Switchable planar chirality and spin texture in highly ordered ferroelectric hybrid perovskite domains DOI Creative Commons

Chuanzhao Li,

Mykola Telychko, Yue Zheng

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 25, 2024

Chiral organic-inorganic hybrid perovskites offer a promising platform for developing non-linear chiro-optical applications and chiral-induced spin selectivity. Here, we show that achiral have highly ordered ferroelectric domains with orthogonal polarization exhibit planar chirality, as manifested by second harmonic generation strong circular dichroism. Interestingly, the handedness of dichroism response can be alternatingly switched between orthogonally polarized domain walls. To correlate origin chirality in these domains, atom-resolved atomic force microscopy is used to reveal distinct arrangements rows crystals indicate symmetry breaking. Remarkably, large SHG anisotropy factor 0.41 measured at wall. Additionally, spatially resolved two-photon photoluminescence excitation measurement provide evidence larger Rashba spin-splitting chiral compared domain-free areas. Our discoveries domain-dependent texture hold great promise advancement domain-specific applications.

Language: Английский

Unlocking the Potential of Organic‐Inorganic Hybrid Manganese Halides for Advanced Optoelectronic Applications DOI Open Access
Wei Zhang, Wei Zheng, Lingyun Li

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 5, 2024

Organic-inorganic hybrid manganese(II) halides (OIMnHs) have garnered tremendous interest across a wide array of research fields owing to their outstanding optical properties, abundant structural diversity, low-cost solution processibility, and low toxicity, which make them extremely suitable for use as new class luminescent materials various optoelectronic applications. Over the past years, plethora OIMnHs with different dimensionalities multifunctionalities such efficient photoluminescence (PL), radioluminescence, circularly polarized luminescence, mechanoluminescence been newly created by judicious screening organic cations inorganic Mn(II) polyhedra. Specifically, through precise molecular engineering, series near-unity PL quantum yields, high anti-thermal quenching excellent stability in harsh conditions devised explored applications light-emitting diodes (LEDs), X-ray scintillators, multimodal anti-counterfeiting, fluorescent sensing. In this review, latest advancements development are summarized, covers from fundamental physicochemical properties advanced applications, an emphasis on functionality design especially LEDs detection imaging. Current challenges future efforts unlock potentials these promising also envisioned.

Language: Английский

Citations

18
Free Halogen Substitution of Chiral Hybrid Metal Halides for Activating the Linear and Nonlinear Chiroptical Properties DOI

Junjie Guan,

Yongshen Zheng,

Puxin Cheng

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(49), P. 26833 - 26842

Published: Dec. 1, 2023

Halogen substitution has been proven as an effective approach to the band gap engineering and optoelectronic modulation of organic–inorganic hybrid metal halide (OIHMH) materials. Various high-performance mixed OIHMH film materials have primarily obtained through coordinated halogens in their inorganic octahedra. Herein, we propose a new strategy free halogen outside octahedra for constructing single crystals with chiral structures, resulting boost linear nonlinear chiroptical properties. The from DMA4[InCl6]Cl (DMA = dimethylammonium) DMA4[InCl6]Br facile antisolvent vaporization method produces centimeter-scale high thermal stability along quantum yield photoluminescence, conspicuous circularly polarized luminescence, greatly enhanced second harmonic generation (SHG). In particular, crystal features intrinsic structure, exhibiting significant SHG circular dichroism (SHG-CD) response highest reported anisotropy factor (gSHG-CD) 1.56 among enhancements both properties are directly attributed octahedral distortion. by confine introduced within sites lattice, thereby ensuring compositions successful employment such may broaden horizon regulation structures

Language: Английский

Citations

36
Direct Observation of Circularly Polarized Nonlinear Optical Activities in Chiral Hybrid Lead Halides DOI Creative Commons

Sunhao Liu,

Xiaoming Wang, Yixuan Dou

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(17), P. 11835 - 11844

Published: April 3, 2024

Circularly polarized light emission is a crucial application in imaging, sensing, and photonics. However, utilizing low-energy photons to excite materials, as opposed high-energy excitation, can facilitate deep-tissue imaging sensing applications. The challenge lies finding materials capable of directly generating circularly nonlinear optical effects. In this study, we introduce chiral hybrid lead halide (CHLH) material system, R/S-DPEDPb3Br8·H2O (DPED = 1,2-diphenylethylenediammonium), which produce second harmonic generation (CP-SHG) through linearly infrared exhibiting polarization efficiency high 37% at room temperature. To understand the spin relaxation mechanisms behind efficiency, utilized two models, so-called D'yakonov–Perel' (DP) Bir–Aronov–Pikus (BAP) mechanisms. unique zigzag inorganic frameworks within structure are believed reduce dielectric confinement exciton binding energy, thus enhancing polarization, especially regions with excitation pump fluence based on DP mechanism. case low fluence, BAP mechanism dominates, evidenced by observed decrease ratio from CP-SHG measurement. Using density functional theory analysis, elucidate how distinctive 8-coordination environment bromide building blocks effectively suppresses spin–orbit coupling conduction band minimum. This suppression significantly diminishes spin-splitting, thereby slowing rate.

Language: Английский

Citations

14
Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand DOI

Puxin Cheng,

Xiaodi Jia,

Siqian Chai

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(19)

Published: March 12, 2024

Abstract Chiral hybrid organic–inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second‐order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement nonlinearity chiral HOMHs could be achieved by matching free exciton and/or self‐trapped energy levels with desired NLO frequencies. However, current scarcity resonance modes and low ratio hamper further improvements performance. Herein, we propose a new resonant channel charge transfer (CT) excited states from halide polyhedra organic ligand boost HOMHs. model lead (C 7 H 10 N)PbBr 3 N=1‐ethylpyridinium) exhibits drastically enhanced second harmonic generation in deep CT energy, intensity up 111.0 times that KDP 10.9 urea. effective coefficient has been determined as high ~40.2 pm V −1 , balanced large polarization laser damage threshold. This work highlights contribution ligands construction enhancing coefficients halides, thus provides guidelines designing advanced photonic applications.

Language: Английский

Citations

13
Wafer-Scale Patterning Integration of Chiral 3D Perovskite Single Crystals toward High-Performance Full-Stokes Polarimeter DOI

Junli Bai,

Hebin Wang, Jianpeng Ma

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(27), P. 18771 - 18780

Published: June 27, 2024

Chiral three-dimensional (3D) perovskites exhibit exceptional optoelectronic characteristics and inherent chiroptical activity, which may overcome the limitations of low-dimensional chiral devices achieve superior performance. The integrated chip high-performance arbitrary polarized light detection is one aims be achieved by 3D perovskites. Herein, we first fabricate wafer-scale full-Stokes polarimeter synergy unprecedented (

Language: Английский

Citations

12
Magneto‐chiral Nonlinear Optical Effect with Large Anisotropic Response in Two‐Dimensional Halide Perovskite DOI
Daichi Okada, Fumito Araoka

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(21)

Published: March 28, 2024

Abstract The chiral organic–inorganic halide perovskites (OIHPs) are vital candidates for superior nonlinear optical (NLO) effects associated with circularly polarized (CP) light. NLO in materials often couples magnetic dipole (MD) transition, as well the conventional electric (ED) transition. However, importance of MD transition process OIHPs has not yet been recognized. Here, circular probe analysis second harmonic generation dichroism (SHG‐CD) provides direct evidence that contribution leads to a large anisotropic response CP lights OIHPs, (R‐/S‐MBACl) 2 PbI 4 . thin films exhibit great sensitivity over wide wavelength range, and g‐value reaches up 1.57 at where is maximized. Furthermore, it also effective light generator, outputting CP‐SHG maximum g‐factor 1.76 upon stimulation linearly This study deepens understanding relation between chirality magneto‐optical effect, such an efficient discrimination signal highly applicable chirality‐based sensor communication devices.

Language: Английский

Citations

10
Mechanical Twisting-Induced Enhancement of Second-Order Optical Nonlinearity in a Flexible Molecular Crystal DOI
Zhihua Wang,

Wenqing Han,

Bona Fu

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 7, 2025

Flexible molecular crystals are essential for advancing smart materials, providing unique functionality and adaptability applications in next-generation electronics, pharmaceuticals, energy storage. However, the optical of flexible have been largely restricted to linear optics, with nonlinear (NLO) properties rarely explored. Herein, we report on application mechanical twisting second-order optics. The crystal formed through self-assembly model compound 9-anthraldehyde (AA) features an intrinsic chiral noncentrosymmetric structure, demonstrating high efficiency second harmonic generation (SHG) NLO circular dichroism, which could be greatly enhanced by macroscopic twisting. anisotropic stacking imparts AA flexibility combined elastic bending plastic isochiral enhance SHG intensities order magnitude depending their M- or P-configuration. Meanwhile, dichroism factor gSHG-CD twisted is increased, achieving highest reported anisotropy among organic materials. These boosted performances intensity chiroptical response expected expand photonic crystals.

Language: Английский

Citations

1
In Situ Chiral Template Approach to Synthesize Homochiral Lead Iodides for Second‐Harmonic Generation DOI

Juan Cheng,

Gangji Yi,

Zhizhuan Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(6)

Published: Dec. 21, 2023

Abstract Homochiral halide perovskites have gained increasing attention because of their fascinating optoelectronic properties and prospective applications in laser technologies. However, the limited choice chiral organic templates severely restricts structural diversity second‐harmonic generation (SHG) effects. Here, we present an situ template approach for synthesis one‐dimensional (1D) homochiral lead iodides. A imine (L‐ipp) was generated by reacting L‐proline (L‐pro) acetone under ambient conditions. Notably, L‐ipp can cooperate with L‐pro to direct formation a iodide dual templates, which is unprecedented crystalline metal halides. The containing both shows strong SHG response 8.0 times that KH 2 PO 4 (8.0×KDP). efficiency one largest values reported date any halides 1064 nm irradiation. comparative study 1D iodides either or exhibit relatively weak responses (≤1.0×KDP). This work demonstrates advantage using two different over single enhancing materials.

Language: Английский

Citations

17
Synthesis and Characterization of Cu-Containing Chiral Metal Halides and Role of Halogenation of the Organic Ligand DOI

Andrea Dibenedetto,

Clarissa Coccia,

Massimo Boiocchi

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(11), P. 4803 - 4808

Published: March 7, 2024

We report herein novel chiral copper metal chlorides, namely, (R/S-ClMBA)2CuCl4 [ClMBA = 4-(chloromethyl)benzylammonium], together with the corresponding racemic compound. The two samples are composed of isolated CuCl4 tetrahedra crystallizing in noncentrosymmetric C2 space group and present a significant absorption visible region spectrum band gap around 2.50 eV. compound, on other hand, gives origin to different structural topology characterized by presence quite unusual five coordination for Cu(II), Cu2Cl6– dimers forming infinite chains along b axis presents, addition, strong reduction (around 1.76 eV). display circular dichroism response anisotropy factor values 0.02. actual investigated comparison MBA-based (MBA methylbenzylammonium) system order unveil effect benzene ring halogenation chiroptical properties, indicating that chlorine leads doubling factor.

Language: Английский

Citations

7
Chiral Ruthenium Halide Semiconductor with Strong Antiferromagnetic Coupling DOI Open Access

Haolin Lu,

Tengfei He, Haolin Wu

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(1)

Published: Sept. 15, 2023

Abstract Chiral hybrid organic–inorganic metal halides have attracted wide attention owing to their superior chiroptoelectronic and chirospintronic properties. Here, a new class of chiral lead‐free halides, ( R / S ‐MBA) 3 Ru 2 Br 9 (MBA = methylbenzylammonium), with unique magnetic properties is reported. composed surface‐shared octahedron dimer separated by cations crystallizes into the Sohncke space group P2 1 . The crystal structures, chiroptical, properties, circular dichroism are systematically investigated. Owing strong antiferromagnetic coupling between atom through bromine bridge in [Ru ] 3− weak ferromagnetic neighboring dimer, exhibits property Néel temperature at 7 K. Considering ruthenium, together rapid progress spintronics optospintronics recently, this work provides novel multifunctional candidate toward optoelectronics spintronics.

Language: Английский

Citations

14