Solution‐Processed Low Threshold Vertical Cavity Surface Emitting Lasers from All‐Inorganic Perovskite Nanocrystals

Recently, newly engineered all‐inorganic cesium lead halide perovskite nanocrystals (IPNCs) (CsPbX₃, X = Cl, Br, I) are discovered to possess superior optical gain properties appealing for solution‐processed cost‐effective lasers. Yet, the potential of such materials has not been exploited for practical laser devices, rendering the prospect as laser media elusive. Herein, the challenging but practically desirable vertical cavity surface emitting lasers (VCSELs) based on the CsPbX₃ IPNCs, featuring low threshold (9 µJ cm^?2), directional output (beam divergence of ≈3.6°), and favorable stability, are realized for the first time. Notably, the lasing wavelength can be tuned across the red, green, and blue region maintaining comparable thresholds, which is promising in developing single‐source‐pumped full‐color visible lasers. It is fully demonstrated that the characteristics of the VCSELs can be versatilely engineered by independent adjustment of the cavity and solution‐processable nanocrystals. The results unambiguously reveal the feasibility of the emerging CsPbX₃ IPNCs as practical laser media and represent a significant leap toward CsPbX₃ IPNC‐based laser devices.     

Record‐Low‐Threshold Lasers Based on Atomically Smooth Triangular Nanoplatelet Perovskite

Single‐crystalline perovskites are ideal candidates for lasing and other optoelectronic applications. Although significant efforts have been made to grow both bulk single‐crystalline perovskites in liquid solution, their dimensions are still too large to make nanoscale whispering‐gallery‐mode (WGM) resonator based lasers that possess high quality (Q) factor and small volume. Besides, most reported perovskite resonators do not possess atomically smooth surfaces and facets, which limits the Q and thereby increases the lasing threshold. Here, atomically smooth triangular PbI₂ templates are fabricated on a mica substrate by the vapor phase deposition method and are converted to atomically smooth perovskites which have regular and unwrinkled facets with average surface roughness less than 2 nm. By using a CH₃NH₃PbI₃ nanoplatelet with a side length of 27 µm and thickness of 80 nm, room temperature WGM lasing with a Q up to 2600 is demonstrated, the highest reported for hybrid organic–inorganic perovskite nanoplatelets. In addition, the volume of the WGM mode is reduced significantly in comparison with the prior reports. The realized high‐quality triangular CH₃NH₃PbI₃ perovskite nanoplatelets with high Q factor and small volume are expected to perform as ideal cavities for long pulse durations lasers and would find potential applications in integrated optoelectronic devices.     

Low-Threshold,External-Cavity-Free Flexible Perovskite Lasers

A distinct advantage of halide perovskite semiconductors is their potential as gain media in high-performance, all-solution-processed flexible lasers. However, most perovskite microlasers employ external optical resonators with rigid and high-temperature/vaccum-processed structures unsuitable for flexible applications. Here, low-threshold, external-cavity-free perovskite lasers (≈550 nm, linewidth: ≈0.3 nm, quality factor: ≈1900, room temperature), prepared with excellent reproducibility using simple one-step spin-coating and low-temperature annealing, are demonstrated. Exceptionally low lasing thresholds of 9.3 and 14.6 µJ cm⁻² are achieved for external-cavity-free perovskite lasers on rigid and flexible substrates, respectively. The thresholds and quality factors are on par with that of high-performance perovskite microlasers with well-designed external cavities. The lasers exhibit good operational stability, showing half-life of >1.8 × 10⁸ pulses under optical pumping in air. Transient optical experiments reveal that the low thresholds stem from enhanced band-to-band spontaneous and stimulated emission processes in the high-quality microcrystalline perovskite, effectively out-pacing trap-mediated and Auger processes detrimental to the lasing action. The flexible perovskite lasers retain >95% of the initial intensity after 10000 bending cycles, showing outstanding mechanical durability. As these lasers can be produced from solution within minutes at low costs, the findings are expected to enable high-throughput, scalable fabrication of perovskite lasers for emerging applications.     

Tunable Near‐Infrared Organic Nanowire Nanolasers

Organic semiconductor nanowires have inherent advantages, such as amenability to low‐cost, low‐temperature processing, and inherent four‐level energy systems, which will significantly contribute to the organic solid‐state lasers (OSSLs) and miniaturized laser devices. However, the realization of near‐infrared (NIR) organic nanowire lasers is always a big challenge due to the difficultly in fabrication of organic nanowires with diameters of ≈100 nm and material issues such as low photoluminescence quantum efficiency in the red‐NIR region. What is more, the achievement of wavelength‐tunable OSSLs has also encountered enormous challenge. This study first demonstrates the 720 nm NIR lasing with a low lasing threshold of ≈1.4 µJ cm^?2 from the organic single‐crystalline nanowires, which are self‐assembled from small organic molecules of (E )‐3‐(4‐(dimethylamino)‐2‐methoxyphenyl)‐1‐(1‐hydroxynaphthalen‐2‐yl)prop‐2‐en‐1‐one through a facile solution‐phase growth method. Notably, these individual nanowires' Fabry–Pérot cavity can alternatively provide the red‐NIR lasing action at 660 or 720 nm from the 0–1 or 0–2 radiative transition channels, and the single (660 or 720 nm)/dual‐wavelength (660 and 720 nm) laser action can be achieved by modulating the length of these organic nanowires due to the intrinsic self‐absorption. These easily‐fabricated organic nanowires are natural laser sources, which offer considerable promise for coherent light devices integrated on the optics microchip.     

Multiphoton‐Pumped Highly Polarized Polariton Microlasers from Single Crystals of a Dye‐Coordinated Metal–Organic Framework

Room‐temperature, low‐threshold, photostable, cost‐effective, efficient, miniaturized, and all‐solid‐state lasers are highly desirable in many technological and medicinal applications. Here, an archetypical dye laser is introduced, with the above attributes, based on single‐crystalline microplates of a dye‐coordinated metal–organic framework (MOF) without an external cavity, holding a potential to be the next‐generation laser. With an exciton–polariton lasing mechanism combined with large multiphoton absorption cross sections, the lasing thresholds of the three microplates are in the range from 0.34 to 0.12 µJ cm^?2 under various optical pumping schemes. The lasing threshold is observed to be reduced with an increment in the order of optical nonlinearity involved in the pumping scheme. Lasing at an extreme‐red region is demonstrated, with a high photostability (with a drop in lasing output as low as 25% after 1.8 × 10⁶ cycles), a large degree of polarization (up to 92%), and an excellent conversion efficiency (up to 12%), thereby realizing a crucial milestone in the field of laser technology.     

Low‐Threshold Distributed‐Feedback Lasers Based on Pyrene‐Cored Starburst Molecules with 1,3,6,8‐Attached Oligo(9,9‐Dialkylfluorene) Arms

Here, a detailed characterization of the optical gain properties of sky‐blue‐light‐emitting pyrene‐cored 9,9‐dialkylfluorene starbursts is reported; it is shown that these materials possess encouragingly low laser thresholds and relatively high thermal and environmental stability. The materials exhibit high solid‐state photoluminescence (PL) quantum efficiencies (>90%) and near‐single‐exponential PL decay transients with excited state lifetimes of ～1.4 ns. The thin‐film slab waveguide amplified spontaneous emission (ASE)‐measured net gain reaches 75–78 cm^?1. The ASE threshold energy is found to remain unaffected by heating at temperatures up to 130 °C, 40 to 50 °C above T_g. The ASE remained observable for annealing temperatures up to 170 or 200 °C. 1D distributed feedback lasers with 75% fill factor and 320 nm period show optical pumping thresholds down to 38–65 Wcm^?2, laser slope efficiencies up to 3.9%, and wavelength tuning ranges of ～40 nm around 471–512 nm. In addition, these lasers have relatively long operational lifetimes, with N_1/2 ≥ 1.1 × 10⁵ pulses for unencapsulated devices operated at ten times threshold in air.     

High‐Quality Whispering‐Gallery‐Mode Lasing from Cesium Lead Halide Perovskite Nanoplatelets

Semiconductor micro/nano‐cavities with high quality factor (Q) and small modal volume provide critical platforms for exploring strong light‐matter interactions and quantum optics, enabling further development of coherent and quantum photonic devices. Constrained by exciton binding energy and thermal fluctuation, only a handful of wide‐band semiconductors such as ZnO and GaN have stable excitons at room temperature. Metal halide perovskite with cubic lattice and well‐controlled exciton may provide solutions. In this work, high‐quality single‐crystalline cesium lead halide CsPbX₃ (X = Cl, Br, I) whispering‐gallery‐mode (WGM) microcavities are synthesized by vapor‐phase van der Waals epitaxy method. The as‐grown perovskites show strong emission and stable exciton at room temperature over the whole visible spectra range. By varying the halide composition, multi‐color (400–700 nm).WGM excitonic lasing is achieved at room temperature with low threshold (~ 2.0 μJ cm^?2) and high spectra coherence (~0.14–0.15 nm). The results advocate the promise of inorganic perovskites towards development of optoelectronic devices and strong light‐matter coupling in quantum optics.     

Pyrene‐Capped Conjugated Amorphous Starbursts: Synthesis,Characterization, and Stable Lasing Properties in Ambient Atmosphere

A family of trigonal starburst conjugated molecules (TrFPy, TrFPy, and TrF2Py) composed of a truxene core and pyrene cappers with various bridge lengths is synthesized and characterized. The incorporation of pyrene cappers successfully depress the crystallization tendency, resulting in enhanced glassy temperature and improved morphological stability of the thin films. The high photoluminescence yield in neat films and excellent thermal stability render these pyrene‐capped starbursts promising lasing optical gain media. Low amplified spontaneous emission (ASE) thresholds (E_th^ASE) of 180 nJ pulse^‐1 and 101 nJ pulse^–1 were recorded for TrFPy and TrF2Py, respectively. One dimensional distributed feedback (1D DFB) lasers demonstrated lasing threshold of 9.3 kW/cm² and 7.3 kW/cm² for TrFPy (at 457 nm) and TrF2Py lasers (at 451 nm), respectively. The ASE performance of TrFPy and TrF2Py in an ambient condition was recorded with various annealing temperature (from 80 to 250 °C, 10 min). Surprisingly, TrFPy exhibited excellent ASE stability in an ambient condition, which is still detectable even after annealing at 250 °C for 10 min. The results suggest the pyrene‐capped molecular design strategy is positive on improving the optical gain stability and meanwhile maintaining excellent lasing properties.     

Cyano‐Substituted Oligo(p‐phenylene vinylene) Single Crystals: A Promising Laser Material

Organic crystals that combine high charge‐carrier mobility and excellent light‐emission characteristics are expected to be of interest for light‐emitting transistors and diodes, and may offer renewed hope for electrically pumped laser action. High‐luminescence‐efficiency cyano‐substituted oligo(p‐ phenylene vinylene) (CN‐DPDSB) crystals (η ≈ 95%) grown by the physical vapor transport method is reported here, with high mobilities (at ≈10^?2 cm² V^?1 s^?1 order of magnitude) as measured by time‐of‐flight. The CN‐DPDSB crystals have well‐balanced bipolar carrier‐transport characteristics (μ_hole≈ 2.5–5.5 × 10^?2 cm² V^?1 s^?1; μ_electron ≈ 0.9–1.3 × 10^?2 cm² V^?1 s^?1) and excellent optically pumped laser properties. The threshold for amplified spontaneous emission (ASE) is about 4.6 μJ per pulse (23 KW cm^?2), while the gain coefficient at the peak wavelength of ASE and the loss coefficient caused by scattering are ≈35 and ≈1.7 cm^?1, respectively. This indicates that CN‐DPDSB crystals are promising candidates for organic laser diodes.     

Ultrahigh‐Strength Ultrahigh Molecular Weight Polyethylene (UHMWPE)‐Based Fiber Electrode for High Performance Flexible Supercapacitors

Flexible fiber‐based supercapacitor (FSC) with excellent electrochemical performance and high tensile strength and modulus is strongly desired for some special circumstances, such as load‐bearing, abrasion resistant, and anticutting fabrics. Here, a series of ultrahigh‐strength fiber electrodes are prepared for flexible FSCs based on ultrahigh molecular weight polyethylene fibers, on which the polydopamine, Ag, and poly (3,4‐ethylene dioxythiophene): poly(styrenesulfonate) are deposited in sequence. The modified fiber‐based electrode exhibits superhigh strength up to 3.72 GPa, which is the highest among fiber‐based electrodes reported to date. In addition, FSCs fabricated with the optimized fiber electrode shows a specific areal capacity as high as 563 mF cm^?2 at 0.17 mA cm^?2, which corresponds to a high areal energy density of ≈50.1 µWh cm^?2 at a power density of ≈124 µW cm^?2. The specific areal capacity only decrease 8% after 1000 times bending test, indicating the outstanding bending performance of this composite fiber electrode. Furthermore, several FSCs can be connected in series or in parallel to get higher working voltage or higher capacity respectively, which demonstrates its potential for broad applications in flexible devices.     

Host Exciton Confinement for Enhanced Förster‐Transfer‐Blend Gain Media Yielding Highly Efficient Yellow‐Green Lasers

This paper reports state‐of‐the‐art fluorene‐based yellow‐green conjugated polymer blend gain media using Förster resonant‐energy‐transfer from novel blue‐emitting hosts to yield low threshold (≤7 kW cm^?2) lasers operating between 540 and 590 nm. For poly(9,9‐dioctylfluorene‐co‐benzothiadiazole) (F8BT) (15 wt%) blended with the newly synthesized 3,6‐bis(2,7‐di([1,1′‐biphenyl]‐4‐yl)‐9‐phenyl‐9H‐fluoren‐9‐yl)‐9‐octyl‐9H–carbazole (DBPhFCz) a highly desirable more than four times increase (relative to F8BT) in net optical gain to 90 cm^?1 and 34 times reduction in amplified spontaneous emission threshold to 3 µJ cm^?2 is achieved. Detailed transient absorption studies confirm effective exciton confinement with consequent diffusion‐limited polaron‐pair generation for DBPhFCz. This delays formation of host photoinduced absorption long enough to enable build‐up of the spectrally overlapped, guest optical gain, and resolves a longstanding issue for conjugated polymer photonics. The comprehensive study further establishes that limiting host conjugation length is a key factor therein, with 9,9‐dialkylfluorene trimers also suitable hosts for F8BT but not pentamers, heptamers, or polymers. It is additionally demonstrated that the host highest occupied and lowest unoccupied molecular orbitals can be tuned independently from the guest gain properties. This provides the tantalizing prospect of enhanced electron and hole injection and transport without endangering efficient optical gain; a scenario of great interest for electrically pumped amplifiers and lasers.     

Enhanced Photocatalytic Activity using Layer‐by‐Layer Electrospun Constructs for Water Remediation

Endocrine disruptors such as bisphenol A (BPA) are environmental pollutants that interfere with the body's endocrine system because of their structural similarity to natural and synthetic hormones. Due to their strong oxidizing potential to decompose such organic pollutants, colloidal metal oxide photocatalysts have attracted increasing attention for water detoxification. However, achieving both long‐term physical stability and high efficiency simultaneously with such photocatalytic systems poses many challenges. Here a layer‐by‐layer (LbL) deposition approach is reported for immobilizing TiO₂ nanoparticles (NPs) on a porous support while maintaining a high catalytic efficiency for photochemical decomposition of BPA. Anatase TiO₂ NPs ≈7 nm in diameter self‐assemble in consecutive layers with positively charged polyhedral oligomeric silsesquioxanes on a high surface area, porous electrospun polymer fiber mesh. The TiO₂ LbL nanofibers decompose approximately 2.2 mg BPA per mg of TiO₂ in 40 h of illumination (AM 1.5G illumination), maintaining first‐order kinetics with a rate constant (k) of 0.15 h^?1 for over 40 h. Although the colloidal TiO₂ NPs initially show significantly higher photocatalytic activity (k ≈ 0.84 h^?1), the rate constant drops to k ≈ 0.07 h^?1 after 4 h of operation, seemingly due to particle agglomeration. In the BPA solution treated with the multilayered TiO₂ nanofibers for 40 h, the estrogenic activity, based on human breast cancer cell proliferation, is significantly lower than that in the BPA solution treated with colloidal TiO₂ NPs under the same conditions. This study demonstrates that water‐based, electrostatic LbL deposition effectively immobilizes and stabilizes TiO₂ NPs on electrospun polymer nanofibers for efficient extended photochemical water remediation.     

Phthalocyanine‐Based 2D Conjugated Metal‐Organic Framework Nanosheets for High‐Performance Micro‐Supercapacitors

2D conjugated metal‐organic frameworks (2D c‐MOFs) are emerging as a novel class of conductive redox‐active materials for electrochemical energy storage. However, developing 2D c‐MOFs as flexible thin‐film electrodes have been largely limited, due to the lack of capability of solution‐processing and integration into nanodevices arising from the rigid powder samples by solvothermal synthesis. Here, the synthesis of phthalocyanine‐based 2D c‐MOF (Ni₂[CuPc(NH)₈]) nanosheets through ball milling mechanical exfoliation method are reported. The nanosheets feature with average lateral size of ≈160 nm and mean thickness of ≈7 nm (≈10 layers), and exhibit high crystallinity and chemical stability as well as a p‐type semiconducting behavior with mobility of ≈1.5 cm² V^?1 s^?1 at room temperature. Benefiting from the ultrathin feature, the nanosheets allow high utilization of active sites and facile solution‐processability. Thus, micro‐supercapacitor (MSC) devices are fabricated mixing Ni₂[CuPc(NH)₈] nanosheets with exfoliated graphene, which display outstanding cycling stability and a high areal capacitance up to 18.9 mF cm^?2; the performance surpasses most of the reported conducting polymers‐based and 2D materials‐based MSCs.     

Analysis of Cavity‐Mode Lasing Characteristics from a Resonator with Broadband Cholesteric Liquid‐Crystal Bragg Reflectors

Detailed optical lasing characteristics in liquid crystal (LC) microlasers consisting of multiple polymer cholesteric LC (PCLC) layers are presented as broadband resonators sandwiching a layer of thick gain media, dye‐containing nematic LC (NLC) or isotropic liquid, in between. Multiple lasing emission peaks due to Fabry‐Perot cavity modes are observed for both gain media, and their polarization characteristics investigated. To analyze lasing characteristics, specified eigen modes are defined, the polarization states of which are maintained before and after passing through the broadband resonator, and obtained for the present full system by using the Berreman 4 × 4 matrix method. Using these specified eigen modes, the optical density for each mode is calculated and compared with the experimental results, and shows good agreement. Finally, lasing characteristics between the resonators with NLC and isotropic gain media are compared, and the advantages of adopting dye‐doped NLC gain medium are shown for tunable red, green, blue lasing in a microlaser system with a broadband resonator.     

Optical Gain in the Near Infrared by Light‐Emitting Electrospun Fibers

The potential integration of polymer nanofibers in photonic devices and circuits is a major driver for research on their waveguiding and optical gain properties. Emission in the near‐infrared is especially important in this framework in view of the realization of nanofiber‐based optical amplifiers. Here, the optical gain properties of electrospun fibers embedding near‐infrared light‐emitting molecules are investigated. Upon pulsed optical pumping, line narrowing typical of amplified spontaneous emission is observed, with gain of 5.5 cm^?1 and threshold fluence down to 0.25 mJ cm^?2. Importantly, the stimulated emission characteristics are strongly dependent on individual fiber characteristics and on the mutual alignment of nanofibers in arrays, thus being tailorable through the fiber architecture and assembling. These results open interesting perspectives for the exploitation of electrospun fibers as active components in the near‐infrared range.     

Long Minority‐Carrier Diffusion Length and Low Surface‐Recombination Velocity in Inorganic Lead‐Free CsSnI3 Perovskite Crystal for Solar Cells

Sn‐based perovskites are promising Pb‐free photovoltaic materials with an ideal 1.3 eV bandgap. However, to date, Sn‐based thin film perovskite solar cells have yielded relatively low power conversion efficiencies (PCEs). This is traced to their poor photophysical properties (i.e., short diffusion lengths (<30 nm) and two orders of magnitude higher defect densities) than Pb‐based systems. Herein, it is revealed that melt‐synthesized cesium tin iodide (CsSnI₃) ingots containing high‐quality large single crystal (SC) grains transcend these fundamental limitations. Through detailed optical spectroscopy, their inherently superior properties are uncovered, with bulk carrier lifetimes reaching 6.6 ns, doping concentrations of around 4.5 × 10¹⁷ cm^?3, and minority‐carrier diffusion lengths approaching 1 µm, as compared to their polycrystalline counterparts having ≈54 ps, ≈9.2 × 10¹⁸ cm^?3, and ≈16 nm, respectively. CsSnI₃ SCs also exhibit very low surface recombination velocity of ≈2 × 10³ cm s^?1, similar to Pb‐based perovskites. Importantly, these key parameters are comparable to high‐performance p‐type photovoltaic materials (e.g., InP crystals). The findings predict a PCE of ≈23% for optimized CsSnI₃ SCs solar cells, highlighting their great potential.     

An Organic Laser Dye having a Small Singlet‐Triplet Energy Gap Makes the Selection of a Host Material Easier

Quenching of singlets by long‐lived triplets is a serious issue for lasing from organic laser dyes, especially under long pulse excitation. As a strategy to scavenge or manage unnecessary triplets, an organic laser dye is dispersed into a host material having high singlet and low triplet energy levels [a large singlet‐triplet energy gap (ΔE_ST)]. However, finding such a host material having a triplet scavenging capability is limited. In this study, an organic laser dye, 2,6‐dicyano‐1,1‐diphenyl‐λ⁵σ⁴‐phosphinine (DCNP), having a small ΔE_ST of ≈0.44 eV is synthesized, and thus 4‐4′‐bis[(N‐carbazole)styryl] biphenyl (BSBCz) can be employed as a triplet scavenging host, i.e., the triplets formed on DCNP are easily transferred to BSBCz. A 1 wt%‐DCNP‐doped BSBCz film is formed on a mixed‐order distributed feedback grating, showing lasing with a low threshold value of ≈0.86 µJ cm^?2 and a full‐width‐at‐half‐maximum value of ≈0.5 nm. Because of the suppressed singlet‐triplet annihilation, DCNP‐based laser devices operating under a continuous‐wave regime, with a low threshold of 72 W cm^?2 and a long laser half‐lifetime of ≈3 min, are demonstrated. These results indicate a possibility of the wider selection of host materials, easing a material design strategy of fabricating high‐performance laser devices in future.     

Low Amplified Spontaneous Emission Threshold from Organic Dyes Based on Bis‐stilbene

Advanced organic laser dyes exhibiting high solubility and bipolar behavior are developed based on a structure combining bis‐stilbene with carbazole (BSBCz). The materials show high photoluminescence quantum yields and large radiative rate constants in solutions, crystals, and blend and neat films. The introduction of alkyl groups significantly improves the solubility of BSBCz, and solution‐processed films of the alkyl‐substituted derivatives exhibit amplified spontaneous emission thresholds as low as 0.59 µJ cm^?2, which is comparable to those of vacuum‐deposited BSBCz films. On the other hand, cyano‐substitution on BSBCz (BSBCz‐CN) increases electron‐accepting properties, resulting in a bathochromic shift of the emission wavelength and improved bipolar behavior. In a BSBCz‐CN‐doped film, a low ASE threshold of 0.63 µJ cm^?2 is achieved, which is one of the lowest values for organic laser dyes with green emission. In addition, organic light‐emitting diodes based on BSBCz‐CN neat films exhibit external quantum efficiencies of 1.8% and could withstand injection of high current densities of up to 500 A cm^?2 under pulse operation. These properties along with low excited‐state absorption cross sections make these materials an outstanding addition to the existing library of organic laser dyes, especially for consideration in electrically pumped lasers.     

Non‐Lithographic Fabrication of All‐2D α‐MoTe2 Dual Gate Transistors

As one of the emerging new transition‐metal dichalcogenides materials, molybdenum ditelluride (α‐MoTe₂) is attracting much attention due to its optical and electrical properties. This study fabricates all‐2D MoTe₂‐based field effect transistors (FETs) on glass, using thin hexagonal boron nitride and thin graphene in consideration of good dielectric/channel interface and source/drain contacts, respectively. Distinguished from previous works, in this study, all 2D FETs with α‐MoTe₂ nanoflakes are dual‐gated for driving higher current. Moreover, for the present 2D dual gate FET fabrications on glass, all thermal annealing and lithography processes are intentionally exempted for fully non‐lithographic method using only van der Waal's forces. The dual‐gate MoTe₂ FET displays quite a high hole and electron mobility over ≈20 cm² V^?1 s^?1 along with ON/OFF ratio of ≈10⁵ in maximum as an ambipolar FET and also demonstrates high drain current of a few tens‐to‐hundred μA at a low operation voltage. It appears promising enough to drive organic light emitting diode pixels and NOR logic functions on glass.     

Interfacial Approach toward Benzene‐Bridged Polypyrrole Film–Based Micro‐Supercapacitors with Ultrahigh Volumetric Power Density

2D soft nanomaterials are an emerging research field due to their versatile chemical structures, easily tunable properties, and broad application potential. In this study, a benzene‐bridged polypyrrole film with a large area, up to a few square centimeters, is synthesized through an interfacial polymerization approach. As‐prepared semiconductive films exhibit a bandgap of ≈2 eV and a carrier mobility of ≈1.5 cm² V^?1 s^?1, inferred from time‐resolved terahertz spectroscopy. The samples are employed to fabricate in‐plane micro‐supercapacitors (MSCs) by laser scribing and exhibit an ultrahigh areal capacitance of 0.95 mF cm^?2, using 1‐ethyl‐3‐methylimidazolium tetrafluoroborate ([EMIM][BF₄]) as an electrolyte. Importantly, the maximum energy and power densities of the developed MSCs reach values up to 50.7 mWh cm^?3 and 9.6 kW cm^?3, respectively; the performance surpassing most of the 2D material‐based MSCs is reported to date.