 pJ at 30 Hz.

A Thin-Film Pinned-Photodiode Imager Pixel with Fully Monolithic Fabrication and beyond 1Me- Full Well Capacity.

Thin-film photodiodes (TFPD) monolithically integrated on the Si Read-Out Integrated Circuitry (ROIC) are promising imaging platforms when beyond-silicon optoelectronic properties are required. Although TFPD device performance has improved significantly, the pixel development has been limited in terms of noise characteristics compared to the Si-based image sensors. Here, a thin-film-based pinned photodiode (TF-PPD) structure is presented, showing reduced kTC noise and dark current, accompanied with a high conversion gain (CG). Indium-gallium-zinc oxide (IGZO) thin-film transistors and quantum dot photodiodes are integrated sequentially on the Si ROIC in a fully monolithic scheme with the introduction of photogate (PG) to achieve PPD operation. This PG brings not only a low noise performance, but also a high full well capacity (FWC) coming from the large capacitance of its metal-oxide-semiconductor (MOS). Hence, the FWC of the pixel is boosted up to 1.37 Me- with a 5 µm pixel pitch, which is 8.3 times larger than the FWC that the TFPD junction capacitor can store. This large FWC, along with the inherent low noise characteristics of the TF-PPD, leads to the three-digit dynamic range (DR) of 100.2 dB. Unlike a Si-based PG pixel, dark current contribution from the depleted semiconductor interfaces is limited, thanks to the wide energy band gap of the IGZO channel material used in this work. We expect that this novel 4 T pixel architecture can accelerate the deployment of monolithic TFPD imaging technology, as it has worked for CMOS Image sensors (CIS).

Image sensors using thin-film absorbers.

Image sensors are must-have components of most consumer electronics devices. They enable portable camera systems, which find their way into billions of devices annually. Such high volumes are possible thanks to the complementary metal-oxide semiconductor (CMOS) platform, leveraging wafer-scale manufacturing. Silicon photodiodes, at the core of CMOS image sensors, are perfectly suited to replicate human vision. Thin-film absorbers are an alternative family of photoactive materials, distinguished by the layer thickness comparable with or smaller than the wavelength of interest. They allow design of imagers with functionalities beyond Si-based sensors, such as transparency or detectivity at wavelengths above Si cutoff (e.g., short-wave infrared). Thin-film image sensors are an emerging device category. While intensive research is ongoing to achieve sufficient performance of thin-film photodetectors, to our best knowledge, there have been few complete studies on their integration into advanced systems. In this paper, we will describe several types of image sensors being developed at imec, based on organic, quantum dot, and perovskite photodiode and show their figures of merit. We also discuss the methodology for selecting the most appropriate sensor architecture (integration with thin-film transistor or CMOS). Application examples based on imec proof-of-concept sensors are demonstrated to showcase emerging use cases.

Electric Field-Induced Quenching of MAPbI3 Photoluminescence in PeLED Architecture.

Photoluminescence (PL) measurements are a widely used technique for the investigation of perovskite-based materials and devices. Although electric field-induced PL quenching provides additional useful information, this phenomenon is quite complex and not yet clearly understood. Here, we address the PL quenching of methylammonium lead iodide (MAPbI3) perovskite in a light-emitting diode (PeLED) architecture. We distinguish two quenching mechanisms: (a) indirect quenching by slow irreversible or partially reversible material changes that occur gradually under the applied light and electric field and (b) direct quenching by the influence of the electric field on the charge carrier densities, their spatial distributions, and radiative recombination rates. Direct quenching, observed under the abrupt application of negative voltage, causes a decrease of the PL intensity. However, the PL intensity then partially recovers within tens of milliseconds as mobile ions screen the internal electric field. The screening time increases to hundreds of seconds at low temperatures, indicating activation energies for ion motion of about 80 meV. On the other hand, ultrafast time-resolved PL measurements revealed two main phases of direct quenching: an instantaneous reduction in the radiative carrier recombination rate, which we attribute to the electron and hole displacement within individual perovskite grains, followed by a second phase lasting hundreds of picoseconds, which is due to the charge carrier extraction and spatial separation of electron and hole "clouds" within the entire perovskite layer thickness.

Interface-Engineered Organic Near-Infrared Photodetector for Imaging Applications.

We report a high-speed low dark current near-infrared (NIR) organic photodetector (OPD) on a silicon substrate with amorphous indium gallium zinc oxide (a-IGZO) as the electron transport layer (ETL). In-depth understanding of the origin of dark current is obtained using an elaborate set of characterization techniques, including temperature-dependent current-voltage measurements, current-based deep-level transient spectroscopy (Q-DLTS), and transient photovoltage decay measurements. These characterization results are complemented by energy band structures deduced from ultraviolet photoelectron spectroscopy. The presence of trap states and a strong dependency of activation energy on the applied reverse bias voltage point to a dark current mechanism based on trap-assisted field-enhanced thermal emission (Poole-Frenkel emission). We significantly reduce this emission by introducing a thin interfacial layer between the donor: acceptor blend and the a-IGZO ETL and obtain a dark current as low as 125 pA/cm2 at an applied reverse bias of -1 V. Thanks to the use of high-mobility metal-oxide transport layers, a fast photo response time of 639 ns (rise) and 1497 ns (fall) is achieved, which, to the best of our knowledge, is among the fastest reported for NIR OPDs. Finally, we present an imager integrating the NIR OPD on a complementary metal oxide semiconductor read-out circuit, demonstrating the significance of the improved dark current characteristics in capturing high-quality sample images with this technology.

Efficient OLEDs Based on Slot-Die-Coated Multicomponent Emissive Layer.

The optimization of multicomponent emissive layer (EML) deposition by slot-die coating for organic light-emitting diodes (OLEDs) is presented. In the investigated EMLs, the yellow-green iridium complex (Ir) was doped in two types of host: a commonly used mixture of poly(N-vinylcarbazole) (PVK) with oxadiazole derivative (PBD) or PVK with thermally activated delayed fluorescence-assisted dopant (10-(4-(4,6-diphenyl-1,3,5-triazin-2-yl)phenyl)-10H-spiro[acridine-9,9'-fluorene], SpiroAC-TRZ). In this article, OLEDs with EML prepared in air by slot-die coating, facilitating industrial manufacturing, are confronted with those with spin-coated EML in nitrogen. OLEDs based on PVK:PBD + 2 wt.% Ir-dopant exhibit comparable performance: ~13 cd A-1, regardless of the used method. The highest current efficiency (21 cd A-1) is shown by OLEDs based on spin-coated PVK with 25 wt.% SpiroAC-TRZ and 2 wt.% Ir-dopant. It is three times higher than the efficiency of OLEDs with slot-die-coated EML in air. The performance reduction, connected with the adverse oxygen effect on the energy transfer from TADF to emitter molecules, is minimized by the rapid EML annealing in a nitrogen atmosphere. This post-treatment causes more than a doubling of the OLED efficiency, from 7 cd A-1 to over 15 cd A-1. Such an approach may be easily implemented in other printing techniques and result in a yield enhancement.

A Thermally Activated Delayed Fluorescence Green OLED with 4500 h Lifetime and 20% External Quantum Efficiency by Optimizing the Emission Zone using a Single-Emission Spectrum Technique.

Device optimization of light-emitting diodes (LEDs) targets the most efficient conversion of electrically injected charges into emitted light. The emission zone in an LED is where charges recombine and light is emitted from. It is believed that the emission zone is strongly linked to device efficiency and lifetime. However, the emission zone size is below the optical diffraction limit, so it is difficult to measure. An accessible method based on a single emission spectrum that enables emission zone measurements with sub-second time resolution is shown. A procedure is introduced to study and control the emission zone of an LED system and correlate it with device performance. A thermally activated delayed fluorescence organic LED emission zone is experimentally measured over all luminescing current densities, while varying the device structure and while ageing. The emission zone is shown to be finely controlled by emitter doping because electron transport via the emitter is the charge-transport bottleneck of the system. Suspected quenching/degradation mechanisms are linked with the emission zone changes, device structure variation, and ageing. Using these findings, a device with an ultralong 4500 h T95 lifetime at 1000 cd m-2 with 20% external quantum efficiency is shown.

Effect of TADF Assistance on Performance Enhancement in Solution Processed Green Phosphorescent OLEDs.

Many methods have been proposed to increase the efficiency of organic electroluminescent materials applied as an emissive layer in organic light emitting diodes (OLEDs). Herein, we demonstrate enhancement of electroluminescence efficiency and operational stability solution processed OLEDs by employing thermally activated delayed fluorescence (TADF) molecules as assistant dopants in host-guest systems. The TADF assistant dopant (SpiroAC-TRZ) is used to facilitate efficient energy transfer from host material poly(N-vinylcarbazole) (PVK) to a phosphorescent Ir(III) emitter. We present the analysis of energy transfer and charge trapping-two main processes playing a crucial role in light generation in host-guest structure OLEDs. The investigation of photo-, electro- and thermoluminescence for the double-dopant layer revealed that assistant dopant does not only harvest and transfer the electrically generated excitons to phosphorescent emitter molecules but also creates exciplexes. The triplet states of formed PVK:SpiroAC-TRZ exciplexes are involved in the transport process of charge carriers and promote long-range exciton energy transfer to the emitter, improving the efficiency of electroluminescence in a single emissive layer OLED, resulting in devices with luminance exceeding 18 000 cd/m2 with a luminous efficiency of 23 cd/A and external quantum efficiency (EQE) of 7.4%.

Mitigating Dark Current for High-Performance Near-Infrared Organic Photodiodes via Charge Blocking and Defect Passivation.

Thin-film organic near-infrared (NIR) photodiodes can be essential building blocks in the rapidly emerging fields including the internet of things and wearable electronics. However, the demonstration of NIR organic photodiodes with not only high responsivity but also low dark current density that is comparable to that of inorganic photodiodes, for example, below 1 nA cm-2 for silicon photodiodes, remains a challenge. In this work, we have demonstrated non-fullerene acceptor-based NIR photodiodes with an ultralow dark current density of 0.2 nA cm-2 at -2 V by innovating on charge transport layers to mitigate the reverse charge injection and interfacial defect-induced current generation. The same device also shows a high external quantum efficiency approaching 70% at 850 nm and a specific detectivity of over 1013 Jones at wavelengths up to 940 nm. Furthermore, the versatility of our approach for mitigating dark current is demonstrated using a NIR photodetector utilizing different non-fullerene systems. Finally, the practical application of NIR organic photodiodes is demonstrated with an image sensor integrated on a silicon CMOS readout. This work provides new insight into the device stack design of low-dark current NIR organic photodiodes for weak light detection.

Carrier Mobility, Lifetime, and Diffusion Length in Optically Thin Quantum Dot Semiconductor Films.

We propose a method to measure the fundamental parameters that govern diffusion transport in optically thin quantum dot semiconductor films and apply it to quantum dot materials with different ligands. Thin films are excited optically, and the profile of photogenerated carriers is modeled using diffusion-based transport equations and taking into account the optical cavity effects. Correlation with steady-state photoluminescence experiments on different stacks comprising a quenching layer allows the extraction of the carrier diffusion length accurately from the experimental data. In the time domain, the mapping of the transient PL data with the solutions of the time-dependent diffusion equation leads to accurate calculations of the photogenerated carrier mobility. These findings allow the estimation of the speed limitations for diffusion-based transport in QD absorbers.

Two-dimensional perovskites with alternating cations in the interlayer space for stable light-emitting diodes.

Lead halide perovskites have attracted tremendous attention in photovoltaics due to their impressive optoelectronic properties. However, the poor stability of perovskite-based devices remains a bottleneck for further commercial development. Two-dimensional perovskites have great potential in optoelectronic devices, as they are much more stable than their three-dimensional counterparts and rapidly catching up in performance. Herein, we demonstrate high-quality two-dimensional novel perovskite thin films with alternating cations in the interlayer space. This innovative perovskite provides highly stable semiconductor thin films for efficient near-infrared light-emitting diodes (LEDs). Highly efficient LEDs with tunable emission wavelengths from 680 to 770 nm along with excellent operational stability are demonstrated by varying the thickness of the interlayer spacer cation. Furthermore, the best-performing device exhibits an external quantum efficiency of 3.4% at a high current density (J) of 249 mA/cm2 and remains above 2.5% for a J up to 720 mA cm-2, leading to a high radiance of 77.5 W/Sr m2 when driven at 6 V. The same device also shows impressive operational stability, retaining almost 80% of its initial performance after operating at 20 mA/cm2 for 350 min. This work provides fundamental evidence that this novel alternating interlayer cation 2D perovskite can be a promising and stable photonic emitter.

Inorganic and Layered Perovskites for Optoelectronic Devices.

Organic-inorganic halide perovskites are making breakthroughs in a range of optoelectronic devices. Reports of >23% certified power conversion efficiency in photovoltaic devices, external quantum efficiency >21% in light-emitting diodes (LEDs), continuous-wave lasing and ultralow lasing thresholds in optically pumped lasers, and detectivity in photodetectors on a par with commercial GaAs rivals are being witnessed, making them the fastest ever emerging material technology. Still, questions on their toxicity and long-term stability raise concerns toward their market entry. The intrinsic instability in these materials arises due to the organic cation, typically the volatile methylamine (MA), which contributes to hysteresis in the current-voltage characteristics and ion migration. Alternative inorganic substitutes to MA, such as cesium, and large organic cations that lead to a layered structure, enhance structural as well as device operational stability. These perovskites also provide a high exciton binding energy that is a prerequisite to enhance radiative emission yield in LEDs. The incorporation of inorganic and layered perovskites, in the form of polycrystalline films or as single-crystalline nanostructure morphologies, is now leading to the demonstration of stable devices with excellent performance parameters. Herein, key developments made in various optoelectronic devices using these perovskites are summarized and an outlook toward stable yet efficient devices is presented.

Mixed Lead-Tin Halide Perovskites for Efficient and Wavelength-Tunable Near-Infrared Light-Emitting Diodes.

Near-infrared (NIR) light-emitting diodes (LEDs), with emission wavelengths between 800 and 950 nm, are useful for various applications, e.g., night-vision devices, optical communication, and medical treatments. Yet, devices using thin film materials like organic semiconductors and lead based colloidal quantum dots face certain fundamental challenges that limit the improvement of external quantum efficiency (EQE), making the search of alternative NIR emitters important for the community. In this work, efficient NIR LEDs with tunable emission from 850 to 950 nm, using lead-tin (Pb-Sn) halide perovskite as emitters are demonstrated. The best performing device exhibits an EQE of 5.0% with a peak emission wavelength of 917 nm, a turn-on voltage of 1.65 V, and a radiance of 2.7 W Sr-1 m-2 when driven at 4.5 V. The emission spectra of mixed Pb-Sn perovskites are tuned either by changing the Pb:Sn ratio or by incorporating bromide, and notably exhibit no phase separation during device operation. The work demonstrates that mixed Pb-Sn perovskites are promising next generation NIR emitters.

Thin-Film Quantum Dot Photodiode for Monolithic Infrared Image Sensors.

Imaging in the infrared wavelength range has been fundamental in scientific, military and surveillance applications. Currently, it is a crucial enabler of new industries such as autonomous mobility (for obstacle detection), augmented reality (for eye tracking) and biometrics. Ubiquitous deployment of infrared cameras (on a scale similar to visible cameras) is however prevented by high manufacturing cost and low resolution related to the need of using image sensors based on flip-chip hybridization. One way to enable monolithic integration is by replacing expensive, small-scale III-V-based detector chips with narrow bandgap thin-films compatible with 8- and 12-inch full-wafer processing. This work describes a CMOS-compatible pixel stack based on lead sulfide quantum dots (PbS QD) with tunable absorption peak. Photodiode with a 150-nm thick absorber in an inverted architecture shows dark current of 10-6 A/cm² at -2 V reverse bias and EQE above 20% at 1440 nm wavelength. Optical modeling for top illumination architecture can improve the contact transparency to 70%. Additional cooling (193 K) can improve the sensitivity to 60 dB. This stack can be integrated on a CMOS ROIC, enabling order-of-magnitude cost reduction for infrared sensors.

Highly Crystalline C8-BTBT Thin-Film Transistors by Lateral Homo-Epitaxial Growth on Printed Templates.

Highly crystalline thin films of organic semiconductors offer great potential for fundamental material studies as well as for realizing high-performance, low-cost flexible electronics. The fabrication of these films directly on inert substrates is typically done by meniscus-guided coating techniques. The resulting layers show morphological defects that hinder charge transport and induce large device-to-device variability. Here, a double-step method for organic semiconductor layers combining a solution-processed templating layer and a lateral homo-epitaxial growth by a thermal evaporation step is reported. The epitaxial regrowth repairs most of the morphological defects inherent to meniscus-guided coatings. The resulting film is highly crystalline and features a mobility increased by a factor of three and a relative spread in device characteristics improved by almost half an order of magnitude. This method is easily adaptable to other coating techniques and offers a route toward the fabrication of high-performance, large-area electronics based on highly crystalline thin films of organic semiconductors.

Growth Of Organic Semiconductor Thin Films with Multi-Micron Domain Size and Fabrication of Organic Transistors Using a Stencil Nanosieve.

To grow small molecule semiconductor thin films with domain size larger than modern-day device sizes, we evaporate the material through a dense array of small apertures, called a stencil nanosieve. The aperture size of 0.5 µm results in low nucleation density, whereas the aperture-to-aperture distance of 0.5 µm provides sufficient crosstalk between neighboring apertures through the diffusion of adsorbed molecules. By integrating the nanosieve in the channel area of a thin-film transistor mask, we show a route for patterning both the organic semiconductor and the metal contacts of thin-film transistors using one mask only and without mask realignment.

Charge carrier mobility in thin films of organic semiconductors by the gated van der Pauw method.

Thin film transistors based on high-mobility organic semiconductors are prone to contact problems that complicate the interpretation of their electrical characteristics and the extraction of important material parameters such as the charge carrier mobility. Here we report on the gated van der Pauw method for the simple and accurate determination of the electrical characteristics of thin semiconducting films, independently from contact effects. We test our method on thin films of seven high-mobility organic semiconductors of both polarities: device fabrication is fully compatible with common transistor process flows and device measurements deliver consistent and precise values for the charge carrier mobility and threshold voltage in the high-charge carrier density regime that is representative of transistor operation. The gated van der Pauw method is broadly applicable to thin films of semiconductors and enables a simple and clean parameter extraction independent from contact effects.

Predictive Model for the Meniscus-Guided Coating of High-Quality Organic Single-Crystalline Thin Films.

A model that describes solvent evaporation dynamics in meniscus-guided coating techniques is developed. In combination with a single fitting parameter, it is shown that this formula can accurately predict a processing window for various coating conditions. Organic thin-film transistors (OTFTs), fabricated by a zone-casting setup, indeed show the best performance at the predicted coating speeds with mobilities reaching 7 cm2 V-1 s-1 .

Dopant-Free Hole-Transporting Material with a C3h Symmetrical Truxene Core for Highly Efficient Perovskite Solar Cells.

Herein we present a new structural design of hole-transporting material, Trux-OMeTAD, which consists of a C3h Truxene-core with arylamine terminals and hexyl side-chains. This planar, rigid, and fully conjugated molecule exhibits excellent hole mobility and desired surface energy to the perovskite uplayer. Perovskite solar cells fabricated using the p-i-n architecture with Trux-OMeTAD as the p-layer, show a high PCE of 18.6% with minimal hysteresis.

On the Extraction of Charge Carrier Mobility in High-Mobility Organic Transistors.

Transistor parameter extraction by the conventional transconductance method can lead to a mobility overestimate. Organic transistors undergoing major contact resistance experience a significant drop in mobility upon mild annealing. Before annealing, strong field-dependent contact resistance yields nonlinear transfer curves with locally high transconductances, resulting in a mobility overestimate. After annealing, a contact resistance below 200 Ω cm is achieved, which is stable over a wide V(G) range.