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@ARTICLE{Singh:128614,
      author       = {Singh, Pradyumna S. and Kätelhön, Enno and Mathwig, Klaus
                      and Wolfrum, Bernhard and Lemay, Serge G.},
      title        = {{S}tochasticity in {S}ingle-{M}olecule
                      {N}anoelectrochemistry: {O}rigins, {C}onsequences, and
                      {S}olutions},
      journal      = {ACS nano},
      volume       = {6},
      number       = {11},
      issn         = {1936-086X},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {FZJ-2013-00348},
      pages        = {9662 - 9671},
      year         = {2012},
      abstract     = {Electrochemical detection of single molecules is being
                      actively pursued as an enabler of new fundamental
                      experiments and sensitive analytical capabilities. Most
                      attempts to date have relied on redox cycling in a nanogap,
                      which consists of two parallel electrodes separated by a
                      nanoscale distance. While these initial experiments have
                      demonstrated single-molecule detection at the
                      proof-of-concept level, several fundamental obstacles need
                      to be overcome to transform the technique into a realistic
                      detection tool suitable for use in more complex settings
                      (e.g., studying enzyme dynamics at single catalytic event
                      level, probing neuronal exocytosis, etc.). In particular, it
                      has become clearer that stochasticity—the hallmark of most
                      single-molecule measurements—can become the key limiting
                      factor on the quality of the information that can be
                      obtained from single-molecule electrochemical assays. Here
                      we employ random-walk simulations to show that this
                      stochasticity is a universal feature of all single-molecule
                      experiments in the diffusively coupled regime and emerges
                      due to the inherent properties of Brownian motion. We
                      further investigate the intrinsic coupling between
                      stochasticity and detection capability, paying particular
                      attention to the role of the geometry of the detection
                      device and the finite time resolution of measurement
                      systems. We suggest concrete, realizable experimental
                      modifications and approaches to mitigate these limitations.
                      Overall, our theoretical analyses offer a roadmap for
                      optimizing single-molecule electrochemical experiments,
                      which is not only desirable but also indispensable for their
                      wider employment as experimental tools for electrochemical
                      research and as realistic sensing or detection systems.},
      cin          = {PGI-8 / JARA-FIT / ICS-8},
      ddc          = {540},
      cid          = {I:(DE-Juel1)PGI-8-20110106 / $I:(DE-82)080009_20140620$ /
                      I:(DE-Juel1)ICS-8-20110106},
      pnm          = {423 - Sensorics and bioinspired systems (POF2-423) / 453 -
                      Physics of the Cell (POF2-453)},
      pid          = {G:(DE-HGF)POF2-423 / G:(DE-HGF)POF2-453},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000311521700035},
      pubmed       = {pmid:23106647},
      doi          = {10.1021/nn3031029},
      url          = {https://juser.fz-juelich.de/record/128614},
}