State Key Laboratory on Integrated Optoelectronics

Shine on you crazy dots: A rapid and high-output strategy allows the fabrication of polymer-like carbon dots (CDs) with quantum yields as high as ca. 80 %. This value is the highest reported to date for fluorescent carbon-based materials, and gives promise for their application in multicolor-patterning and biosensors. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Abstract In this review, the factors influencing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) is emphasized. The PCE of PSCs has remarkably increased from 3.8% to 23.7%, but on the other hand, poor stability is one of the main facets that creates a huge barrier in the commercialization of PSCs. Herein, a concise overview of the current efforts to enhance the stability of PSCs is provided; moreover, the degradation causes and mechanisms are summarized. The strategies to improve device stability are portrayed in terms of structural effects, a photoactive layer, hole‐ and electron‐transporting layers, electrode materials, and device encapsulation. Last but not least, the economic feasibility of PSCs is also vividly discussed.

Abstract The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based fluorescent material. Here, the surface chemistry of small size graphene (graphene quantum dots, GQDs) is tuned programmably through modification or reduction and green luminescent GQDs are changed to blue luminescent GQDs. Several tools are employed to characterize the composition and morphology of resultants. More importantly, using this system, the luminescence mechanism (the competition between both the defect state emission and intrinsic state emission) is explored in detail. Experiments demonstrate that the chemical structure changes during modification or reduction suppresses non‐radiative recombination of localized electron‐hole pairs and/or enhances the integrity of surface π electron network. Therefore the intrinsic state emission plays a leading role, as opposed to defect state emission in GQDs. The results of time‐resolved measurements are consistent with the suggested PL mechanism. Up‐conversion PL of GQDs is successfully applied in near‐IR excitation for bioimaging.

In recent years, semiconducting polymer nanoparticles have attracted considerable attention because of their outstanding characteristics as fluorescent probes. These nanoparticles, which primarily consist of π-conjugated polymers and are called polymer dots (Pdots) when they exhibit small particle size and high brightness, have demonstrated utility in a wide range of applications such as fluorescence imaging and biosensing. In this review, we summarize recent findings of the photophysical properties of Pdots which speak to the merits of these entities as fluorescent labels. This review also highlights the surface functionalization and biomolecular conjugation of Pdots, and their applications in cellular labeling, in vivo imaging, single-particle tracking, biosensing, and drug delivery. We discuss the relationship between the physical properties and performance, and evaluate the merits and limitations of the Pdot probes for certain imaging tasks and fluorescence assays. We also tackle the current challenges of Pdots and share our perspective on the future directions of the field.

The past 20 years have witnessed unprecedented progress in brain-computer interfaces (BCIs). However, low communication rates remain key obstacles to BCI-based communication in humans. This study presents an electroencephalogram-based BCI speller that can achieve information transfer rates (ITRs) up to 5.32 bits per second, the highest ITRs reported in BCI spellers using either noninvasive or invasive methods. Based on extremely high consistency of frequency and phase observed between visual flickering signals and the elicited single-trial steady-state visual evoked potentials, this study developed a synchronous modulation and demodulation paradigm to implement the speller. Specifically, this study proposed a new joint frequency-phase modulation method to tag 40 characters with 0.5-s-long flickering signals and developed a user-specific target identification algorithm using individual calibration data. The speller achieved high ITRs in online spelling tasks. This study demonstrates that BCIs can provide a truly naturalistic high-speed communication channel using noninvasively recorded brain activities.

A white light-emitting diode (0.33, 0.33) is fabricated using perovskite quantum dot/silica composites. It is shown to have greatly improved stability. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Farbenspiele: Polymerartige Kohlenstoffpunkte (CDs) können schnell und in großen Mengen hergestellt werden. Mit ca. 80 % erzielen die CDs die bisher höchsten Quantenausbeuten für fluoreszierende Kohlenstoffmaterialien, woraus sich Anwendungsmöglichkeiten in Vielfarben-Musterbildung und Biosensoren ergeben könnten. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

OBJECTIVE: This study proposes and evaluates a novel data-driven spatial filtering approach for enhancing steady-state visual evoked potentials (SSVEPs) detection toward a high-speed brain-computer interface (BCI) speller. METHODS: Task-related component analysis (TRCA), which can enhance reproducibility of SSVEPs across multiple trials, was employed to improve the signal-to-noise ratio (SNR) of SSVEP signals by removing background electroencephalographic (EEG) activities. An ensemble method was further developed to integrate TRCA filters corresponding to multiple stimulation frequencies. This study conducted a comparison of BCI performance between the proposed TRCA-based method and an extended canonical correlation analysis (CCA)-based method using a 40-class SSVEP dataset recorded from 12 subjects. An online BCI speller was further implemented using a cue-guided target selection task with 20 subjects and a free-spelling task with 10 of the subjects. RESULTS: The offline comparison results indicate that the proposed TRCA-based approach can significantly improve the classification accuracy compared with the extended CCA-based method. Furthermore, the online BCI speller achieved averaged information transfer rates (ITRs) of 325.33 ± 38.17 bits/min with the cue-guided task and 198.67 ± 50.48 bits/min with the free-spelling task. CONCLUSION: This study validated the efficiency of the proposed TRCA-based method in implementing a high-speed SSVEP-based BCI. SIGNIFICANCE: The high-speed SSVEP-based BCIs using the TRCA method have great potential for various applications in communication and control.

OBJECTIVE: Recently, canonical correlation analysis (CCA) has been widely used in steady-state visual evoked potential (SSVEP)-based brain-computer interfaces (BCIs) due to its high efficiency, robustness, and simple implementation. However, a method with which to make use of harmonic SSVEP components to enhance the CCA-based frequency detection has not been well established. APPROACH: This study proposed a filter bank canonical correlation analysis (FBCCA) method to incorporate fundamental and harmonic frequency components to improve the detection of SSVEPs. A 40-target BCI speller based on frequency coding (frequency range: 8-15.8 Hz, frequency interval: 0.2 Hz) was used for performance evaluation. To optimize the filter bank design, three methods (M1: sub-bands with equally spaced bandwidths; M2: sub-bands corresponding to individual harmonic frequency bands; M3: sub-bands covering multiple harmonic frequency bands) were proposed for comparison. Classification accuracy and information transfer rate (ITR) of the three FBCCA methods and the standard CCA method were estimated using an offline dataset from 12 subjects. Furthermore, an online BCI speller adopting the optimal FBCCA method was tested with a group of 10 subjects. MAIN RESULTS: The FBCCA methods significantly outperformed the standard CCA method. The method M3 achieved the highest classification performance. At a spelling rate of ∼33.3 characters/min, the online BCI speller obtained an average ITR of 151.18 ± 20.34 bits min(-1). SIGNIFICANCE: By incorporating the fundamental and harmonic SSVEP components in target identification, the proposed FBCCA method significantly improves the performance of the SSVEP-based BCI, and thereby facilitates its practical applications such as high-speed spelling.

High photoluminescence quantum yield, easily tuned emission colors, and high color purity of perovskite nanocrystals make this class of material attractive for light source or display applications. Here, green light-emitting devices (LEDs) were fabricated using inorganic cesium lead halide perovskite nanocrystals as emitters. By introducing a thin film of perfluorinated ionomer (PFI) sandwiched between the hole transporting layer and perovskite emissive layer, the device hole injection efficiency has been significantly enhanced. At the same time, PFI layer suppressed charging of the perovskite nanocrystal emitters thus preserving their superior emissive properties, which led to the three-fold increase in peak brightness reaching 1377 cd m(-2). The full width at half-maximum of the symmetric emission peak with color coordinates of (0.09, 0.76) was 18 nm, the narrowest value among perovskite based green LEDs.

Two-photon-pumped lasers have been regarded as a promising strategy to achieve frequency up-conversion for situations where the condition of phase matching required by conventional approaches cannot be fulfilled. However, their practical applications have been hindered by the lack of materials holding both efficient two-photon absorption and ease of achieving population inversion. Here, we show that this challenge can be tackled by employing colloidal nanocrystals of perovskite semiconductors. We observe highly efficient two-photon absorption (with a cross section of 2.7 × 10(6) GM) in toluene solutions of CsPbBr3 nanocrystals that can excite large optical gain (>500 cm(-1)) in thin films. We have succeeded in demonstrating stable two-photon-pumped lasing at a remarkable low threshold by coupling CsPbBr3 nanocrystals with microtubule resonators. Our findings suggest perovskite nanocrystals can be used as excellent gain medium for high-performance frequency-up-conversion lasers toward practical applications.

Organic-inorganic hybrid perovskite (OIHP) photodetectors that simultaneously achieve an ultrafast response and high sensitivity in the near-infrared (NIR) region are prerequisites for expanding current monitoring, imaging, and optical communication capbilities. Herein, we demonstrate photodetectors constructed by OIHP and an organic bulk heterojunction (BHJ) consisting of a low-bandgap nonfullerene and polymer, which achieve broadband response spectra up to 1 μm with a highest external quantum efficiency of approximately 54% at 850 nm, an ultrafast response speed of 5.6 ns and a linear dynamic range (LDR) of 191 dB. High sensitivity, ultrafast speed and a large LDR are preeminent prerequisites for the practical application of photodetectors. Encouragingly, due to the high-dynamic-range imaging capacity, high-quality visible-NIR actual imaging is achieved by employing the OIHP photodetectors. We believe that state-of-the-art OIHP photodetectors can accelerate the translation of solution-processed photodetector applications from the laboratory to the imaging market.

Recent years have witnessed the rise of graphene and its applications in various electronic devices. Specifically, featuring excellent flexibility, transparency, conductivity, and mechanical robustness, graphene has emerged as a versatile material for flexible electronics. In the past decade, facilitated by various laser processing technologies, including the laser-treatment-induced photoreduction of graphene oxides, flexible patterning, hierarchical structuring, heteroatom doping, controllable thinning, etching, and shock of graphene, along with laser-induced graphene on polyimide, graphene has found broad applications in a wide range of electronic devices, such as power generators, supercapacitors, optoelectronic devices, sensors, and actuators. Here, the recent advancements in the laser fabrication of graphene-based flexible electronic devices are comprehensively summarized. The various laser fabrication technologies that have been employed for the preparation, processing, and modification of graphene and its derivatives are reviewed. A thorough overview of typical laser-enabled flexible electronic devices that are based on various graphene sources is presented. With the rapid progress that has been made in the research on graphene preparation methodologies and laser micronanofabrication technologies, graphene-based electronics may soon undergo fast development.

Carbon-dot based light-emitting diodes (LEDs) with driving current controlled color change are reported. These devices consist of a carbon-dot emissive layer sandwiched between an organic hole transport layer and an organic or inorganic electron transport layer fabricated by a solution-based process. By tuning the device structure and the injecting current density (by changing the applied voltage), we can obtain multicolor emission of blue, cyan, magenta, and white from the same carbon dots. Such a switchable EL behavior with white emission has not been observed thus far in single emitting layer structured nanomaterial LEDs. This interesting current density-dependent emission is useful for the development of colorful LEDs. The pure blue and white emissions are obtained by tuning the electron transport layer materials and the thickness of electrode.

We alloyed Zn2+ into CsPbI3 perovskite nanocrystals by partial substitution of Pb2+ with Zn2+, which does not change their crystalline phase. The resulting alloyed CsPb0.64Zn0.36I3 nanocrystals exhibited an improved, close-to-unity photoluminescence quantum yield of 98.5% due to the increased radiative decay rate and the decreased non-radiative decay rate. They also showed an enhanced stability, which correlated with improved effective Goldschmidt tolerance factors, by the incorporation of Zn2+ ions with a smaller radius than the Pb2+ ions. Simultaneously, the nanocrystals switched from n-type (for CsPbI3) to nearly ambipolar for the alloyed nanoparticles. The hole injection barrier of electroluminescent LEDs was effectively eliminated by using alloyed CsPb0.64Zn0.36I3 nanocrystals, and a high peak external quantum efficiency of 15.1% has been achieved.

Abstract Quantum cutting can realize the emission of multiple near‐infrared photons for each ultraviolet/visible photon absorbed, and has potential to significantly improve the photoelectric conversion efficiency (PCE) of solar cells. However, due to the lack of an ideal downconversion material, it has merely served as a principle in the laboratory until now. Here, the fabrication of a novel type of quantum cutting material, CsPbCl 1.5 Br 1.5 :Yb 3+ , Ce 3+ nanocrystals is presented. Benefiting from the larger absorption cross‐section, weaker electron–phonon coupling, and higher inner luminescent quantum yield (146%), the doped perovskite nanocrystals are successfully explored as a downconverter of commercial silicon solar cells (SSCs). Noticeably, the PCE of the SSCs is improved from 18.1% to 21.5%, with a relative enhancement of 18.8%. This work exhibits a cheap, convenient, and effective way to enhance the PCE of SSCs, which may be commercially popularized in the future.

Abstract Actuators that can convert environmental stimuli into mechanical work are widely used in intelligent systems, robots, and micromechanics. To produce robust and sensitive actuators of different scales, efforts are devoted to developing effective actuating schemes and functional materials for actuator design. Carbon‐based nanomaterials have emerged as preferred candidates for different actuating systems because of their low cost, ease of processing, mechanical strength, and excellent physical/chemical properties. Especially, due to their excellent photothermal activity, which includes both optical absorption and thermal conductivities, carbon‐based materials have shown great potential for use in photothermal actuators. Herein, the recent advances in photothermal actuators based on various carbon allotropes, including graphite, carbon nanotubes, amorphous carbon, graphene and its derivatives, are reviewed. Different photothermal actuating schemes, including photothermal effect–induced expansion, desorption, phase change, surface tension gradient creation, and actuation under magnetic levitation, are summarized, and the light‐to‐heat and heat‐to‐work conversion mechanisms are discussed. Carbon‐based photothermal actuators that feature high light‐to‐work conversion efficiency, mechanical robustness, and noncontact manipulation hold great promise for future autonomous systems.

This paper presents a benchmark steady-state visual evoked potential (SSVEP) dataset acquired with a 40-target brain- computer interface (BCI) speller. The dataset consists of 64-channel Electroencephalogram (EEG) data from 35 healthy subjects (8 experienced and 27 naïve) while they performed a cue-guided target selecting task. The virtual keyboard of the speller was composed of 40 visual flickers, which were coded using a joint frequency and phase modulation (JFPM) approach. The stimulation frequencies ranged from 8 Hz to 15.8 Hz with an interval of 0.2 Hz. The phase difference between two adjacent frequencies was . For each subject, the data included six blocks of 40 trials corresponding to all 40 flickers indicated by a visual cue in a random order. The stimulation duration in each trial was five seconds. The dataset can be used as a benchmark dataset to compare the methods for stimulus coding and target identification in SSVEP-based BCIs. Through offline simulation, the dataset can be used to design new system diagrams and evaluate their BCI performance without collecting any new data. The dataset also provides high-quality data for computational modeling of SSVEPs. The dataset is freely available fromhttp://bci.med.tsinghua.edu.cn/download.html.

Abstract Cesium‐based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses ( E loss ) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI 2 Br absorber and polythiophene hole‐acceptor to minimize the E loss is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI 2 Br, can significantly reduce electron‐hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole‐injection into the hole‐acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed‐halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open‐circuit voltage ( V OC ) of up to 1.32 V and E loss of down to 0.5 eV, which both are the optimal values reported among cesium‐lead mixed‐halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the E loss .

Two-dimensional covalent–organic frameworks (2D COFs) have recently emerged as great prospects for their applications as new photocatalytic platforms in solar-to-hydrogen conversion; nevertheless, their inefficient solar energy capture and fast charge recombination hinder the improvement of photocatalytic hydrogen production performance. Herein, two photoactive three-component donor−π–acceptor (TCDA) materials were constructed using a multicomponent synthesis strategy by introducing electron-deficient triazine and electron-rich benzotrithiophene moieties into frameworks through sp2 carbon and imine linkages, respectively. Compared with two-component COFs, the novel TCDA-COFs are more convenient in regulating the inherent photophysical properties, thereby realizing outstanding photocatalytic activity for hydrogen evolution from water. Remarkably, the first sp2 carbon-linked TCDA-COF displays an impressive hydrogen evolution rate of 70.8 ± 1.9 mmol g–1 h–1 with excellent reusability in the presence of 1 wt % Pt under visible-light illumination (420–780 nm). Utilizing the combination of diversified spectroscopy and theoretical prediction, we show that the full π-conjugated linkage not only effectively broadens the visible-light harvesting of COFs but also enhances charge transfer and separation efficiency.