Method of producing fluorescent diamond particles

Patent metadata

Field	Value
Publication number	US-12031072-B2
Application number	US-202117233843-A
Country	US
Kind code	B2
Filing date	Apr 19, 2021
Priority date	Oct 19, 2018
Publication date	Jul 9, 2024
Grant date	Jul 9, 2024

Abstract

A method of controlled production of luminescent diamond particles exhibiting luminescence in selected specific spectral ranges is provided. The method comprises taking diamond particles containing dopant atoms in the diamond core, irradiating the particles with high energy radiation, and annealing the irradiated diamond particles at a target temperature in the temperature range of about 1400° C.-2200° C. to form luminescent diamond particles where the specific spectral range of luminescence is controlled by the target temperature of the annealing process, the irradiation dose, and the type of dopant atoms. Duration of the annealing and the temperature ramp up and ramp down times should be short enough to minimize or prevent significant graphitization of the particles. Duration of the temperature ramp up time should be short enough to minimize formation of color centers that might form at temperatures below the target temperature.

First claim

What is claimed is:

1. A method of processing diamond particles to form a plurality of luminescent diamond particles exhibiting luminescence in specific selected spectral ranges, comprising:
a. providing diamond particles with sizes below about 100 microns having a surface and a diamond lattice and containing a plurality of impurity atoms in the diamond lattice;
b. irradiating the diamond particles with high energy species in a dose of about 1×10 10 species/cm 2 to 1×10 21 species/cm 2 ;
c. annealing the irradiated diamond particles in at least one of an inert gas environment, vacuum, or hydrogen environment at a target temperature in the temperature range from about 1400° C. to about 2200° C. to form luminescent diamond particles with emission in the specific selected spectral range where the specific spectral range is controlled by the temperature and duration of the annealing process and the irradiation dose;
d. purifying the irradiated and annealed diamond particles to remove sp 2 carbon from the surface of the diamond particles; and
e. where the luminescence is excited by electromagnetic radiation in the wavelength range comprising at least one selected from the group consisting of optical and X-ray radiation.

2. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the specific selected spectral ranges correspond to emission spectral ranges of at least one of the luminescent centers formed by an impurity atom and a vacancy; at least two impurity atoms and a vacancy; and a combination thereof.

3. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the luminescence is excited by optical radiation comprising wavelengths from the range about 190 nm to 2000 nm.

4. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the impurity atoms are N atoms and the target temperature facilitates the formation of a plurality of H3 luminescent color centers.

5. The method of processing diamond particles to form color centers according to claim 4 , wherein the target temperature is a temperature above about 1700° C.

6. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the impurity atoms are N atoms and the target temperature is selected to cause the formation of a plurality of N3 luminescent color centers.

7. The method of processing diamond particles to form color centers according to claim 6 , wherein the target temperature is a temperature above about 1900° C.

8. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the target temperature facilitates the formation of a plurality of nickel-containing luminescent color centers.

9. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the diamond particles contain less than about 200 ppm of nitrogen.

10. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the diamond particles comprise particles produced by at least one of the methods selected from the group consisting of detonation, shock wave, chemical vapor deposition, laser ablation, ultrasonic treatment, nucleation of diamond powder in the gas phase, ion irradiation of graphite, chlorination of carbides, high-pressure-high-temperature diamond synthesis and fragmentation of synthetic, or natural bulk diamond.

11. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the irradiating comprises at least one species selected from the group consisting of irradiating with high energy electrons, protons, ions, neutrons, and gamma rays.

12. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , further comprising:
functionalizing the purified diamond particles with at least one functional group selected from the group consisting of carboxylic, hydroxyl, amino, hydrogen, epoxy, polyethylene glycol, hydrocarbon chain, hydrocarbon, aromatic, nucleophile, thiol, sulfur, acid, base, halogen and fluoro-containing.

13. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , further comprising:
after the purification from sp 2 carbon, conjugating with the diamond particles or attaching to the diamond particles at least one material selected from the group consisting of biological molecules, a nucleic acid, a protein, an antibody, a ligand, a dye, a fluorescent specie, a radioactive specie, a paramagnetic specie, an image contrast agent, an isotope, a drug molecule, and a polymer.

14. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , further comprising incorporation of the luminescent diamond particles into a cell, organism, tissue, matrix or a substrate.

15. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the impurity is selected from the group consisting of N, Ni, Co, a transition metal, non-carbon isotope, 19F, 15N, a rare earth element, a noble gas atom, Sn, Ag, Tl, Zn, Si, and Ge.

16. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the irradiating comprises irradiating with electrons having energy between about 300 keV and about 10 MeV providing irradiation dose between about 1×10 16 e/cm 2 to 1×10 21 e/cm 2 .

17. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , wherein the target temperature is selected to cause the formation of at least one of NV, H3, N3, SiV, Ni-containing luminescent color centers, and a mixture thereof.

18. The method of processing diamond particles to form luminescent diamond particles according to claim 1 , further comprising after the step b) annealing the irradiated diamond particles in at least one of an inert gas environment, vacuum, or hydrogen environment at a target temperature below approximately 1400° C. and then performing steps c) and d).

19. A plurality of luminescent diamond particles with sizes below about 100 microns having a surface and a diamond lattice and containing nitrogen dopant atoms at concentration below about 200 ppm and at least one non-nitrogen dopant atom, where particles contain a plurality of at least one of H3 centers, N3 centers, a non-nitrogen dopant atom related luminescent center, and a mixture of the thereof.

20. A plurality of luminescent diamond particles according to claim 19 , further comprising NV centers.

21. A plurality of luminescent diamond particles according to claim 19 , wherein the non-nitrogen dopant is selected from the group consisting of Ni, Co, a transition metal, carbon isotope, 13C, non-carbon isotope, 19F, 15N, a rare earth element, a noble gas atom, Sn, Ag, Tl, Zn, Si, and Ge.

22. A plurality of luminescent diamond particles according to claims 1 and 19 , wherein the concentration of nitrogen dopant atoms is below about 100 ppm.

23. A plurality of luminescent diamond particles according to claims 1 and 19 , wherein the concentration of nitrogen dopant atoms is below about 50 ppm.

24. The method of processing diamond particles to form color centers according to claim 1 , wherein anneali

Assignees

• Shenderova Olga A
• Zaitsev Alexander M
• Nunn Nicholas A
• Torelli Marco Diego
• Adamas Nanotechnologies Inc
• Univ City New York Res Found

Inventors

• Shenderova Olga A
• Zaitsev Alexander M
• Nunn Nicholas A
• Torelli Marco Diego

Classifications

• C30B29/04

  Diamond · CPC title

• C30B1/02

  by thermal treatment, e.g. strain annealing (C30B1/12 takes precedence) · CPC title

• C01B32/28 Primary

  After-treatment, e.g. purification, irradiation, separation or recovery · CPC title

• C09K11/65 Primary

  containing carbon (in organic compounds C09K11/06) · CPC title