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Yang, Sang Mo,Strelcov, Evgheni,Paranthaman, M. Parans,Tselev, Alexander,Noh, Tae Won,Kalinin, Sergei V. American Chemical Society 2015 NANO LETTERS Vol.15 No.2
<P>Scanning probe microscopy (SPM) is a powerful tool to investigate electrochemistry in nanoscale volumes. While most SPM-based studies have focused on reactions at the tip–surface junction, charge and mass conservation requires coupled and intrinsically nonlocal cathodic and anodic processes that can be significantly affected by ambient humidity. Here, we explore the role of water in both cathodic and anodic processes, associated charge transport, and topographic volume changes depending on the polarity of tip bias. The first-order reversal curve current–voltage technique combined with simultaneous detection of the sample topography, referred to as FORC-IVz, was applied to a silver solid ion conductor. We found that the protons generated from water affect silver ionic conduction, silver particle formation and dissolution, and mechanical integrity of the material. This work highlights the dual nature (simultaneously local and nonlocal) of electrochemical SPM studies, which should be considered for comprehensive understanding of nanoscale electrochemistry.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/nalefd/2015/nalefd.2015.15.issue-2/nl5040286/production/images/medium/nl-2014-040286_0009.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/nl5040286'>ACS Electronic Supporting Info</A></P>
Mechanical Control of Electroresistive Switching
Kim, Yunseok,Kelly, Simon J.,Morozovska, Anna,Rahani, Ehsan Kabiri,Strelcov, Evgheni,Eliseev, Eugene,Jesse, Stephen,Biegalski, Michael D.,Balke, Nina,Benedek, Nicole,Strukov, Dmitri,Aarts, J.,Hwang, I American Chemical Society 2013 Nano letters Vol.13 No.9
<P>Hysteretic metal–insulator transitions (MIT) mediated by ionic dynamics or ferroic phase transitions underpin emergent applications for nonvolatile memories and logic devices. The vast majority of applications and studies have explored the MIT coupled to the electric field or temperarture. Here, we argue that MIT coupled to ionic dynamics should be controlled by mechanical stimuli, the behavior we refer to as the piezochemical effect. We verify this effect experimentally and demonstrate that it allows both studying materials physics and enabling novel data storage technologies with mechanical writing and current-based readout.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/nalefd/2013/nalefd.2013.13.issue-9/nl401411r/production/images/medium/nl-2013-01411r_0005.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/nl401411r'>ACS Electronic Supporting Info</A></P>
Nanoparticle Shape Evolution and Proximity Effects During Tip-Induced Electrochemical Processes
Yang, Sang Mo,Paranthaman, Mariappan Parans,Noh, Tae Won,Kalinin, Sergei V.,Strelcov, Evgheni American Chemical Society 2016 ACS NANO Vol.10 No.1
<P>Voltage spectroscopies in scanning probe microscopy (SPM) techniques are widely used to investigate the electrochemical processes in nanoscale volumes, which are important for current key applications, such as batteries, fuel cells, catalysts, and memristors. The spectroscopic measurements are commonly performed on a grid of multiple points to yield spatially resolved maps of reversible and irreversible electrochemical functionalities. Hence, the spacing between measurement points is an important parameter to be considered, especially for irreversible electrochemical processes. Here, we report nonlocal electrochemical dynamics in chains of Ag particles fabricated by the SPM tip on a silver ion solid electrolyte. When the grid spacing is small compared with the size of the formed Ag particles,, anomalous chains of unequally sized particles with double periodicity evolve. This behavior is ascribed to a proximity effect during the tip-induced electrochemical process, specifically, size-dependent silver particle growth following the contact between the particles. In addition, fractal shape evolution of the formed Ag structures indicates that the growth-limiting process changes from Ag+/Ag redox reaction to Ag+-ion diffusion with the increase in the applied voltage and pulse duration. This study shows that characteristic shapes of the electrochemical products are good indicators for determining the underlying growth-limiting process, and emergence of complex phenomena during spectroscopic mapping of electrochemical functionalities.</P>