Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite

@article{Duan2020PhotoinducedVD,
  title={Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite},
  author={Hong-Guang Duan and Vandana Tiwari and Ajay Jha and Golibjon R. Berdiyorov and Alexey V. Akimov and Oriol Vendrell and Pabitra K. Nayak and Henry James Snaith and Michael Thorwart and Zheng Li and Mohamed El-Amine Madjet and R. J. Dwayne Miller},
  journal={Journal of the American Chemical Society},
  year={2020},
  volume={142},
  pages={16569 - 16578}
}
The success of organic–inorganic perovskites in optoelectronics is dictated by the complex interplay between various underlying microscopic phenomena. The structural dynamics of organic cations and the inorganic sublattice after photoexcitation are hypothesized to have a direct effect on the material properties, thereby affecting the overall device performance. Here, we use ultrafast heterodyne-detected two-dimensional (2D) electronic spectroscopy to reveal impulsively excited vibrational modes… 

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References

SHOWING 1-10 OF 73 REFERENCES

Probing femtosecond lattice displacement upon photo-carrier generation in lead halide perovskite

TLDR
Two new phonon modes with impulsive vibrational spectroscopy are observed providing the evidence of the polaronic nature of the photo-excitation, demonstrating the presence ofPolaronic effects in lead halide perovskites.

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

TLDR
The important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites is shown and new understanding of hot carrier—lattices interactions, which fundamentally determine solar cell efficiencies is provided.

Direct Observation of Ultrafast Exciton Dissociation in Lead Iodide Perovskite by 2D Electronic Spectroscopy

The unprecedented success of hybrid organic–inorganic lead halide perovskites in photovoltaics motivates fundamental research to unravel the underlying microscopic mechanism for photoinduced charge

Real-Time Observation of Organic Cation Reorientation in Methylammonium Lead Iodide Perovskites.

TLDR
This work uses ultrafast 2D vibrational spectroscopy of methylammonium (MA) lead iodide to directly resolve the rotation of the organic cations within the MAPbI3 lattice and reveals two characteristic time constants of motion.

Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite

TLDR
The polaron formation via nuclear dynamics that may be important for efficient charge separation is revealed and elucidating electron-phonon coupling in hybrid organic-inorganic perovskites may help to understand the high photovoltaic efficiency.

Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices

TLDR
The results suggest that the attractive optoelectronic properties of CH3NH3PbI3 mainly derive from the inorganic lead-halide framework, and employ infrared-pump electronic-probe spectroscopy to show that pump-induced atomic motions of the organic cations do not substantially alter optoelection properties.

Organic Cation Rotation and Immobilization in Pure and Mixed Methylammonium Lead-Halide Perovskites.

TLDR
This work combines ultrafast two-dimensional vibrational spectroscopy and molecular dynamics simulations to study the dynamics of the organic methylammonium cation orientation in a range of pure and mixed trihalide perovskite materials.

Polaron Stabilization by Cooperative Lattice Distortion and Cation Rotations in Hybrid Perovskite Materials.

TLDR
An in-depth computational study of small polaron formation, electronic structure, charge density, and reorganization energies using both periodic boundary conditions and isolated structures suggests formamidinium and cesium based crystals and alloys are potentially better materials for solar cell and other optoelectronic applications.

Direct observation of collective modes coupled to molecular orbital–driven charge transfer

TLDR
The ultrafast photoresponse of the molecular crystal Me4P[Pt(dmit)2]2 is reported, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and how femtosecond electron diffraction can be applied to directly observe the associated molecular motions.

How Lattice Dynamics Moderate the Electronic Properties of Metal-Halide Perovskites.

  • L. Herz
  • Materials Science
    The journal of physical chemistry letters
  • 2018
TLDR
This Perspective outlines how the dynamic response of the ionic lattice affects key electronic properties such as exciton binding energies and charge-carrier mobilities in hybrid perovskites.
...