The broad tunability of the energy band gap through size control makes colloidal quantum dots (QDs) promising for the development of photovoltaic devices. Large-size lead sulfide (PbS) QDs, exhibiting a narrow energy band gap, are particularly interesting as they can be used to augment perovskite and c-Si solar cells due to their complementary NIR absorption. However, their complex surface chemistry makes them difficult to process for the development of solar cells. The shape of the QDs transformed from octahedron to cuboctahedron as their size increases, a phenomenon guided by surface energy minimization. As a result, the surface properties change drastically for large-size QDs, which exhibit nonpolar (200) facets and polar (111) facets, as opposed to only (111) facets in small-size QDs. Recent advancements in solution-phase surface passivation strategies, used for the development of high-performance solar cells using the small size and wide band gap QDs, failed to translate a similar enhancement in the case of large-size and narrow band gap QDs. Here, we report a hybrid passivation strategy for large-size and narrow band gap QDs to passivate both ( 111) and ( 200) facets, respectively, using inorganic lead triiodide (PbI 3 − ) and organic 3-chloro-1-propanethiol (CPT). By employing charge balance calculation, we identified the desired narrow band gap for QDs to complement the perovskite and c-Si absorption. The distinct choice of the organic ligand CPT enhances the colloidal stability of QDs in the solution phase and improves surface passivation to stop QD fusion in solid films. Photophysical properties show narrower excitonic and emission peaks and a reduction in the Stokes shift. Hybrid passivation leads to a 94% increase in the power conversion efficiency of solar cells and a 74% increase in the external quantum efficiency at the excitonic peak.
RetractionThis article was mistakenly published twice. For this reason this duplicate article has now been retracted. For citation purposes please cite the original: http://www.inljournal.com/?_action=articleInfo&article=21 Abstract Al-doped and un-doped ZnO thin films deposited on quartz substrates by the nebulized spray pyrolysis method were studied to investigate the wettability of the surface. The main objective of the present study was to investigate the wettability of ZnO thin film by changing the concentration of Al doping. Microstructure and water contact angles of the films were measured by scanning electron microscopy (SEM) and using a contact angle goniometer. SEM studies revealed that the grain size within the film increases with the doping concentration. The contact angles were studied to see the effect of aluminum doping on the hydrophilicity of the film. ZnO films were found to be hydrophobic in nature. A good correlation was observed between the SEM micrographs and contact angle results. The nature of the film was found to change from being hydrophobic to hydrophilic after the treatment in low-pressure DC glow discharge plasma, which, however, was reversible with the storage time.
Conventional memory technologies are facing enormous problems with downscaling, and are hence unable to fulfill the requirement of big data storage generated by a huge explosion of digital information. A resistive random access memory device (RRAM) is one of the most emerging technologies for next-generation computing data storage owing to its high-density stacking, ultrafast switching speed, high non-volatility, multilevel data storage, low power consumption, and simple device structure. In this work, colloidal MoS2 quantum dots (QDs) embedded in an insulating matrix of poly-(4vinylpyridine) (PVP) were used as an active layer to fabricate a RRAM device. The MoS2 QDs-PVP based RRAM device reveals an excellent nonvolatile resistive switching (RS) behavior with a maximum current on-off ratio (ION/IOFF) of 105. High endurance, long retention time, and successive “write-read-erase-read” cycles indicate high-performance RRAM characteristics. The ultimate power consumption by this RRAM device is considerably low for energy saving. In addition, the MoS2 QDs-PVP based device shows RS behavior even at 130 °C. High ION/IOFF, low operating power, high endurance, long retention time, and excellent stability with temperatures reveal that the MoS2 QDs-PVP based device can be a promising candidate for high-performance low power RRAM devices that can be operated at relatively higher temperatures.
Colloidal quantum dots (QDs) benefit from solution-phase processing and band-gap tuning for their application in solar cell development. Today's QD solar cells rely on solid-state ligand exchange (SLE) to replace bulky oleic acid (OA) ligands with small 1,2-ethanedithiol (EDT) ligands to develop a conducting hole transport layer (HTL). High volume contraction in EDT conjugated QD films, however, leads to crack and porosity in the HTL, which is a major cause of concern for the device reproducibility and large-area solar cell development. We show that partial removal of the OA ligands in the solution phase reduces the volume contraction in solid films, thereby allowing the growth of crack-free QD films in the SLE process. The cleaning of QDs by repeated precipitation and redispersion using a protic methanol (MeOH) solvent helps with partial removal of the OA ligands, but it is detrimental to the electronic properties of QDs. We develop a one-step solution-phase partial ligand-exchange process using ammonium salts, which enable partial replacement of the OA ligands and passivation of the QD surface. Introduction of the facile partial ligand-exchange process eliminates the need for tedious and wasteful multiple cleaning steps with MeOH, while improving the photophysical properties of QDs. The advancement in QD processing helps to build crackfree, smooth, and conjugated QD films for their deployment as HTLs in solar cell development. Partial ligand exchange with NH 4 SCN leads to a 1.5 times increase in p doping and mobility over multiple MeOH-cleaned PbS QD films. HTLs developed using NH 4 SCN QDs show an improved photovoltaic performance to attain a 10.5% power conversion efficiency. Improvement in the depletion width and hole collection efficiency leads to a superior photovoltaic performance, as confirmed from experimental studies and one-dimensional solar cell capacitance simulation.
Material composition plays a crucial role in the device performance; thus, nonvolatile memory devices from a small molecule named 5-mercapto-1-methyl tetrazole (MMT) in an insulating polymer matrix of poly(4-vinyl pyridine) (PVP) were fabricated. The composition of the active material in the device was varied to observe its influence on the device’s electronic properties. The device with a more or less weight ratio of MMT has a much smoother surface morphology, whereas when the contributions of MMT and PVP were equal, the average surface roughness increased. However, the maximum on–off current ratio for all the devices is 105, suggesting that the MMT molecule does not show any change in its characteristic properties when surrounded by an insulating material. When the device was fabricated without the polymer matrix, the surface morphology of the device completely changed as it was filled with large holes. These holes provide short-circuited pathways for the current by forming the direct metal contact between the top and bottom electrodes. The carrier transport through these devices follows various conduction mechanisms. Some of the dominating conduction mechanisms are direct tunneling and trap-free and trap-assisted space–charge-limited conduction.
Progress in device engineering and surface passivation strategies has led to steady progress in colloidal quantum dot (QD) solar cells. Bulk homojunction (BHJ) device architecture has several advantages over the conventional planar junction in developing QD solar cells. Herein, surface ligand chemistry is utilized to control the doping type and dispersibility of oppositely doped PbS QDs to develop BHJ solar cells. Thiocyanate and thiol ligand combination is introduced to develop p‐PbS QD ink, which is blended with halide‐passivated n‐PbS QDs to build BHJ solar cells. It is shown that BHJ solar cells are benefited from high energy offset and higher hole mobility. This leads to the superior carrier extraction from a thicker active layer without compromising fill factor and open circuit voltage. Power conversion efficiency has reached 10.7% in 530 nm‐thick BHJ solar cells, a 24% improvement over the best performing planar solar cells. With the help of the 1D solar cell capacitance simulator, it is shown that a 15% efficient QD solar cell can be realized by further improving the hole mobility above 0.1 cm2 V−1 s−1.
The explosion in digital communication with the huge amount of data and the internet of things (IoT) led to the increasing demand for data storage technology with faster operation speed, high-density stacking, nonvolatility, and low power consumption for saving energy. Metal chalcogenide-based quantum dots (QDs) show excellent nonvolatile resistive memory behavior owing to their tunable electronic states and control in trap states by passivating the surface with different ligands. Here, we synthesized high-quality colloidal monodispersed CdSe QDs by the hot injection method. The CdSe QDs were blended with an organic polymer, poly(4-vinylpyridine) (PVP), to fabricate an Al\CdSe-PVP\Al device. Our device shows excellent bipolar nonvolatile resistive random access memory (RRAM) switching behavior with a high current ON/OFF ratio (I ON/OFF) of 6.1 × 104, and it consumes ultralow power. The charge trapping and detrapping in the potential well formed by the CdSe QD and PVP combination result in resistive switching. This CdSe-PVP-based resistive random access memory (RRAM) device with a high I ON/OFF, ultrafast switching speed, high endurance, low operating voltage, and long retention period can be used as a high-performance and ultralow-power memristive device.
Control over surface passivation is a key to manage the optoelectronic properties in low-dimensional nanomaterials because of their high surface-to-volume ratios. Tunable band gap quantum dots (QDs) are a potential building block for the development of optoelectronic devices like solar cells, photodetectors, and light-emitting diodes. Long and insulating surface ligands of colloidally synthesized QDs are exchanged by short ligands to attain compact arrangement in thin films to facilitate the charge transport process. However, the ligand exchange process often resulted in reduced surface passivation, inhomogeneous QD fusion, and deterioration of energy band gap, which adversely impact their performance in solar cells. Here, we introduce a surface passivation strategy where the QDs are mutually passivated by the organic ligand 3-methyl mercapto propionate and inorganic halometallate ligands to develop a conducting QD ink. The mutually passivated QDs (MPQDs) show significant improvement in optoelectronic properties in maintaining the trap-free energy band gap and size monodispersity. The photovoltaic performance of MPQDs shows a 33% average increase in power conversion efficiency (PCE) over the conventional halometallate passivation to attain 9.6% PCE in MPQD solar cells. The improvements in photovoltaic parameters are corroborated by the reduction in density of the intermediate trap states and an increase in depletion width and diffusion length in MPQD-based solar cells.
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