Coherent Phonon‐Induced Modulation of Charge Transfer in 2D Hybrid Perovskites

Seyitliyev, Dovletgeldi; Qin, Xixi; Jana, Manoj K.; Janke, Svenja M.; Zhang, Xiaowei; You, Wei; Mitzi, David B.; Blüm, Volker; Gündoğdu, Kenan

doi:10.1002/adfm.202213021

Cited by 4 publications

(1 citation statement)

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“…Desired charge transport properties may be tuned by altering the dimensionality and connectivity of the inorganic lattice, which influences the extended electronic structure. While the electronic states of small organic cations typically reside outside of the band edges, changing the organic (A-site) cation can impact the structure and dimensionality of the inorganic lattice through hydrogen bonding and organic–organic interactions that template particular structures. − In some cases, the organic cation can directly influence material properties, − such as in charge transfer semiconductors, − or in hybrid systems with chiral organic cations. ,− …”

Section: Introductionmentioning

confidence: 99%

Impact of Chiral Symmetry Breaking on Spin-Texture and Lone Pair Expression in Chiral Crystals of Hybrid Antimony and Bismuth Halides

Maughan,

Koknat,

Sercel

et al. 2023

Chem. Mater.

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Chiral organic building blocks can be incorporated into hybrid organic−inorganic metal-halide crystalline semiconductors so as to control and impact the interconversion between light, charge, and spin. Here, we report a series of hybrid antimony and bismuth halide materials of the general formula MBA 4 B 2 X 10 (B = Sb 3+ , Bi 3+ ; X = Br − , I − ) and study how chiral symmetry breaking imposed by the templating organic chiral methylbenzylammonium (MBA) cations induces symmetry breaking within the inorganic sublattice and leads to a unique spintexture. The chiral MBA cations introduce two structural modifications to the metal-halide sublattice that consists of isolated edge-sharing dimers of B 2 X 10 octahedra: (1) the dimers have a chiral spatial arrangement with respect to one another and (2) there is an asymmetric distortion of the two subunits within the individual dimers with a higher distortion caused by strong stereochemical activity of the Sb 5s 2 lone pair electrons. The structural distortions and chiral arrangement result in circular dichroism (CD) at the band edge of the inorganic framework with dissymmetry factors in the range of 10 −4 . Chiral spin-splitting of the inorganic states, caused by breaking of the inversion symmetry and large spin−orbit coupling, is studied via density functional theory (DFT), and a multiband effective mass theory was developed that links the DFT-derived spin-splitting of helical character (i.e., spin expectation value not perpendicular to the crystal momentum) to the observed CD. We also find broad red photoluminescence from the MBA 4 Sb 2 Br 10 compounds, which we attribute to self-trapped excitonic emission driven by the large distortion due to the lone pair expression.

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Section: Introductionmentioning

confidence: 99%

Impact of Chiral Symmetry Breaking on Spin-Texture and Lone Pair Expression in Chiral Crystals of Hybrid Antimony and Bismuth Halides

Maughan,

Koknat,

Sercel

et al. 2023

Chem. Mater.

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Controlling Ultrafast Magnetization Dynamics via Coherent Phonon Excitation in a Ferromagnet Monolayer

Zhou,

Li,

Frauenheim

et al. 2024

Nano Lett.

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Measuring carrier diffusion in MAPbI3 solar cells with photocurrent-detected transient grating spectroscopy

Ouyang,

Gan,

Yan

et al. 2023

The Journal of Chemical Physics

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Conventional time-of-flight methods can be used to determine carrier mobilities for photovoltaic cells in which the transit time between electrodes is greater than the RC time constant of the device. To measure carrier drift on sub-ns timescales, we have recently developed a two-pulse time-of-flight technique capable of detecting drift velocities with 100-ps time resolution in perovskite materials. In this method, the rates of carrier transit across the active layer of a device are determined by varying the delay time between laser pulses and measuring the magnitude of the recombination-induced nonlinearity in the photocurrent. Here, we present a related experimental approach in which diffractive optic-based transient grating spectroscopy is combined with our two-pulse time-of-flight technique to simultaneously probe drift and diffusion in orthogonal directions within the active layer of a photovoltaic cell. Carrier density gratings are generated using two time-coincident pulse-pairs with passively stabilized phases. Relaxation of the grating amplitude associated with the first pulse-pair is detected by varying the delay and phase of the density grating corresponding to the second pulse-pair. The ability of the technique to reveal carrier diffusion is demonstrated with model calculations and experiments conducted using MAPbI3 photovoltaic cells.

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Coherent Phonon‐Induced Modulation of Charge Transfer in 2D Hybrid Perovskites

Cited by 4 publications

References 50 publications

Impact of Chiral Symmetry Breaking on Spin-Texture and Lone Pair Expression in Chiral Crystals of Hybrid Antimony and Bismuth Halides

Impact of Chiral Symmetry Breaking on Spin-Texture and Lone Pair Expression in Chiral Crystals of Hybrid Antimony and Bismuth Halides

Controlling Ultrafast Magnetization Dynamics via Coherent Phonon Excitation in a Ferromagnet Monolayer

Measuring carrier diffusion in MAPbI3 solar cells with photocurrent-detected transient grating spectroscopy

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