skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • Simultaneous Enhancement of Efficiency and Operational‐Stability of Mesoscopic Perovskite Solar Cells via Interfacial Toughening
Title: Simultaneous Enhancement of Efficiency and Operational‐Stability of Mesoscopic Perovskite Solar Cells via Interfacial Toughening
The combined effects of compact TiO2 (c-TiO2) electron-transport layer (ETL) are investigated without and with mesoscopic TiO2 (m-TiO2) on top, and without and with an iodine-terminated silane self-assembled monolayer (SAM), on the mechanical behavior, opto–electronic properties, photovoltaic (PV) performance, and operational-stability of solar cells based on metal-halide perovskites (MHPs). The interfacial toughness increases almost threefold in going from c-TiO2 without SAM to m-TiO2 with SAM. This is attributed to the synergistic effect of the m-TiO2/MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine-terminated silane SAM. The combination of m-TiO2 and SAM also offers a significant beneficial effect on the photocarriers extraction at the ETL/MHP interface, resulting in perovskite solar cells (PSCs) with power-conversion efficiency (PCE) of over 24% and 20% for 0.1 and 1 cm2 active areas, respectively. These PSCs also have exceptionally long operational-stability lives: extrapolated T80 (duration at 80% initial PCE retained) is ≈18 000 and 10 000 h for 0.1 and 1 cm2 active areas, respectively. Postmortem characterization and analyses of the operational-stability-tested PSCs are performed to elucidate the possible mechanisms responsible for the long operational-stability.  more » « less
Award ID(s):
2313648
PAR ID:
10504179
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Wiley, Wiley-VCH
Date Published:
Journal Name:
Advanced Materials
Volume:
36
Issue:
3
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; (, Science)
    null (Ed.)
    Iodine-terminated self-assembled monolayer (I-SAM) was used in perovskite solar cells (PSCs) to achieve a 50% increase of adhesion toughness at the interface between the electron transport layer (ETL) and the halide perovskite thin film to enhance mechanical reliability. Treatment with I-SAM also increased the power conversion efficiency from 20.2% to 21.4%, reduced hysteresis, and improved operational stability with a projected T80 (time to 80% initial efficiency retained) increasing from ~700 hours to 4000 hours under 1-sun illumination and with continuous maximum power point tracking. Operational stability–tested PSC without SAMs revealed extensive irreversible morphological degradation at the ETL/perovskite interface, including voids formation and delamination, whereas PSCs with I-SAM exhibited minimal damage accumulation. This difference was attributed to a combination of a decrease in hydroxyl groups at the interface and the higher interfacial toughness. 
    more » « less
  2. ; (, RSC Advances)
    The work proposed here aims to describe the dynamics of photoexcited charge carriers at the interface between the perovskite and electron transport layer (ETL) in perovskite solar cells (PSCs) and the effect that the interface morphology has on these dynamics. This is done in an effort to further develop the understanding of these materials so that their chemical composition and morphology may be better utilized to improve PSCs by means of increasing the power conversion efficiency (PCE), maximizing the chemical stability of PSCs to lengthen their lifespan, finding the cheapest and easiest materials to synthesize which have beneficial properties in photovoltaics, etc. This is done by using density functional theory to model the interface and open system Redfield theory to describe the charge carrier dynamics. We find that the charge transfer characteristics at the perovskite/ETL interface depend greatly on the choice of ligands adsorbed on the ETL that act as a bridge between the perovskite and ETL. The two ligand choices discussed here go so far as to determine whether the system will undergo a Förster energy transfer or a Dexter energy transfer upon photoexcitation. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; (, Advanced Energy Materials)
    Abstract High‐performance tin‐lead perovskite solar cells (PSCs) are needed for all‐perovskite‐tandem solar cells. However, iodide related fast photodegradation severely limits the operational stability of Sn‐Pb perovskites despite the demonstrated high efficiency and thermal stability. Herein, this work employs an alkylammonium pseudo‐halogen additive to enhance the power conversion efficiency (PCE) and photostability of methylammonium (MA)‐free, Sn‐Pb PSCs. Density functional theory (DFT) calculations reveal that the pseudo‐halogen tetrafluoroborate (BF4−) has strong binding capacity with metal ions (Sn2+/Pb2+) in the Sn‐Pb perovskite lattice, which lowers iodine vacancy formation. Upon combining BF4−with an octylammonium (OA+) cation, the PCE of the device with a built‐in light‐scattering layer is boosted to 23.7%, which represents a new record for Sn‐Pb PSCs. The improved efficiency benefits from the suppressed defect density. Under continuous 1 sun illumination, the OABF4embodied PSCs show slower generation of interstitial iodides and iodine, which greatly improves the device photostability under open‐circuit condition. Moreover, the device based on OABF4retains 88% of the initial PCE for 1000 h under the maximum‐power‐point tracking (MPPT) without cooling. 
    more » « less
  4. ; ; ; ; ; (, Energy & Environmental Science)
    null (Ed.)
    While typical perovskite solar cells (PSCs) with doped Spiro-OMeTAD as a hole transport material (HTM) have shown rapid increase in their power-conversion efficiencies (PCEs), their poor stability remains a big concern as the dopants and additives used with Spiro-OMeTAD have a strong tendency to diffuse into and degrade the perovskite active layer under normal operating conditions. Aiming to push forward the development of PSCs, many dopant-free small-molecular HTMs have been reported based on energetic considerations for charge transfer and criteria for charge transport. However, the PCEs of the state-of-the-art PSCs with dopant-free small-molecular HTMs are still inferior to those using doped Spiro-OMeTAD, and little attention has been paid to the interactions between the HTM and perovskite absorber in PSCs. Here, we report a facile design concept to functionalize HTMs so that they can passivate perovskite surface defects and enable perovskite active layers with lower density of surface trap states and more efficient charge transfer to the hole transport layer. As a consequence, perovskite solar cells with a functionalized HTM exhibit a champion PCE of 22.4%, the highest value for PSCs using dopant-free small molecular HTMs to date, and substantively improved operational stability under continuous illumination. With a T 80 of (1617 ± 7) h for encapsulated cells tested at 30 °C in air, the PSCs containing the functionalized HTM are among the most stable PSCs using dopant-free small-molecular HTMs. The effectiveness of our strategy is demonstrated in PSCs comprising both a state-of-the-art MA-free perovskite and MAPbI, a system having more surface defects, and implies the potential generality of our strategy for a broad class of perovskite systems, to further advance highly efficient and stable solar cells. 
    more » « less
  5. ; ; ; ; ; ; ; (, Advanced Functional Materials)
    The long‐term operational stability of perovskite solar cells (PSCs) remains a key challenge impeding their commercialization, particularly due to ambient environments (e.g., moisture, oxygen, heat)‐induced degradation. Carbon electrode‐based PSCs have emerged as cost‐effective and relatively stable alternatives to metal electrode‐based devices due to carbon materials' hydrophobic behavior, yet they still lag in both long‐term durability and power conversion efficiency (PCE). In this work, an ultrathin hydrophobic ligand‐modified core–shell Cd(S,Se)/ZnS quantum dots (QDs) capping layer is introduced as a multifunctional interfacial modifier for carbon‐electrode‐based PSCs. This oleic acid ligand‐modified QDs capping layer exhibits inherent hydrophobicity, effectively serving as a moisture barrier to retard perovskite degradation under ambient conditions. Furthermore, the strong interfacial bonding between the QDs and perovskite halide surfaces leads to efficient trap state passivation, reducing trap density and creating a more uniform electrical contact. The modified QDs/perovskite interface also features an elevated conduction band edge, promoting improved charge extraction. As a result, devices incorporating this quantum dot capping layer retain 98% of their initial PCE after 450 h of ambient aging and achieve a champion efficiency of 20.74%. This strategy highlights the potential of hydrophobic ligand‐modified chalcogenide QDs as surface modifiers to enhance both the stability and performance of carbon‐based PSCs, offering a promising route toward scalable fabrication of durable perovskite solar modules. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email