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Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets

Sushant Ghimire Orcid Logo, Chris Rehhagen Orcid Logo, Saskia Fiedler, Urvi Parekh, Rostyslav Lesyuk, Stefan Lochbrunner Orcid Logo, Christian Klinke Orcid Logo

Nanoscale, Volume: 15, Issue: 5, Pages: 2096 - 2105

Swansea University Author: Christian Klinke Orcid Logo

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DOI (Published version): 10.1039/d2nr06048e

Abstract

Non-toxicity and stability make two-dimensional (2D) bismuth halide perovskites better alternatives to lead-based ones for optoelectronic applications and catalysis. In this work, we synthesize sub-micron size colloidal quasi-2D Cs3Bi2I9 perovskite nanosheets and study their generation and relaxatio...

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Published in: Nanoscale
ISSN: 2040-3364 2040-3372
Published: Royal Society of Chemistry (RSC) 2022
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URI: https://cronfa.swan.ac.uk/Record/cronfa62450
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In this work, we synthesize sub-micron size colloidal quasi-2D Cs3Bi2I9 perovskite nanosheets and study their generation and relaxation of charge carriers. Steady-state absorption spectroscopy reveals an indirect bandgap of 2.07 eV, which is supported by the band structure calculated using density functional theory. The nanosheets show no detectable photoluminescence at room temperature at near bandgap excitation which is attributed to the indirect bandgap. However, cathodoluminescence spanning a broad range from 500 nm to 750 nm with an asymmetric and Stokes-shifted emission is observed, indicating the phonon- and trap-assisted recombination of charge carriers. We study the ultrafast charge carrier dynamics in Cs3Bi2I9 nanosheets using femtosecond transient absorption spectroscopy. The samples are excited with photon energies higher than their bandgap, and the results are interpreted in terms of hot carrier generation (&lt;1 ps), thermalization with local phonons (∼1 ps), and cooling (&gt;30 ps). Further, a relatively slow relaxation of excitons (≳3 ns) at the band edge suggests the formation of stable polarons which decay nonradiatively by releasing phonons.</abstract><type>Journal Article</type><journal>Nanoscale</journal><volume>15</volume><journalNumber>5</journalNumber><paginationStart>2096</paginationStart><paginationEnd>2105</paginationEnd><publisher>Royal Society of Chemistry (RSC)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>2040-3364</issnPrint><issnElectronic>2040-3372</issnElectronic><keywords/><publishedDay>30</publishedDay><publishedMonth>12</publishedMonth><publishedYear>2022</publishedYear><publishedDate>2022-12-30</publishedDate><doi>10.1039/d2nr06048e</doi><url>http://dx.doi.org/10.1039/d2nr06048e</url><notes/><college>COLLEGE NANME</college><department>Chemistry</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>CHEM</DepartmentCode><institution>Swansea University</institution><apcterm>Other</apcterm><funders>S. G. acknowledges Alexander von Humboldt-Stiftung/ Foundation for the postdoctoral research fellowship. C. K. acknowledges the European Regional Development Fund of the European Union for funding the PL spectrometer (GHS-20- 0035/P000376218) and X-ray diffractometer (GHS-20-0036/ P000379642) and the Deutsche Forschungsgemeinschaft (DFG) for funding an electron microscope ThermoFisher Talos L120C (INST 264/188-1 FUGG) and for supporting the collaborative research center SFB 1477 “Light-Matter Interactions at Interfaces (LiMatI)”, project number 441234705. C. 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spelling v2 62450 2023-01-26 Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets c10c44238eabfb203111f88a965f5372 0000-0001-8558-7389 Christian Klinke Christian Klinke true false 2023-01-26 CHEM Non-toxicity and stability make two-dimensional (2D) bismuth halide perovskites better alternatives to lead-based ones for optoelectronic applications and catalysis. In this work, we synthesize sub-micron size colloidal quasi-2D Cs3Bi2I9 perovskite nanosheets and study their generation and relaxation of charge carriers. Steady-state absorption spectroscopy reveals an indirect bandgap of 2.07 eV, which is supported by the band structure calculated using density functional theory. The nanosheets show no detectable photoluminescence at room temperature at near bandgap excitation which is attributed to the indirect bandgap. However, cathodoluminescence spanning a broad range from 500 nm to 750 nm with an asymmetric and Stokes-shifted emission is observed, indicating the phonon- and trap-assisted recombination of charge carriers. We study the ultrafast charge carrier dynamics in Cs3Bi2I9 nanosheets using femtosecond transient absorption spectroscopy. The samples are excited with photon energies higher than their bandgap, and the results are interpreted in terms of hot carrier generation (<1 ps), thermalization with local phonons (∼1 ps), and cooling (>30 ps). Further, a relatively slow relaxation of excitons (≳3 ns) at the band edge suggests the formation of stable polarons which decay nonradiatively by releasing phonons. Journal Article Nanoscale 15 5 2096 2105 Royal Society of Chemistry (RSC) 2040-3364 2040-3372 30 12 2022 2022-12-30 10.1039/d2nr06048e http://dx.doi.org/10.1039/d2nr06048e COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University Other S. G. acknowledges Alexander von Humboldt-Stiftung/ Foundation for the postdoctoral research fellowship. C. K. acknowledges the European Regional Development Fund of the European Union for funding the PL spectrometer (GHS-20- 0035/P000376218) and X-ray diffractometer (GHS-20-0036/ P000379642) and the Deutsche Forschungsgemeinschaft (DFG) for funding an electron microscope ThermoFisher Talos L120C (INST 264/188-1 FUGG) and for supporting the collaborative research center SFB 1477 “Light-Matter Interactions at Interfaces (LiMatI)”, project number 441234705. C. R. acknowledges the financial support by the DFG via the priority program SPP 2102 (LO 714/11-1) and the Friedrich-Naumann Foundation for the graduate scholarship. 2023-06-12T14:44:18.4656020 2023-01-26T11:48:33.7222468 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Sushant Ghimire 0000-0002-4845-1236 1 Chris Rehhagen 0000-0001-5308-7910 2 Saskia Fiedler 3 Urvi Parekh 4 Rostyslav Lesyuk 5 Stefan Lochbrunner 0000-0001-9729-8277 6 Christian Klinke 0000-0001-8558-7389 7 62450__26524__d63a3684de324d21b43b3d70f729c478.pdf Ghimire-Klinke-2023-Manuscript.pdf 2023-02-10T15:45:50.0015531 Output 1861826 application/pdf Accepted Manuscript true true eng
title Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
spellingShingle Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
Christian Klinke
title_short Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
title_full Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
title_fullStr Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
title_full_unstemmed Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
title_sort Synthesis, optoelectronic properties, and charge carrier dynamics of colloidal quasi-two-dimensional Cs3Bi2I9 perovskite nanosheets
author_id_str_mv c10c44238eabfb203111f88a965f5372
author_id_fullname_str_mv c10c44238eabfb203111f88a965f5372_***_Christian Klinke
author Christian Klinke
author2 Sushant Ghimire
Chris Rehhagen
Saskia Fiedler
Urvi Parekh
Rostyslav Lesyuk
Stefan Lochbrunner
Christian Klinke
format Journal article
container_title Nanoscale
container_volume 15
container_issue 5
container_start_page 2096
publishDate 2022
institution Swansea University
issn 2040-3364
2040-3372
doi_str_mv 10.1039/d2nr06048e
publisher Royal Society of Chemistry (RSC)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
url http://dx.doi.org/10.1039/d2nr06048e
document_store_str 1
active_str 0
description Non-toxicity and stability make two-dimensional (2D) bismuth halide perovskites better alternatives to lead-based ones for optoelectronic applications and catalysis. In this work, we synthesize sub-micron size colloidal quasi-2D Cs3Bi2I9 perovskite nanosheets and study their generation and relaxation of charge carriers. Steady-state absorption spectroscopy reveals an indirect bandgap of 2.07 eV, which is supported by the band structure calculated using density functional theory. The nanosheets show no detectable photoluminescence at room temperature at near bandgap excitation which is attributed to the indirect bandgap. However, cathodoluminescence spanning a broad range from 500 nm to 750 nm with an asymmetric and Stokes-shifted emission is observed, indicating the phonon- and trap-assisted recombination of charge carriers. We study the ultrafast charge carrier dynamics in Cs3Bi2I9 nanosheets using femtosecond transient absorption spectroscopy. The samples are excited with photon energies higher than their bandgap, and the results are interpreted in terms of hot carrier generation (<1 ps), thermalization with local phonons (∼1 ps), and cooling (>30 ps). Further, a relatively slow relaxation of excitons (≳3 ns) at the band edge suggests the formation of stable polarons which decay nonradiatively by releasing phonons.
published_date 2022-12-30T14:44:17Z
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score 11.012678

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