Localized holes and delocalized electrons in photoexcited inorganic perovskites: Watching each atomic actor by picosecond X-ray absorption spectroscopy | Zendy

Fabio Santomauro | Zendy; Jakob Grilj | Zendy; Lars Mewes | Zendy; Georgian Nedelcu | Zendy; Sergii Yakunin | Zendy; Thomas Rossi | Zendy; Gloria Capano | Zendy; André Al Haddad | Zendy; James Budarz | Zendy; Dominik Kinschel | Zendy; Darío Ferreira Sánchez | Zendy; Giacomo Rossi | Zendy; Mario Gutiérrez | Zendy; Daniel Grolimund | Zendy; Vallerie Ann Samson | Zendy; Maarten Nachtegaal | Zendy; Grigory Smolentsev | Zendy; Maksym V. Kovalenko | Zendy; Majed Chergui | Zendy

Open Access

Localized holes and delocalized electrons in photoexcited inorganic perovskites: Watching each atomic actor by picosecond X-ray absorption spectroscopy

Author(s) -

Fabio Santomauro,

Jakob Grilj,

Lars Mewes,

Georgian Nedelcu,

Sergii Yakunin,

Thomas Rossi,

Gloria Capano,

André Al Haddad,

James Budarz,

Dominik Kinschel,

Darío Ferreira Sánchez,

Giacomo Rossi,

Mario Gutiérrez,

Daniel Grolimund,

Vallerie Ann Samson,

Maarten Nachtegaal,

Grigory Smolentsev,

Maksym V. Kovalenko,

Majed Chergui

Publication year - 2016

Publication title -

structural dynamics

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 1.415

H-Index - 29

ISSN - 2329-7778

DOI - 10.1063/1.4971999

Subject(s) - delocalized electron , polaron , exciton , xanes , electron , spectroscopy , perovskite (structure) , charge carrier , valence (chemistry) , picosecond , absorption spectroscopy , absorption (acoustics) , absorption edge , materials science , chemistry , molecular physics , atomic physics , condensed matter physics , crystallography , band gap , physics , optoelectronics , optics , laser , organic chemistry , quantum mechanics , composite material

We report on an element-selective study of the fate of charge carriers in photoexcited inorganic CsPbBr 3 and CsPb(ClBr) 3 perovskite nanocrystals in toluene solutions using time-resolved X-ray absorption spectroscopy with 80 ps time resolution. Probing the Br K-edge, the Pb L 3 -edge, and the Cs L 2 -edge, we find that holes in the valence band are localized at Br atoms, forming small polarons, while electrons appear as delocalized in the conduction band. No signature of either electronic or structural changes is observed at the Cs L 2 -edge. The results at the Br and Pb edges suggest the existence of a weakly localized exciton, while the absence of signatures at the Cs edge indicates that the Cs + cation plays no role in the charge transport, at least beyond 80 ps. This first, time-resolved element-specific study of perovskites helps understand the rather modest charge carrier mobilities in these materials.

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