Toward Nonepitaxial Laser Diodes.

Thin-film organic, colloidal quantum dot, and metal halide perovskite semiconductors are all being pursued in the quest for a wavelength-tunable diode laser technology that does not require epitaxial growth on a traditional semiconductor substrate. Despite promising demonstrations of efficient light-emitting diodes and low-threshold optically pumped lasing in each case, there are still fundamental and practical barriers that must be overcome to reliably achieve injection lasing. This review outlines the historical development and recent advances of each material system on the path to a diode laser. Common challenges in resonator design, electrical injection, and heat dissipation are highlighted, as well as the different optical gain physics that make each system unique. The evidence to date suggests that continued progress for organic and colloidal quantum dot laser diodes will likely hinge on the development of new materials or indirect pumping schemes, while improvements in device architecture and film processing are most critical for perovskite lasers. In all cases, systematic progress will require methods that can quantify how close new devices get with respect to their electrical lasing thresholds. We conclude by discussing the current status of nonepitaxial laser diodes in the historical context of their epitaxial counterparts, which suggests that there is reason to be optimistic for the future.

Hot-Casting-Assisted Liquid Additive Engineering for Efficient and Stable Perovskite Solar Cells.

High-performance inorganic-organic lead halide perovskite solar cells (PSCs) are often fabricated with a liquid additive such as dimethyl sulfoxide (DMSO), which retards crystallization and reduces roughness and pinholes in the perovskite layers. However, DMSO can be trapped during perovskite film formation and induce voids and undesired reaction byproducts upon later processing steps. Here, it is shown that the amount of residual DMSO can be reduced in as-spin-coated films significantly through use of preheated substrates, or a so-called hot-casting method. Hot casting increases the perovskite film thickness given the same concentration of solutions, which allows for reducing the perovskite solution concentration. By reducing the amount of DMSO in proportion to the concentration of perovskite precursors and using hot casting, it is possible to fabricate perovskite layers with improved perovskite-substrate interfaces by suppressing the formation of byproducts, which increase trap density and accelerate degradation of the perovskite layers. The best-performing PSCs exhibit a power conversion efficiency (PCE) of 23.4% (23.0% stabilized efficiency) under simulated solar illumination. Furthermore, encapsulated devices show considerably reduced post-burn-in decay, retaining 75% and 90% of their initial and post-burn-in efficiencies after 3000 h of operation with maximum power point tracking (MPPT) under high power of ultraviolet (UV)-containing continuous light exposure.

Nanosecond-Pulsed Perovskite Light-Emitting Diodes at High Current Density.

While metal-halide perovskite light-emitting diodes (PeLEDs) hold the potential for a new generation of display and lighting technology, their slow operation speed and response time limit their application scope. Here, high-speed PeLEDs driven by nanosecond electrical pulses with a rise time of 1.2 ns are reported with a maximum radiance of approximately 480 kW sr-1  m-2 at 8.3 kA cm-2 , and an external quantum efficiency (EQE) of 1% at approximately 10 kA cm-2 , through improved device configuration designs and material considerations. Enabled by the fast operation of PeLEDs, the temporal response provides access to transient charge carrier dynamics under electrical excitation, revealing several new electroluminescence quenching pathways. Finally, integrated distributed feedback (DFB) gratings are explored, which facilitate more directional light emission with a maximum radiance of approximately 1200 kW sr-1  m-2 at 8.5 kA cm-2 , a more than two-fold enhancement to forward radiation output.

Thermal Management Enables Bright and Stable Perovskite Light-Emitting Diodes.

The performance of lead-halide perovskite light-emitting diodes (LEDs) has increased rapidly in recent years. However, most reports feature devices operated at relatively small current densities (<500 mA cm-2 ) with moderate radiance (<400 W sr-1 m-2 ). Here, Joule heating and inefficient thermal dissipation are shown to be major obstacles toward high radiance and long lifetime. Several thermal management strategies are proposed in this work, such as doping charge-transport layers, optimizing device geometry, and attaching heat spreaders and sinks. Combining these strategies, high-performance perovskite LEDs are demonstrated with maximum radiance of 2555 W sr-1 m-2 , peak external quantum efficiency (EQE) of 17%, considerably reduced EQE roll-off (EQE > 10% to current densities as high as 2000 mA cm-2 ), and tenfold increase in operational lifetime (when driven at 100 mA cm-2 ). Furthermore, with proper thermal management, a maximum current density of 2.5 kA cm-2 and an EQE of ≈1% at 1 kA cm-2 are shown using electrical pulses, which represents an important milestone toward electrically driven perovskite lasers.

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.

Improved Outcoupling Efficiency and Stability of Perovskite Light-Emitting Diodes using Thin Emitting Layers.

Hybrid organic-inorganic perovskite semiconductors have shown potential to develop into a new generation of light-emitting diode (LED) technology. Herein, an important design principle for perovskite LEDs is elucidated regarding optimal perovskite thickness. Adopting a thin perovskite layer in the range of 35-40 nm is shown to be critical for both device efficiency and stability improvements. Maximum external quantum efficiencies (EQEs) of 17.6% for Cs0.2 FA0.8 PbI2.8 Br0.2 , 14.3% for CH3 NH3 PbI3 (MAPbI3 ), 10.1% for formamidinium lead iodide (FAPbI3 ), and 11.3% for formamidinium lead bromide (FAPbBr3 )-based LEDs are demonstrated with optimized perovskite layer thickness. Optical simulations show that the improved EQEs source from improved light outcoupling. Furthermore, elevated device temperature caused by Joule heating is shown as an important factor contributing to device degradation, and that thin perovskite emitting layers maintain lower junction temperature during operation and thus demonstrate increased stability.

Hybrid perovskite light emitting diodes under intense electrical excitation.

Hybrid perovskite semiconductors represent a promising platform for color-tunable light emitting diodes (LEDs) and lasers; however, the behavior of these materials under the intense electrical excitation required for electrically-pumped lasing remains unexplored. Here, we investigate methylammonium lead iodide-based perovskite LEDs under short pulsed drive at current densities up to 620 A cm-2. At low current density (J < 10 A cm-2), we find that the external quantum efficiency (EQE) depends strongly on the time-averaged history of the pulse train and show that this curiosity is associated with slow ion movement that changes the internal field distribution and trap density in the device. The impact of ions is less pronounced in the high current density regime (J > 10 A cm-2), where EQE roll-off is dominated by a combination of Joule heating and charge imbalance yet shows no evidence of Auger loss, suggesting that operation at kA cm-2 current densities relevant for a laser diode should be within reach.

A Photonic Crystal Laser from Solution Based Organo-Lead Iodide Perovskite Thin Films.

Perovskite semiconductors are actively investigated for high performance solar cells. Their large optical absorption coefficient and facile solution-based, low-temperature synthesis of thin films make perovskites also a candidate for light-emitting devices across the visible and near-infrared. Specific to their potential as optical gain medium for lasers, early work has demonstrated amplified spontaneous emission and lasing at attractively low thresholds of photoexcitation. Here, we take an important step toward practically usable perovskite lasers where a solution-processed thin film is embedded within a two-dimensional photonic crystal resonator. We demonstrate high degree of temporally and spatially coherent lasing whereby well-defined directional emission is achieved near 788 nm wavelength at optical pumping energy density threshold of 68.5 ± 3.0 µJ/cm(2). The measured power conversion efficiency and differential quantum efficiency of the perovskite photonic crystal laser are 13.8 ± 0.8% and 35.8 ± 5.4%, respectively. Importantly, our approach enables scalability of the thin film lasers to a two-dimensional multielement pixelated array of microlasers which we demonstrate as a proof-of-concept for possible projection display applications.

Surface-emitting red, green, and blue colloidal quantum dot distributed feedback lasers.

We demonstrate surface emitting distributed feedback (DFB) lasers across the red, green, and blue from densely packed colloidal quantum dot (CQD) films. The solid CQD films were deposited on periodic grating patterns to enable 2nd-order DFB lasing action at mere 120, 280, and 330 µJ/cm2 of optical pumping energy densities for red, green, and blue DFB lasers, respectively. The lasers operated in single mode operation with less than 1 nm of full-width-half-maximum. We measured far-field patterns showing high degree of spatial beam coherence. Specifically, by taking advantage of single exciton optical gain regime from our engineered CQDs, we can significantly suppress the Auger recombination to reduce lasing threshold and achieve quasi-steady state, optically pumped operation.