# US 11,306,244 B2 · Two-dimensional perovskite phosphor and method of formation

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- Number: US 11,306,244 B2
- Document ID: US11306244B2
- Status: Granted
- Kind: B2
- Application number: 16/142,756
- Filed: 2018-09-26
- Published: 2019-01-24
- Granted: 2022-04-19
- Earliest claimed: 2013-10-23
- Assignees: The Board of Trustees of the Leland Stanford Junior University
- Applicants: The Board of Trustees of the Leland Stanford Junior University
- Inventors: Emma Rose Dohner; Hemamala Indivari Karunadasa
- Web page: https://patentgrep.com/patent/US11306244B2

## CPC

- C09K 11/06: containing organic luminescent materials
- C09K 11/664: {Halogenides (C09K11/661 takes precedence)}
- C09K 11/08: containing inorganic luminescent materials
- C09K 11/66: containing germanium, tin or lead
- C09K 2211/188: of other metals not provided for in one of the previous groups
- Y02B 20/00: Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps
- C09K: MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- Y02B: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS

## Abstract

Intrinsic broadband white-light emitting phosphors and a solution-state method for producing them are disclosed. Emitters in accordance with the present invention include layered perovskite-based phosphors that comprise metals and halides and have an emission spectrum that spans the entire visible-light spectrum.

## Claims

### Claim 1

A phosphor comprising:
a layered hybrid perovskite comprising:
at least one metal-halide sheet that comprises [PbCl4]2−, [PbBr4]2− or a mixture of [PbCl4]2− and [PbBr4]2−; and
at least one organic layer that comprises organic molecules;
wherein the phosphor has a two-dimensional (100) perovskite crystal structure or a two-dimensional (110) perovskite crystal structure;
wherein the phosphor emits light having an emission spectrum that is continuous and spans at least the wavelength range from approximately 400 nm to approximately 700 nm; and
wherein the light is emitted by the at least one metal-halide sheet.

### Claim 2 (depends on 1)

The phosphor of claim 1 wherein the organic molecules are selected from the group consisting of (2,2′(ethylenedioxy)bis(ethylammonium)) (EDBE) and (N1-methylethane-1,2-diammonium) (N-MEDA).

### Claim 3 (depends on 1)

The phosphor of claim 1, wherein the at least one metal-halide sheet further includes a second halide, wherein the metal, the first halide, and second halide are arranged in the two-dimensional perovskite crystal structure, and wherein a shape of the emission spectrum is influenced by the ratio of the first halide and the second halide.

### Claim 4 (depends on 1)

The phosphor of claim 1, wherein the at least one metal-halide sheet is the (110) perovskite crystal structure, and wherein the (110) perovskite crystal structure is corrugated.

### Claim 5 (depends on 1)

The phosphor of claim 1 wherein the at least one metal-halide sheet is the (100) perovskite crystal structure.

### Claim 6

A method comprising:
selecting organic molecules having an organic chain of a certain length;
mixing a first solution and a second solution to form a third solution, the first solution comprising a inorganic compound dissolved in a first hydrohalic acid and the second solution comprising the organic molecules dissolved in the first hydrohalic acid, wherein the inorganic compound comprises a metal and a first halide comprising [PbCl4]2−, [PbBr4]2− or a mixture of [PbCl4]2− and [PbBr4]2− and wherein the first hydrohalic acid comprises the first halide; and
precipitating a first phosphor from the third solution, wherein the first phosphor comprises a layered two-dimensional perovskite that includes at least one metal-halide sheet comprising the metal and the first halide, and wherein the at least one metal-halide sheet emits light having a first emission spectrum that is continuous and spans at least the wavelength range from approximately 400 nm to approximately 700 nm;
wherein the organic molecules templates a two-dimensional (100) perovskite structure or a two-dimensional (110) perovskite crystal structure.

### Claim 7 (depends on 6)

The method of claim 6 further comprising:
dissolving the first phosphor in a fourth solution including the first hydrohalic acid and a second hydrohalic acid that comprises a second halide;
adding a liquid to the fourth solution to form a fifth solution, the liquid containing an organic solvent, wherein the liquid is added while at a temperature below room temperature; and
precipitating a second phosphor from the fifth solution, wherein the second phosphor a layered two-dimensional perovskite that includes the metal, the first halide, and the second halide, wherein the second phosphor is operative for emitting light having a second emission spectrum that includes a visible-light spectrum, and wherein a shape of the second emission spectrum is influenced by a ratio of the first halide and second halide in the second phosphor.

### Claim 8 (depends on 6)

The method of claim 6 wherein the precipitation of the first phosphor is by an operation selected from the group consisting of:
maintaining the temperature of the third solution at or below room temperature;
diffusing an organic solvent into the third solution; and
sub-operations including;
(i) forming the third solution such that it is a saturated solution at a first temperature that is greater than room temperature; and
(ii) cooling the third solution to a second temperature that is less than the first temperature.

### Claim 9 (depends on 6)

The method of claim 6 wherein the organic molecules are selected from the group consisting of (2,2′-(ethylenedioxy)bis(ethylammonium)) (EDBE) and (N1-methylethane-1,2-diammonium) (N-MEDA).

### Claim 10 (depends on 6)

The method of claim 6 wherein the at least one metal-halide sheet is the (110) perovskite crystal structure, and wherein the (110) perovskite crystal structure is corrugated.

### Claim 11 (depends on 6)

The method of claim 6 wherein the at least one metal-halide sheet is the (100) perovskite crystal structure.

### Claim 12

A phosphor comprising:
an inorganic sheet comprising a metal and a first halide comprising [PbCl4]2−, [PbBr4]2− or a mixture of [PbCl4]2− and [PbBr4]2−; and
an organic layer that comprises organic molecules;
wherein the inorganic sheet and organic layer collectively define a layered hybrid perovskite crystal structure, the crystal structure based on the organic molecules in the organic layer, and wherein the crystal structure is a (100) perovskite crystal structure or a (110) perovskite crystal structure; and
wherein the phosphor emits light having a spectrum that is continuous and spans at least the wavelength range from approximately 400 nm to approximately 700 nm, and wherein the emission arises from a bulk effect within the first inorganic sheet.

### Claim 13 (depends on 12)

The phosphor of claim 12 wherein the organic molecules are selected from the group consisting of (2,2′-(ethylenedioxy)bis(ethylammonium)) (EDBE) and (N1-methylethane-1,2-diammonium) (N-MEDA).

### Claim 14 (depends on 12)

The phosphor of claim 12 wherein the inorganic sheet further comprises a second halide, wherein the shape of the spectrum is influenced by the ratio of the first halide and the second halide.

### Claim 15 (depends on 12)

The phosphor of claim 12 wherein the inorganic sheet is the (110) perovskite crystal structure, and wherein the (110) perovskite crystal structure is corrugated.

### Claim 16 (depends on 12)

The phosphor of claim 12 wherein the inorganic sheet is the (100) perovskite crystal structure.