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\n\n \n \n \n \n \n Stochastic Pore Blocking and Gating in PDMS-Glass Nanopores from Vapor-Liquid Phase Transitions.\n \n \n \n\n\n \n Shimizu, S.; Ellison, M.; Aziz, K.; Wang, Q. H.; Ulissi, Z. W.; Gunther, Z.; Bellisario, D.; and Strano, M.\n\n\n \n\n\n\n
Journal of Physical Chemistry C, 117(19): 9641–9651. 5 2013.\n
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@Article{ISI:000319649100015,\n Title = {Stochastic Pore Blocking and Gating in PDMS-Glass Nanopores from Vapor-Liquid Phase Transitions},\n Author = {Shimizu, Steven and Ellison, Mark and Aziz, Kimberly and Wang, Qing Hua and Ulissi, Zachary W. and Gunther, Zachary and Bellisario, Darin and Strano, Michael},\n Journal = {Journal of Physical Chemistry C},\n Year = {2013},\n\n Month = {5},\n Number = {19},\n Pages = {9641--9651},\n Volume = {117},\n\n Abstract = {Polydimethylsiloxane (PDMS) is commonly used in research for microfluidic devices and for making elastomeric stamps for soft lithography. Its biocompatibility and nontoxicitiy also allow it to be used in personal care, food, and medical products. Herein we report a phenomenon observed when patch clamp, a technique normally used to study biological ion channels, is performed on both grooved and planar PDMS surfaces, resulting in stochastic current fluctuations that are due to a nanopore being formed at the interface of the PDMS and glass surfaces and being randomly blocked. Deformable pores between 1.9 +/- 0.7 and 7.4 +/- 2.1 nm in diameter, depending on the calculation method, form upon patching to the surface. Coulter blocking and nanoprecipitation are ruled out, and we instead propose a mechanism of stochastic current fluctuations arising from transitions between vapor and liquid phases, consistent with similar observations and theory from statistical mechanics literature. Interestingly, we find that {[}Ru(bpy)(3)](2+), a common probe molecule employed in nanopore research, physisorbs inside these hydrophobic nanopores blocking all ionic current flow at concentrations higher than 1 X 10(-4) M, despite the considerably larger pore diameter relative to the molecule. Patch clamp methods are promising for the study of stochastic current fluctuations and other transport phenomenon in synthetic nanopore systems.},\n Doi = {10.1021/jp312659m},\n ISSN = {1932-7447},\n Unique-id = {ISI:000319649100015}\n}\n\n
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\n Polydimethylsiloxane (PDMS) is commonly used in research for microfluidic devices and for making elastomeric stamps for soft lithography. Its biocompatibility and nontoxicitiy also allow it to be used in personal care, food, and medical products. Herein we report a phenomenon observed when patch clamp, a technique normally used to study biological ion channels, is performed on both grooved and planar PDMS surfaces, resulting in stochastic current fluctuations that are due to a nanopore being formed at the interface of the PDMS and glass surfaces and being randomly blocked. Deformable pores between 1.9 +/- 0.7 and 7.4 +/- 2.1 nm in diameter, depending on the calculation method, form upon patching to the surface. Coulter blocking and nanoprecipitation are ruled out, and we instead propose a mechanism of stochastic current fluctuations arising from transitions between vapor and liquid phases, consistent with similar observations and theory from statistical mechanics literature. Interestingly, we find that [Ru(bpy)(3)](2+), a common probe molecule employed in nanopore research, physisorbs inside these hydrophobic nanopores blocking all ionic current flow at concentrations higher than 1 X 10(-4) M, despite the considerably larger pore diameter relative to the molecule. Patch clamp methods are promising for the study of stochastic current fluctuations and other transport phenomenon in synthetic nanopore systems.\n
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\n\n \n \n \n \n \n Control of nano and microchemical systems.\n \n \n \n\n\n \n Ulissi, Z. W.; Strano, M. S.; and Braatz, R. D.\n\n\n \n\n\n\n
Computers & Chemical Engineering, 51(SI): 149-156. 4 2013.\n
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@Article{ISI:000314993000014,\n Title = {Control of nano and microchemical systems},\n Author = {Ulissi, Zachary W. and Strano, Michael S. and Braatz, Richard D.},\n Journal = {Computers \\& Chemical Engineering},\n Year = {2013},\n\n Month = {4},\n Number = {SI},\n Pages = {149-156},\n Volume = {51},\n\n Abstract = {Many advances in the development of nano and microchemical systems have occurred in the last decade. These systems have significant associated identification and control challenges, including high state dimensionality, limitations in real-time measurements and manipulated variables, and significant uncertainties described by non-Gaussian distributions. Some strategies for addressing these challenges are summarized, which include exploiting structure within the stochastic Master equations that describe molecular interactions, manipulating molecular bonds at system boundaries, and manipulating molecules and nanoscale objects through magnetic and electric fields. The strategies are illustrated in a variety of applications that include the estimation of nucleation kinetics of protein and pharmaceutical crystals within fluidic devices, the estimation of concentration fields using DNA-wrapped single-walled carbon nanotube-based sensor arrays, the simultaneous control of nanoscale geometry and electrical activation during thermal annealing in a semiconductor material, and the control of nanostructure formation on surfaces. Promising directions for research and technology development are identified for the next decade. (C) 2012 Elsevier Ltd. All rights reserved.},\n Doi = {10.1016/j.compchemeng.2012.07.004},\n ISSN = {0098-1354},\n Unique-id = {ISI:000314993000014}\n}\n\n
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\n Many advances in the development of nano and microchemical systems have occurred in the last decade. These systems have significant associated identification and control challenges, including high state dimensionality, limitations in real-time measurements and manipulated variables, and significant uncertainties described by non-Gaussian distributions. Some strategies for addressing these challenges are summarized, which include exploiting structure within the stochastic Master equations that describe molecular interactions, manipulating molecular bonds at system boundaries, and manipulating molecules and nanoscale objects through magnetic and electric fields. The strategies are illustrated in a variety of applications that include the estimation of nucleation kinetics of protein and pharmaceutical crystals within fluidic devices, the estimation of concentration fields using DNA-wrapped single-walled carbon nanotube-based sensor arrays, the simultaneous control of nanoscale geometry and electrical activation during thermal annealing in a semiconductor material, and the control of nanostructure formation on surfaces. Promising directions for research and technology development are identified for the next decade. (C) 2012 Elsevier Ltd. All rights reserved.\n
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\n\n \n \n \n \n \n Diameter-dependent ion transport through the interior of isolated single-walled carbon nanotubes.\n \n \n \n\n\n \n Choi, W.; Ulissi, Z. W; Shimizu, S. F.; Bellisario, D. O; Ellison, M. D; and Strano, M. S\n\n\n \n\n\n\n
Nature Communications, 4: 2397. 2013.\n
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@article{choi2013diameter,\n title={Diameter-dependent ion transport through the interior of isolated single-walled carbon nanotubes},\n author={Choi, Wonjoon and Ulissi, Zachary W and Shimizu, Steven FE and Bellisario, Darin O and Ellison, Mark D and Strano, Michael S},\n journal={Nature Communications},\n volume={4},\n pages={2397},\n year={2013},\n doi={10.1038/ncomms3397},\n publisher={Nature Publishing Group}\n}\n\n
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\n\n \n \n \n \n \n Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes.\n \n \n \n\n\n \n Zhang, J.; Landry, M. P.; Barone, P. W.; Kim, J.; Lin, S.; Ulissi, Z. W.; Lin, D.; Mu, B.; Boghossian, A. A.; Hilmer, A. J.; Rwei, A.; Hinckley, A. C.; Kruss, S.; Shandell, M. A.; Nair, N.; Blake, S.; Sen, F.; Sen, S.; Croy, R. G.; Li, D.; Yum, K.; Ahn, J.; Jin, H.; Heller, D. A.; Essigmann, J. M.; Blankschtein, D.; and Strano, M. S.\n\n\n \n\n\n\n
Nature Nanotechnology, 8(12): 959–968. 12 2013.\n
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@Article{ISI:000327943400026,\n Title = {Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes},\n Author = {Zhang, Jingqing and Landry, Markita P. and Barone, Paul W. and Kim, Jong-Ho and Lin, Shangchao and Ulissi, Zachary W. and Lin, Dahua and Mu, Bin and Boghossian, Ardemis A. and Hilmer, Andrew J. and Rwei, Alina and Hinckley, Allison C. and Kruss, Sebastian and Shandell, Mia A. and Nair, Nitish and Blake, Steven and Sen, Fatih and Sen, Selda and Croy, Robert G. and Li, Deyu and Yum, Kyungsuk and Ahn, Jin-Ho and Jin, Hong and Heller, Daniel A. and Essigmann, John M. and Blankschtein, Daniel and Strano, Michael S.},\n Journal = {Nature Nanotechnology},\n Year = {2013},\n\n Month = {12},\n Number = {12},\n Pages = {959--968},\n Volume = {8},\n\n Abstract = {Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.},\n Doi = {10.1038/NNANO.2013.236},\n ISSN = {1748-3387},\n Unique-id = {ISI:000327943400026}\n}\n\n
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\n Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.\n
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