PMID- 38086659 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20240102 IS - 1477-9234 (Electronic) IS - 1477-9226 (Linking) VI - 53 IP - 2 DP - 2024 Jan 2 TI - Critical role of dopant in NiO(x) hole transport layer for mitigating redox reactivity at NiO(x)/absorber interface in mixed cation perovskite solar cells. PG - 781-797 LID - 10.1039/d3dt03012a [doi] AB - Redox chemistry transpiring at the interface of NiO(x) hole transport layer (HTL) and perovskite absorber is a critical phenomenon leading to relatively low values of open circuit voltage (V(OC)) and fill factor (FF), in turn hampering the overall device performance and stability. In this work, for the first time, the hard acid electronic nature of vanadium (V) dopant in nickel oxide HTL is opportunely exploited to mitigate the undesirable Lewis acid-base reactions occurring at the HTL/mixed-cation perovskite interface. The findings of the study show that vanadium doping results in improved interfacial energetics along with decreased V(OC) loss, confirming that despite the increase in Ni(3+)/Ni(2+) ratio with the vanadium dopant, the redox reaction catalyzed by Ni(3+) ions is kept under check. Vanadium doping also aided in the realization of superior perovskite films with lower Urbach energy, which translated into one order increase in maximum photoinduced carrier generation rate per unit volume. Carrier dynamics investigations show fewer defect states (lower V(TFL)) and trap-assisted recombination (lower diode ideality factor), which optimize the devices' photovoltaic performance. These benefits collectively contribute to low-loss charge transfer across the NiO(x)/mixed-cation perovskite interface, which increases the relative efficiency by approximately 30% for 5 wt% V-doped NiO(x) devices compared to pristine NiO(x) devices, augmented by an increase in device J-V parameters like open circuit voltage (V(OC)), short circuit current density (J(SC)), and fill factor (FF). FAU - Sudhakaran Menon, Vidya AU - Sudhakaran Menon V AUID- ORCID: 0000-0002-7368-1500 AD - Organic and Perovskite Photovoltaics Laboratory (OPPV), Department of Chemistry, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu, 603203, India. ananthak@srmist.edu.in. FAU - Ganesan, Saraswathi AU - Ganesan S AUID- ORCID: 0000-0002-2335-2143 AD - Organic and Perovskite Photovoltaics Laboratory (OPPV), Department of Chemistry, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu, 603203, India. ananthak@srmist.edu.in. FAU - Raman, Rohith Kumar AU - Raman RK AUID- ORCID: 0000-0003-2965-4684 AD - Department of Physics and Nanotechnology, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu, 603203, India. FAU - Alagumalai, Ananthan AU - Alagumalai A AUID- ORCID: 0000-0002-8308-0864 AD - Organic and Perovskite Photovoltaics Laboratory (OPPV), Department of Chemistry, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu, 603203, India. ananthak@srmist.edu.in. FAU - Krishnamoorthy, Ananthanarayanan AU - Krishnamoorthy A AUID- ORCID: 0000-0002-4079-4576 AD - Organic and Perovskite Photovoltaics Laboratory (OPPV), Department of Chemistry, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu, 603203, India. ananthak@srmist.edu.in. LA - eng PT - Journal Article DEP - 20240102 PL - England TA - Dalton Trans JT - Dalton transactions (Cambridge, England : 2003) JID - 101176026 SB - IM EDAT- 2023/12/13 00:42 MHDA- 2023/12/13 00:43 CRDT- 2023/12/12 21:27 PHST- 2023/12/13 00:43 [medline] PHST- 2023/12/13 00:42 [pubmed] PHST- 2023/12/12 21:27 [entrez] AID - 10.1039/d3dt03012a [doi] PST - epublish SO - Dalton Trans. 2024 Jan 2;53(2):781-797. doi: 10.1039/d3dt03012a.