Transient High-Harmonic Spectroscopy in an Inorganic-Organic Lead Halide Perovskite

Maarten L.S. van der Geest; Jeroen J. de Boer; Kevin Murzyn; Peter Jürgens; Bruno Ehrler; Peter M. Kraus

doi:10.1021/acs.jpclett.3c02588

Transient High-Harmonic Spectroscopy in an Inorganic-Organic Lead Halide Perovskite

Maarten L.S. van der Geest
, Jeroen J. de Boer
, Kevin Murzyn
, Peter Jürgens
, Bruno Ehrler
, Peter M. Kraus^*

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

High-harmonic generation is the frequency upconversion of an intense femtosecond infrared laser in a material. In condensed-phase high-harmonic generation, laser-driven currents of coherently excited charge carriers map the electronic structure onto the emitted light. This promises a thus far scarcely explored potential of condensed-phase time-resolved high-harmonic spectroscopy for probing carrier dynamics. Here, we realize this potential and use time-resolved solid-state high-harmonic spectroscopy from a laser-excited methylammonium lead bromide (MAPbBr₃) thin film, a key material in perovskite solar cells, for measuring carrier cooling and relaxation on femto- and picosecond time scales. Through comparison with transient absorption, we show the links between carrier dynamics and experimental observables of generated harmonics.

Original language	English
Pages (from-to)	10810-10818
Number of pages	9
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	48
Early online date	28 Nov 2023
DOIs	https://doi.org/10.1021/acs.jpclett.3c02588
Publication status	Published - 7 Dec 2023

Bibliographical note

Funding Information:
This work has been carried out at the Advanced Research Center for Nanolithography (ARCNL), a public-private partnership of the University of Amsterdam (UvA), the Vrije Universiteit Amsterdam (VU), The Netherlands Organisation for Scientific Research (NWO), and the semiconductor equipment manufacturer ASML, and was partly financed by “Toeslag voor Topconsortia voor Kennis en Innovatie (TKI)” from the Dutch Ministry of Economic Affairs and Climate Policy. The work of J.J.d.B. and B.E. was carried out at the research institute AMOLF, which is part of NWO. P.J. acknowledges funding by the German Research Foundation - SFB1477 “Light-Matter Interaction at Interfaces”, project no. 441234705. We acknowledge support from ERC Starting Grants ANACONDA (Grant No. 101041819) and SHAPE (Grant No. 999624092). The authors acknowledge assistance from the software engineering department and mechanical workshops at AMOLF and ARCNL for construction and implementation of the experimental setup. Furthermore, the authors would like to thank Dr. W.G. Roeterdink for extensive help with the TA measurements. Finally, the authors thank Dr. C.S. Lehmann for technical assistance and Dr. Z. Nie for valuable comments and discussion.

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

Funding

This work has been carried out at the Advanced Research Center for Nanolithography (ARCNL), a public-private partnership of the University of Amsterdam (UvA), the Vrije Universiteit Amsterdam (VU), The Netherlands Organisation for Scientific Research (NWO), and the semiconductor equipment manufacturer ASML, and was partly financed by “Toeslag voor Topconsortia voor Kennis en Innovatie (TKI)” from the Dutch Ministry of Economic Affairs and Climate Policy. The work of J.J.d.B. and B.E. was carried out at the research institute AMOLF, which is part of NWO. P.J. acknowledges funding by the German Research Foundation - SFB1477 “Light-Matter Interaction at Interfaces”, project no. 441234705. We acknowledge support from ERC Starting Grants ANACONDA (Grant No. 101041819) and SHAPE (Grant No. 999624092). The authors acknowledge assistance from the software engineering department and mechanical workshops at AMOLF and ARCNL for construction and implementation of the experimental setup. Furthermore, the authors would like to thank Dr. W.G. Roeterdink for extensive help with the TA measurements. Finally, the authors thank Dr. C.S. Lehmann for technical assistance and Dr. Z. Nie for valuable comments and discussion.

Funders	Funder number
AMOLF
Physics of Nanolithography
Toeslag voor Topconsortia voor Kennis en Innovatie
European Research Council	101041819, 999624092
Deutsche Forschungsgemeinschaft	SFB1477, 441234705
Universiteit van Amsterdam
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Ministerie van Economische Zaken en Klimaat

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title = "Transient High-Harmonic Spectroscopy in an Inorganic-Organic Lead Halide Perovskite",

abstract = "High-harmonic generation is the frequency upconversion of an intense femtosecond infrared laser in a material. In condensed-phase high-harmonic generation, laser-driven currents of coherently excited charge carriers map the electronic structure onto the emitted light. This promises a thus far scarcely explored potential of condensed-phase time-resolved high-harmonic spectroscopy for probing carrier dynamics. Here, we realize this potential and use time-resolved solid-state high-harmonic spectroscopy from a laser-excited methylammonium lead bromide (MAPbBr3) thin film, a key material in perovskite solar cells, for measuring carrier cooling and relaxation on femto- and picosecond time scales. Through comparison with transient absorption, we show the links between carrier dynamics and experimental observables of generated harmonics.",

author = "\{van der Geest\}, \{Maarten L.S.\} and \{de Boer\}, \{Jeroen J.\} and Kevin Murzyn and Peter J{\"u}rgens and Bruno Ehrler and Kraus, \{Peter M.\}",

note = "Funding Information: This work has been carried out at the Advanced Research Center for Nanolithography (ARCNL), a public-private partnership of the University of Amsterdam (UvA), the Vrije Universiteit Amsterdam (VU), The Netherlands Organisation for Scientific Research (NWO), and the semiconductor equipment manufacturer ASML, and was partly financed by “Toeslag voor Topconsortia voor Kennis en Innovatie (TKI)” from the Dutch Ministry of Economic Affairs and Climate Policy. The work of J.J.d.B. and B.E. was carried out at the research institute AMOLF, which is part of NWO. P.J. acknowledges funding by the German Research Foundation - SFB1477 “Light-Matter Interaction at Interfaces”, project no. 441234705. We acknowledge support from ERC Starting Grants ANACONDA (Grant No. 101041819) and SHAPE (Grant No. 999624092). The authors acknowledge assistance from the software engineering department and mechanical workshops at AMOLF and ARCNL for construction and implementation of the experimental setup. Furthermore, the authors would like to thank Dr. W.G. Roeterdink for extensive help with the TA measurements. Finally, the authors thank Dr. C.S. Lehmann for technical assistance and Dr. Z. Nie for valuable comments and discussion. Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

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AU - Jürgens, Peter

AU - Ehrler, Bruno

AU - Kraus, Peter M.

N1 - Funding Information: This work has been carried out at the Advanced Research Center for Nanolithography (ARCNL), a public-private partnership of the University of Amsterdam (UvA), the Vrije Universiteit Amsterdam (VU), The Netherlands Organisation for Scientific Research (NWO), and the semiconductor equipment manufacturer ASML, and was partly financed by “Toeslag voor Topconsortia voor Kennis en Innovatie (TKI)” from the Dutch Ministry of Economic Affairs and Climate Policy. The work of J.J.d.B. and B.E. was carried out at the research institute AMOLF, which is part of NWO. P.J. acknowledges funding by the German Research Foundation - SFB1477 “Light-Matter Interaction at Interfaces”, project no. 441234705. We acknowledge support from ERC Starting Grants ANACONDA (Grant No. 101041819) and SHAPE (Grant No. 999624092). The authors acknowledge assistance from the software engineering department and mechanical workshops at AMOLF and ARCNL for construction and implementation of the experimental setup. Furthermore, the authors would like to thank Dr. W.G. Roeterdink for extensive help with the TA measurements. Finally, the authors thank Dr. C.S. Lehmann for technical assistance and Dr. Z. Nie for valuable comments and discussion. Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.

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N2 - High-harmonic generation is the frequency upconversion of an intense femtosecond infrared laser in a material. In condensed-phase high-harmonic generation, laser-driven currents of coherently excited charge carriers map the electronic structure onto the emitted light. This promises a thus far scarcely explored potential of condensed-phase time-resolved high-harmonic spectroscopy for probing carrier dynamics. Here, we realize this potential and use time-resolved solid-state high-harmonic spectroscopy from a laser-excited methylammonium lead bromide (MAPbBr3) thin film, a key material in perovskite solar cells, for measuring carrier cooling and relaxation on femto- and picosecond time scales. Through comparison with transient absorption, we show the links between carrier dynamics and experimental observables of generated harmonics.

AB - High-harmonic generation is the frequency upconversion of an intense femtosecond infrared laser in a material. In condensed-phase high-harmonic generation, laser-driven currents of coherently excited charge carriers map the electronic structure onto the emitted light. This promises a thus far scarcely explored potential of condensed-phase time-resolved high-harmonic spectroscopy for probing carrier dynamics. Here, we realize this potential and use time-resolved solid-state high-harmonic spectroscopy from a laser-excited methylammonium lead bromide (MAPbBr3) thin film, a key material in perovskite solar cells, for measuring carrier cooling and relaxation on femto- and picosecond time scales. Through comparison with transient absorption, we show the links between carrier dynamics and experimental observables of generated harmonics.

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JF - Journal of Physical Chemistry Letters

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ER -

Transient High-Harmonic Spectroscopy in an Inorganic-Organic Lead Halide Perovskite

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