Abstract
Two-dimensional Ruddlesden-Popper (2D RP) halide perovskites, C2MAn-1PbnI3n+1 (C = bulky ammonium cation; MA = methylammonium) with low n-members (n < 5), have been garnering sensational attention for photovoltaic and optoelectronic applications because of the long carrier diffusion lengths, long-term stability, and tunable bandgap. Yet, the surface modification of 2D RP under kinetic particle irradiation, such as light or electron irradiation, is ambiguous, even though it is imperative to elucidate long-stabilized conversion efficiency. Herein, we present molecular-scale observations of dynamic surface reconstruction of BA2MA2Pb3I10 (n = 3) 2D RP induced by the electron beam. The surface dynamics reveal lateral growth of polytypic PbI2 with 3R, 4H, and 2H structures at the edge and surface of the 2D perovskite, accompanied by simultaneous annihilation at the other edges. Local radiolysis occurs dominantly by the internal energy increase of electron momentum transfer, which triggers a sequential layer-by-layer degradation into PbI2. In situ observation of the polytypic PbI2 growth at the whole surface and edges of 2D RP under electron irradiation elucidates how the outer PbI2 self-passivation can protect inner 2D RP, causing longer operando stability.
| Original language | English |
|---|---|
| Pages (from-to) | 6109-6117 |
| Number of pages | 9 |
| Journal | Nano letters |
| Volume | 19 |
| Issue number | 9 |
| DOIs | |
| Publication status | Published - Sep 11 2019 |
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Keywords
- 2D Ruddlesden−Popper halide perovskite
- BAMAPbI 2D halide perovskite
- electron beam irradiation
- in situ TEM
- long-term stability
- polytypic PbI surface self-passivation
ASJC Scopus subject areas
- Bioengineering
- Chemistry(all)
- Materials Science(all)
- Condensed Matter Physics
- Mechanical Engineering
Cite this
Self-Passivation of 2D Ruddlesden-Popper Perovskite by Polytypic Surface PbI2 Encapsulation. / Jung, Hee Joon; Stompus, Constantinos C.; Kanatzidis, Mercouri G; Dravid, Vinayak P.
In: Nano letters, Vol. 19, No. 9, 11.09.2019, p. 6109-6117.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Self-Passivation of 2D Ruddlesden-Popper Perovskite by Polytypic Surface PbI2 Encapsulation
AU - Jung, Hee Joon
AU - Stompus, Constantinos C.
AU - Kanatzidis, Mercouri G
AU - Dravid, Vinayak P.
PY - 2019/9/11
Y1 - 2019/9/11
N2 - Two-dimensional Ruddlesden-Popper (2D RP) halide perovskites, C2MAn-1PbnI3n+1 (C = bulky ammonium cation; MA = methylammonium) with low n-members (n < 5), have been garnering sensational attention for photovoltaic and optoelectronic applications because of the long carrier diffusion lengths, long-term stability, and tunable bandgap. Yet, the surface modification of 2D RP under kinetic particle irradiation, such as light or electron irradiation, is ambiguous, even though it is imperative to elucidate long-stabilized conversion efficiency. Herein, we present molecular-scale observations of dynamic surface reconstruction of BA2MA2Pb3I10 (n = 3) 2D RP induced by the electron beam. The surface dynamics reveal lateral growth of polytypic PbI2 with 3R, 4H, and 2H structures at the edge and surface of the 2D perovskite, accompanied by simultaneous annihilation at the other edges. Local radiolysis occurs dominantly by the internal energy increase of electron momentum transfer, which triggers a sequential layer-by-layer degradation into PbI2. In situ observation of the polytypic PbI2 growth at the whole surface and edges of 2D RP under electron irradiation elucidates how the outer PbI2 self-passivation can protect inner 2D RP, causing longer operando stability.
AB - Two-dimensional Ruddlesden-Popper (2D RP) halide perovskites, C2MAn-1PbnI3n+1 (C = bulky ammonium cation; MA = methylammonium) with low n-members (n < 5), have been garnering sensational attention for photovoltaic and optoelectronic applications because of the long carrier diffusion lengths, long-term stability, and tunable bandgap. Yet, the surface modification of 2D RP under kinetic particle irradiation, such as light or electron irradiation, is ambiguous, even though it is imperative to elucidate long-stabilized conversion efficiency. Herein, we present molecular-scale observations of dynamic surface reconstruction of BA2MA2Pb3I10 (n = 3) 2D RP induced by the electron beam. The surface dynamics reveal lateral growth of polytypic PbI2 with 3R, 4H, and 2H structures at the edge and surface of the 2D perovskite, accompanied by simultaneous annihilation at the other edges. Local radiolysis occurs dominantly by the internal energy increase of electron momentum transfer, which triggers a sequential layer-by-layer degradation into PbI2. In situ observation of the polytypic PbI2 growth at the whole surface and edges of 2D RP under electron irradiation elucidates how the outer PbI2 self-passivation can protect inner 2D RP, causing longer operando stability.
KW - 2D Ruddlesden−Popper halide perovskite
KW - BAMAPbI 2D halide perovskite
KW - electron beam irradiation
KW - in situ TEM
KW - long-term stability
KW - polytypic PbI surface self-passivation
UR - http://www.scopus.com/inward/record.url?scp=85072133527&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85072133527&partnerID=8YFLogxK
U2 - 10.1021/acs.nanolett.9b02069
DO - 10.1021/acs.nanolett.9b02069
M3 - Article
VL - 19
SP - 6109
EP - 6117
JO - Nano Letters
JF - Nano Letters
SN - 1530-6984
IS - 9
ER -