Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI

Michael Andreas Kempf; Philipp Moser; Maximilian Tomoscheit; Julian Schröer; Jean Christophe Blancon; Rico Schwartz; Swarup Deb; Aditya Mohite; Andreas V. Stier; Jonathan J. Finley; Tobias Korn

doi:10.1021/acsnano.3c09001

Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI

Michael Andreas Kempf, Philipp Moser, Maximilian Tomoscheit, Julian Schröer, Jean Christophe Blancon, Rico Schwartz, Swarup Deb, Aditya Mohite, Andreas V. Stier, Jonathan J. Finley, Tobias Korn

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

We report temperature-dependent spectroscopy on the layered (n = 4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneously recorded time-resolved differential reflectivity (TRΔR) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin relaxation time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, spin relaxation is nearly T-independent. Our results highlight that spin relaxation in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aiming to utilize this degree of freedom.

Original language	English
Pages (from-to)	25459-25467
Number of pages	9
Journal	ACS Nano
Volume	17
Issue number	24
DOIs	https://doi.org/10.1021/acsnano.3c09001
State	Published - 26 Dec 2023

Keywords

(BA)(MA)PbI
layered perovskites
photocarrier dynamics
spin dynamics
time-resolved spectroscopy

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10.1021/acsnano.3c09001

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@article{4887ef223ac942b3ac8a0af3c494e10c,

title = "Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI",

abstract = "We report temperature-dependent spectroscopy on the layered (n = 4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneously recorded time-resolved differential reflectivity (TRΔR) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin relaxation time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, spin relaxation is nearly T-independent. Our results highlight that spin relaxation in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aiming to utilize this degree of freedom.",

keywords = "(BA)(MA)PbI, layered perovskites, photocarrier dynamics, spin dynamics, time-resolved spectroscopy",

author = "Kempf, {Michael Andreas} and Philipp Moser and Maximilian Tomoscheit and Julian Schr{\"o}er and Blancon, {Jean Christophe} and Rico Schwartz and Swarup Deb and Aditya Mohite and Stier, {Andreas V.} and Finley, {Jonathan J.} and Tobias Korn",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = dec,

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doi = "10.1021/acsnano.3c09001",

language = "English",

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T1 - Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI

AU - Kempf, Michael Andreas

AU - Moser, Philipp

AU - Tomoscheit, Maximilian

AU - Schröer, Julian

AU - Blancon, Jean Christophe

AU - Schwartz, Rico

AU - Deb, Swarup

AU - Mohite, Aditya

AU - Stier, Andreas V.

AU - Finley, Jonathan J.

AU - Korn, Tobias

PY - 2023/12/26

Y1 - 2023/12/26

N2 - We report temperature-dependent spectroscopy on the layered (n = 4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneously recorded time-resolved differential reflectivity (TRΔR) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin relaxation time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, spin relaxation is nearly T-independent. Our results highlight that spin relaxation in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aiming to utilize this degree of freedom.

AB - We report temperature-dependent spectroscopy on the layered (n = 4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneously recorded time-resolved differential reflectivity (TRΔR) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin relaxation time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, spin relaxation is nearly T-independent. Our results highlight that spin relaxation in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aiming to utilize this degree of freedom.

KW - (BA)(MA)PbI

KW - layered perovskites

KW - photocarrier dynamics

KW - spin dynamics

KW - time-resolved spectroscopy

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JO - ACS Nano

JF - ACS Nano

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ER -

Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI

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