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1.
Adv Mater ; : e2405572, 2024 May 29.
Article in English | MEDLINE | ID: mdl-38809575

ABSTRACT

The non-uniform distribution of colloidal particles in perovskite precursor results in an imbalanced response to the shear force during flexible printing process. Herein, it is observed that the continuous disordered migration occurring in perovskite inks significantly contributes to the enlargement of colloidal particles size and diminishes the crystallization activity of the inks. Therefore, a molecular encapsulation architecture by glycerol monostearate to mitigate colloidal particles collisions in the precursor ink, while simultaneously homogenizing the size distribution of perovskite colloids to minimize their diffusion disparities, is devised. The utilization of colloidal particles with a molecular encapsulation structure enables the achievement of uniform deposition during the printing process, thereby effectively balancing the crystallization rate and phase transition in the film and facilitating homogeneous crystallization of perovskite films. The large-area flexible perovskite device (1.01 cm2 and 100 cm2) fabricated through printing processes, achieves an efficiency of 24.45% and 15.87%, respectively, and manifests superior environmental stability, maintaining an initial efficiency of 91% after being stored in atmospheric ambiences for 150 days (unencapsulated). This work demonstrates that the dynamic evolution process of colloidal particles in both the precursor ink and printing process represents a crucial stride toward achieving uniform crystallization of perovskite films.

2.
Adv Mater ; 36(15): e2310752, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38183338

ABSTRACT

Organic-inorganic hybrid perovskites are considered ideal candidates for future photovoltaic applications due to their excellent photovoltaic properties. Although solution-printed manufacturing has shown inherent potential for the low-cost, high-throughput production of thin-film semiconductor electronics, the high-quality and high-reproducibility deposition of large-area perovskite remains a bottleneck that restricts their commercialization due to the droplet coffee-ring effect (CRE). In this study, these issues are addressed by introducing an in situ polymer framework. The 3D framework formed by spontaneous cross-linking improves the precursor viscosity and homogenizes its heat diffusion coefficient, counteracting the lateral capillary flow of the colloidal particles and anchoring their flocculent movement. Thus, the Marangoni convection intensity is properly controlled to ensure high-quality perovskite films, which significantly enhances reproducibility in printing efficient photovoltaics by mitigating the CRE. Subsequently, the perovskite solar cells and modules achieve power conversion efficiencies of 23.94 and 17.53%, and exhibit positive environmental stability, retaining over 90 and 78% efficiency after storage for 2500 and 1600 h, respectively. This work may serves as a foundation for exploring precursor rheology to match the homogeneous deposition requirements of perovskite photovoltaics and facilitating the advancement of their printing manufacturing and commercialization transition.

3.
Angew Chem Int Ed Engl ; 62(24): e202303177, 2023 Jun 12.
Article in English | MEDLINE | ID: mdl-37069478

ABSTRACT

The multiple quantum wells (QWs) distribution in low-dimensional perovskite films hinders charge transport due to the fundamental difficulty of controlling crystal growth from precursor solutions, yielding poorly homogeneous low-dimensional perovskite solar cells (PSCs), especially in upscaling fabrication. Here, efficient low-dimensional PSCs are realized by modulating the colloidal assembly behavior in the precursor solution to induce intermediate structures. In combination with in situ liquid time-of-flight secondary ion mass spectrometry, the assembly behavior of organic cations involved lead iodide-dominated colloidal soft framework is visualized by investigating the precursor species differences under hydrogen bonding interactions. Subsequently, solid-state reactions emerge and the formamidine (FA)-based perovskite films exhibit significantly suppressed multiple QWs distribution. Encouragingly, the FA device (n=9, by meniscus-assisted coating) achieves a power conversion efficiency (PCE) of 20.28 % for a size of 0.04 cm2 and a PCE of 15.35 % for a mini-module of 16.94 cm2 with superior stability.

4.
Nat Commun ; 14(1): 1204, 2023 Mar 02.
Article in English | MEDLINE | ID: mdl-36864062

ABSTRACT

In a flexible perovskite solar cell, the bottom interface between perovskite and the electron-transporting layer is critical in determining its efficiency and reliability. High defect concentrations and crystalline film fracturing at the bottom interface substantially reduce the efficiency and operational stability. In this work, a liquid crystal elastomer interlayer is intercalated into a flexible device with the charge transfer channel toughened by the aligned mesogenic assembly. The molecular ordering is instantly locked upon photopolymerization of liquid crystalline diacrylate monomers and dithiol-terminated oligomers. The optimized charge collection and the minimized charge recombination at the interface boost the efficiency up to 23.26% and 22.10% for rigid and flexible devices, respectively. The liquid crystal elastomer-induced suppression of phase segregation endows the unencapsulated device maintaining >80% of the initial efficiency for 1570 h. Moreover, the aligned elastomer interlayer preserves the configuration integrity with remarkable repeatability and mechanical robustness, which enables the flexible device to retain 86% of its original efficiency after 5000 bending cycles. The flexible solar cell chips are further integrated into a wearable haptic device with microneedle-based arrays of sensors to demonstrate a pain sensation system in virtual reality.

5.
ACS Nano ; 16(10): 16563-16573, 2022 10 25.
Article in English | MEDLINE | ID: mdl-36201316

ABSTRACT

Precise diagnosis of the boundary and grade of tumors is especially important for surgical dissection. Recently, visible and near-infrared (Vis-NIR) absorption differences of tumors are demonstrated for a precise tumor diagnosis. Here, a template-assisted sequential printing strategy is investigated to construct lateral heterostructured Vis-NIR photodetectors, relying on the up-conversion nanoparticles (UCNPs)/perovskite arrays. Under the sequential printing process, the synergistic effect and co-confinement are demonstrated to induce the UCNPs to cover both sides of the perovskite microwire. The side-wrapped lateral heterogeneous UCNPs/perovskite structure exhibits more satisfactory responsiveness to Vis-NIR light than the common fully wrapped structure, due to sufficient visible-light-harvesting ability. The Vis-NIR photodetectors with R reaching 150 mA W-1 at 980 nm and 1084 A W-1 at 450 nm are employed for the rapid classification of glioma. The detection accuracy rate of 99.3% is achieved through a multimodal analysis covering the Vis-NIR light, which provides a reliable basis for glioma grade diagnosis. This work provides a concrete example for the application of photodetectors in tumor detection and surgical diagnosis.


Subject(s)
Glioma , Titanium , Humans , Oxides , Calcium Compounds , Glioma/diagnostic imaging
6.
Phys Chem Chem Phys ; 24(13): 7969-7977, 2022 Mar 30.
Article in English | MEDLINE | ID: mdl-35311859

ABSTRACT

Quasi-two-dimensional (quasi-2D) perovskites are emerging as promising materials for highly stable light-emitting diodes (LEDs). However, their lower charge transport mobilities and higher defect densities may constrain their light-emitting efficiency. Here, we combine an excessive-salt-assisted (ESA) process with antisolvent treatments to inhibit the defects in Dion-Jacobson-type perovskite LEDs. Such a method could improve the film quality and recombination efficiency. By further investigation, we found that artificially building a bulk junction interface and enhancing surface polarization could play a more important role in promoting the ability of charge carrier injection and recombination for high-performance LED devices. Accordingly, the DJ-type quasi-2D perovskite LED can achieve a high external quantum efficiency (EQE) of 7.1%.

7.
BMC Microbiol ; 21(1): 281, 2021 10 18.
Article in English | MEDLINE | ID: mdl-34657588

ABSTRACT

BACKGROUND: Bloodstream infection (BSI) caused by Staphylococcus aureus (S. aureus) can be life-threatening and pose a great challenge to infection control and clinical treatment. However, little information exists regarding the characterization of S. aureus in BSI patients in Shandong, China. To identify the clonality, virulence genes, and antibiotic resistance of S. aureus in blood, a total of 101 nonrepetitive blood isolates were collected. The antibiotic resistance phenotypes were determined, and virulence genes were analyzed with polymerase chain reaction (PCR). Finally, the genetic relatedness was investigated with Staphylococcus chromosomal cassette mec (SCCmec) typing for methicillin-resistant S. aureus (MRSA) isolates, Staphylococcal protein A (spa), and multilocus sequence typing (MLST) for all of 101 isolates. RESULTS: Of the 101 S. aureus isolates, 24 MRSA isolates and 77 methicillin-susceptible S. aureus (MSSA) isolates were identified. Overall, MRSA isolates had higher resistance rates than MSSA isolates when exposed to any of the 15 antibiotics tested in this study except for trimethoprim/sulfamethoxazole. Among the 17 virulence genes tested in this study, hla, hld, and hlg could be detected in all isolates. MRSA isolates were more likely to carry seb and hlb genes, while MSSA isolates were more likely to carry seg and sei genes. Thirty-five sequence types (STs) and 49 spa types were identified, of which ST59-t437 and ST398-t571 were the most abundant. These two genotypes were also the most abundant ST-spa types in MRSA and MSSA isolates, but their abundances shifted over time, with ST398-t571 being the predominant genotype from 2016 to 2017, and ST59-t437 from 2018 to 2020. Besides, all the ST59-t437 isolates harbored hlgb gene, whereas most (88.9%) ST398-t571 did not. In addition, twenty-four MRSA isolates were subject to SCCmec typing. SCCmec IVa was the most prevalent SCCmec type, and all the ST59-t437 MRSA isolates were SCCmec IVa. We also observed 15 new STs, and some of them were MRSA. CONCLUSION: These findings provide additional observations and epidemiological data for blood S. aureus isolates, which can improve future infection-control measures and aid in potential clinical treatments in hospitals and other clinical settings.


Subject(s)
Bacteremia/microbiology , Staphylococcal Infections/microbiology , Staphylococcus aureus/drug effects , Staphylococcus aureus/pathogenicity , Anti-Bacterial Agents/pharmacology , China/epidemiology , Drug Resistance, Bacterial/drug effects , Drug Resistance, Bacterial/genetics , Genes, Bacterial/genetics , Genotype , Hospitals , Humans , Methicillin-Resistant Staphylococcus aureus/drug effects , Methicillin-Resistant Staphylococcus aureus/genetics , Methicillin-Resistant Staphylococcus aureus/isolation & purification , Methicillin-Resistant Staphylococcus aureus/pathogenicity , Microbial Sensitivity Tests , Multilocus Sequence Typing , Staphylococcal Protein A/genetics , Staphylococcus aureus/genetics , Staphylococcus aureus/isolation & purification , Virulence/genetics
8.
Chem Commun (Camb) ; 57(51): 6320-6323, 2021 Jun 24.
Article in English | MEDLINE | ID: mdl-34076656

ABSTRACT

A washable perovskite solar cell with high efficiency (over 11%) and outstanding crumpling durability (maintaining 81.2% after 100 cycles crumpling) is demonstrated herein by combining the flexible self-encapsulation method with a waterproof glue coated substrate.

9.
ACS Appl Mater Interfaces ; 13(17): 19959-19969, 2021 May 05.
Article in English | MEDLINE | ID: mdl-33884873

ABSTRACT

Dramatic development in perovskite solar cells (PSCs) and the widespread application of wearable electronics have attracted extensive research in the area of large-scale flexible solar power sources based on PSCs. Manufacturing of flexible PSCs by printing is considered to be one of the most potential methods. However, it is still a great challenge to print large-area uniform hole transport layers (HTLs) on a rough and soft plastic substrate to achieve flexible PSCs with high efficiency and good stability. Herein, we synthesized a viscous poly(3,4-ethylene dioxythiophene):graphene oxide (PEDOT:GO) gel and then blade-coated the gel by high-speed shearing to achieve high-quality HTLs with scalable size. The glued HTLs exhibit high viscosity, electrical conductivity, and mechanical flexibility, which enhance the adhesive ability and protect the brittle ITO electrode and perovskite crystals. Due to the gelatinous HTLs, we achieved an optimal efficiency of the flexible PSCs (1.01 cm2) of 19.7%, while that of the large-area flexible perovskite module (25 cm2) exceeded 10%. This is the highest efficiency for reported flexible MAPbI3 PSCs (1.01 cm2). Furthermore, the efficiency retention of the PSCs remains over 85% after 5000 bending cycles, which is of great significance for the practical application of PSCs in portable and wearable electronics.

10.
Sci Bull (Beijing) ; 66(6): 527-535, 2021 Mar 30.
Article in English | MEDLINE | ID: mdl-36654422

ABSTRACT

The power conversion effciency (PCE) of flexible perovskite solar cells (PSCs) has increased rapidly, while the mechanical flexibility and environmental stability are still far from satisfactory. Previous studies show the environmental degradation and ductile cracks of perovskite films usually begin at the grain boundaries (GBs). Herein, sulfonated graphene oxide (s-GO) is employed to construct a cementitious GBs by interacting with the [PbI6]4- at GBs. The resultant s-GO-[PbI6]4- complex can effectively passivate the defects of vacant iodine, and the devices with s-GO exhibit remarkable waterproofness and flexibility due to the tough and water-insoluble GBs. The champion PCE of 20.56% (1.01 cm2) in a device treated with s-GO is achieved. This device retains 90% of its original PCE after 180 d stored in the ambient condition, as well as over 80% retention after 10,000 bending cycles at a curvature radius of 3 mm.

11.
ACS Appl Mater Interfaces ; 12(50): 56151-56160, 2020 Dec 16.
Article in English | MEDLINE | ID: mdl-33263982

ABSTRACT

Perovskite polycrystalline films contain numerous intrinsic and interfacial defects ascribed to the solution preparation process, which are harmful to both the photovoltaic performance and the stability of perovskite solar cells (PVSCs). Although various passivators have been proved to be promising materials for passivating perovskite films, there is still a lack of deeper understanding of the effectiveness of the different passivation methods. Here, the mechanism between antisolvent dripping and additive doping strategies on the passivation effects in PVSCs is systematically investigated with a nonfullerene small molecule (F8IC). Such a passivated effect of F8IC is realized via coordination interactions between the carbonyl (C═O) and nitrile (C-N) groups of F8IC with Pb2+ ion of MAPbI3. Interestingly, F8IC antisolvent dripping can effectively passivate the surface defects and thus inhibit the nonradiative charge recombination on the upper part of the perovskite layer, whereas F8IC additive doping significantly reduces the surface and bulk defects and produces a compact perovskite film with denser crystal grains, thus facilitating charge transmission and extraction. Therefore, these benefits are translated into significant improvements in the short-circuit current density (Jsc) to 21.86 mA cm-2 and a champion power conversion efficiency of 18.40%. The selection of an optimal passivation strategy should also be considered according to the energy level matching between the passivators and the perovskite. The large energetic disparity is unsuitable for additive doping, whereas it is expected in antisolvent dripping.

12.
Nat Commun ; 11(1): 3016, 2020 06 15.
Article in English | MEDLINE | ID: mdl-32541859

ABSTRACT

The translation of unparalleled efficiency from the lab-scale devices to practical-scale flexible modules affords a huge performance loss for flexible perovskite solar cells (PSCs). The degradation is attributed to the brittleness and discrepancy of perovskite crystal growth upon different substrates. Inspired by robust crystallization and flexible structure of vertebrae, herein, we employ a conductive and glued polymer between indium tin oxide and perovskite layers, which simultaneously facilitates oriented crystallization of perovskite and sticks the devices. With the results of experimental characterizations and theoretical simulations, this bionic interface layer accurately controls the crystallization and acts as an adhesive. The flexible PSCs achieve the power conversion efficiencies of 19.87% and 17.55% at effective areas of 1.01 cm2 and 31.20 cm2 respectively, retaining over 85% of original efficiency after 7000 narrow bending cycles with negligible angular dependence. Finally, the modules are assembled into a wearable solar-power source, enabling the upscaling of flexible electronics.

13.
Adv Mater ; 32(26): e2000617, 2020 Jul.
Article in English | MEDLINE | ID: mdl-32449256

ABSTRACT

Sequential deposition is certified as an effective technology to obtain high-performance perovskite solar cells (PVSCs), which can be derivatized into large-scale industrial production. However, dense lead iodide (PbI2 ) causes incomplete reaction and unsatisfactory solution utilization of perovskite in planar PVSCs without mesoporous titanium dioxide as a support. Here, a novel autonomously longitudinal scaffold constructed by the interspersion of in situ self-polymerized methyl methacrylate (sMMA) in PbI2 is introduced to fabricate efficient PVSCs with excellent flexural endurance and environmental adaptability. By this strategy perovskite solution can be confined within an organic scaffold with vertical crystal growth promoted, effectively inhibiting exciton accumulation and recombination at grain boundaries. Additionally, sMMA cross-linked perovskite network can release mechanical stress and occupy the main channels for ion migration and water/oxygen permeation to significantly improve operational stability, which opens up a new strategy for the commercial development of large-area PVSCs in flexible electronics.

14.
Angew Chem Int Ed Engl ; 59(38): 16602-16608, 2020 Sep 14.
Article in English | MEDLINE | ID: mdl-32472623

ABSTRACT

Perovskite solar cells (PSCs) are a promising photovoltaic technology for stretchable applications because of their flexible, light-weight, and low-cost characteristics. However, the fragility of crystals and poor crystallinity of perovskite on stretchable substrates results in performance loss. In fact, grain boundary defects are the "Achilles' heel" of optoelectronic and mechanical stability. We incorporate a self-healing polyurethane (s-PU) with dynamic oxime-carbamate bonds as a scaffold into the perovskite films, which simultaneously enhances crystallinity and passivates the grain boundary of the perovskite films. The stretchable PSCs with s-PU deliver a stabilized efficiency of 19.15 % with negligible hysteresis, which is comparable to the performance on rigid substrates. The PSCs can maintain over 90 % of their initial efficiency after 3000 hours in air because of their self-encapsulating structure. Importantly, the self-healing function of the s-PU scaffold was verified in situ. The s-PU can release mechanical stress and repair cracks at the grain boundary on multiple levels. The devices recover 88 % of their original efficiency after 1000 cycles at 20 % stretch. We believe that this ingenious growth strategy for crystalline semiconductors will facilitate development of flexible and stretchable electronics.

15.
ACS Appl Mater Interfaces ; 12(12): 14049-14056, 2020 Mar 25.
Article in English | MEDLINE | ID: mdl-32129060

ABSTRACT

Tin-based perovskite solar cells (PVSCs) have emerged as the most promising lead-free perovskite materials owing to their superior optoelectronic properties. However, the deficiency of accurate control of the tin-based perovskite crystallization process increases the possibility of unexpected perovskite film morphology and defects, resulting in inferior power conversion efficiency (PCE). Meanwhile, the poor environmental stability of tin-based perovskite films hinders its further development. In this work, a unique polymer [poly(ethylene-co-vinyl acetate) (EVA)] is introduced into anti-solvent during spin coating of formamidinium tin tri-iodide (FASnI3) precursor solution. The C═O groups contained in EVA have a powerful Lewis acid-base complexation with uncoordinated tin atoms in perovskite grains, which can greatly improve the grain size, optimize the grain orientation, and decrease the surface defects of FASnI3 films. This strategy offers an impressive PCE of 7.72% with favorable reproducibility. More importantly, the PVSC devices based on FASnI3-EVA absorbers have a self-encapsulation effect, which exhibits distinguished moisture and oxygen barrier property, thereby retaining 62.4% of the original efficiency value after aging for 48 h in the air with a humidity of 60%. Such a convenient strategy provides a new inspiration for the establishment of stable and high-performance tin-based PVSCs.

16.
Adv Mater ; 31(41): e1903649, 2019 Oct.
Article in English | MEDLINE | ID: mdl-31423693

ABSTRACT

The blossoming of organic solar cells (OSCs) has triggered enormous commercial applications, due to their high-efficiency, light weight, and flexibility. However, the lab-to-manufacturing translation of the praisable performance from lab-scale devices to industrial-scale modules is still the Achilles' heel of OSCs. In fact, it is urgent to explore the mechanism of morphological evolution in the bulk heterojunction (BHJ) with different coating/printing methods. Here, a general approach to upscale flexible organic photovoltaics to module scale without obvious efficiency loss is demonstrated. The shear impulse during the coating/printing process is first applied to control the morphology evolution of the BHJ layer for both fullerene and nonfullerene acceptor systems. A quantitative transformation factor of shear impulse between slot-die printing and spin-coating is detected. Compelling results of morphological evolution, molecular stacking, and coarse-grained molecular simulation verify the validity of the impulse translation. Accordingly, the efficiency of flexible devices via slot-die printing achieves 9.10% for PTB7-Th:PC71 BM and 9.77% for PBDB-T:ITIC based on 1.04 cm2 . Furthermore, 15 cm2 flexible modules with effective efficiency up to 7.58% (PTB7-Th:PC71 BM) and 8.90% (PBDB-T:ITIC) are demonstrated with satisfying mechanical flexibility and operating stability. More importantly, this work outlines the shear impulse translation for organic printing electronics.

17.
Chem Commun (Camb) ; 55(25): 3666-3669, 2019 Mar 21.
Article in English | MEDLINE | ID: mdl-30855051

ABSTRACT

Bendable nickel oxide (NiOx) was first fabricated via polydopamine (PDA) modification and applied as an interfacial layer in flexible perovskite solar cells. PDA cross-linked NiOx could release mechanical stress to eliminate the inherent brittleness of inorganic crystals, leading to a flexible device exhibit over 70% retention of efficiency after 1000 bending cycles.

18.
ACS Appl Mater Interfaces ; 10(2): 1909-1916, 2018 Jan 17.
Article in English | MEDLINE | ID: mdl-29271205

ABSTRACT

Solar cells based on hybrid organic-inorganic metal halide perovskites are being developed to achieve high efficiency and stability. However, inevitably, there are defects in perovskite films, leading to poor device performance. Here, we employ an additive-engineering strategy to modify the grain boundary (GB) defects and crystal lattice defects by introducing a strong electron acceptor of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) into perovskite functional layer. Importantly, it has been found that F4TCNQ is filled in GBs and there is a significant reduction of metallic lead defects and iodide vacancies in the perovskite crystal lattice. The bulk heterojunction perovskite-F4TCNQ film exhibits superior electronic quality with improved charge separation and transfer, enhanced and balanced charge mobility, as well as suppressed recombination. As a result, the F4TCNQ doped perovskite device shows excellent device performance, especially the reproducible high fill factor (up to 80%) and negligible hysteresis effect.

19.
Adv Mater ; 29(42)2017 Nov.
Article in English | MEDLINE | ID: mdl-28885738

ABSTRACT

Dramatic advances in perovskite solar cells (PSCs) and the blossoming of wearable electronics have triggered tremendous demands for flexible solar-power sources. However, the fracturing of functional crystalline films and transmittance wastage from flexible substrates are critical challenges to approaching the high-performance PSCs with flexural endurance. In this work, a nanocellular scaffold is introduced to architect a mechanics buffer layer and optics resonant cavity. The nanocellular scaffold releases mechanical stresses during flexural experiences and significantly improves the crystalline quality of the perovskite films. The nanocellular optics resonant cavity optimizes light harvesting and charge transportation of devices. More importantly, these flexible PSCs, which demonstrate excellent performance and mechanical stability, are practically fabricated in modules as a wearable solar-power source. A power conversion efficiency of 12.32% for a flexible large-scale device (polyethylene terephthalate substrate, indium tin oxide-free, 1.01 cm2 ) is achieved. This ingenious flexible structure will enable a new approach for development of wearable electronics.

20.
Adv Mater ; 29(27)2017 Jul.
Article in English | MEDLINE | ID: mdl-28481051

ABSTRACT

Corrosive precursors used for the preparation of organic-inorganic hybrid perovskite photoactive layers prevent the application of ultrathin metal layers as semitransparent bottom electrodes in perovskite solar cells (PVSCs). This study introduces tin-oxide (SnOx ) grown by atomic layer deposition (ALD), whose outstanding permeation barrier properties enable the design of an indium-tin-oxide (ITO)-free semitransparent bottom electrode (SnOx /Ag or Cu/SnOx ), in which the metal is efficiently protected against corrosion. Simultaneously, SnOx functions as an electron extraction layer. We unravel the spontaneous formation of a PbI2 interfacial layer between SnOx and the CH3 NH3 PbI3 perovskite. An interface dipole between SnOx and this PbI2 layer is found, which depends on the oxidant (water, ozone, or oxygen plasma) used for the ALD growth of SnOx . An electron extraction barrier between perovskite and PbI2 is identified, which is the lowest in devices based on SnOx grown with ozone. The resulting PVSCs are hysteresis-free with a stable power conversion efficiency (PCE) of 15.3% and a remarkably high open circuit voltage of 1.17 V. The ITO-free analogues still achieve a high PCE of 11%.

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