# US 2014/0150966 A1 · High dielectric nanosheet laminate, high dielectric element and method for producing the same

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- Number: US 2014/0150966 A1
- Document ID: US20140150966A1
- Status: Published application
- Kind: A1
- Application number: 14/118,354
- Filed: 2012-05-18
- Published: 2014-06-05
- Earliest claimed: 2011-05-19
- Assignees: National Institute for Materials Science
- Inventors: Minoru Osada; Yasuo Ebina; Takayoshi Sasaki
- Web page: https://patentgrep.com/patent/US20140150966A1

## CPC

- H01G 4/10: Metal-oxide dielectrics {(H01G4/085 takes precedence)}
- B32B 18/00: Layered products essentially comprising ceramics, e.g. refractory products
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- C01G 33/006: {Compounds containing niobium, with or without oxygen or hydrogen, and containing two or more other elements}
- C01G 35/006: {Compounds containing tantalum, with or without oxygen or hydrogen, and containing two or more other elements}
- C04B 35/495: based on vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates
- C04B 35/62685: {characterised by the order of addition of constituents or additives}
- H10D 1/684: {the dielectrics comprising multiple layers, e.g. comprising buffer layers, seed layers or gradient layers}
- H10P 14/6344: {using Langmuir-Blodgett techniques}
- H10P 14/69398: {the material having a perovskite structure, e.g. BaTiO3}
- C01P 2002/34: perovskite-type (ABO3)
- C01P 2004/24: Nanoplates, i.e. plate-like particles with a thickness from 1-100 nanometer
- C01P 2006/40: Electric properties
- C04B 2235/3201: Alkali metal oxides or oxide-forming salts thereof
- C04B 2235/3208: Calcium oxide or oxide-forming salts thereof, e.g. lime
- C04B 2235/768: Perovskite structure ABO3
- C04B 2237/34: Oxidic
- C04B 2237/345: Refractory metal oxides
- C04B 2237/704: of one or more of the ceramic layers or articles
- H10D 84/0144: {Manufacturing their gate insulating layers}
- H10D 84/038: {using silicon technology, e.g. SiGe}
- H10D 84/212: {of only capacitors}
- Y10T 156/10: Methods of surface bonding and/or assembly therefor
- H01G: CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE (selection of specified materials as dielectric H01B3/00; capacitors having potential barriers H10D1/62, H10K10/10)
- B32B: LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- C04B: LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE {(roofing granules E04D7/005)}; CERAMICS (devitrified glass-ceramics C03C10/00); REFRACTORIES; TREATMENT OF NATURAL STONE
- H10D: INORGANIC ELECTRIC SEMICONDUCTOR DEVICES
- H10P: GENERIC PROCESSES OR APPARATUS FOR THE MANUFACTURE OR TREATMENT OF DEVICES COVERED BY CLASS H10
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION

## Abstract

A high dielectric nanosheet laminate is produced by laminating nanosheets, each of which has a thickness of 10 nm or less and is formed of an oxide that has a perovskite structure wherein at least four NbO6 octahedrons, TaO6 octahedrons or TiO6 octahedrons are included in a unit lattice. Consequently, the high dielectric nanosheet laminate is capable of achieving a high dielectric constant and a satisfactory insulation property, which are preferable for high dielectric nanosheet multilayer capacitors or the like, at the same time even if formed very thin.

## Claims

### Claim 1

A high dielectric nanosheet laminate produced by laminating nanosheets each of which has a thickness of 10 nm or less and is formed of an oxide that has a perovskite structure wherein at least four NbO6 octahedrons, TaO6 octahedrons or TiO6 octahedrons are included in a unit lattice.

### Claim 2 (depends on 1)

The high dielectric nanosheet laminate according to claim 1, wherein each of the nanosheets has a lateral size of 10 nm to 1000 μm.

### Claim 3 (depends on 1)

The high dielectric nanosheet laminate according to claim 1, wherein the nanosheets is one produced by exfoliating any of the layered oxides represented by the following formula or a hydrate thereof:
formula A[Ca2Nan−3NbnO3n+1−d], A[(Ca1−xSrx)2Nan−3NbnO3n+1−d], or A[Mn−1A′n−3M′nO3n+1−d](A, A′ are at least one selected from H, Li, Na, K, Rb and Cs; M is at least one selected from Sr, Ba, Pb, Bi, or rare earth elements La, Ce, Pr, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb and Lu; M′ is at least one selected from Ti, Mg, Mn, Zn, Nb and Ta; x=0 to 1; n=3 to 8; and d=0 to 2).

### Claim 4 (depends on 1)

The high dielectric nanosheet laminate according to claim 1, wherein the nanosheets is a perovskite oxide represented by the following compositional formula:
formula [Ca2Nan−3NbnO3n+1−d], [(Ca1−xSrx)2Nan−3NbnO3n+1−d], or [Mn−1A′n−3M′nO3n+1−d] (A′ is at least one selected from H, Li, Na, K, Rb and Cs; M is at least one selected from Sr, Ba, Bi, or rare earth elements La, Ce, Pr, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb and Lu; M′ is at least one selected from Ti, Mg, Mn, Zn, Nb and Ta; x=0 to 1; n=3 to 8; and d=0 to 2).

### Claim 5 (depends on 1)

The high dielectric nanosheet laminate according to claim 1, which has a thickness of 1 nm to 100 nm.

### Claim 6 (depends on 1)

A high dielectric element produced by adhering a high dielectric nanosheet laminate according to claim 1 onto an electrode substrate.

### Claim 7 (depends on 1)

A high dielectric element wherein a high dielectric nanosheet laminate according to claim 1 is disposed between a first electrode substrate and a second electrode substrate.

### Claim 8 (depends on 1)

A method for producing a high dielectric element wherein a high dielectric nanosheet laminate according to claim 1 is disposed between a first electrode substrate and a second electrode substrate, wherein the high dielectric nanosheet laminate according to claim 1 is adhered onto at least one electrode substrate of the first and second electrode substrates, and the first and second electrode substrates are so disposed that the high dielectric nanosheet laminate is located therebetween.

### Claim 9 (depends on 8)

The method for producing a high dielectric element according to claim 8 in which the high dielectric nanosheet laminate is produced by repeating a step of forming a monolayer film in which a surface of a substrate is covered with the oxide closely and with no gap by the Langmuir-Blodgett process, and then adhering the monolayer film onto the electrode substrate.

### Claim 10 (depends on 8)

The method for producing a high dielectric element according to claim 8 in which the high dielectric nanosheet laminate is produced by dipping the electrode substrate into a cationic organic polymer solution to allow an organic polymer to be adsorbed onto a substrate surface thereof, and then dipping the electrode substrate into a colloid solution in which the nanosheets are suspended, so as to allow the nanosheets to be adsorbed onto the polymer by electrostatic interaction.

### Claim 11 (depends on 10)

The method for producing a high dielectric element according to claim 10, wherein the overlapping parts of the nanosheets are removed by applying ultrasonic waves thereto in the step of allowing the nanosheets to be adsorbed onto the electrode substrate by electrostatic interaction.

### Claim 12 (depends on 10)

The method for producing a high dielectric element according to claim 10, wherein the organic polymer is removed through irradiation with UV rays after the high dielectric nanosheet laminate is produced.

### Claim 13 (depends on 10)

The method for producing a high dielectric element according to claim 10, wherein the organic polymer is removed by heating after the high dielectric nanosheet laminate is produced.