Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals: the effect of surface layer

Weihua Lin; Mingli Liang; Yuran Niu; Zhesheng Chen; Marie Cherasse; Jie Meng; Xianshao Zou; Qian Zhao; Huifang Geng; Evangelos Papalazarou; Marino Marsi; Luca Perfetti; Sophie E. Canton; Kaibo Zheng; Tönu Pullerits

doi:10.1039/D2TC03111F

Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals: the effect of surface layer†

Weihua Lin,

‡^a Mingli Liang,‡^ab Yuran Niu,^c Zhesheng Chen,^d Marie Cherasse,^de Jie Meng,

^ab Xianshao Zou,^a Qian Zhao,^b Huifang Geng,^f Evangelos Papalazarou,^g Marino Marsi,^g Luca Perfetti,^d Sophie E. Canton,*^bh Kaibo Zheng*^ab and Tönu Pullerits

*^a

Author affiliations

* Corresponding authors

^a Chemical Physics and NanoLund, Lund University, Box 124, 22100 Lund, Sweden
E-mail: tonu.pullerits@chemphys.lu.se, kaibo.zheng@chemphys.lu.se

^b Department of Chemistry, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark

^c MAX IV Laboratory, Lund University, P.O. Box 118, 22100 Lund, Sweden

^d Laboratoire des Solides Irradiés, CEA/DRF/IRAMIS, CNRS, Ecole polytechnique, Institut Polytechnique de Paris, 91120 Palaiseau, France

^e Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany

^f Ultrafast Electron Microscopy Laboratory, The MOE Key Laboratory of Weak-Light Nonlinear Photonics, School of Physics, Nankai University, Tianjin 300071, China

^g Laboratoire de Physique des Solides, CNRS, Université Paris Saclay, Orsay 91405, France

^h European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany
E-mail: sophie.canton@xfel.eu

Abstract

We investigate hot carrier (HC) cooling in two-dimensional (2D) perovskite single crystals by applying two complementary ultrafast spectroscopy techniques – transient absorption (TA) and time-resolved two-photon photoemission (TR-2PPE) spectroscopies. TR-2PPE directly maps the hot electron distribution and its dynamics in the conduction band to the detected photoelectron distribution. While TR-2PPE selectively probes the upper layer of the material, TA provides information on the whole bulk. Two cooling regimes are resolved in both techniques. The fast timescale of 100–200 fs is related to the electron scattering by longitudinal optical (LO) phonons and the slow timescale of 3–4 ps corresponds to the LO phonon relaxation. The HC cooling dynamic of TA measurement has faster initial stage and higher starting temperature for the slower stage than in TR-2PPE measurements. Conclusions about spatial sensitivity of the cooling dynamics across the 2D perovskite single crystals constitute valuable information that can guide the future development of HC solar cells and thermoelectric applications based on 2D perovskites.

Journal of Materials Chemistry C

Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals: the effect of surface layer†

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Combining two-photon photoemission and transient absorption spectroscopy to resolve hot carrier cooling in 2D perovskite single crystals: the effect of surface layer

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