Saiful I. Khondaker

Ultralight Multiwalled Carbon Nanotube Aerogel

Ultralight multiwalled carbon nanotube (MWCNT) aerogel is fabricated from a wet gel of well-dispersed pristine MWCNTs. On the basis of a theoretical prediction that increasing interaction potential between CNTs lowers their critical concentration to form an infinite percolation network, poly(3-(trimethoxysilyl) propyl methacrylate) (PTMSPMA) is used to disperse and functionalize MWCNTs where the subsequent hydrolysis and condensation of PTMSPMA introduces strong and permanent chemical bonding between MWCNTs. The interaction is both experimentally and theoretically proven to facilitate the formation of a MWCNT percolation network, which leads to the gelation of MWCNT dispersion at ultralow MWCNT concentration. After removing the liquid component from the MWCNT wet gel, the lightest ever free-standing MWCNT aerogel monolith with a density of 4 mg/cm(3) is obtained. The MWCNT aerogel has an ordered macroporous honeycomb structure with straight and parallel voids in 50-150 μm separated by less than 100 nm thick walls. The entangled MWCNTs generate mesoporous structures on the honeycomb walls, creating aerogels with a surface area of 580 m(2)/g which is much higher than that of pristine MWCNTs (241 m(2)/g). Despite the ultralow density, the MWCNT aerogels have an excellent compression recoverable property as demonstrated by the compression test. The aerogels have an electrical conductivity of 3.2 × 10(-2) S·cm(-1) that can be further increased to 0.67 S·cm(-1) by a high-current pulse method without degrading their structures. The excellent compression recoverable property, hierarchically porous structure with large surface area, and high conductivity grant the MWCNT aerogels exceptional pressure and chemical vapor sensing capabilities.

Ultrahigh Density Alignment of Carbon Nanotube Arrays by Dielectrophoresis

We report ultrahigh density assembly of aligned single-walled carbon nanotube (SWNT) two-dimensional arrays via AC dielectrophoresis using high-quality surfactant-free and stable SWNT solutions. After optimization of frequency and trapping time, we can reproducibly control the linear density of the SWNT between prefabricated electrodes from 0.5 SWNT/μm to more than 30 SWNT/μm by tuning the concentration of the nanotubes in the solution. Our maximum density of 30 SWNT/μm is the highest for aligned arrays via any solution processing technique reported so far. Further increase of SWNT concentration results in a dense array with multiple layers. We discuss how the orientation and density of the nanotubes vary with concentrations and channel lengths. Electrical measurement data show that the densely packed aligned arrays have low sheet resistances. Selective removal of metallic SWNTs via controlled electrical breakdown produced field-effect transistors with high current on-off ratio. Ultrahigh density alignment reported here will have important implications in fabricating high-quality devices for digital and analog electronics.

Position dependent photodetector from large area reduced graphene oxide thin films

We fabricated large area infrared photodetector devices from thin film of chemically reduced graphene oxide (RGO) sheets and studied their photoresponse as a function of laser position. We found that the photocurrent either increases, decreases, or remain almost zero depending upon the position of the laser spot with respect to the electrodes. The position sensitive photoresponse is explained by Schottky barrier modulation at the RGO film-electrode interface. The time response of the photocurrent is dramatically slower than single sheet of graphene possibly due to disorder from the chemical synthesis and interconnecting sheets.

High yield fabrication of chemically reduced graphene oxide field effect transistors by dielectrophoresis

We demonstrate high yield fabrication of field effect transistors (FET) using chemically reduced graphene oxide (RGO) sheets. The RGO sheets suspended in water were assembled between prefabricated gold source and drain electrodes using ac dielectrophoresis. With the application of a backgate voltage, 60% of the devices showed p-type FET behavior, while the remaining 40% showed ambipolar behavior. After mild thermal annealing at 200 degrees C, all ambipolar RGO FET remained ambipolar with increased hole and electron mobility, while 60% of the p-type RGO devices were transformed to ambipolar. The maximum hole and electron mobilities of the devices were 4.0 and 1.5 cm(2) V( - 1) s( - 1) respectively. High yield assembly of chemically derived RGO FET will have significant impact in scaled up fabrication of graphene based nanoelectronic devices.

Space charge limited conduction with exponential trap distribution in reduced graphene oxide sheets

We elucidate on the low mobility and charge traps of the chemically reduced graphene oxide (RGO) sheets by measuring and analyzing temperature dependent current-voltage characteristics. The RGO sheets were assembled between source and drain electrodes via dielectrophoresis. At low bias voltage the conduction is Ohmic while at high bias voltage and low temperatures the conduction becomes space charge limited with an exponential distribution of traps. We estimate an average trap density of 1.75×1016 cm−3. Quantitative information about charge traps will help develop optimization strategies of passivating defects in order to fabricate high quality solution processed graphene devices.

Photoluminescence quenching in gold - MoS2 hybrid nanoflakes

Achieving tunability of two dimensional (2D) transition metal dichalcogenides (TMDs) functions calls for the introduction of hybrid 2D materials by means of localized interactions with zero dimensional (0D) materials. A metal-semiconductor interface, as in gold (Au) - molybdenum disulfide (MoS2), is of great interest from the standpoint of fundamental science as it constitutes an outstanding platform to investigate plasmonic-exciton interactions and charge transfer. The applied aspects of such systems introduce new options for electronics, photovoltaics, detectors, gas sensing, catalysis, and biosensing. Here we consider pristine MoS2 and study its interaction with Au nanoislands, resulting in local variations of photoluminescence (PL) in Au-MoS2 hybrid structures. By depositing monolayers of Au on MoS2, we investigate the electronic structure of the resulting hybrid systems. We present strong evidence of PL quenching of MoS2 as a result of charge transfer from MoS2 to Au: p-doping of MoS2. The results suggest new avenues for 2D nanoelectronics, active control of transport or catalytic properties.

Fabrication of nanometer-spaced electrodes using gold nanoparticles

A simple and highly reproducible technique is demonstrated for the fabrication of metallic electrodes with nanometer separation. Commercially available bare gold colloidal nanoparticles are first trapped between prefabricated large-separation electrodes to form a low-resistance bridge by an ac electric field. A large dc voltage is then applied to break the bridge via electromigration at room temperature, which consistently produces gaps in the sub-10 nm range. The technique is readily applied to prefabricated electrodes with separation up to 1 μm, which can be defined using optical lithography. The simple fabrication scheme will facilitate electronic transport studies of individual nanostructures made by chemical synthesis. As an example, measurement of a thiol-coated gold nanoparticle showing a clear Coulomb staircase is presented.

Semiconducting enriched carbon nanotube aligned arrays of tunable density and their electrical transport properties.

We demonstrate assembly of solution-processed semiconducting enriched (99%) single-walled carbon nanotubes (s-SWNTs) in an array with varying linear density via ac dielectrophoresis (DEP) and investigate detailed electronic transport properties of the fabricated devices. We show that (i) the quality of the alignment varies with frequency of the applied voltage and that (ii) by varying the frequency and concentration of the solution, we can control the linear density of the s-SWNTs in the array from 1/μm to 25/μm. The DEP assembled s-SWNT devices provide the opportunity to investigate the transport property of the arrays in the direct transport regime. Room temperature electron transport measurements of the fabricated devices show that with increasing nanotube density the device mobility increases while the current on-off ratio decreases dramatically. For the dense array, the device current density was 16 μA/μm, on-conductance was 390 μS, and sheet resistance was 30 kΩ/◻. These values are the best reported so far for any semiconducting nanotube array.

High performance organic phototransistor based on regioregular poly(3-hexylthiophene)

We fabricated solution processed organic phototransistors (OPT) by drop casting regioregular poly 3-hexylthiophene (P3HT) from three different solvents: p-xylene, dichlorobenzene and chloroform. The best performance was obtained for films drop-casted from p-xylene with a maximum photosensitivity (P) of 3.8 x 10(3) and responsivity (R) of 250 A W(-1) under white light illumination. For films deposited from dichlorobenzene and chloroform the values of P were 1.1 x 10(3) and 30, respectively, while the values of R were 150 and 35, respectively. The maximum responsivity value reported here is at least one order of magnitude higher than that of previously reported solution processed OPT devices. By analyzing the absorption spectra of different films, we conclude that the better device performance of OPT from p-xylene is due to better crystallinity of P3HT. Demonstration of high performance OPTs is a significant step forward in integrating these devices in various optoelectronic circuits.

Quantum chemistry of quantum dots: Effects of ligands and oxidation

We report Gaussian basis set density functional theory (DFT) calculations of the structure and spectra of several colloidal quantum dots (QDs) with a (CdSe)(n) core (n=6,15,17), that are either passivated by trimethylphosphine oxide ligands, or unpassivated and oxidized. From the ground state geometry optimization results we conclude that trimethylphosphine oxide ligands preserve the wurtzite structure of the QDs. Evaporation of the ligands may lead to surface reconstruction. We found that the number of two-coordinated atoms on the nanoparticles surface is the critical parameter defining the optical absorption properties. For (CdSe)(15) wurtzite-derived QD this number is maximal among all considered QDs and the optical absorption spectrum is strongly redshifted compared to QDs with threefold coordinated surface atoms. According to the time-dependent DFT results, surface reconstruction is accompanied by a significant decrease in the linear absorption. Oxidation of QDs destroys the perfection of the QD surface, increases the number of two-coordinated atoms and results in the appearance of an infrared absorption peak close to 700 nm. The vacant orbitals responsible for this near infrared transition have strong Se-O antibonding character. Conclusions of this study may be used in optimization of engineered nanoparticles for photodetectors and photovoltaic devices.