PMID- 35025199
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20221109
IS  - 1936-086X (Electronic)
IS  - 1936-0851 (Linking)
VI  - 16
IP  - 1
DP  - 2022 Jan 25
TI  - Guanidinium-Pseudohalide Perovskite Interfaces Enable Surface Reconstruction of 
      Colloidal Quantum Dots for Efficient and Stable Photovoltaics.
PG  - 1649-1660
LID - 10.1021/acsnano.1c10636 [doi]
AB  - Complete surface passivation of colloidal quantum dots (CQDs) and their strong 
      electronic coupling are key factors toward high-performance CQD-based 
      photovoltaics (CQDPVs). Also, the CQD matrices must be protected from oxidative 
      environments, such as ambient air and moisture, to guarantee air-stable operation 
      of the CQDPVs. Herein, we devise a complementary and effective approach to 
      reconstruct the oxidized CQD surface using guanidinium and pseudohalide. Unlike 
      conventional halides, thiocyanate anions provide better surface passivation with 
      effective replacement of surface oxygen species and additional filling of 
      defective sites, whereas guanidinium cations promote the construction of 
      epitaxial perovskite bridges within the CQD matrix and augment electronic 
      coupling. Additionally, we replace a defective 1,2-ethanedithiol-treated CQD hole 
      transport layer (HTL) with robust polymeric HTLs, based on a judicious 
      consideration of the energy level alignment established at the CQD/HTL interface. 
      These efforts collectively result in high-performance and stable CQDPVs with 
      photocurrents over 30 mA cm(-2),  approximately 80% quantum efficiency at excitonic peaks and 
      stable operation under humid and ambient conditions. Elucidation of carrier 
      dynamics further reveals that interfacial recombination associated with band 
      alignment governs both the CQDPV performance and stability.
FAU - Yang, Jonghee
AU  - Yang J
AUID- ORCID: 0000-0001-7013-6761
AD  - Institute for Advanced Materials and Manufacturing, Department of Materials 
      Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, 
      United States.
FAU - Cho, Seong Chan
AU  - Cho SC
AD  - Department of Applied Chemistry, Center for Bionano Intelligence Education and 
      Research, Hanyang University, Ansan 15588, Republic of Korea.
FAU - Lee, Seungjin
AU  - Lee S
AUID- ORCID: 0000-0002-6318-0702
AD  - Department of Electrical and Computer Engineering, University of Toronto, 
      Toronto, Ontario M5S 3G4, Canada.
FAU - Yoon, Jung Won
AU  - Yoon JW
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Jeong, Woo Hyeon
AU  - Jeong WH
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Song, Hochan
AU  - Song H
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Oh, Jae Taek
AU  - Oh JT
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Lim, Seul Gi
AU  - Lim SG
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Bae, Sung Yong
AU  - Bae SY
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
FAU - Lee, Bo Ram
AU  - Lee BR
AUID- ORCID: 0000-0002-4670-6717
AD  - Department of Physics, Pukyong National University, Busan 48513, Republic of 
      Korea.
FAU - Ahmadi, Mahshid
AU  - Ahmadi M
AUID- ORCID: 0000-0002-3268-7957
AD  - Institute for Advanced Materials and Manufacturing, Department of Materials 
      Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, 
      United States.
FAU - Sargent, Edward H
AU  - Sargent EH
AUID- ORCID: 0000-0003-0396-6495
AD  - Department of Electrical and Computer Engineering, University of Toronto, 
      Toronto, Ontario M5S 3G4, Canada.
FAU - Yi, Whikun
AU  - Yi W
AUID- ORCID: 0000-0001-8402-9289
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
AD  - Research Institute for Natural Sciences, Hanyang University, Seoul 04763, 
      Republic of Korea.
FAU - Lee, Sang Uck
AU  - Lee SU
AUID- ORCID: 0000-0001-9596-2349
AD  - Department of Applied Chemistry, Center for Bionano Intelligence Education and 
      Research, Hanyang University, Ansan 15588, Republic of Korea.
FAU - Choi, Hyosung
AU  - Choi H
AUID- ORCID: 0000-0003-4573-9012
AD  - Department of Chemistry, Hanyang University, Seoul 04763, Republic of Korea.
AD  - Research Institute for Natural Sciences, Hanyang University, Seoul 04763, 
      Republic of Korea.
AD  - Research Institute for Convergence of Basic Science, Hanyang University, Seoul 
      04763, Republic of Korea.
LA  - eng
PT  - Journal Article
DEP - 20220113
PL  - United States
TA  - ACS Nano
JT  - ACS nano
JID - 101313589
SB  - IM
OTO - NOTNLM
OT  - Colloidal Quantum Dots
OT  - Guanidinium
OT  - Perovskites
OT  - Photovoltaics
OT  - Pseudohalides
EDAT- 2022/01/14 06:00
MHDA- 2022/01/14 06:01
CRDT- 2022/01/13 17:12
PHST- 2022/01/14 06:00 [pubmed]
PHST- 2022/01/14 06:01 [medline]
PHST- 2022/01/13 17:12 [entrez]
AID - 10.1021/acsnano.1c10636 [doi]
PST - ppublish
SO  - ACS Nano. 2022 Jan 25;16(1):1649-1660. doi: 10.1021/acsnano.1c10636. Epub 2022 
      Jan 13.