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Perovskite light-emitting diodes (PeLEDs) have emerged as a strong contender for next-generation display and information technologies. However, similar to perovskite solar cells, the poor operational stability remains the main obstacle toward commercial applications. Here we demonstrate ultra-stable and efficient PeLEDs with extraordinary operational lifetimes (T50) of 1.0x10^4 h, 2.8x10^4 h, 5.4x10^5 h, and 1.9x10^6 h at initial radiance (or current densities) of 3.7 W/sr/m2 (~5 mA/cm2), 2.1 W/sr/m2 (~3.2 mA/cm2), 0.42 W/sr/m2 (~1.1 mA/cm2), and 0.21 W/sr/m2 (~0.7 mA/cm2) respectively, and external quantum efficiencies of up to 22.8%. Key to this breakthrough is the introduction of a dipolar molecular stabilizer, which serves two critical roles simultaneously. First, it prevents the detrimental transformation and decomposition of the alpha-phase FAPbI3 perovskite, by inhibiting the formation of lead and iodide intermediates. Secondly, hysteresis-free device operation and microscopic luminescence imaging experiments reveal substantially suppressed ion migration in the emissive perovskite. The record-long PeLED lifespans are encouraging, as they now satisfy the stability requirement for commercial organic LEDs (OLEDs). These results remove the critical concern that halide perovskite devices may be intrinsically unstable, paving the path toward industrial applications., Comment: This is a preprint of the paper prior to peer review. New and updated results may be available in the final version from the publisher

Quantum-dot light-emitting diodes (QD-LEDs) promise a new generation of efficient, low-cost, large-area, and flexible electroluminescent devices. However, the inferior performance of green and blue QD-LEDs is hindering the commercialization of QD-LEDs in display and solid-state lighting. Here, we demonstrate best-performing green and blue QD-LEDs with ~100% conversion of the injected charge carriers into emissive excitons. Key to this success is eliminating electron leakage at the organic/inorganic interface by using hole-transport polymers with low electron affinity and reduced energetic disorder. Our devices exhibit record-high peak external quantum efficiencies (28.7% for green, 21.9% for blue), exceptionally high efficiencies in wide ranges of luminance, and unprecedented stability (T95 lifetime: 580,000 h for green, 4,400 h for blue). The overall performance surpasses previously reported solution-processed green and blue LEDs.

The radiative recombination of injected charge carriers gives rise to electroluminescence (EL), a central process for light-emitting diode (LED) operation. It is often presumed in some emerging fields of optoelectronics, including perovskite and organic LEDs, that the minimum voltage required for light emission is the semiconductor bandgap divided by the elementary charge. Here we show for many classes of LEDs, including those based on metal halide perovskite, organic, chalcogenide quantum-dot and commercial III-V semiconductors, photon emission can be generally observed at record-low driving voltages of 36%-60% of their bandgaps, corresponding to a large apparent energy gain of 0.6-1.4 eV per emitted photon. Importantly, for various classes of LEDs with very different modes of charge injection and recombination (dark saturation current densities ranging from ~10^-35 to ~10^-21 mA/cm2), their EL intensity-voltage curves under low voltages exhibit similar behaviors, revealing a universal origin of ultralow-voltage device operation. Finally, we demonstrate as a proof-of-concept that perovskite LEDs can transmit data efficiently to a silicon detector at 1V, a voltage below the silicon bandgap. Our work provides a fresh insight into the operational limits of electroluminescent diodes, highlighting the significant potential of integrating low-voltage LEDs with silicon electronics for next-generation communications and computational applications.

The Shockley-Queisser (SQ) limit, introduced by W. Shockley and H. J. Queisser in 1961, is the most well-established fundamental efficiency limit for single-junction photovoltaic solar cells. For widely-studied semiconductors such as Si, GaAs and lead-halide perovskite, the SQ limits under standard solar illumination (1-sun) are 32.7%, 32.5% and 31% for bandgaps of 1.12 eV, 1.43 eV and 1.55 eV, respectively. Here, we propose that the fundamental efficiency limits for single-junction solar cells may be surpassed via photon confinement, substantially raising the theoretical limits to 49%, 45.2% and 42.1% for Si, GaAs and methylammonium lead iodide (MAPbI3) perovskite cells under 1-sun. Such enhancement is possible through the containment of luminescent photons within the solar cell, allowing the suppression of both non-radiative and radiative recombination losses, which were considered inevitable in the classical SQ model. Importantly, restricting photon emission from the solar cells raises the open-circuit voltage (VOC) to values approaching the semiconductor bandgaps, surpassing the theoretical VOC values predicted by the SQ model. The fill factors of the cells are expected to increase substantially, resulting in current-voltage characteristics with very-high squareness for ideal diode operation. Our work introduces a new framework for improving solar cell performance beyond the conventional limits.

Electroluminescence (EL) of colloidal nanocrystals promises a new generation of high-performance and solution-processable light-emitting diodes (LEDs). The operation of nanocrystal-based LEDs relies on the recombination of electrically-generated excitons. However, a fundamental question, i.e, how excitons are electrically generated in individual nanocrystals, remains unanswered. Here, we reveal a molecular mechanism of sequential electron-hole injection for the exciton generation in nanocrystal-based EL devices. To decipher the corresponding elementary processes, we develop electrically-pumped single-nanocrystal spectroscopy. While hole injection into neutral quantum dots (QDs) is generally-considered to be inefficient, we find that the intermediate negatively-charged state of QD triggers confinement-enhanced Coulomb interactions, which simultaneously accelerate hole injection and hinder excessive electron injection. In-situ/operando spectroscopy on state-of-the-art QD-LEDs demonstrate that exciton generation at the ensemble level is consistent with the charge-confinement-enabled sequential electron-hole injection mechanism revealed at the single-nanocrystal level. Our findings provide a universal mechanism for enhancing charge balance in nanocrystal-based EL devices.

Electronic skin, a class of wearable electronic sensors that mimic the functionalities of human skin, has made remarkable success in applications including health monitoring, human-machine interaction and electronic-biological interfaces. While electronic skin continues to achieve higher sensitivity and faster response, its ultimate performance is fundamentally limited by the nature of low-frequency AC currents in electronic circuitries. Here we demonstrate highly sensitive optical skin (O-skin) in which the primary sensory elements are optically driven. The simple construction of the sensors is achieved by embedding glass micro/nanofibers (MNFs) in thin layers of polydimethylsiloxane (PDMS). Enabled by the highly sensitive power-leakage response of the guided modes from the MNF upon external stimuli, our optical sensors show ultrahigh sensitivity (1870/kPa), low detection limit (7 mPa) and fast response (10 microseconds) for pressure sensing, significantly exceeding the performance metrics of state-of-the-art electronic skins. Electromagnetic interference (EMI)-free detection of high-frequency vibrations, wrist pulse and human voice are realized. Moreover, a five-sensor optical data glove and a 2x2-MNF tactile sensor are demonstrated. Our results pave the way toward wearable optical devices ranging from ultrasensitive flexible sensors to optical skins.

Perovskite-based optoelectronic devices have gained significant attention due to their remarkable performance and low processing cost, particularly for solar cells. However, for perovskite light-emitting diodes (LEDs), non-radiative charge carrier recombination has limited electroluminescence (EL) efficiency. Here we demonstrate perovskite-polymer bulk heterostructure LEDs exhibiting record-high external quantum efficiencies (EQEs) exceeding 20%, and an EL half-life of 46 hours under continuous operation. This performance is achieved with an emissive layer comprising quasi-2D and 3D perovskites and an insulating polymer. Transient optical spectroscopy reveals that photogenerated excitations at the quasi-2D perovskite component migrate to lower-energy sites within 1 ps. The dominant component of the photoluminescence (PL) is primarily bimolecular and is characteristic of the 3D regions. From PL quantum efficiency and transient kinetics of the emissive layer with/without charge-transport contacts, we find non-radiative recombination pathways to be effectively eliminated. Light outcoupling from planar LEDs, as used in OLED displays, generally limits EQE to 20-30%, and we model our reported EL efficiency of over 20% in the forward direction to indicate the internal quantum efficiency (IQE) to be close to 100%. Together with the low drive voltages needed to achieve useful photon fluxes (2-3 V for 0.1-1 mA/cm2), these results establish that perovskite-based LEDs have significant potential for light-emission applications.

The efficiency of an organic light-emitting diode (OLED) is fundamentally governed by the spin of recombining electron-hole pairs (singlet and triplet excitons), since triplets cannot usually emit light. The singlet-triplet energy gap, a key factor for efficient utilization of triplets, is normally positive. Here we show that in a family of materials with amide donor and carbene acceptor moieties linked by a metal, this energy gap for singlet and triplet excitons with charge-transfer character can be tuned from positive to negative values via the rotation of donor and acceptor about the metal-amide bond. When the gap is close to zero, facile intersystem crossing is possible, enabling efficient emission from singlet excitons. We demonstrate solution-processed LEDs with exceptionally high quantum efficiencies (near-100% internal and >27% external quantum efficiencies), and current and power efficiencies (87 cd/A and 75 lm/W) comparable to, or exceeding, those of state-of-the-art vacuum-processed OLEDs and quantum dot LEDs.