Gill Sang Han

Highly efficient and bending durable perovskite solar cells: toward a wearable power source

Perovskite solar cells are promising candidates for realizing an efficient, flexible, and lightweight energy supply system for wearable electronic devices. For flexible perovskite solar cells, achieving high power conversion efficiency (PCE) while using a low-temperature technology for the fabrication of a compact charge collection layer is a critical issue. Herein, we report on a flexible perovskite solar cell exhibiting 12.2% PCE as a result of the employment of an annealing-free, 20 nm thick, amorphous, compact TiOx layer deposited by atomic layer deposition. The excellent performance of the cell was attributed to fast electron transport, verified by time-resolved photoluminescence and impedance studies. The PCE remained the same down to 0.4 sun illumination, as well as to a 45° tilt to incident light. Mechanical bending of the devices worsened device performance by only 7% when a bending radius of 1 mm was used. The devices maintained 95% of the initial PCE after 1000 bending cycles for a bending radius of 10 mm. Degradation of the device performance by the bending was the result of crack formation from the transparent conducting oxide layer, demonstrating the potential of the low-temperature-processed TiOx layer to achieve more efficient and bendable perovskite solar cells, which becomes closer to a practical wearable power source.

Retarding charge recombination in perovskite solar cells using ultrathin MgO-coated TiO2 nanoparticulate films

MgO-coated TiO2 nanoparticle (NP)-based electron collecting layers were fabricated to prevent charge recombination at the methylamine lead iodide/TiO2 interface in perovskite solar cells. The open circuit voltage (Voc) and fill factor (ff) of perovskite solar cells based on MgO-coated TiO2 charge collectors were 0.89 V and 71.2%, respectively. These values were 4.7% and 6.1% higher than the pure TiO2 based perovskite solar cells. Transient photovoltage decay data exhibited recombination times for MgO-coated TiO2 NP-based perovskite solar cells about three times longer than those of TiO2 NP based solar cells. The longer recombination time was responsible for enhancing the Voc and ff of MgO-coated TiO2 NP-based perovskite solar cells. By employing a MgO nanolayer, we observed that the power conversion efficiency (PCE) was increased from 11.4% to 12.7%, demonstrating that MgO ultrathin nanolayers are able to efficiently retard charge recombination in perovskite solar cells.

Niobium Doping Effects on TiO2 Mesoscopic Electron Transport Layer-Based Perovskite Solar Cells.

Perovskite solar cells (PSCs) are the most promising candidates as next-generation solar energy conversion systems. To design a highly efficient PSC, understanding electronic properties of mesoporous metal oxides is essential. Herein, we explore the effect of Nb doping of TiO2 on electronic structure and photovoltaic properties of PSCs. Light Nb doping (0.5 and 1.0 at %) increased the optical band gap slightly, but heavy doping (5.0 at %) distinctively decreased it. The relative Fermi level position of the conduction band is similar for the lightly Nb-doped TiO2 (NTO) and the undoped TiO2 whereas that of the heavy doped NTO decreased by as much as ∼0.3 eV. The lightly doped NTO-based PSCs exhibit 10 % higher efficiency than PSCs based on undoped TiO2 (from 12.2 % to 13.4 %) and 52 % higher than the PSCs utilizing heavy doped NTO (from 8.8 % to 13.4 %), which is attributed to fast electron injection/transport and preserved electron lifetime, verified by transient photocurrent decay and impedance studies.

Reduced Graphene Oxide/Mesoporous TiO2 Nanocomposite Based Perovskite Solar Cells

We report on reduced graphene oxide (rGO)/mesoporous (mp)-TiO2 nanocomposite based mesostructured perovskite solar cells that show an improved electron transport property owing to the reduced interfacial resistance. The amount of rGO added to the TiO2 nanoparticles electron transport layer was optimized, and their impacts on film resistivity, electron diffusion, recombination time, and photovoltaic performance were investigated. The rGO/mp-TiO2 nanocomposite film reduces interfacial resistance when compared to the mp-TiO2 film, and hence, it improves charge collection efficiency. This effect significantly increases the short circuit current density and open circuit voltage. The rGO/mp-TiO2 nanocomposite film with an optimal rGO content of 0.4 vol % shows 18% higher photon conversion efficiency compared with the TiO2 nanoparticles based perovskite solar cells.

Simple Large-Scale Synthesis of Hydroxyapatite Nanoparticles: In Situ Observation of Crystallization Process

The noble synthesis method for hydroxyapatite (HAp) nanoparticles was exploited using a fairly simple reaction of Ca(OH)(2) and H(3)PO(4), which does not generate residual harmful anions and consequently does not need an additional washing process. HAp nanoparticles were found to yield from dicalcium phosphate dehydrate (DCPD) as the only intermediate phase, which was monitored by in situ observation study using X-ray diffraction (XRD), Fourier transform infrared (FT-IR), (1)H and (31)P magic-angle spinning (MAS) NMR. Furthermore, we found that the phase evolution of HAp was preceded by heteronucleation of HAp onto the DCPD surface. The combination of scanning electron microscopy (SEM) and inductively coupled plasma atomic emission spectroscopy (ICP-ES) analysis gave more information on the HAp crystallization process, which was found to be retarded by the residual Ca(OH)(2) and slow diffusion process of Ca ions into the interface between HAp and DCPD. These results demonstrate that the synthesis of pure HAp nanoparticles with high throughput can be achieved by controlling the residual Ca(OH)(2) and diffusion process of Ca ions.

BiVO4/WO3/SnO2 Double-Heterojunction Photoanode with Enhanced Charge Separation and Visible-Transparency for Bias-Free Solar Water-Splitting with a Perovskite Solar Cell

Coupling dissimilar oxides in heterostructures allows the engineering of interfacial, optical, charge separation/transport and transfer properties of photoanodes for photoelectrochemical (PEC) water splitting. Here, we demonstrate a double-heterojunction concept based on a BiVO4/WO3/SnO2 triple-layer planar heterojunction (TPH) photoanode, which shows simultaneous improvements in the charge transport (∼93% at 1.23 V vs RHE) and transmittance at longer wavelengths (>500 nm). The TPH photoanode was prepared by a facile solution method: a porous SnO2 film was first deposited on a fluorine-doped tin oxide (FTO)/glass substrate followed by WO3 deposition, leading to the formation of a double layer of dense WO3 and a WO3/SnO2 mixture at the bottom. Subsequently, a BiVO4 nanoparticle film was deposited by spin coating. Importantly, the WO3/(WO3+SnO2) composite bottom layer forms a disordered heterojunction, enabling intimate contact, lower interfacial resistance, and efficient charge transport/transfer. In addition, the top BiVO4/WO3 heterojunction layer improves light absorption and charge separation. The resultant TPH photoanode shows greatly improved internal quantum efficiency (∼80%) and PEC water oxidation performance (∼3.1 mA/cm2 at 1.23 V vs RHE) compared to the previously reported BiVO4/WO3 photoanodes. The PEC performance was further improved by a reactive-ion etching treatment and CoOx electrocatalyst deposition. Finally, we demonstrated a bias-free and stable solar water-splitting by constructing a tandem PEC device with a perovskite solar cell (STH ∼3.5%).

Screening effect on photovoltaic performance in ferroelectric CH3NH3PbI3 perovskite thin films

Organic and inorganic hybrid materials of CH3NH3PbX3 with a perovskite crystal structure have been conceived as emerging light absorbing materials for high efficiency photovoltaic devices. Here, we demonstrate the screening effect of polarization states on charge redistribution related to the photovoltaic performance of ferroelectric CH3NH3PbI3 thin films using atomic force microscopy. We show the interplay between polarization and injected charges to have significant effects on charge transfer which potentially influences photovoltaic performance. The obtained results reveal that the direction and the amount of charge transfer can be influenced by the screening of polarization states at the interface. These results could deliver fundamental information regarding the influence of ferroelectricity on CH3NH3PbX3 solar cells.

The novel design of a remote phosphor ceramic plate for white light generation in high power LEDs

Here, we report a phosphor ceramic plate (PCP) constructed using Y3Al5O12:Ce3+ (YAG:Ce) nanoparticles (NPs) with a uniformly spherical size distribution for high-power light emitting diode (LED) applications. YAG:Ce NPs with diameters of 600 nm were synthesized using the forced hydrolysis method, and the typical excitation and emission of the PCP constructed using YAG:Ce NPs were observed on blue light emitting InGaN chips, as a conversion process for the generation of white LEDs with high luminous flux and thermal stability. In addition, for the improvement of the PCP characteristics, a novel design using graphene-embedded red phosphor (GRP) layer was utilized. The GRP-coated PCP displayed a higher CRI value of 82 and warm white light with a correlated colour temperature (CCT) of 3952 K compared to the general PCP. This type of PCP is expected to be an outstanding candidate for the production of luminescent materials in various fields of optoelectronics.

Low-Temperature Modification of ZnO Nanoparticles Film for Electron-Transport Layers in Perovskite Solar Cells

An electron-transport layer (ETL) that selectively collects photogenerated electrons is an important constituent of halide perovskite solar cells (PSCs). Although TiO2 films are widely used as ETL of PSCs, the processing of TiO2 films with high electron mobility requires high-temperature annealing and TiO2 dissociates the perovskite layer through a photocatalytic reaction. Here, we report an effective surface-modification method of a room-temperature processed ZnO nanoparticles (NPs) layer as an alternative to the TiO2 ETL. A combination of simple UV exposure and nitric acid treatment effectively removes the hydroxyl group and passivates surface defects in ZnO NPs. The surface modification of ZnO NPs increases the power conversion efficiency (PCE) of PSCs to 14 % and decreases the aging of PSCs under light soaking. These results suggest that the surface-modified ZnO film can be a good ETL of PSCs and provide a path toward low-temperature processing of efficient and stable PSCs that are compatible with flexible electronics.

Green-emitting Lu3Al5O12:Ce3+ phosphor as a visible light amplifier for dye-sensitized solar cells

A down convertor Lu3Al5O12:Ce3+ (LuAG) phosphor was used as a visible light amplifier for dye-sensitized solar cells (DSSCs). LuAG particles emitting green light with a wavelength of 470 to 650 nm, which is capable of stimulating Ru-dye molecules, enhanced the light-harvesting properties of a DSSC. The average short-circuit current density (Jsc) of the DSSC containing LuAG down conversion layers was approximately 9.6% higher than that of the mesoporous (mp) TiO2-based DSSC. Therefore, the average power conversion efficiency (PCE) for the DSSC with LuAG was 7.5% under AM 1.5 conditions, which was 8.7% higher than that for the mp-TiO2 based DSSC. The superior photovoltaic properties of the DSSC containing LuAG down conversion layers under UV light illumination revealed the effective wavelength down-converting properties of the LuAG down conversion layers.