IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v9y2018i1d10.1038_s41467-018-06009-3.html
   My bibliography  Save this article

Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics

Author

Listed:
  • Jasmine P. H. Rivett

    (University of Cambridge)

  • Liang Z. Tan

    (University of Pennsylvania)

  • Michael B. Price

    (University of Cambridge)

  • Sean A. Bourelle

    (University of Cambridge)

  • Nathaniel J. L. K. Davis

    (Victoria University of Wellington)

  • James Xiao

    (University of Cambridge)

  • Yatao Zou

    (Soochow University)

  • Rox Middleton

    (University of Cambridge)

  • Baoquan Sun

    (Soochow University)

  • Andrew M. Rappe

    (University of Pennsylvania)

  • Dan Credgington

    (University of Cambridge)

  • Felix Deschler

    (University of Cambridge)

Abstract

Anharmonic crystal lattice dynamics have been observed in lead halide perovskites on picosecond timescales. Here, we report that the soft nature of the perovskite crystal lattice gives rise to dynamic fluctuations in the electronic properties of excited states. We use linear polarization selective transient absorption spectroscopy to study the charge carrier relaxation dynamics in lead-halide perovskite films and nanocrystals. We find that photo-excited charge carriers maintain an initial polarization anisotropy for several picoseconds, independent of crystallite size and composition, and well beyond the reported timescales of carrier scattering. First-principles calculations find intrinsic anisotropies in the transition dipole moment, which depend on the orientation of light polarization and the polar distortion of the local crystal lattice. Lattice dynamics are imprinted in the optical transitions and anisotropies arise on the time-scales of structural motion. The strong coupling between electronic states and structural dynamics requires a unique interpretation of recombination and transport mechanisms.

Suggested Citation

  • Jasmine P. H. Rivett & Liang Z. Tan & Michael B. Price & Sean A. Bourelle & Nathaniel J. L. K. Davis & James Xiao & Yatao Zou & Rox Middleton & Baoquan Sun & Andrew M. Rappe & Dan Credgington & Felix , 2018. "Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-06009-3
    DOI: 10.1038/s41467-018-06009-3
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-018-06009-3
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-018-06009-3?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-06009-3. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.