Ultrafast Excitonic Response in Two-Dimensional Hybrid Perovskites Driven by Intense Midinfrared Pulses

Li, Shunran; Li, Xiaotong; Kocoj, Conrad A.; Ji, Xiaoqin; Yuan, Shaofan; Macropulos, Eleni C.; Stoumpos, Constantinos C.; Xia, Fengnian; Mao, Lingling; Kanatzidis, Mercouri G.; Guo, Peijun

doi:10.1103/physrevlett.129.177401

Cited by 9 publications

(9 citation statements)

References 65 publications

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“…These solution-processed films, despite the presence of cracks that are spaced hundreds of microns apart, still exhibit good uniformity within each domain and feature large grain sizes. The reflectance spectra of both samples shown in Figure b exhibit pronounced reflection dips around 500 nm, which are characteristic of exciton resonances in these materials. − The exciton resonance in (PEA) 2 PbI 4 is slightly red-shifted compared to (BA) 2 PbI 4 . The reflection dips at wavelengths beyond 520 nm, which fall below the absorption spectral window, are attributed to interference fringes …”

Section: Resultsmentioning

confidence: 98%

“…We attribute this observed transient response to the heat-induced broadening of the exciton resonance, a phenomenon we recently demonstrated for (BA) 2 PbBr 4 under MIR vibrational excitation. 36 In essence, lattice heating enhances electron−phonon interactions, leading to a stronger damping factor for the exciton resonance. 46 The rapid, subnanosecond interband carrier relaxation times and the nanosecond time resolution of our PPM setup prevent us from observing the initial blue shift under 380 nm excitation and the electronic dynamics in these strongly excitonic materials.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Li,

Xu,

Kocoj

et al. 2024

J. Am. Chem. Soc.

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In recent years, optical pump–probe microscopy (PPM) has become a vital technique for spatiotemporally imaging electronic excitations and charge-carrier transport in metals and semiconductors. However, existing methods are limited by mechanical delay lines with a probe time window up to several nanoseconds (ns) or monochromatic pump and probe sources with restricted spectral coverage and temporal resolution, hindering their amenability in studying relatively slow processes. To bridge these gaps, we introduce a dual-hyperspectral PPM setup with a time window spanning from nanoseconds to milliseconds and single-nanosecond resolution. Our method features a wide-field probe tunable from 370 to 1000 nm and a pump spanning from 330 nm to 16 μm. We apply this PPM technique to study various two-dimensional metal-halide perovskites (2D-MHPs) as representative semiconductors by imaging their transient responses near the exciton resonances under both above-band gap electronic pump excitation and below-band gap vibrational pump excitation. The resulting spatially and temporally resolved images reveal insights into heat dissipation, film uniformity, distribution of impurity phases, and film–substrate interfaces. In addition, the single-nanosecond temporal resolution enables the imaging of in-plane strain wave propagation in 2D-MHP single crystals. Our method, which offers extensive spectral tunability and significantly improved time resolution, opens new possibilities for the imaging of charge carriers, heat, and transient phase transformation processes, particularly in materials with spatially varying composition, strain, crystalline structure, and interfaces.

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Section: Resultsmentioning

confidence: 98%

Section: ■ Results and Discussionmentioning

confidence: 99%

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Li,

Xu,

Kocoj

et al. 2024

J. Am. Chem. Soc.

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“…Instances involving OIHPs with n = 1 often exhibit robust quantum and dielectric confinement effects, accompanied by a somewhat subdued photoluminescence, often attributed to Auger recombination . A more in-depth understanding of Auger recombination hinges on a thorough delineation of quantum and dielectric confinement facilitated by 2D structures. , There is a growing anticipation for the development of advanced characterization techniques tailored for OIHPs, which not only enrich the understanding of dielectric-related phenomena but also serve as a theoretical compass for practical applications of these OIHPs.…”

Section: Discussionmentioning

confidence: 99%

Dielectric Engineering of 2D Organic–Inorganic Hybrid Perovskites

Chen,

Yu,

Xing

et al. 2023

ACS Energy Lett.

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Manipulating excitons in semiconductors has driven the evolution of today's optoelectronic and photovoltaic devices. Engineering the dielectric constant, a key parameter that is highly associated with the Coulomb force of excitons, has recently emerged as a fresh avenue to regulate excitons from the root. Unlike three-dimensional (3D) bulk semiconductors featuring uniformly distributed dielectric constants, the dielectric constants of two-dimensional (2D) layered semiconductors exhibit spatial variability. Particularly, organic−inorganic hybrid perovskites (OIHPs) assembled with alternating organic and inorganic layers show a cyclic variation in the dielectric property, which substantially impacts exciton dynamics, including recombination and separation, offering an opportunity for the regulation of exciton-related physical attributes by dielectric engineering and the cutting-edge applications thereof. This Review documents the recent advances in the rational design of organic and inorganic constituents of 2D OIHPs for dielectric engineering. We show that dielectrically engineered OIHPs are pivotal in driving the advancements in optoelectrical and photovoltaic applications.

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“…[31] In contrast, 2D layered perovskite materials have a multiple quantum well-like structure with general formula (A´) m A n-1 B n X 3n+1 , where A´is bulky cations that form a monolayer or bilayer connecting the conductor (A) n-1 B n X 3n+1 2D sheets. [32][33][34] 2D perovskite structures are mostly categorized into Ruddlesden-Popper (R-P) and Dion-Jacobson (D-J) phases. [35] The optoelectronic properties of 2D halide perovskites can be synergistically tuned by the number of inorganic layers and by changing the size, shape, charge, and location of bulky organic cations.…”

Section: Introductionmentioning

confidence: 99%

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Ghosh

Parveen

Sellin

et al. 2023

Adv Materials Technologies

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Layered metal halide perovskites have attracted enormous research attention over the last few years, befitting their unique optical and electronic properties. Low‐dimensional layered perovskites demonstrate great potential for various optoelectronic and sensing applications beyond photovoltaics. Herein, the recent progress and opportunities in 2D and quasi‐2D perovskites for light‐emitting diodes (LEDs), lasers, memristors, neuromorphic/synaptic applications, UV–vis photodetection, X‐ray detection, scintillators, and photocatalytic applications are reviewed. First, the crystal structure, characteristics, and fundamental properties of 2D layered perovskites are discussed. Recent efforts and developments of 2D and quasi‐2D metal halide perovskite for light‐emitting applications with excellent luminescence properties are reviewed. Unique properties of 2D perovskites, such as negligible leakage current due to restricted carrier transport, high stability, and hydrophobicity, make them viable for memristor devices. After discussing the memristor and neuromorphic devices using 2D perovskites, the outstanding performance of 2D perovskites in UV–vis photodetection including polarization‐sensitive photodetection is discussed. 2D perovskites recently proved as a superior candidate in X‐ray detection with high stability. Further, the scintillation properties of 2D perovskites for the detection of ionizing radiation are discussed. Finally, some of the very recent achievements and present future outlook, including exciting opportunities in this burgeoning field are highlighted.

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Ultrafast Excitonic Response in Two-Dimensional Hybrid Perovskites Driven by Intense Midinfrared Pulses

Cited by 9 publications

References 65 publications

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Dielectric Engineering of 2D Organic–Inorganic Hybrid Perovskites

Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

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