Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals

Maryna I. Bodnarchuk, Simon C. Boehme, Stephanie Ten Brinck, Caterina Bernasconi, Yevhen Shynkarenko, Franziska Krieg, Roland Widmer, Beat Aeschlimann, Detlef Günther, Maksym V. Kovalenko, Ivan Infante

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and luminescent properties are challenged by the lability of their surfaces, i.e., the interface of the NC core and the ligand shell. On the example of CsPbBr3 NCs, we model the nanocrystal surface structure and its effect on the emergence of trap states using density functional theory. We rationalize the typical observation of a degraded luminescence upon aging or the luminescence recovery upon postsynthesis surface treatments. The conclusions are corroborated by the elemental analysis. We then propose a strategy for healing the surface trap states and for improving the colloidal stability by the combined treatment with didodecyldimethylammonium bromide and lead bromide and validate this approach experimentally. This simple procedure results in robust colloids, which are highly pure and exhibit high photoluminescence quantum yields of up to 95-98%, retained even after three to four rounds of washing.

Original languageEnglish
Pages (from-to)63-74
Number of pages12
JournalACS Energy Letters
Volume4
Issue number1
Early online date27 Nov 2018
DOIs
Publication statusPublished - 11 Jan 2019

Fingerprint

Cesium
Passivation
Surface structure
Nanocrystals
Lead
Luminescence
Colloids
Quantum yield
Washing
Perovskite
Photonics
Density functional theory
Surface treatment
Photoluminescence
Aging of materials
Ligands
Recovery
Processing
Chemical analysis

Cite this

Bodnarchuk, Maryna I. ; Boehme, Simon C. ; Ten Brinck, Stephanie ; Bernasconi, Caterina ; Shynkarenko, Yevhen ; Krieg, Franziska ; Widmer, Roland ; Aeschlimann, Beat ; Günther, Detlef ; Kovalenko, Maksym V. ; Infante, Ivan. / Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals. In: ACS Energy Letters. 2019 ; Vol. 4, No. 1. pp. 63-74.
@article{b36f8cb24da5459cbfc9d4763fed86c3,
title = "Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals",
abstract = "Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and luminescent properties are challenged by the lability of their surfaces, i.e., the interface of the NC core and the ligand shell. On the example of CsPbBr3 NCs, we model the nanocrystal surface structure and its effect on the emergence of trap states using density functional theory. We rationalize the typical observation of a degraded luminescence upon aging or the luminescence recovery upon postsynthesis surface treatments. The conclusions are corroborated by the elemental analysis. We then propose a strategy for healing the surface trap states and for improving the colloidal stability by the combined treatment with didodecyldimethylammonium bromide and lead bromide and validate this approach experimentally. This simple procedure results in robust colloids, which are highly pure and exhibit high photoluminescence quantum yields of up to 95-98{\%}, retained even after three to four rounds of washing.",
author = "Bodnarchuk, {Maryna I.} and Boehme, {Simon C.} and {Ten Brinck}, Stephanie and Caterina Bernasconi and Yevhen Shynkarenko and Franziska Krieg and Roland Widmer and Beat Aeschlimann and Detlef G{\"u}nther and Kovalenko, {Maksym V.} and Ivan Infante",
year = "2019",
month = "1",
day = "11",
doi = "10.1021/acsenergylett.8b01669",
language = "English",
volume = "4",
pages = "63--74",
journal = "ACS Energy Letters",
issn = "2380-8195",
publisher = "American Chemical Society",
number = "1",

}

Bodnarchuk, MI, Boehme, SC, Ten Brinck, S, Bernasconi, C, Shynkarenko, Y, Krieg, F, Widmer, R, Aeschlimann, B, Günther, D, Kovalenko, MV & Infante, I 2019, 'Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals' ACS Energy Letters, vol. 4, no. 1, pp. 63-74. https://doi.org/10.1021/acsenergylett.8b01669

Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals. / Bodnarchuk, Maryna I.; Boehme, Simon C.; Ten Brinck, Stephanie; Bernasconi, Caterina; Shynkarenko, Yevhen; Krieg, Franziska; Widmer, Roland; Aeschlimann, Beat; Günther, Detlef; Kovalenko, Maksym V.; Infante, Ivan.

In: ACS Energy Letters, Vol. 4, No. 1, 11.01.2019, p. 63-74.

Research output: Contribution to JournalArticleAcademicpeer-review

TY - JOUR

T1 - Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals

AU - Bodnarchuk, Maryna I.

AU - Boehme, Simon C.

AU - Ten Brinck, Stephanie

AU - Bernasconi, Caterina

AU - Shynkarenko, Yevhen

AU - Krieg, Franziska

AU - Widmer, Roland

AU - Aeschlimann, Beat

AU - Günther, Detlef

AU - Kovalenko, Maksym V.

AU - Infante, Ivan

PY - 2019/1/11

Y1 - 2019/1/11

N2 - Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and luminescent properties are challenged by the lability of their surfaces, i.e., the interface of the NC core and the ligand shell. On the example of CsPbBr3 NCs, we model the nanocrystal surface structure and its effect on the emergence of trap states using density functional theory. We rationalize the typical observation of a degraded luminescence upon aging or the luminescence recovery upon postsynthesis surface treatments. The conclusions are corroborated by the elemental analysis. We then propose a strategy for healing the surface trap states and for improving the colloidal stability by the combined treatment with didodecyldimethylammonium bromide and lead bromide and validate this approach experimentally. This simple procedure results in robust colloids, which are highly pure and exhibit high photoluminescence quantum yields of up to 95-98%, retained even after three to four rounds of washing.

AB - Colloidal lead halide perovskite nanocrystals (NCs) have recently emerged as versatile photonic sources. Their processing and luminescent properties are challenged by the lability of their surfaces, i.e., the interface of the NC core and the ligand shell. On the example of CsPbBr3 NCs, we model the nanocrystal surface structure and its effect on the emergence of trap states using density functional theory. We rationalize the typical observation of a degraded luminescence upon aging or the luminescence recovery upon postsynthesis surface treatments. The conclusions are corroborated by the elemental analysis. We then propose a strategy for healing the surface trap states and for improving the colloidal stability by the combined treatment with didodecyldimethylammonium bromide and lead bromide and validate this approach experimentally. This simple procedure results in robust colloids, which are highly pure and exhibit high photoluminescence quantum yields of up to 95-98%, retained even after three to four rounds of washing.

UR - http://www.scopus.com/inward/record.url?scp=85058177905&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85058177905&partnerID=8YFLogxK

U2 - 10.1021/acsenergylett.8b01669

DO - 10.1021/acsenergylett.8b01669

M3 - Article

VL - 4

SP - 63

EP - 74

JO - ACS Energy Letters

JF - ACS Energy Letters

SN - 2380-8195

IS - 1

ER -