Scintillation compound including a rare earth element and a process of forming the same
A scintillation compound can include a rare earth element that is in a divalent (RE 2+ ) or a tetravalent state (RE 4+ ). The scintillation compound can include another element to allow for better change balance. The other element may be a principal constituent of the scintillation compound or may be a dopant or a co-dopant. In an embodiment, a metal element in a trivalent state (M 3+ ) may be replaced by RE 4+ and a metal element in a divalent state (M 2+ ). In another embodiment, M 3+ may be replaced by RE 2+ and M 4+ . In a further embodiment, M 2+ may be replaced by a RE 3+ and a metal element in a monovalent state (M 1+ ). The metal element used for electronic charge balance may have a single valance state, rather than a plurality of valence states, to help reduce the likelihood that the valance state would change during formation of the scintillation compound.
1. A scintillation apparatus including a luminescent material comprising a rare earth (Ln) orthosilicate doped with an element RE different from Ln, RE being chosen among Ce, Pr, and Tb, wherein the element RE is at least partially in its 4+ oxidation state (RE 4+ ), the quantity of RE 4+ in the luminescent material being between 0.0001% and 0.1% in mass.
2. The scintillation apparatus of claim 1 , wherein the quantity of RE 4+ in the luminescent material is between 0.0005% and 0.05% in mass.
3. The scintillation apparatus of claim 1 , wherein a molar ratio RE 4+ /(RE 3+ +RE 4+ ) is between 0.05 and 1.
4. The scintillation apparatus of claim 1 , wherein the quantity of RE in the luminescent material is between 0.001% and 0.1% in mass.
5. The scintillation apparatus of claim 1 , wherein the luminescent material has the formula
Ln (2-z-x1-x2) RE 3+ x1 RE 4+ x2 M z M′ v Si (1-v) O (5) , wherein:
Ln represents a rare earth different than RE;
M represents a divalent alkaline-earth element;
M′ represents a trivalent element such as Al, Ga, Sc, In, or any combination thereof;
(z+v) is greater than or equal to 0.0001 and lower than or equal to 0.2;
z is greater than or equal to 0 and lower than or equal to 0.2;
v is greater than or equal to 0 and lower than or equal to 0.2;
x1 is greater than or equal to 0.00005 and lower than 0.1;
x2 is greater than or equal to 0.00005 and lower than 0.1;
x2/(x1+x2) is greater than or equal to 0.05 and lower than 1;
x1+x2 is lower than 0.1.
6. The scintillation apparatus of claim 5 , wherein x1 is greater than or equal to 0.0005 and lower than 0.01, and x2 is greater than or equal to 0.0005 and lower than 0.01.
7. The scintillation apparatus of claim 5 , wherein z lower than or equal to 0.1.
8. The scintillation apparatus of claim 7 , wherein z is greater than or equal to 0.00003.
9. The scintillation apparatus of claim 5 , wherein x2/(x1+x2) is greater than or equal to 0.1.
10. The scintillation apparatus of claim 5 , wherein v is greater than 0.
11. The scintillation apparatus of claim 5 , wherein RE is Ce, and a sum of masses of M and M′ in the luminescent material is less than a mass of Ce in the luminescent material.
12. The scintillation apparatus of claim 5 , wherein the quantity of M′ in the luminescent material is in a proportion from 0.005 mol % to 25 mol % of a sum of moles of Si and of RE 3+ in the luminescent material.
13. The scintillation apparatus of claim 5 , wherein:
Ln is a rare earth chosen among Y, La, Gd, Er, Ho, Lu, or any combination thereof;
M is a divalent alkaline-earth element chosen among Ca, Mg, Sr, Ba, or any combination thereof;
v is 0;
z is greater than or equal to 0.00003 and lower than or equal to 0.1;
x1 is greater than or equal to 0.00005 and lower than 0.01;
x2 is greater than or equal to 0.00005 and lower than 0.01; and
x2/(x1+x2) is greater than or equal to 0.1 and lower than or equal to 1.
14. The scintillation apparatus of claim 1 , wherein Ln is chosen among one or more elements of the group: Y, La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, or Lu.
15. The scintillation apparatus of claim 14 , wherein cerium represents 0.005 mol % to 20 mol % of all the rare earths in the luminescent material.
16. The scintillation apparatus of claim 14 , wherein the luminescent material is codoped with a divalent alkaline earth element present in a proportion from 0.0025 mol % to 15 mol % of the sum of all the rare earths included in the luminescent material.
17. The scintillation apparatus of claim 1 , wherein the apparatus includes an ionizing particle detector, a luminescence emitter, or a medical imaging apparatus.
18. A method of forming a luminescent material, the method comprising:
an oxidizing heat treatment at a temperature between 1100° C. and 2200° C. in an atmosphere containing at least 10 vol % of oxygen; and
cooling after heating that results in the luminescent material,
wherein:
the heat treatment and the cooling both being carried out in an atmosphere containing at least 10 vol % of oxygen when the temperature is greater than 1100° C.;
the luminescent material includes a rare earth (Ln) silicate doped with an element RE different from Ln, RE being chosen among Ce, Pr, Tb, wherein the element RE is at least partially in its 4+ oxidation state (RE 4+ ), the quantity of RE 4+ in the luminescent material being between 0.0001% and 0.1% in mass; and
the luminescent material is formed from raw materials, one of which includes an oxide of RE 4+ .
19. The method of claim 18 , further comprising melting the raw materials, wherein the melting of the raw materials is carried out in an atmosphere containing less than 1 vol % of oxygen.