Publications

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2016
Lorenz, M., M. S. {Ramachandra Rao}, T. Venkatesan, E. Fortunato, P. Barquinha, R. Branquinho, D. Salgueiro, R. Martins, E. Carlos, A. Liu, et al., "{The 2016 oxide electronic materials and oxide interfaces roadmap}", Journal of Physics D: Applied Physics, vol. 49, no. 43: IOP Publishing, pp. 433001, nov, 2016. AbstractWebsite

Oxide electronic materials provide a plethora of possible applications and offer ample opportunity for scientists to probe into some of the exciting and intriguing phenomena exhibited by oxide systems and oxide interfaces. In addition to the already diverse spectrum of properties, the nanoscale form of oxides provides a new dimension of hitherto unknown phenomena due to the increased surface-to-volume ratio. Oxide electronic materials are becoming increasingly important in a wide range of applications including transparent electronics, optoelectronics, magnetoelectronics, photonics, spintronics, thermoelectrics, piezoelectrics, power harvesting, hydrogen storage and environmental waste management. Synthesis and fabrication of these materials, as well as processing into particular device structures to suit a specific application is still a challenge. Further, characterization of these materials to understand the tunability of their properties and the novel properties that evolve due to their nanostructured nature is another facet of the challenge. The research related to the oxide electronic field is at an impressionable stage, and this has motivated us to contribute with a roadmap on 'oxide electronic materials and oxide interfaces'. This roadmap envisages the potential applications of oxide materials in cutting edge technologies and focuses on the necessary advances required to implement these materials, including both conventional and novel techniques for the synthesis, characterization, processing and fabrication of nanostructured oxides and oxide-based devices. The contents of this roadmap will highlight the functional and correlated properties of oxides in bulk, nano, thin film, multilayer and heterostructure forms, as well as the theoretical considerations behind both present and future applications in many technologically important areas as pointed out by Venkatesan. The contributions in this roadmap span several thematic groups which are represented by the following authors: novel field effect transistors and bipolar devices by Fortunato, Grundmann, Boschker, Rao, and Rogers; energy conversion and saving by Zaban, Weidenkaff, and Murakami; new opportunities of photonics by Fompeyrine, and Zuniga-Perez; multiferroic materials including novel phenomena by Ramesh, Spaldin, Mertig, Lorenz, Srinivasan, and Prellier; and concepts for topological oxide electronics by Kawasaki, Pentcheva, and Gegenwart. Finally, Miletto Granozio presents the European action 'towards oxide-based electronics' which develops an oxide electronics roadmap with emphasis on future nonvolatile memories and the required technologies. In summary, we do hope that this oxide roadmap appears as an interesting up-to-date snapshot on one of the most exciting and active areas of solid state physics, materials science, and chemistry, which even after many years of very successful development shows in short intervals novel insights and achievements.

2015
Kiazadeh, A., D. Salgueiro, R. Branquinho, J. Pinto, H. L. Gomes, P. Barquinha, R. Martins, and E. Fortunato, "{Operational stability of solution based zinc tin oxide/SiO2 thin film transistors under gate bias stress}", APL Materials, vol. 3, no. 6: AIP Publishing, pp. 062804, jun, 2015. AbstractWebsite

In this study, we report solution-processed amorphous zinc tin oxide transistors exhibiting high operational stability under positive gate bias stress, translated by a recoverable threshold voltage shift of about 20{%} of total applied stress voltage. Under vacuum condition, the threshold voltage shift saturates showing that the gate-bias stress is limited by trap exhaustion or balance between trap filling and emptying mechanism. In ambient atmosphere, the threshold voltage shift no longer saturates, stability is degraded and the recovering process is impeded. We suggest that the trapping time during the stress and detrapping time in recovering are affected by oxygen adsorption/desorption processes. The time constants extracted from stretched exponential fitting curves are ≈106 s and 105 s in vacuum and air, respectively.

Alexa, A., N. Tigau, P. Alexandru, A. Pimentel, R. Branquinho, D. Salgueiro, T. Calmeiro, R. Martins, E. Fortunato, and V. Musat, "{Morphological and optical characterization of transparent thin films obtained at low temperature using ZnO nanoparticles}", Journal of Optoelectronic and Advanced Materials, vol. 17, no. 9, pp. 1288–1295, 2015. Abstract

Transparent metal oxides thin films are a class of inorganic conductors and semiconductors with significant importance for use in portable electronics, displays, flexible electronics, multi-functional windows and solar cells. Due to the recent development of transparent and flexible electronics, there is a growing interest in depositing metal-oxide thin-film on plastic substrates that can offer flexibility, lighter weight, and potentially lead to cheaper manufacturing by allowing printing and roll- to-roll processing. The plastic substrates, however, limit device processing to below 200oC. In this context, the deposition of high-performance semiconductor thin films from dispersions of pre-prepared oxide nanoparticles at temperatures below 200oC represents a potential key route. This paper reports on the preparation of ZnO transparent thin films using solution- processed nanoparticles (NPs) precipitated from zinc acetate alcoholic solution with potassium hydroxide. The nanoparticles size distribution, microstructure and crystallinity were measured by dynamic light scattering (DLS), Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD). The thin films were deposited by spin-coating onto soda lima glass substrate, using a dispersion of 1wt{%} ZnO NPs. The morphology of the films annealed at 120 and 180oC, observed by atomic force microscopy and cross-section scanning electron microscopy, shows columnar grains with diameter ranging between 20 and 70 nm, depending on the conditions of depositions. Optical measurements indicated high transparency, between 85 and 94 {%}, in the visible range, a direct nature of band-to-band transitions and band gap values between 3,22 and 3,32 eV. The refractive index and extinction coefficient have been calculated from optical transmittance and reflectance spectra.

Branquinho, R., D. Salgueiro, A. Santa, A. Kiazadeh, P. Barquinha, L. Í. Pereira, R. Martins, and E. Fortunato, "{Towards environmental friendly solution- based ZTO / AlO x TFTs}", Semicond. Sci. Technol., vol. 30: IOP Publishing, pp. 024007, 2015. AbstractWebsite

Solution based deposition has been recently considered as a viable option for low-cost flexible electronics. In this context research efforts have been increasingly centred on the development of suitable solution-processed materials for oxide based transistors. Nevertheless, the majority of synthetic routes reported require the use of toxic organic solvents. In this work we report on a new environmental friendly solution combustion synthesis route, using ethanol as solvent, for the preparation of indium/gallium free amorphous zinc-tin oxide (ZTO) thin film transistors (TFTs) including AlOx gate dielectric. The decomposition of ZTO and AlOx precursor solutions, electrical characterization and stability of solution processed ZTO/AlOx TFTs under gate-bias stress, in both air and vacuum atmosphere, were investigated. The devices demonstrated low hysteresis ($Δ$V = 0.23 V), close to zero turn on voltage, low threshold voltage (VT = 0.36 V) and a saturation mobility of 0.8 cm2 V−1 s−1 at low operation voltages. Ethanol based ZTO/AlOx TFTs are a promising alternative for applications in disposable, low cost and environmental friendly electronics.

2014
Branquinho, R., D. Salgueiro, L. Santos, P. Barquinha, L. Pereira, R. F. D. P. Martins, and E. Fortunato, "{Aqueous Combustion Synthesis of Aluminum Oxide Thin Films and Application as Gate Dielectric in GZTO Solution-based TFTs.}", ACS applied materials {&} interfaces, vol. 6: American Chemical Society, pp. 195592–9, oct, 2014. AbstractWebsite

Solution processing has been recently considered as an option when trying to reduce the costs associated to deposition under vacuum. In this context most of the research efforts have been centered in the development of the semiconductors processes nevertheless the development of the most suitable dielectrics for oxide based transistors is as relevant as the semiconductor layer itself. In this work we explore the solution combustion synthesis and report on a completely new and green route for the preparation of amorphous aluminum oxide thin films; introducing water as solvent. Optimized dielectric layers were obtained for a water based precursor solution with 0.1 M concentration and demonstrated high capacitance, 625 nF cm-2 at 10 kHz, and a permittivity of 7.1. These thin films were successfully applied as gate dielectric in solution processed gallium-zinc-tin oxide (GZTO) thin film transistors (TFTs) yielding good electrical performance such as subthreshold slope of about 0.3 V dec-1 and mobility above 1.3 cm2 V-1 s-1.

Veigas, B., R. Branquinho, J. V. Pinto, P. J. Wojcik, R. Martins, E. Fortunato, and P. V. Baptista, "{Ion sensing (EIS) real-time quantitative monitorization of isothermal DNA amplification}", Biosensors and Bioelectronics, vol. 52: Elsevier, pp. 50–55, 2014. AbstractWebsite

Field-effect-based devices are becoming a basic structural element in a new generation of microbiosensors. Reliable molecular characterization of DNA and/or RNA is of paramount importance for disease diagnostics and to follow up alterations in gene expression profiles. The use of such devices for point-of-need diagnostics has been hindered by the need of standard or real-time PCR amplification procedures. The present work focuses on the development of a tantalum pentoxide (Ta2O5) based sensor for the real-time label free detection of DNA amplification via loop mediated isothermal amplification (LAMP) allowing for quantitative analysis of the cMYC proto-oncogene. The strategy based on the field effect sensor was tested within a range of 1??108-1011 copies of target DNA, and a linear relationship between the log copy number of the initial template DNA and threshold time was observed allowing for a semi-quantitative analysis of DNA template. The concept offers many of the advantages of isothermal quantitative real-time DNA amplification in a label free approach and may pave the way to point-of-care quantitative molecular analysis focused on ease of use and low cost. ?? 2013 Elsevier B.V.

2013
Pinto, J. V., R. Branquinho, P. Barquinha, E. Alves, R. Martins, and E. Fortunato, "{Extended-gate ISFETs based on sputtered amorphous oxides}", IEEE/OSA Journal of Display Technology, vol. 9, no. 9, pp. 729–734, 2013. Abstract

We present the results obtained with an extended-gate ISFET totally based on amorphous oxides (GIZO as the semiconductor, {\textless}formula formulatype="inline"{\textgreater}{\textless}tex Notation="TeX"{\textgreater}{\$}{\{}hbox{\{}Ta{\}}{\}}{\_}{\{}2{\}}{\{}hbox{\{}O{\}}{\}}{\_}{\{}5{\}}{\{}hbox{\{}:SiO{\}}{\}}{\_}{\{}2{\}}{\$}{\textless}/tex{\textgreater} {\textless}/formula{\textgreater} as the dielectric and {\textless}formula formulatype="inline"{\textgreater}{\textless}tex Notation="TeX"{\textgreater}{\$}{\{}hbox{\{}Ta{\}}{\}}{\_}{\{}2{\}}{\{}hbox{\{}O{\}}{\}}{\_}{\{}5{\}}{\$}{\textless}/tex{\textgreater} {\textless}/formula{\textgreater} as the sensitive layer). A full characterization of the device was performed with constant ionic strength pH buffer solutions, revealing a sensitivity of 40 mV/pH with small hysteresis, and good linearity in the pH 4{&}{\#}x2013;pH 10 range buffer solutions. These results clearly show that it is possible to produce room-temperature disposable and low cost bio-sensors.

Branquinho, R., J. V. Pinto, T. Busani, P. Barquinha, L. Pereira, P. V. Baptista, R. Martins, and E. Fortunato, "{Plastic compatible sputtered Ta2O5 sensitive layer for oxide semiconductor tft sensors}", IEEE/OSA Journal of Display Technology, vol. 9, no. 9, pp. 723–728, 2013. AbstractWebsite

The effect of post-deposition annealing temperature on the pH sensitivity of room temperature RF sputtered Ta2O5 was investigated. Structural and morphological features of these films were analyzed before and after annealing at various temperatures. The deposited films are amorphous up to 600 °C and crystallize at 700 °C in an orthorhombic phase. Electrolyte-insulator-semiconductor (EIS) field effect based sensors with an amorphous Ta2O5 sensing layer showed pH sensitivity above 50 mV/pH. For sensors annealed above 200 °C pH sensitivity decreased with increasing temperature. Stabilized sensor response and maximum pH sensitivity was achieved after low temperature annealing at 200 °C, which is compatible with the use of polymeric substrates and application as sensitive layer in oxides TFT-based sensors.

Ramos, A. M., S. Pereira, M. T. Cidade, G. Pereira, R. Branquinho, L. Pereira, R. Martins, and E. Fortunato, "{Preparation and characterization of cellulose nanocomposite hydrogels as functional electrolytes}", Solid State Ionics, vol. 242: Elsevier B.V., pp. 26–32, 2013. AbstractWebsite

In this work Laponite was combined with a modified abundant natural polymer, (caboxymethyl cellulose), acrylic sodium salt polymer and lithium perchlorate aiming to produce inexpensive and sustainable nanocomposite electrolytes for functional electrochemical devices. Optical, electrochemical, structural, morphological and rheological characterization was performed in order to evaluate their properties and potential advantages as electrolyte. It was verified that the addition of Laponite led to an ionic conductivity at room temperature (25 C) in the range of 6 to 9 ?? 10- 5 Scm - 1 this value being then determined by the composition of the nanocomposite. These electrolytes were applied to electrochromic devices using evaporated nickel oxide thin film as the electrochromic layer. The devices exhibited a significant transmittance modulation that exceeds 45 {%} at 600 nm. ?? 2013 Elsevier B.V.

2011
Branquinho, R., B. Veigas, J. V. Pinto, R. Martins, E. Fortunato, and P. V. Baptista, "{Real-time monitoring of PCR amplification of proto-oncogene c-MYC using a Ta2O5 electrolyte-insulator-semiconductor sensor}", Biosensors and Bioelectronics, vol. 28, no. 1: Elsevier B.V., pp. 44–49, 2011. AbstractWebsite

We present a new approach for real-time monitoring of PCR amplification of a specific sequence from the human c-MYC proto-oncogene using a Ta 2O 5 electrolyte-insulator-semiconductor (EIS) sensor. The response of the fabricated EIS sensor to cycle DNA amplification was evaluated and compared to standard SYBR-green fluorescence incorporation, showing it was possible to detect DNA concentration variations with 30mV/??M sensitivity. The sensor's response was then optimized to follow in real-time the PCR amplification of c-MYC sequence from a genomic DNA sample attaining an amplification profile comparable to that of a standard real-time PCR. Owing to the small size, ease of fabrication and low-cost, the developed Ta 2O 5 sensor may be incorporated onto a microfluidic device and then used for real-time PCR. Our approach may circumvent the practical and economical obstacles posed by current platforms that require an external fluorescence detector difficult to miniaturize and incorporate into a lab-on-chip system. ?? 2011 Elsevier B.V.