Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels
This dissertation presents the development of ultra-sensitive fluidic sensors and molecular dynamics studies of ion and water distribution in highly confined nanochannels. <p>The fluidic sensor is based on resistive pulse sensing, i.e., when a non-conducting particle flows through an electroly...
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ndltd-VANDERBILT-oai-VANDERBILTETD-etd-07112008-0943122013-01-08T17:16:21Z Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels XU, DONGYAN Mechanical Engineering This dissertation presents the development of ultra-sensitive fluidic sensors and molecular dynamics studies of ion and water distribution in highly confined nanochannels. <p>The fluidic sensor is based on resistive pulse sensing, i.e., when a non-conducting particle flows through an electrolyte-filled aperture, it displaces a volume of the electrolyte equal to its own volume, which results in an increase in the electrical resistance of the aperture. This resistance increase can be measured as current or voltage pulses to detect the translocation of particles. Instead of direct measurement of the ionic current or electrical potential modulation, the new ultra-sensitive fluidic sensor integrates the fluidic circuit with a MOSFET and monitors the MOSFET drain current to detect particles. The minimum volume ratio of the particle to the sensing channel detected is 0.006%, about ten times smaller than the lowest detected volume ratio previously reported in the literature. <p>To understand the complex system of the electrolyte in highly confined nanochannels with charged surfaces, molecular dynamics studies of ion distribution in a nanochannel were performed using a three-region simulation domain to include two bulk regions on each side of the nanochannel. Results show that both the concentrations of counter-ions and co-ions inside the nanochannel could be significantly different from the bulk concentration, challenging the common practice in the literature of regarding the co-ion concentration as that of the bulk electrolyte. In addition, the ion and water distribution near charged (100) and (111) silicon surfaces were examined. It was shown that, under high surface charge densities, the water molecules within ~ 5 Å from the charged (100) silicon surface can be split from one layer into two layers because of the strong electrostatic interactions between surface charges and water molecules. This phenomenon was not observed for the (111) silicon surface, consistent with results in the literature, which indicates that in addition to the surface charge density, the surface atom density may also affect the near-wall water distribution. Leonard C. Feldman Deyu Li Yongsheng Leng Ronald D. Schrimpf Greg Walker VANDERBILT 2008-07-11 text application/pdf http://etd.library.vanderbilt.edu/available/etd-07112008-094312/ http://etd.library.vanderbilt.edu/available/etd-07112008-094312/ en unrestricted I hereby certify that, if appropriate, I have obtained and attached hereto a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee. I hereby grant to Vanderbilt University or its agents the non-exclusive license to archive and make accessible, under the conditions specified below, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report. |
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Mechanical Engineering XU, DONGYAN Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
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This dissertation presents the development of ultra-sensitive fluidic sensors and molecular dynamics studies of ion and water distribution in highly confined nanochannels. <p>The fluidic sensor is based on resistive pulse sensing, i.e., when a non-conducting particle flows through an electrolyte-filled aperture, it displaces a volume of the electrolyte equal to its own volume, which results in an increase in the electrical resistance of the aperture. This resistance increase can be measured as current or voltage pulses to detect the translocation of particles. Instead of direct measurement of the ionic current or electrical potential modulation, the new ultra-sensitive fluidic sensor integrates the fluidic circuit with a MOSFET and monitors the MOSFET drain current to detect particles. The minimum volume ratio of the particle to the sensing channel detected is 0.006%, about ten times smaller than the lowest detected volume ratio previously reported in the literature. <p>To understand the complex system of the electrolyte in highly confined nanochannels with charged surfaces, molecular dynamics studies of ion distribution in a nanochannel were performed using a three-region simulation domain to include two bulk regions on each side of the nanochannel. Results show that both the concentrations of counter-ions and co-ions inside the nanochannel could be significantly different from the bulk concentration, challenging the common practice in the literature of regarding the co-ion concentration as that of the bulk electrolyte. In addition, the ion and water distribution near charged (100) and (111) silicon surfaces were examined. It was shown that, under high surface charge densities, the water molecules within ~ 5 Å from the charged (100) silicon surface can be split from one layer into two layers because of the strong electrostatic interactions between surface charges and water molecules. This phenomenon was not observed for the (111) silicon surface, consistent with results in the literature, which indicates that in addition to the surface charge density, the surface atom density may also affect the near-wall water distribution.
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author2 |
Leonard C. Feldman |
author_facet |
Leonard C. Feldman XU, DONGYAN |
author |
XU, DONGYAN |
author_sort |
XU, DONGYAN |
title |
Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
title_short |
Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
title_full |
Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
title_fullStr |
Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
title_full_unstemmed |
Development of Ultra-Sensitive Fluidic Sensors and Molecular Dynamics Studies of Ion and Water Distribution in Nanochannels |
title_sort |
development of ultra-sensitive fluidic sensors and molecular dynamics studies of ion and water distribution in nanochannels |
publisher |
VANDERBILT |
publishDate |
2008 |
url |
http://etd.library.vanderbilt.edu/available/etd-07112008-094312/ |
work_keys_str_mv |
AT xudongyan developmentofultrasensitivefluidicsensorsandmoleculardynamicsstudiesofionandwaterdistributioninnanochannels |
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1716570326952837120 |