arXiv subjects

Shane Ardo

Publications and source records attributed to Shane Ardo.

3 recordsLinked to original sources

arXiv2025

Imaging nanoscale photocarrier traps in solar water-splitting catalysts

Defects trap photocarriers and hinder solar water splitting. The nanoscale photocarrier transport, trapping, and recombination mechanisms are usually inferred from ensemble-averaged measurements and remain elusive. Because an individual high-performing nanoparticle photocatalyst may outperform the ensemble average, design rules that would otherwise enhance catalytic efficiency remain unclear. Here, we introduce photomodulated electron energy-loss spectroscopy (EELS) in an optically coupled scanning transmission electron microscope (STEM) to map photocarrier localization. Using rhodium-doped strontium titanate (SrTiO3:Rh) solar water-splitting nanoparticles, we directly image the carrier densities concentrated at oxygen-vacancy surface trap states. This is achieved by separating photothermal heating from photocarrier populations through experimental and computational analyses of low-loss spectra. Photomodulated STEM-EELS enables angstrom-scale imaging of defect-induced photocarrier traps and their impact on photocatalytic efficiency.

physics.chem-ph↗

arXiv2023

A nanoporous capacitive electrochemical ratchet for continuous ion separations

Directed ion transport in liquid electrolyte solutions underlies many phenomena in Nature and industry. While Nature has devised structures that drive continuous ion flow without Faradaic redox reactions, artificial analogs do not exist. Here we report the first demonstration of an ion pump that drives aqueous ions against a force using a capacitive ratchet mechanism that does not require redox reactions. Modulation of an electric potential between thin metallic layers on either face of a nanoporous alumina wafer immersed in solution resulted in persistent voltages and ionic currents. This occurs due to the non-linear capacitive nature of electric double layers, whose repeated charging and discharging sustains a continuous ion flux. Ratchet driven electrodialysis was demonstrated reaching a 50% decrease in the conductivity of the solution in a dilution cell. These ratchet-based ion pumps can enable continuous desalination and selective ion separation using an electrically powered device with no moving parts.

physics.app-ph↗

arXiv2022

Ratchet based ion pumps for selective ion separations

The development of a selective, membrane-based ion separation technology may prove useful in a wide range of applications such as water treatment, battery recycling, ion specific chemical sensors, extraction of valuable metals from sea water, and bio-medical devices. In this work we show that a flashing ratchet mechanism can be used for high precision ion separation. The suggested ratchet-based ion pumps utilize a unique feature of ratchets, the frequency dependent current reversals, to drive ions with the same charge but different diffusion coefficients in opposite directions. We show that for the prevalent ions in water, ions with a relative diffusion coefficient difference as small as 1% can be separated by driving them in opposite directions with a velocity difference as high as 1.2 mm/s. Since the pumping properties of the ratchet are determined by an electric input signal, the proposed ion pumps can pave the way for simple large-scale, fit-to-purpose selective ion separation systems.

physics.app-ph↗