School of Chemistry - Research Publications
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ItemA reflective display based on the electro-microfluidic assembly of particles within suppressed water-in-oil droplet array(SPRINGERNATURE, 2023-12-05)Reflective displays have stimulated considerable interest because of their friendly readability and low energy consumption. Herein, we develop a reflective display technique via an electro-microfluidic assembly of particles (eMAP) strategy whereby colored particles assemble into annular and planar structures inside a dyed water droplet to create "open" and "closed" states of a display pixel. Water-in-oil droplets are compressed within microwells to form a pixel array. The particles dispersed in droplets are driven by deformation-strengthened dielectrophoretic force to achieve fast and reversible motion and assemble into multiple structures. This eMAP based device can display designed information in three primary colors with ≥170° viewing angle, ~0.14 s switching time, and bistability with an optimized material system. This proposed technique demonstrates the basis of a high-performance and energy-saving reflective display, and the display speed and color quality could be further improved by structure and material optimization; exhibiting a potential reflective display technology.
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ItemNo Preview AvailableEnergy dissipation during homogeneous wetting of surfaces with randomly and periodically distributed cylindrical pillars(ACADEMIC PRESS INC ELSEVIER SCIENCE, 2024-04)HYPOTHESIS: Understanding contact angle hysteresis on rough surfaces is important as most industrially relevant and naturally occurring surfaces possess some form of random or structured roughness. We hypothesise that hysteresis can be described by the dilute defect model of Joanny & de Gennes [1] and that the energy dissipation occurring during the stick-slip motion of the contact line is key to developing a predictive equation for hysteresis. EXPERIMENTS: We measured hysteresis on surfaces with randomly distributed and periodically arranged microscopic cylindrical pillars for a variety of different liquids in air. The inherent (flat surface) contact angles tested range from lyophilic (θe=33.8°) to lyophobic (θe=112.0°). FINDINGS: A methodology for averaging the measured advancing and receding contact angles on random surfaces is presented. Based on these results correlations for roughness-induced energy dissipation are derived, and an equation for predicting the advancing and receding contact angles during homogeneous (Wenzel) wetting on random surfaces is presented. Equations that predict the onset of the alternate wetting conditions of hemiwicking, split-advancing, split-receding and heterogeneous (Cassie) wetting are also derived, thus defining the range of validity for the homogeneous wetting equation. A 'cluster' concept is proposed to explain the measurably higher hysteresis exhibited by structured surfaces compared to random surfaces.
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ItemNo Preview AvailableElectrophoretic Deposition of Single Nanoparticles(AMER CHEMICAL SOC, 2024-02-01)The controlled assembly of colloid particles on a solid substrate has always been a major challenge in colloid and surface science. Here we provide an overview of electrophoretic deposition (EPD) of single charge-stabilized nanoparticles. We demonstrate that surface templated EPD (STEPD) assembly, which combines EPD with top-down nanofabrication, allows a wide range of nanoparticles to be built up into arbitrary structures with high speed, scalability, and excellent fidelity. We will also discuss some of the current colloid chemical limitations and challenges in STEPD assembly for sub-10 nm nanoparticles and for the fabrication of densely packed single particle arrays.
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ItemNo Preview AvailableSpectroelectrochemistry of CdSe/CdS Core-Shell Quantum Dots(AMER CHEMICAL SOC, 2024-02-16)
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ItemNo Preview AvailableThe Multiple Roles of Na Ions in Highly Efficient CZTSSe Solar Cells(WILEY-V C H VERLAG GMBH, 2024-02-11)Sodium (Na) doping is a well-established technique employed in chalcopyrite and kesterite solar cells. While various improvements can be achieved in crystalline quality, electrical properties, or defect passivation of the absorber materials by incorporating Na, a comprehensive demonstration of the desired Na distribution in CZTSSe is still lacking. Herein, a straightforward Na doping approach by dissolving NaCl into the CZTS precursor solution is proposed. It is demonstrated that a favorable Na ion distribution should comprise a precisely controlled Na+ concentration at the front surface and an enhanced distribution within the bottom region of the absorber layer. These findings demonstrated that Na ions play several positive roles within the device, leading to an overall power conversion efficiency of 12.51%.
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ItemPolarity-Tunable Field Effect Phototransistors(AMER CHEMICAL SOC, 2023-05-30)Field-effect phototransistors feature gate voltage modulation, allowing dynamic performance control and significant signal amplification. A field-effect phototransistor can be designed to be inherently either unipolar or ambipolar in its response. However, conventionally, once a field-effect phototransistor has been fabricated, its polarity cannot be changed. Herein, a polarity-tunable field-effect phototransistor based on a graphene/ultrathin Al2O3/Si structure is demonstrated. Light can modulate the gating effect of the device and change the transfer characteristic curve from unipolar to ambipolar. This photoswitching in turn produces a significantly improved photocurrent signal. The introduction of an ultrathin Al2O3 interlayer also enables the phototransistor to achieve a responsivity in excess of 105 A/W, a 3 dB bandwidth of 100 kHz, a gain-bandwidth product of 9.14 × 1010 s-1, and a specific detectivity of 1.91 × 1013 Jones. This device architecture enables the gain-bandwidth trade-off in current field-effect phototransistors to be overcome, demonstrating the feasibility of simultaneous high-gain and fast-response photodetection.
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ItemSize, Diffusion, and Sedimentation of Gold Nanorods(AMER CHEMICAL SOC, 2023-11-08)We have used four different analytical techniques (electron microscopy (TEM), dynamic light scattering (DLS), analytical ultracentrifugation (AUC), and small angle X-ray scattering (SAXS) to measure the length and width as well as the diffusion coefficients of gold nanorods of different aspect ratio. All four methods could reproduce the trends in aspect ratio, and both length and width could be extracted once the ligand shell was accounted for. The CTAB bilayer coating was determined to have a thickness of 3.34, 3.02, and 3.26 nm by SAXS, DLS, and AUC, respectively. TEM nevertheless yielded the best predictions for the nanorod ensemble surface plasmon resonance by using COMSOL simulations. All four methods yielded better fits when the rods were treated as spherically capped cylinders.
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ItemGold Nanodrum Resonators(AMER CHEMICAL SOC, 2023-10-12)Nanodrum resonators have been fabricated using nanometer-thick gold films as the drumheads. The fabrication method is favorable for large-area array manufacture of arbitrary shapes. The drum resonators exhibit fundamental mode vibration frequencies in the MHz regime. We use the stretched-plate model to describe the natural vibrations of the drum. The Q factor of the fundamental mode increases as the thickness of the drum increases and decreases as the drum diameter goes up. The highest Q factor of the fundamental mode reaches 290 at room temperature and atmospheric pressure. Based on the deduced material properties we estimate that the resonator has a mass sensitivity of 1.11 × 10-22 g/Hz.
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ItemNo Preview AvailableRoom Temperature Bias-Selectable, Dual-Band Infrared Detectors Based on Lead Sulfide Colloidal Quantum Dots and Black Phosphorus(AMER CHEMICAL SOC, 2023-06-15)A single photodetector capable of switching its peak spectral photoresponse between two wavelength bands is highly useful, particularly for the infrared (IR) bands in applications such as remote sensing, object identification, and chemical sensing. Technologies exist for achieving dual-band IR detection with bulk III-V and II-VI materials, but the high cost and complexity as well as the necessity for active cooling associated with some of these technologies preclude their widespread adoption. In this study, we leverage the advantages of low-dimensional materials to demonstrate a bias-selectable dual-band IR detector that operates at room temperature by using lead sulfide colloidal quantum dots and black phosphorus nanosheets. By switching between zero and forward bias, these detectors switch peak photosensitive ranges between the mid- and short-wave IR bands with room temperature detectivities of 5 × 109 and 1.6 × 1011 cm Hz1/2 W-1, respectively. To the best of our knowledge, these are the highest reported room temperature values for low-dimensional material dual-band IR detectors to date. Unlike conventional bias-selectable detectors, which utilize a set of back-to-back photodiodes, we demonstrate that under zero/forward bias conditions the device's operation mode instead changes between a photodiode and a phototransistor, allowing additional functionalities that the conventional structure cannot provide.
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ItemNo Preview AvailableTuning the Photoluminescence Anisotropy of Semiconductor Nanocrystals(AMER CHEMICAL SOC, 2023-09-25)Semiconductor nanocrystals are promising optoelectronic materials. Understanding their anisotropic photoluminescence is fundamental for developing quantum-dot-based devices such as light-emitting diodes, solar cells, and polarized single-photon sources. In this study, we experimentally and theoretically investigate the photoluminescence anisotropy of CdSe semiconductor nanocrystals with various shapes, including plates, rods, and spheres, with either wurtzite or zincblende structures. We use defocused wide-field microscopy to visualize the emission dipole orientation and find that spheres, rods, and plates exhibit the optical properties of 2D, 1D, and 2D emission dipoles, respectively. We rationalize the seemingly counterintuitive observation that despite having similar aspect ratios (width/length), rods and long nanoplatelets exhibit different defocused emission patterns by considering valence band structures calculated using multiband effective mass theory and the dielectric effect. The principles are extended to provide general relationships that can be used to tune the emission dipole orientation for different materials, crystalline structures, and shapes.