Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

Timo Neumann; Sascha Feldmann; Philipp Moser; Alex Delhomme; Jonathan Zerhoch; Tim van de Goor; Shuli Wang; Mateusz Dyksik; Thomas Winkler; Jonathan J. Finley; Paulina Plochocka; Martin S. Brandt; Clément Faugeras; Andreas V. Stier; Felix Deschler

doi:10.1038/s41467-021-23602-1

Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

Timo Neumann, Sascha Feldmann, Philipp Moser, Alex Delhomme, Jonathan Zerhoch, Tim van de Goor, Shuli Wang, Mateusz Dyksik, Thomas Winkler, Jonathan J. Finley, Paulina Plochocka, Martin S. Brandt, Clément Faugeras, Andreas V. Stier, Felix Deschler

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

53 Scopus citations

Abstract

Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)₂PbI₄ (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn²⁺ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

Original language	English
Article number	3489
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-23602-1
State	Published - 1 Dec 2021

Access to Document

10.1038/s41467-021-23602-1

Cite this

Neumann, T., Feldmann, S., Moser, P., Delhomme, A., Zerhoch, J., van de Goor, T., Wang, S., Dyksik, M., Winkler, T., Finley, J. J., Plochocka, P., Brandt, M. S., Faugeras, C., Stier, A. V., & Deschler, F. (2021). Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites. Nature Communications, 12(1), Article 3489. https://doi.org/10.1038/s41467-021-23602-1

@article{75b05f5076a340b69c856eeebceadb05,

title = "Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites",

abstract = "Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13\% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.",

author = "Timo Neumann and Sascha Feldmann and Philipp Moser and Alex Delhomme and Jonathan Zerhoch and \{van de Goor\}, Tim and Shuli Wang and Mateusz Dyksik and Thomas Winkler and Finley, \{Jonathan J.\} and Paulina Plochocka and Brandt, \{Martin S.\} and Cl{\'e}ment Faugeras and Stier, \{Andreas V.\} and Felix Deschler",

note = "Publisher Copyright: {\textcopyright} 2021, The Author(s).",

year = "2021",

month = dec,

day = "1",

doi = "10.1038/s41467-021-23602-1",

language = "English",

volume = "12",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

Neumann, T, Feldmann, S, Moser, P, Delhomme, A, Zerhoch, J, van de Goor, T, Wang, S, Dyksik, M, Winkler, T, Finley, JJ, Plochocka, P, Brandt, MS, Faugeras, C, Stier, AV & Deschler, F 2021, 'Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites', Nature Communications, vol. 12, no. 1, 3489. https://doi.org/10.1038/s41467-021-23602-1

TY - JOUR

T1 - Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

AU - Neumann, Timo

AU - Feldmann, Sascha

AU - Moser, Philipp

AU - Delhomme, Alex

AU - Zerhoch, Jonathan

AU - van de Goor, Tim

AU - Wang, Shuli

AU - Dyksik, Mateusz

AU - Winkler, Thomas

AU - Finley, Jonathan J.

AU - Plochocka, Paulina

AU - Brandt, Martin S.

AU - Faugeras, Clément

AU - Stier, Andreas V.

AU - Deschler, Felix

PY - 2021/12/1

Y1 - 2021/12/1

N2 - Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

AB - Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

UR - https://www.scopus.com/pages/publications/85107495896

U2 - 10.1038/s41467-021-23602-1

DO - 10.1038/s41467-021-23602-1

M3 - Article

C2 - 34108469

AN - SCOPUS:85107495896

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 3489

ER -

Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

Abstract

Access to Document

Other files and links

Fingerprint

Cite this