Effect of film morphology on circular dichroism of low-dimensional chiral hybrid perovskites DOI Open Access

Urmila Makhija,

Parikshit Kumar Rajput,

P. Parthiban

et al.

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 160(2)

Published: Jan. 12, 2024

Chiral hybrid lead halide perovskites show interesting chiral optoelectronic properties. The extent of chirality is often estimated by their circular dichroism (CD) response. Here, we that the CD data depend strongly on film morphology. Four six films prepared, 2D (R- and S-MBA)2PbI4 1D S-MBA)PbI3 (MBA: methylbenzylammonium), form homogenous non-textured an isotropic signal. In contrast, other two samples, S-MBA)PbBr3, textured films, showing uncorrelated signals from different parts film. Therefore, role morphology needs to be verified before designing comparing chiroptic properties perovskites.

Language: Английский

Chiral materials and mechanisms for circularly polarized light-emitting diodes DOI
Francesco Furlan, Juan Manuel Moreno-Naranjo, Nicola Gasparini

et al.

Nature Photonics, Journal Year: 2024, Volume and Issue: 18(7), P. 658 - 668

Published: March 25, 2024

Language: Английский

Citations

71
The first chiral cerium halide towards circularly-polarized luminescence in the UV region DOI
Xinyi Niu, Zhichao Zeng, Zhaoyu Wang

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(6), P. 1961 - 1968

Published: Feb. 7, 2024

Language: Английский

Citations

30
Efficient Green Spin Light-Emitting Diodes Enabled by Ultrafast Energy- and Spin-Funneling in Chiral Perovskites DOI
Jingwen Yao, Zhiyu Wang, Yuling Huang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(20), P. 14157 - 14165

Published: May 10, 2024

Introducing molecular chirality into perovskite crystal structures has enabled the control of carrier spin states, giving rise to circularly polarized luminescence (CPL) in thin films and electroluminescence (CPEL) LEDs. Spin-LEDs can be fabricated either through a spin-filtering layer by chiral-induced selectivity or chiral emissive layer. The former requires high degree polarization compatible spinterface for efficient injection, which might not easily integrated Alternatively, also generate electroluminescence, but efficiency remains low fundamental mechanism is elusive. In this work, we report an green LED based on quasi-two-dimensional (quasi-2D) perovskites as emitting (EML), where CPEL directly produced without separate injection. optimized exhibited strong CPL at 535 nm with photoluminescence quantum yield (PLQY) 91% dissymmetry factor (glum) 8.6 × 10–2. Efficient spin-LEDs were successfully demonstrated, large EL (gEL) 7.8 10–2 maximum external (EQE) 13.5% room temperature. Ultrafast transient absorption (TA) spectroscopic study shows that generated from rapid energy transfer accompanied 2D 3D perovskites. Our only demonstrates reliable approach achieve performance reveals

Language: Английский

Citations

22
Chiral Cation Doping for Modulating Structural Symmetry of 2D Perovskites DOI
Yi Xie, Jack Morgenstein, Benjamin G. Bobay

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(32), P. 17831 - 17844

Published: Aug. 2, 2023

Cation mixing in two-dimensional (2D) hybrid organic-inorganic perovskite (HOIP) structures represents an important degree of freedom for modifying organic templating effects and tailoring inorganic structures. However, the limited number known cation-mixed 2D HOIP systems generally employ a 1:1 cation ratio stabilizing structure. Here, we demonstrate chiral-chiral mixed-cation system wherein controlled small amount (<10%) chiral S-2-MeBA (S-2-MeBA = (S)-(-)-2-methylbutylammonium) can be doped into (S-BrMBA)2PbI4 (S-BrMBA (S)-(-)-4-bromo-α-methylbenzylammonium), modulating structural symmetry from higher (C2) to lowest state (P1). This change occurs when concentration S-2-MeBA, measured by solution nuclear magnetic resonance, exceeds critical level─specifically, 1.4 ± 0.6%, structure remains as C2, whereas 3.9 1.4% substitution induces P1 (this is stable ∼7% substitution). Atomic occupancy analysis suggests that one specific S-BrMBA site preferentially substituted unit cell. Density functional theory calculations indicate spin splitting along different k-paths modulated doping. A true circular dichroism band at exciton energy 3.9% doping phase shows polarity inversion ∼45 meV blue shift Cotton-effect-type line-shape relative (S-BrMBA)2PbI4. trend toward suppressed melting temperature with also noted. The associated doping-concentration-induced transition provide material design strategy enhancing those emergent properties are sensitive types breaking.

Language: Английский

Citations

30
Chiral multiferroicity in two-dimensional hybrid organic-inorganic perovskites DOI Creative Commons
Haining Zheng, A. Ghosh,

M. J. Swamynadhan

et al.

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

Published: July 2, 2024

Abstract Chiral multiferroics offer remarkable capabilities for controlling quantum devices at multiple levels. However, these materials are rare due to the competing requirements of long-range orders and strict symmetry constraints. In this study, we present experimental evidence that coexistence ferroelectric, magnetic orders, crystallographic chirality is achievable in hybrid organic-inorganic perovskites [( R / S )- β -methylphenethylamine] 2 CuCl 4 . By employing Landau mode analysis, investigate interplay between ferroic propose a novel mechanism transfer systems. This involves coupling non-chiral distortions, characterized by defining pseudo-scalar quantity, $$\xi={{{{{\bf{p}}}}}}{{\cdot }}{{{{{\bf{r}}}}}}$$ ξ = p ⋅ r ( $${{{{{\bf{p}}}}}}$$ represents ferroelectric displacement vector $${{{{{\bf{r}}}}}}$$ denotes ferro-rotational vector), which distinguishes )-chirality based on its sign. Moreover, reversal descriptor’s sign can be associated with coordinated transitions Jahn-Teller antiferro-distortions, Dzyaloshinskii-Moriya vectors, indicating mediating role magnetoelectric correlations.

Language: Английский

Citations

13
Dimensional and Doping Engineering of Chiral Perovskites with Enhanced Spin Selectivity for Green Emissive Spin Light-Emitting Diodes DOI

Li‐Zhe Feng,

Yong‐Hui Song, Zidu Li

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(20), P. 6084 - 6091

Published: May 8, 2024

Chiral perovskites play a pivotal role in spintronics and optoelectronic systems attributed to their chiral-induced spin selectivity (CISS) effect. Specifically, they allow for spin-polarized charge transport light-emitting diodes (LEDs), yielding circularly polarized electroluminescence at room temperature without external magnetic fields. However, chiral lead bromide-based have yet achieve high-performance green emissive spin-LEDs, owing limited CISS effects transport. Herein, we employ dimensional regulation Sn2+-doping optimize perovskite architecture spin-LEDs. The optimized (PEA)x(S/R-PRDA)2–xSn0.1Pb0.9Br4 film exhibits an enhanced effect, higher hole mobility, better energy level alignment with the layer. These improvements us fabricate spin-LEDs quantum efficiency (EQE) of 5.7% asymmetry factor |gCP-EL| 1.1 × 10–3. This work highlights importance tailored architectures doping strategies advancing applications.

Language: Английский

Citations

12
Large exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite DOI Creative Commons
Shunran Li, Xian Xu, Conrad A. Kocoj

et al.

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

Published: March 22, 2024

Abstract In two-dimensional chiral metal-halide perovskites, organic spacers endow structural and optical chirality to the sublattice, enabling exquisite control of light, charge, electron spin. The chiroptical properties perovskites have been measured by transmissive circular dichroism spectroscopy, which necessitates thin-film samples. Here, developing a reflection-based approach, we characterize intrinsic, polarization-dependent complex refractive index for prototypical lead-bromide perovskite report large single crystals. Comparison with ab initio theory reveals arises from inorganic sublattice rather than ligand is an excitonic phenomenon driven electron-hole exchange interactions, breaks degeneracy transitions between Rashba-Dresselhaus-split bands, resulting in Cotton effect. Our study suggests that previous data spin-coated films largely underestimate provides quantitative insights into intrinsic spintronic applications.

Language: Английский

Citations

9
A chemical perspective on the chiral induced spin selectivity effect DOI Creative Commons
Brian P. Bloom, Zhongwei Chen, Haipeng Lu

et al.

National Science Review, Journal Year: 2024, Volume and Issue: 11(9)

Published: June 20, 2024

This review discusses opportunities in chemistry that are enabled by the chiral induced spin selectivity (CISS) effect. First, begins with a brief overview of seminal studies on CISS. Next, we discuss different material systems whose properties can be tailored through chemical means, special emphasis hybrid organic-inorganic layered materials exhibit some largest filtering to date. Then, promise CISS for reactions and enantioseparation before concluding.

Language: Английский

Citations

9
Efficient Spin‐Light‐Emitting Diodes With Tunable Red to Near‐Infrared Emission at Room Temperature DOI Creative Commons
Jingwen Yao, Yuling Huang, Haifeng Sun

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

Abstract Spin light‐emitting diodes (spin‐LEDs) are important for spin‐based electronic circuits as they convert the carrier spin information to optical polarization. Recently, chiral‐induced selectivity (CISS) has emerged a new paradigm enable spin‐LED it does not require any magnetic components and operates at room temperature. However, CISS‐enabled with tunable wavelengths ranging from red near‐infrared (NIR) yet be demonstrated. Here, chiral quasi‐2D perovskites developed fabricate efficient spin‐LEDs NIR region by tuning halide composition. The optimized perovskite films exhibit circularly polarized luminescence 675 788 nm, photoluminescence quantum yield (PLQY) exceeding 86% dissymmetry factor ( g lum ) 8.5 × 10 −3 2.6 −2 . More importantly, direct electroluminescence (CPEL) is achieved temperature in spin‐LEDs. This work demonstrated highest external efficiency (EQE) reaching 12.4% (EL) factors EL 3.7 1.48 composition‐dependent CPEL performance further attributed prolonged lifetime revealed ultrafast transient absorption spectroscopy.

Language: Английский

Citations

1
Spatially Correlated Chirality in Chiral Two-Dimensional Perovskites Revealed by Second-Harmonic-Generation Circular Dichroism Microscopy DOI
Zhihang Guo, Junzi Li, Rulin Liu

et al.

Nano Letters, Journal Year: 2023, Volume and Issue: 23(16), P. 7434 - 7441

Published: Aug. 8, 2023

Understanding the chiral mechanism of hybrid perovskites is a prerequisite for developing relevant chiroptoelectronic applications. Although conventional circular dichroism (CD) spectroscopy can be used to characterize chirality in perovskites, it has low signal-to-noise ratio and provide only information about macroscopic chirality. Herein, with aim revealing microscopic we utilize spacer cation alloying strategy construct two-dimensional perovskites. For first time, demonstrate second-harmonic-generation CD microarea imaging perovskite thin films unveil their spatially correlated In combination theoretical calculations, revealed that caused by localized out-of-plane supramolecular orientations. This work will not advance understanding chiroptical activity but also inspiration rational design synthesis chirality-related nonlinear optoelectronic devices.

Language: Английский

Citations

18