Excitonic enhancement of optical nonlinearities in perovskite 
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 single crystals

Ohara, Keiichi; Yamada, Takumi; Tahara, Hirokazu; Aharen, Tomoko; Hirori, Hideki; Suzuura, Hidekatsu; Kanemitsu, Yoshihiko

doi:10.1103/physrevmaterials.3.111601

Cited by 48 publications

(44 citation statements)

References 47 publications

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“…This indicates that the cavity effect just plays a minor role in the large optical nonlinear enhancements near the polaritonic wavelengths under strong coupling condition. In addition, the optical nonlinear response of the excitonic resonance also needs to be explored because the exciton effect can potentially enhance the nonlinear response of some organic materials 29 . For this purpose, we investigated Z-scan measurements on a cavity-exciton weak-coupling (WC) system that does not support polaritons.…”

Section: Resultsmentioning

confidence: 99%

Large optical nonlinearity enhancement under electronic strong coupling

et al. 2021

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Nonlinear optical responses provide a powerful way to understand the microscopic interactions between laser fields and matter. They are critical for plenty of applications, such as in lasers, integrated photonic circuits, biosensing and medical tools. However, most materials exhibit weak optical nonlinearities or long response times when they interact with intense optical fields. Here, we strongly couple the exciton of cyanine dye J-aggregates to an optical mode of a Fabry-Perot (FP) cavity, and achieve an enhancement of the complex nonlinear refractive index by two orders of magnitude compared with that of the uncoupled condition. Moreover, the coupled system shows an ultrafast response of ~120 fs that we extract from optical cross-correlation measurements. The ultrafast and large enhancement of the optical nonlinar coefficients in this work paves the way for exploring strong coupling effects on various third-order nonlinear optical phenomena and for technological applications.

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Section: Resultsmentioning

confidence: 99%

Large optical nonlinearity enhancement under electronic strong coupling

et al. 2021

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“…Exciton localization by disorder or impurities (i.e., bound exciton) may further increase its oscillator strength and the nonlinear susceptibility. [52] Recently, such exciton effect enhanced 2PA has been demonstrated in MAPbCl 3 single crystal, [53] which deviates from the standard semiconductor model. For low-dimensional semiconductors with stronger exciton binding energy ranging from NCs [54,55] to free-standing 2D materials, [56,57] this enhancement of third-order NLO will become more remarkable.…”

Section: Dimension Effects On Nlomentioning

confidence: 96%

Advances of Nonlinear Photonics in Low‐Dimensional Halide Perovskites

Wang

Mei

Liao

et al. 2021

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Hybrid halide perovskites emerging as a highly promising class of functional materials for semiconductor optoelectronic applications have drawn great attention from worldwide researchers. In the past few years, prominent nonlinear optical properties have been demonstrated in perovskite bulk structures indicating their bright prospect in the field of nonlinear optics (NLO). Following the surge of 3D perovskites, more recently, the low‐dimensional perovskites (LDPs) materials ranging from two‐, one‐, to zero‐dimension such as quantum‐wells or colloidal nanostructures have displayed unexpectedly attractive NLO response due to the strong quantum confinement, remarkable exciton effect, and structural diversity. In this perspective, the current state of the art is reviewed in the field of NLO for LDP materials. The relationship between confinement effect and NLO is analyzed systematically to give a comprehensive understanding of the function of dimension reduction. Furthermore, future directions and challenges toward the improvement of the NLO in LDP materials are discussed to provide an outlook in this rapidly developing field.

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“…[51] Table 1 summarizes such determinations of 2PA in 3D perovskites. [48,[52][53][54][55][56][57][58][59][60][61][62][63] Notice that the conditions of laser excitation, in particular, laser pulse durations greater than a few ns may result in the inaccurate determination of 2PA coefficients, since other nonlinear mechanisms, such as free-carrier absorptions [64] or thermal effects, [65] complicate the analysis of experimental data. As such, in Table 1, the 2PA measurements with ns laser pulses are excluded.…”

Section: Two-photon Absorption (2pa) In 3d Perovskite Crystalsmentioning

confidence: 99%

Perovskites: Multiphoton Absorption and Applications

Zhou

Ran

Fan

et al. 2021

Advanced Optical Materials

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critical temperature superconductivity, ferroelectric semiconductor-based cells for solar-energy conversion and others. Analogous to the oxide counterparts, metal lead halide perovskites (MLHPs) (represented by CsPbX 3 , X = I, Br, Cl) also exhibit a cubic lattice in 3Ds at room temperature, as illustrated in Figure 1, but with high-defect tolerance. [9,10] Commonly, their defect tolerance is a major enabling factor for their remarkable optoelectronic properties, such as considerable optical absorption coefficients, long carrier diffusion lengths, and high photoluminescence (PL) efficiency. [11][12][13][14] Furthermore, MLHPs can be synthesized cost effectively on large scales through simple solutionbased processes. As a result, the MLHPs have been investigated for optoelectronic applications in photovoltaics, light-emitting diodes, laser devices, and photodetectors. Recently, the lead halide hybrid organic-inorganic perovskites (HOIPs) have been emerging as a new territory of photovoltaic materials. The HOIPs comprise earth-abundant elements, and yet, exhibit outstanding semiconducting and light-absorption properties. [15,16] In particular, the power-conversion efficiency of HOIP-based devices has surpassed 20% over several years of research and development. [17,18] The HOIPs have a large structural diversity. When the A-site is only occupied by small organic cations (typically methylammonium, MA), they ideally exhibit 3D structures in an octahedral coordination.More interestingly, the HOIPs can exist in layered structures, or 2Ds. 2D HOIPs with unique layered structures are constructed from alternately stacked molecular sheets of organic cations and inorganic anions, as illustrated in Figure 1. The stacking sheets in 2D HOIPs can be regarded as a multiquantum-well structure in semiconductor physics, greatly enhancing the quantum and/or dielectric confinements. As a result, the free charge carriers (electrons or holes) can be strongly confined in atomic-thickness layers, readily forming excitons, which can be treated theoretically as hydrogen-like quasi-particles but moving in 2Ds. As a result, NLO effects can be greatly enhanced along with strong exciton-photon coupling. [19][20][21][22] 2D perovskites have opened up a new opportunity for both fundamental research and practical applications in ultrathin and flexible optoelectronics devices.Moreover, perovskites can also be synthesized into various lower-dimensional structures such as nanocrystals with controllable shapes and sizes. [11,23,24] This allows ones to modulate the quantum confinement effect in the lower-dimensional structures to achieve desirable light-to-electrical conversion, light-emitting, lasing, photodetecting, and NLO properties for various optoelectronic applications.Recently, there have been intensive and extensive research works on perovskites because of their excellent electrical and optical properties. This review is focused on their multiphoton absorption (MPA) and applications. All the MPA coefficients or cross-sections reported in the ...

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Excitonic enhancement of optical nonlinearities in perovskite CH3NH3PbCl3 single crystals

Cited by 48 publications

References 47 publications

Large optical nonlinearity enhancement under electronic strong coupling

Large optical nonlinearity enhancement under electronic strong coupling

Advances of Nonlinear Photonics in Low‐Dimensional Halide Perovskites

Perovskites: Multiphoton Absorption and Applications

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