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WO2004032176A1 - Dielectriques nanoporeux pour generateur de plasma - Google Patents

Dielectriques nanoporeux pour generateur de plasma Download PDF

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Publication number
WO2004032176A1
WO2004032176A1 PCT/KR2003/002023 KR0302023W WO2004032176A1 WO 2004032176 A1 WO2004032176 A1 WO 2004032176A1 KR 0302023 W KR0302023 W KR 0302023W WO 2004032176 A1 WO2004032176 A1 WO 2004032176A1
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WIPO (PCT)
Prior art keywords
few
dielectric
plasma
dielectrics
nanoporous
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Ceased
Application number
PCT/KR2003/002023
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English (en)
Inventor
Kyu-Wang Lee
Sung-Jin Park
Jin-Hoon Cho
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Individual
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Priority to AU2003265112A priority Critical patent/AU2003265112A1/en
Publication of WO2004032176A1 publication Critical patent/WO2004032176A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00—Generating plasma; Handling plasma
    • H05H1/24—Generating plasma
    • H05H1/2406—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes
    • H05H1/2441—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes characterised by the physical-chemical properties of the dielectric, e.g. porous dielectric
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
    • H01J37/32—Gas-filled discharge tubes
    • H01J37/32431—Constructional details of the reactor
    • H01J37/32532—Electrodes
    • H01J37/32559—Protection means, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
    • H01J37/32—Gas-filled discharge tubes
    • H01J37/32009—Arrangements for generation of plasma specially adapted for examination or treatment of objects, e.g. plasma sources
    • H01J37/32018—Glow discharge

Definitions

  • the present invention relates to a method for generating a highly efficient and stable plasma and a device thereof using nanoporous dielectrics.
  • the present invention is suitable for wide range of applications of plasma induced physical and chemical processes such as lamp, surface treatment, thin film deposition, etching, cleaning and sterilization etc.
  • Plasma is a collection of electrons, ions and excited neutral species.
  • a glow discharge plasma is non-thermal and highly reactive while gas remains ambient temperature and finds its many applications in lamp, surface treatment, thin film deposition, etching, cleaning and sterilization etc.
  • pin or brush type electrodes (Akishev et al: J. Phys. D., 1630, 1993), insertion of dielectric barrier between electrodes (Kogoma et al: J. Phys. D., 1125,
  • Another object of the present invention is to provide a plasma electrode device that produces a stable glow discharge in various gases up to atmospheric pressure.
  • the distribution and dimension of pores and the thickness of barrier layer etc. affect the density and energy of electrons as well as current density and this results in the prevention of arc and further controls the plasma density. Further, cathode fall is minimized and settled during glow discharge and this prevents transition to arc.
  • Avalanche like propagation of electrons in nano channel increases the electron density significantly and the sharp edge of the nano structures generates very high electric fields.
  • inclusion of conductor, semiconductor and secondary electron emitter inside of pores or pore peripherals enhance the above effects and lowering the breakdown voltage and increasing the plasma efficiency. Further, low work function materials enhance the electron emission efficiency.
  • Still another object ofthe present invention is to provide diverse devices for various applications by simple modification of electrodes. Wider range of dielectric property and capacitance can be varied via modification of dielectric structure, compared to the conventional bulk dielectrics. This enables to generate the low to high density, the low to high pressure and the small and large volume plasma.
  • the dielectrics of the present invention has regular or irregular array of pores with diameter (D) of few nm to um.
  • D diameter
  • this structure will be referred to as a 'nanoporous structure'
  • a dielectric including such structure will be referred to as a 'nanoporous dielectric'.
  • the dielectrics of the present invention contains regular or irregular array of pores with diameter (D) of few nm to um and their pore distribution, pore length (L), pore diameter (D) and inter pore distance (d) can be modified with ease, depending on the dielectric material and processing method. To avoid confusion in wording, thickness and height will be expressed by 'length'.
  • FIG. 1 is a schematic view of a basic structure of an electrode with regular shape nanoporous dielectrics.
  • FIGS. 2A to 2C are cross-sectional views of the structural variation of an electrode with regular shape nanoporous dielectrics.
  • FIG. 3 is a cross-sectional view of a basic structure of an electrode with irregular shape nanoporous dielectrics.
  • FIGS. 4A and 4B are the cross-sectional views of the structural variation of an electrode with irregular shape nanoporous dielectrics.
  • FIGS. 5A to 5D are schematic views of a diode type plasma device with one or more electrodes with nanoporous dielectrics.
  • FIG. 6 is a schematic view of a triode type plasma device with one or more electrode with nanoporous dielectrics.
  • FIG. 7 is a graph showing electrical properties for the FIG 5A type plasma device with porous anodic alumina dielectric (device A) and with porous alumina dielectric (device B).
  • FIG. 8 is a photograph illustrating a homogeneous glow discharge plasma in the FIG 5A type plasma device.
  • FIGS. 9 A and 9B are photographs illustrating a homogeneous glow discharge plasma in the FIG 6 type plasma device with different power supplying scheme.
  • barrier layer 24 barrier layer 24, 24, 54: pore peripherals 26, 26, 66, 66, 56: nano pore 27,28: plasma reforming materials
  • FIG. 1 is a schematic view of a basic structure of the electrode with regular shape nanoporous dielectrics, according to a first embodiment of the present invention.
  • nanoporous dielectric 20 (hereinafter, it is referred to simply as 'dielectric') is formed on the conducting electrode 10.
  • the dielectric 20 is composed of the porous area with pore 26 (hereinafter, it is referred to simply as 'pore') and barrier layer 22 without pore having a designated thickness (t2). Meanwhile, nano peripheral pores 24 indicate a peripheral portion of pores.
  • the cross sectional shape of the pore 26 can be circular or other shape.
  • the ratio of the pore diameter (D) to the length (L) as well as the ratio of the pore length (L) to the thickness of dielectric (tl) affect the effects from nanoporous dielectric and plasma characteristics significantly and can be optimized with respect to the specific plasma application.
  • the variation ofthe thickness (t2) ofthe barrier layer 22 controls the electron flow from conducting electrode 10 and the capacitance of dielectric 20 and consequently controls the plasma characteristics.
  • the shape of the pore also can be modified to vary the electrical property of dielectric 20. For example, whole or certain area ofthe pore mouth can be closed to make a nano chamber.
  • a diameter of the pore (D) can be in the range of few nm to few um and the length (L) is in the range of few tens of nm to few hundreds of um.
  • a inter pore distance (d) is in the range of few nm and few tens of um.
  • a porous anodic alumina is an example of electrode described in FIG 1. Its electrochemical preparation method, forming mechanism and modification of the structure are fairly well known (Yakoleva et al, Inorg. Mat., 34,711, 1998, Jessensky et al. Appl. Phys. Lett., 72, 1773, 1998).
  • a nano structure array was formed on a cleaned and electropolished aluminum substrate by anodization in acidic solution or by specifically shaped nano patterning such as photolithography followed by the removal of patterning layer.
  • This seeded substrate was further anodized to a desirable thickness of dielectric. Pore diameter, pore density and barrier layer thickness were controlled by the applied voltage and the type of electrolyte. Further pore widening can also be achieved by dissolution of anodic alumina. Since anodic alumina grows on the aluminum conducting electrode, the adhesion between the conducting electrode and the dielectric is very strong and results in a very durable and efficient electrode.
  • Nano porous silica is another example which can be prepared by lithography and patterning. (Tonucci et al. Science, 258, 783, 1992)
  • the conducting electrode can be formed on a nano porous silica dielectric.
  • FIGS. 2 A to 2C illustrate cross-sectional views of the structural variation of the electrode with regular shape nanoporous dielectrics, according to the second embodiment of this invention.
  • barrier layer was selectively removed.
  • conductors or semiconductors such as Ni, Au, Ag, graphite, MnO 2 , TiO 2 , conducting polymers, or secondary electron emissive materials, such as MgO, BaO, KCl, NaCl, diamond, SnO 2 etc. are embedded in the nano pore.
  • the length (hi) of the embedding layer 27 that is related to the current density through pore can be adjusted in the range of few nm to few tens of um.
  • conductors or semiconductors such as Ni, W, Mo, Au, Ag, Pt, Al:Li graphite, MnO 2 , TiO 2 , or secondary electron emissive materials, such as MgO, BaO, LiF, KCl, NaCl, diamond, SnO 2 etc. are coated on the nano pore peripherals 24.
  • the length (h2) of this coating layer 28 can be adjusted in the range of few nm to few tens of um.
  • the nanoporous dielectrics can be prepared directly from the dielectric composite of conductors, semiconductors and secondary electron emitting materials. An appropriate amount ofthe above materials can be mixed with dielectric materials in preparation of dielectric layer or their alloy can be used in electrochemical preparation of dielectric layer.
  • the anodic anodization of Al-Mg alloy produces a nanoporous composite of alumina and magnesia.
  • the device with this dielectric layer shows excellent plasma characteristics without adhesion problem that is often observed in the devices of the examples of FIGS. 2B and 2C.
  • FIG. 2A The combination of structural variation as illustrated in FIG. 2A, FIG. 2B and FIG. 2C is also possible.
  • FIG. 3 is a cross-sectional view of a basic structure of the electrode with irregular shape nanoporous dielectrics, according to the third embodiment of this invention.
  • the nm to um size dielectric particles such as alumina, silica and polystyrene are deposit on the conducting electrode 10 to form the dielectric layer 50 with pores 54.
  • This dielectric layer can be deposit by various methods of precipitation, electrochemical, plasma jet, sol-gel and electrophoretic deposition etc.
  • the dielectric materials must have suitable dielectric constant, durability and preferably, good adhesion to conducting electrode.
  • Good secondary electron emitting materials such as Csl and KCl film show a columnar structure with pores, those have been applied to a channel plate (Shikhaliev et al. Nucl. Inst. Met. Phys. Res., 487, 676, 2002), can be used as a dielectric. Since their durability and low or even negative electron affinity, nanoporous diamond and diamond like carbon can be utilized too.
  • FIG. 4A shows a nanoporous conducting layer 60 while FIG. 4B shows a nanoporous dielectric layer 67 as well as nanoporous conducting electrode layer 60, according to the fourth embodiment of this invention.
  • the diameters (D) of pores 66, 66' are in the range of few nm to few hundreds of nm.
  • the thickness and the ration to the diameter are similar to those illustrated in above embodiments and their effects are also similar.
  • An example of FIG. 4B structure can be obtained by electro photochemical etching of silicon.
  • a silicon oxide for dielectric layer was formed via thermal or electrochemical oxidation and followed by forming a conducting electrode.
  • This device is similar to the ballistic electron surface-emitting device (BSD) for field emission display (FED). (Ichihara et al. J. Cryst. Growth, 1915, 2002)
  • nano fiber bundle of conductors, semiconductors and insulators such as Ag, Au, carbon nanotube, CdS, MgO, TiO 2 etc. can be used as conducting electrodes or dielectrics.
  • plasma efficiency can be improved by secondary electron emission or field emission effect from the nanoporous structure or the nano bundle.
  • adhesion is the most concerning factor.
  • Plasma and heat resistant nano porous polymer for example, polycarbonate, polystyrene, or polyester, can also be used as a dielectric for cold plasma device.
  • FIGS. 5 A to 5D illustrate the schematic view of the diode type plasma device with one or more electrode with nano porous dielectrics according to the fifth embodiment of this invention.
  • a conducting electrode 70 such as metal plate and an electrode with nano porous dielectrics are arranged to form a discharge space, such that the discharging electrodes face each other.
  • both of discharging electrodes are electrodes with nano porous dielectrics.
  • a coplanar discharge and a surface discharge type device structures with electrode with nano porous dielectrics are illustrated in FIG. 5C and FIG. 5D, respectively.
  • FIGS. 5 A to 5D Although the electrode with regular shape nanoporous dielectrics was illustrated in FIGS. 5 A to 5D, other types and their combinations of electrode with nano porous dielectrics suggested in this invention, such as illustrated in FIGS. 2 A to
  • DC, pulsed DC, AC, RF and MW power supply can be used.
  • few tens of voltages to few hundreds of voltages, and hundreds of uA/cm 2 to tens of mA/cm 2 of current density can be used.
  • few kV to tens of few kV can be applied.
  • the distance between discharge electrodes can be varied from few hundreds of um to few tens of cm, depending on the discharge gas composition and the pressure. There is no limitation in total thickness and area ofthe electrode. Further, dielectric properties of dielectric layer can be tailored precisely and no external ballast is necessary. In some cases, a gas flow system can be installed inside of the electrode to make gas flow in-between nanoporous structures.
  • FIG. 6 illustrates a schematic view ofthe triode type plasma device with one or more electrode with nano porous dielectrics according to the sixth embodiment of the present invention.
  • a conducting or semi conducting layer 28, acting as a gate is formed on top of nano porous dielectrics.
  • the gate voltage is lower than that of discharge electrodes. If AC was applied between discharge electrodes, DC can be applied to the gate or the gate can be grounded, after shorting the switch 86.
  • FIG. 6 is a graph showing electrical properties for the FIG. 5A type plasma device with porous anodic alumina dielectric (device A) and with porous alumina dielectric (device B).
  • the 25 mm x 30 mm aluminum electrode and the ITO counter electrode was separated by 1 mm.
  • Discharge gas was 50 Torr of Ne gas.
  • device A 17 um thick porous anodic alumina with pore diameter of 50 nm was grew on the aluminum electrode, while 20 um thick sintered alumina paste was prepared on the aluminum electrode in device B. Both of the devices A and B show the stable glow discharge up to atmospheric pressure.
  • FIG. 8 is a photograph illustrating homogeneous glow discharge plasma in the FIG 5A type plasma device with porous anodic alumina dielectric. (Device A) The turn on voltage at 100 Torr neon gas was about 130V (AC, 2KHz).
  • FIGS. 9 A and 9B are photographs illustrating homogeneous glow discharge plasma in the FIG 6 type plasma device with different power supplying scheme.
  • 50 nm thick aluminum was evaporated as a gate. When gate was grounded, much stronger light intensity about
  • nanoporous dielectrics for plasma generator of the present invention has the following advantages. According to the present invention, by introducing the nanoporous dielectrics, stable glow discharge can be obtained in various gases up to atmospheric pressure.
  • the distribution and dimension of pores and the thickness of barrier layer etc. affect the density and energy of electrons as well as current density and this results in a prevention of arc and further the controls the plasma density.
  • cathode fall is minimized and settled during glow discharge and this prevents transition to arc.
  • Avalanche like propagation of electrons in nano channel increases the electron density significantly and the sharp edge of the nano structures generate very high electric fields.
  • inclusion of conductor, semiconductor and secondary electron emitter inside of pores or pore peripherals enhance the above effects and lowering the breakdown voltage and increasing the plasma efficiency.
  • low work function materials enhance the electron emission efficiency.
  • nanoporous dielectrics promotes the heat dissipation ability that enhances the plasma efficiency and device lifetime. Since dielectrics are directly grown on the conducting electrode, adhesion, durability and plasma efficiency are maximized while it minimizes the resistive heat.
  • the process of preparing dielectrics is very simple and large area device can be prepared very easily.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Plasma & Fusion (AREA)
  • Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Plasma Technology (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Abstract

La présente invention concerne une électrode plasma présentant des diélectriques nanoporeux dont la dimension des pores est comprise entre quelques nm et quelques um. Selon un mode de réalisation de la présente invention, des diélectriques nanoporeux réguliers ou irréguliers sont formés sur les électrodes et placés de manière symétrique ou non symétrique afin de produire une décharge luminescente présentant divers modes de volume, de surface et de décharge coplanaire. La simple modification de paramètres du plasma et par conséquent l'amélioration de la stabilité et de l'efficacité du plasma peut être obtenue par modification de l'épaisseur, de homogénéité, du diamètre des pores et de la porosité des diélectriques nanoporeux et par imprégnation ou formation de matière de reformage de plasma telles que des matières conductrices, semi-conductrices ou émissives d'électrons secondaires à l'intérieur du pore ou de la surface des diélectriques.
PCT/KR2003/002023 2002-10-04 2003-10-01 Dielectriques nanoporeux pour generateur de plasma Ceased WO2004032176A1 (fr)

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KR10-2002-0060513A KR100530765B1 (ko) 2002-10-04 2002-10-04 나노 다공성 유전체를 이용한 플라즈마 발생장치
KR10-2002-0060513 2002-10-04

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DE102005002142A1 (de) * 2005-01-12 2006-07-20 Forschungsverbund Berlin E.V. Mikroplasmaarray
US7297041B2 (en) * 2004-10-04 2007-11-20 The Board Of Trustees Of The University Of Illinois Method of manufacturing microdischarge devices with encapsulated electrodes
US7477017B2 (en) 2005-01-25 2009-01-13 The Board Of Trustees Of The University Of Illinois AC-excited microcavity discharge device and method
DE102008024486A1 (de) * 2008-05-21 2009-12-03 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Plasmastempel, Plasmabehandlungsvorrichtung, Verfahren zur Plasmabehandlung und Herstellungsverfahren für einen Plasmastempel
WO2010138103A1 (fr) * 2008-05-30 2010-12-02 Colorado State University Research Foundation Matières de surface d'électrode et structures pour plasmachimie
EP1905057A4 (fr) * 2005-07-15 2012-06-27 Univ Illinois Reseaux de dispositifs a plasma a microcavites comprenant des electrodes encapsulees dans un dielectrique
US8221179B2 (en) 2001-10-26 2012-07-17 The Board Of Trustees Of The University Of Illinois Method of making arrays of thin sheet microdischarge devices
CN102933015A (zh) * 2012-11-16 2013-02-13 上海交通大学 一维纳米结构极化增强放电电极
US8497631B2 (en) 2006-01-23 2013-07-30 The Board Of Trustees Of The University Of Illinois Polymer microcavity and microchannel devices and fabrication method
US8547004B2 (en) 2010-07-27 2013-10-01 The Board Of Trustees Of The University Of Illinois Encapsulated metal microtip microplasma devices, arrays and fabrication methods
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JP2015032401A (ja) * 2013-07-31 2015-02-16 富士フイルム株式会社 ガス電子増倍器およびガス電子増倍装置
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US9028656B2 (en) 2008-05-30 2015-05-12 Colorado State University Research Foundation Liquid-gas interface plasma device
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US9272359B2 (en) 2008-05-30 2016-03-01 Colorado State University Research Foundation Liquid-gas interface plasma device
CZ306217B6 (cs) * 2015-10-06 2016-10-05 Fyzikální ústav AV ČR, v.v.i. Zdroj nízkoteplotního plazmatu s možností kontaktní i bezkontaktní aplikace a způsob výroby sendvičové struktury pro tento zdroj
KR20160146391A (ko) * 2015-06-12 2016-12-21 주식회사 넥스트이앤엠 경사가 있는 나노기공을 포함하는 이온 다이오드막 및 그 제조 방법
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WO1998042002A1 (fr) * 1997-03-18 1998-09-24 Trustees Of The Stevens Institute Of Technology Dispositif de decharge luminescente a plasma
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Cited By (50)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8221179B2 (en) 2001-10-26 2012-07-17 The Board Of Trustees Of The University Of Illinois Method of making arrays of thin sheet microdischarge devices
US7297041B2 (en) * 2004-10-04 2007-11-20 The Board Of Trustees Of The University Of Illinois Method of manufacturing microdischarge devices with encapsulated electrodes
US8545764B2 (en) 2005-01-12 2013-10-01 Forschungsverbund Berlin E.V. Microplasma array
DE102005002142A1 (de) * 2005-01-12 2006-07-20 Forschungsverbund Berlin E.V. Mikroplasmaarray
US7477017B2 (en) 2005-01-25 2009-01-13 The Board Of Trustees Of The University Of Illinois AC-excited microcavity discharge device and method
EP1905057A4 (fr) * 2005-07-15 2012-06-27 Univ Illinois Reseaux de dispositifs a plasma a microcavites comprenant des electrodes encapsulees dans un dielectrique
US8497631B2 (en) 2006-01-23 2013-07-30 The Board Of Trustees Of The University Of Illinois Polymer microcavity and microchannel devices and fabrication method
US8864542B2 (en) 2006-01-23 2014-10-21 The Board Of Trustees Of The University Of Illinois Polymer microcavity and microchannel device and array fabrication method
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