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Resolving the ultrafast charge carrier dynamics of 2D and 3D domains within a mixed 2D/3D lead-tin perovskite

DOI: 10.1002/adfm.202305736 DOI Help

Authors: Jake D. Hutchinson (University of Warwick) , Edoardo Ruggeri (University of Cambridge) , Jack M. Woolley (University of Warwick) , Geraud Delport (University of Cambridge) , Samuel D. Stranks (University of Cambridge) , Rebecca L. Milot (University of Warwick)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Advanced Functional Materials , VOL 32

State: Published (Approved)
Published: August 2023
Diamond Proposal Number(s): 17223

Open Access Open Access

Abstract: Mixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light- emitting diode (LED) communities due to their impressive opto-electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead-tin perovskite containing distinct, self-assembled domains of either 3D structures or highly phase-pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump-terahertz probe spectroscopy, the effective charge-carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long-range charge-transport should not be impeded by the heterogeneous structure of the material.

Journal Keywords: perovskites; photon recycling; recombination; Ruddlesden–Popper; terahertz; ultrafast

Diamond Keywords: Photovoltaics; Semiconductors; Light-Emitting Diodes (LEDs)

Subject Areas: Materials, Physics, Energy

Instruments: I07-Surface & interface diffraction

Added On: 09/08/2023 09:09

Adv Funct Materials - 2023 - Hutchinson.pdf

Discipline Tags:

Surfaces Earth Sciences & Environment Sustainable Energy Systems Energy Physics Climate Change Energy Materials Materials Science interfaces and thin films Perovskites Metallurgy

Technical Tags:

Scattering Wide Angle X-ray Scattering (WAXS) Grazing Incidence Wide Angle Scattering (GIWAXS)