Chellappan Vijila

High performance dye-sensitized solar cells with record open circuit voltage using tin oxide nanoflowers developed by electrospinning

Flower shaped nanostructures of an architypical transparent conducting oxide, SnO2, have been synthesized by an electrospinning technique for the first time by precisely controlling the precursor concentration in a polymeric solution. The flowers were made up of nanofibrils of diameter ∼70–100 nm, which in turn consisted of linear arrays of single crystalline nanoparticles of size 20–30 nm. Mott–Schottkey analysis shows that flowers have an order of magnitude higher electron density compared with the fibers despite their chemical similarity. Dye-sensitized solar cells fabricated using the flowers showed a record open circuit voltage of ∼700 mV and have one of the highest photoconversion efficiencies so far achieved with SnO2 and the iodide/triiodide electrolyte. The photoaction spectra and impedance spectroscopic measurements show that the flowers are characterized by a higher electron lifetime, owing to their enhanced crystallinity, compared to the conventional fibrous structure.

Metal oxide semiconducting interfacial layers for photovoltaic and photocatalytic applications

The present review rationalizes the significance of the metal oxide semiconductor (MOS) interfaces in the field of photovoltaics and photocatalysis. This perspective considers the role of interface science in energy harvesting using organic photovoltaics (OPVs) and dye-sensitized solar cells (DSSCs). These interfaces include large surface area junctions between photoelectrodes and dyes, the interlayer grain boundaries within the photoanodes, and the interfaces between photoactive layers and the top and bottom contacts. Controlling the collection and minimizing the trapping of charge carriers at these boundaries is crucial to overall power conversion efficiency of solar cells. Similarly, MOS photocatalysts exhibit strong variations in their photocatalytic activities as a function of band structure and surface states. Here, the MOS interface plays a vital role in the generation of OH radicals, which forms the basis of the photocatalytic processes. The physical chemistry and materials science of these MOS interfaces and their influence on device performance are also discussed.

Low frequency noise analysis on organic thin film transistors

Bottom-contact organic field-effect transistors (OFETs) based on poly(3-hexylthiophene) with different channel lengths were fabricated under different substrate pretreatment process conditions. These OFET devices were characterized using low frequency noise (LFN) spectroscopy, and the device performance parameters were correlated with the level of LFN. It is observed that the devices with higher noise levels showed poorer device properties when compared with the devices operated at same Ids of the same channel length. It is also observed that the noise level increased with the increase in channel length for devices with the same pretreatment conditions, which is due to increased trapping and detrapping in the channel material interface domain. The OFET device operating around the threshold voltage Vth will have a 1/f noise slope that is flatter, having a gradient that is smaller in magnitude. The threshold voltage of a device can thus be observed to be at the gate voltage in which 1/f noise intensity is t...

Investigation of the Device Degradation Mechanism in Pentacene-Based Thin-Film Transistors Using Low-Frequency-Noise Spectroscopy

The degradation process in pentacene-based organic thin-film transistors (OTFTs) is investigated. Pentacene-based OTFTs were fabricated with and without octadecyl trichlorosilane (OTS) treatment, and their device characteristics during lifetime test are evaluated using low-frequency-noise (LFN) spectroscopy. It is found that the devices exhibited the 1/f type of noise behavior with generation and recombination noise superimposed. The drain-current noise was found to vary proportionally with drain current according to Hooges empirical relation of flicker noise. Devices without any treatment show obvious interface traps and deep-level traps, while devices with OTS treatment show nonexistence of interface traps and suppression of deep-level traps. The LFN intensity is found to decrease during the device lifetime test initially, while upon the device failure, the noise level is observed to increase again. The viability of using LFN as a diagnostic tool in the organic transistor is demonstrated.

Role of dipole moment of solvents in formation and stabilization of the TICT states in Coumarin 445 under nitrogen laser excitation

In this paper we report the observation of dual Amplified Spontaneous Emission (ASE) from solutions of 7-ethylamino-4-methyl coumarin dye (Coumarin 445) in certain solvents such as n-butyl acetate, dioxane etc. when pumped by high power nitrogen laser. The two ASE bands appear to be from two different excited species (ICT and TICT conformation) one of which is the precursor of the other. The spectral characteristics of dye Coumarin 445 depend upon the solvent environment. The TICT coumarin photoisomers, which form exciplexes with the solvent molecules, have enough gain to produce amplified spontaneous emission even when there is apparently no detectable fluorescence. The behaviour of this dye in the excited state is studied by measuring the small signal gain and variation of the gain slope with temperature in different solvents. It is observed that polarity of the solvent plays a more dominant role in formation and stabilization of TICT states.

Enhanced Charge Carrier Transport and Device Performance Through Dual-Cesium Doping in Mixed-Cation Perovskite Solar Cells with Near Unity Free Carrier Ratios

PbI2-enriched mixed perovskite film [FA0.81MA0.15Pb(I0.836Br0.15)3] has been widely studied due to its great potential in perovskite solar cell (PSC) applications. Herein, a FA0.81MA0.15Pb(I0.836Br0.15)3 film has been fabricated with the temperature-dependent optical absorption spectra utilized to determine its exciton binding energy. A ∼13 meV exciton binding energy is estimated, and a near-unity fraction of free carriers out of the total photoexcitons has been obtained in the solar cell operating regime at equilibrium state. PSCs are fabricated with this mixed perovskite film, but a significant electron transport barrier at the TiO2-perovskite interface limited their performance. Cs2CO3 and CsI are then utilized as functional enhancers with which to substantially balance the electron and hole transport and increase the carriers (both electrons and holes) mobilities in PSCs, resulting in much-improved solar-cell performance. The modified PSCs exhibit reproducible power conversion efficiency (PCE) values with little hysteresis effect in the J-V curves, achieving PCEs up to 19.5% for the Cs2CO3-modified PSC and 20.6% when subsequently further doped with CsI.

Nanoscale phase domain structure and associated device performance of organic solar cells based on a diketopyrrolopyrrole polymer

We investigate the blend morphology and performance of bulk heterojunction organic photovoltaic devices comprising the donor polymer, pDPP-TNT (poly{3,6-dithiophene-2-yl-2,5-di(2-octyldodecyl)-pyrrolo[3,4-c]pyrrole-1, 4-dione-alt-naphthalene}) and the fullerene acceptor, [70]PCBM ([6,6]-phenyl C71-butyric acid methyl ester). The blend morphology is heavily dependent upon the solvent system used in the fabrication of thin films. Thin films spin-coated from chloroform possess a cobblestone-like morphology, consisting of thick, round-shaped [70]PCBM-rich mounds separated by thin polymer-rich valleys. The size of the [70]PCBM domains is found to depend on the overall film thickness. Thin films spin-coated from a chloroform:dichlorobenzene mixed solvent system are smooth and consist of a network of pDPP-TNT nanofibers embedded in a [70]PCBM-rich matrix. Rinsing the films in hexane selectively removes [70]PCBM and allows for analysis of domain size and purity. It also provides a means for investigating exciton dissociation efficiency through relative photoluminescence yield measurements. Devices fabricated from chloroform solutions show much poorer performance than the devices fabricated from the mixed solvent system; this disparity in performance is seen to be more pronounced with increasing film thickness. The primary cause for the improved performance of devices fabricated from mixed solvents is attributed to the greater donor-acceptor interfacial area and resulting greater capacity for charge carrier generation.

Charge transport in lightly reduced graphene oxide: A transport energy perspective

Significant variation in the charge transport behaviour in graphene oxide (GO) ranging from Schottky to Poole-Frenkel and to space charge limited transport exists. These have been extensively reported in the literature. However, the validity of such conventional charge transport models meant for delocalized carriers, to study charge transport through localised states in GO, a disordered semiconductor is open to question. In this work, we use the concept of transport energy (TE) to model charge transport in lightly reduced GO (RGO) and demonstrate that the TE calculations match well with temperature dependent experimental I-V data on RGO. We report on a temperature dependent TE ranging from a few 10 meV to 0.1 eV in slightly reduced GO. Last, we point out that, despite the success of several delocalised charge transport models in estimating barrier heights that resemble the TE level, they remain largely accidental and lack the insight in which the TE concept provides in understanding charge transport in RGO.

Impact of self-assembled monolayer on low frequency noise of organic thin film transistors

Bottom-contact organic field-effect transistors (FETs) based on regioregular poly(3-hexylthiophene) were fabricated with different surface treatments and were evaluated using a low frequency noise (LFN) spectroscopy. The oxygen-plasma (OP) treated device shows the highest mobility with the lowest current fluctuation. Octadecyltrichlorosilane and perfluorodecyldimetylchlorosilane treated device gives a higher noise compared with the OP treated device. Hexamethyldisilazane treated devices show the highest noise but the lowest mobility. The LFN results are correlated with organic FET device mobility and stability, proved by channel material crystallinity and degree of dislocations analysis. LFN measurement provides a nondisruptive and direct methodology to characterize device performance.

Correlation of Current Noise Behavior and Dark Spot Formation in Organic Light-Emitting Diodes

A correlation between current 1/f noise and dark spot formation is reported. Our results show that the dark spot is primarily correlated to current 1/f noise slope; the higher the slope, the poorer the interface, and the more abnormal dark spot growth rate and the shorter lifetime. Besides, there is a correlation between current 1/f noise magnitude and the dark spot initial size. A higher 1/f noise magnitude generally indicates a larger dark spot initial size. A seemingly identical current-voltage curve does not render the same characteristics of dark spot formation, which can be clearly distinguished from the subtle difference in 1/f noise behavior. The noise measurement can be used to predicate device lifetime and degradation behavior.