Coherent Random Lasing in Subwavelength Quasi‐2D Perovskites

Fruhling, Colton; Wang, Kang; Chowdhury, Sarah N.; Xu, Xiaohui; Simon, Jeffrey; Kildishev, Alexander V.; Dou, Letian; Meng, Xianwei; Boltasseva, Alexandra; Shalaev, Vladimir M.

doi:10.1002/lpor.202200314

Cited by 11 publications

(7 citation statements)

References 77 publications

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“…We chose FA-based perovskite layers instead of methylammonium (MA) because of their favorable photovoltaic performance (power conversion efficiency over 21%) and room-temperature continuous-wave green lasing . The MQWs are capped with phenylethylammonium bromide (PEABr) organic cations in a configuration that has recently demonstrated random lasing . The surface quality is characterized by atomic force microscopy and the depolarization of ellipsometric measurements, revealing a high-quality surface morphology (RMS roughness of 2.1 nm; see also the Supporting Information (SI) Figure S1), which is beneficial for improved luminescence properties.…”

Section: Resultsmentioning

confidence: 99%

“…Solution-processed lead halide perovskites (LHPs) have been extensively studied for next-generation optoelectronic applications due to their tunable and narrow bandwidth light emission , light-harvesting capabilities, and high photoluminescence quantum yield . Particularly, their low-threshold and tunable amplified spontaneous emissions (ASE) through stoichiometry and composition control have made them ideal candidates for cutting-edge research aiming at light-emitting devices such as light-emitting diodes (LEDs) and lasers. ,− The broad applicability of LHPs has stimulated great efforts to understand excited-state properties such as carrier thermalization and electron–phonon coupling to predict the performance of these materials before optoelectronic devices are made . Moreover, the relative strength and time scale of charge carrier generation–recombination processes like carrier cooling, free-carrier ionization, and exciton formation play vital roles in dictating the overall performance of devices like solar cells, LEDs, and lasers. , …”

Section: Introductionmentioning

confidence: 99%

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Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Chowdhury,

Fruhling,

Diroll

et al. 2024

ACS Photonics

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Quasi-2D perovskites have recently been extensively studied due to their narrow-bandwidth-tunable emission, solution processability, and applicability as optical gain media. Quasi-2D perovskites are composed of inorganic perovskite crystal layers encapsulated with a bulky organic ligand such as phenylethylammonium, endowing the perovskite with a quantum-well structure and improved stability. In this article, we explore the photophysics of a quasi-2D metal halide perovskite as a promising light-harvesting and emitting medium. We find it exhibits high optical absorption (∼105 cm–1) and an optically pumped amplified spontaneous emission threshold at 623 μJ/cm2. We study charge transfer processes in the complex mixed quantum wells of these perovskites through transient absorption and time-resolved photoluminescence measurements and develop a phenomenological model that incorporates optical gain for lasing. While both free carriers and excitons are observed, we show surprisingly that photoluminescence is dominated by excitons despite the relatively small binding energy (∼16 meV) of the low-energy band edge. Additionally, we extract the rates of exciton relaxation pathways, revealing a relatively large radiative term of 4.6 × 108 s–1 as well as an exciton–exciton annihilation term of 3.6 × 10–13 cm3 s–1 that is 3 orders of magnitude smaller than in similar quasi-2D perovskites.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Chowdhury,

Fruhling,

Diroll

et al. 2024

ACS Photonics

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“…Random lasers are a type of laser whose laser mode is not achieved through traditional reflection and resonance, but rather through the scattering of photons in the random microstructure of materials [92]. Compared to traditional lasers, random lasers have irregular resonant cavities, simple preparation, low cost, controllable morphology and easy modulation, making them potentially useful in multiple fields such as optical imaging and biomedicine.…”

Section: Random Lasermentioning

confidence: 99%

Quasi-two dimensional Ruddlesden-Popper halide perovskites for laser applications

Chen,

Zhang,

Liang

et al. 2023

Front. Phys.

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Quasi-two-dimensional (2D) Ruddlesden–Popper (RP) halide perovskites, as a kind of emerged two-dimensional layered materials, have recently achieved great attentions in lasing materials field owing to their large exciton binding energy, high emission yield, large optical gain, and wide-range tuning of optical bandgap. This review will introduce research progresses of RP halide perovskites for lasing applications in aspects of materials, photophysics, and devices with emphasis on emission and lasing properties tailored by the molecular composition and interface. The materials, structures and fabrications are introduced in the first part. Next, the optical transitions and amplified spontaneous emission properties are discussed from the aspects of electronic structure, exciton, gain dynamics, and interface tailoring. Then, the research progresses on lasing devices are summarized and several types of lasers including VCSEL, DFB lasers, microlasers, random lasers, plasmonic lasers, and polariton lasers are discussed. At last, the challenges and perspectives would be provided.

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“…Benefiting from these excellent properties, the quasi-2D perovskites have been successfully employed in several lasers depending on the whispering-gallery mode (WGM), Fabry–Pérot (F–P) mode, distributed feedback (DFB), and distributed Bragg reflector (DBR) cavities at room temperature. ,− Among the various perovskite lasers, quasi-2D perovskite random lasers with low spatial coherence can be generated simply by multiple light scattering in disordered gain media. − In contrast to ordinary lasers, LEDs, and other light sources, random perovskite lasers possess high brightness, a narrow bandwidth, and relatively low spatial coherence, effectively preventing the formation of speckles. These unique characteristics that make random lasers more appropriate for speckle-free imaging applications than conventional lasers with high spatial resolution and LEDs have not been sufficiently explored. − …”

Section: Introductionmentioning

confidence: 99%

Speckle-Free Imaging Based on a Quasi-2D Perovskite Random Laser with a Subwavelength Thickness

Wang,

Qin,

Zhan

et al. 2024

ACS Photonics

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Quasi-two-dimensional (quasi-2D) perovskite materials possess remarkable optical properties, including a large exciton binding energy, enhanced stability, and natural quantumwell structures, which have great potential for lasing applications. However, solution-processed quasi-2D perovskite films encounter challenges such as serious defect states, poor crystal quality, and random phase distribution, thereby hindering the practical application of quasi-2D perovskite lasers. Here, we demonstrate random lasers based on quasi-2D (PEA) 2 MA 3 Pb 4 Br 13 films with preeminent optical gain by introducing adipic acid (AA) as an additive and further explore their speckle-free imaging. By the introduction of AA, the quality of quasi-2D perovskite films is significantly improved, including suppressed defect states, improved crystalline quality, larger grain sizes, a more homogeneous phase distribution, and enhanced photoluminescence (PL) because of the lowering of the crystallization rate. Moreover, the AA-assisted quasi-2D perovskite film exhibits significantly decreased amplified spontaneous emission (ASE) thresholds from 55.4 to 7.8 μJ/cm 2 , along with an increased gain coefficient from 332 to 1404 cm −1 , which is four times that of the pristine one. Accordingly, the threshold of random lasers based on AA-assisted quasi-2D perovskite films can be reduced to 20% of that of pristine films. Benefiting from the high brightness, narrow bandwidth, and relatively low spatial coherence of the random laser, we realized higher speckle-free imaging of quasi-2D perovskite subwavelength random lasers. This work presents an effective strategy for enhancing quasi-2D perovskites as gain media and expanding their practical applications in optoelectronic devices, particularly in semiconductor lasers.

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Coherent Random Lasing in Subwavelength Quasi‐2D Perovskites

Cited by 11 publications

References 77 publications

Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Quasi-two dimensional Ruddlesden-Popper halide perovskites for laser applications

Speckle-Free Imaging Based on a Quasi-2D Perovskite Random Laser with a Subwavelength Thickness

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