Method for detecting the interaction of at least one entity with a dielectric layer

9,746,460

14/350489

October 08, 2012

The invention relates to a method of detecting the interaction between at least one entity and a dielectric layer containing different electron levels in the energy band gap of the dielectric layer, the method comprising the following steps: a) depositing the entity on the dielectric layer; b) subjecting the dielectric layer and the entity deposited thereon to exciting electromagnetic radiation that does not give rise to observable luminescence in the entity itself under the conditions implemented in step c); and c) detecting the luminescence of the dielectric layer, in which the radiative and non-radiative electron transitions between the energy levels of the band gap have been influenced as a result of its interaction with the entity.

UNIVERSITE CLAUDE BERNARD LYON I (Villeurbanne, FR); ECOLE CENTRALE DE LYON (Ecully, FR); INSTITUT NATIONALE DES SCIENCES APPLIQUEES DE LYON (Villeurbanne, FR); CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE (Paris, FR); INSERM (INSTITUT NATIONAL DE LA SANTE ET DE LA RECHERCHE MEDICALE) (Paris, FR)

CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE (Paris, FR), INSERM (INSTITUT NATIONAL DE LA SANTE ET DE LA RECHERCHE MEDICALE) (Paris, FR)

1. A method of detecting the interaction between at least one entity and a dielectric layer containing different electron levels in the energy band gap of the dielectric layer, the method comprising the following steps: a) depositing the at least one entity on the dielectric layer; b) subjecting the dielectric layer and the at least one entity deposited on the dielectric layer to exciting electromagnetic radiation that does not give rise to observable luminescence of the at least one entity itself under the conditions implemented in step c); and c) detecting the luminescence of the dielectric layer, in which the radiative and non-radiative electron transitions between the energy levels of the band gap have been influenced as a result of its interaction with the at least one entity; wherein the dielectric layer is made of a member selected from the group consisting of: silicon oxide, in which silicon nanoparticles are distributed, and wherein said dielectric layer comprises Si—H, Si—O—Si, and Si—OH bonds, with a stoichiometry, in terms of atoms of Si and O, of SiOx, with 0

2. The method according to claim 1 , wherein, by physicochemical interactions with the dielectric layer on which the at least one entity is deposited, the at least one entity is capable of influencing the radiative and non-radiative electron transitions between the energy levels in the band gap as caused by the exciting electromagnetic radiation.

3. The method according to claim 1 , wherein the silicon nanoparticles have a size in a range from 1 nm to 20 nm.

4. The method according to claim 3 , wherein the silicon nanoparticles have a size in a range from 1 nm to 7 nm.

5. The method according to claim 1 , wherein the dielectric layer has a thickness of less than 500 nm.

6. The method according to claim 5 , wherein the dielectric layer has a thickness in a range from 50 to 150 nm.

7. The method according to claim 1 , wherein the dielectric layer is a dielectric layer of silicon nitride having silicon nanoparticles distributed therein, and that is partially hydrogenated, in which the stoichiometry in atoms of silicon and atoms of nitrogen is SiNxa, where xa is in a range from 0.4 to 0.8.

8. The method according to claim 1 , wherein the dielectric layer does not include any metallic particles, neither in material of the dielectric layer, nor on a surface of the dielectric layer.

9. The method according to claim 1 , wherein the exciting electromagnetic radiation is selected from the group consisting of radiation of light visible to the human eye, infrared radiation, ultraviolet radiation, and X-ray radiation.

10. The method according to claim 1 , wherein the luminescence of the dielectric layer is detected in step c) in the form of an image having a plurality of colors.

11. The method according to claim 1 , wherein the dielectric layer is obtained by a plasma excited chemical vapor deposition technique.

12. The method according to claim 1 , wherein detection is carried out without adding a luminescent agent to the at least one entity.

13. The method according to claim 1 , wherein the biological entity is a living cell.

14. The method according to claim 1 , wherein the biological entity is a living cell that is deposited and cultured on the dielectric layer.

15. The method according to claim 1 , wherein the biological entity is a molecule forming part of a cell or a cellular organelle.

16. The method according to claim 15 , wherein the biological entity is a member selected from the group consisting of a protein, a lipid, a DNA, a RNA, a nucleus, and a mitochondrion.

17. The method according to claim 1 , wherein the silicon nanoparticles present a volume fraction lying in a range of 5% to 75% relative to a total volume of the dielectric layer.

2010/0035335 February 2010 Lakowicz et al.
2011/0188733 August 2011 Bardos et al.

Watts et al. “Optical Biosensor for Monitoring Microbial Cells” (1994), Analytical Chemistry, vol. 66: 2465-2470. cited by examiner
Duplan et al., A photoluminescence-based quantum semiconductor biosensor for rapid in situ detection of Escherichia coli, Sensors and Actuators B: Chemical, Jul. 19, 2011, vol. 160, pp. 46-51 and S1-S4. cited by examiner
Salamon et al., Coupled Plasmon-Waveguide Resonators: A New Spectroscopic Tool for Probing Proteolipid Film Structure and Properties, Biophysical Journal, 1997, vol. 73, pp. 2791-2797. cited by examiner
Giebel et al., Imaging of Cell/Substrate Contacts of Living Cells with Surface Plasmon Resonance Microscopy, Biophysical Journal, vol. 76, pp. 509-516. cited by examiner
Nychyporuk, T., et al. “Strong photoluminescence enhancement of silicon quantum dots by their near-resonant coupling with multi-polar plasmonic hot spots.” Nanoscale 3.6 (2011): 2472-2475. cited by examiner
Biteen, Julie S., et al. “Enhanced radiative emission rate and quantum efficiency in coupled silicon nanocrystal-nanostructured gold emitters.” Nano letters 5.9 (2005): 1768-1773. cited by examiner
International Search Report mailed Jan. 16, 2013, corresponding to International Patent Application No. PCT/FR2012/052274. cited by applicant
Pascal Anger et al.: “Enhancement and Quenching of Single-Molecule Fluorescence”, Physical Review Letters, vol. 96, No. 11, Mar. 1, 2006 (Mar. 1, 2006). cited by applicant
F Giorgis et al: “Luminescence processes in amorphous hydrogenated silicon-nitride nanometric multilayers”, Physical Review, vol. 60, No. 16, Oct. 15, 1999, pp. 11572-11576. cited by applicant
Pons T et al: “On the quenching of semiconductor quantum dot photoluminescence by proximal gold nanoparticles”, Nano Letters, ACS, US, vol. 7, No. 10, Oct. 1, 2007, pp. 3157-3164. cited by applicant
T. Serdiuk et al :“Storage of luminescent nanoparticles in porous silicon: Toward a solid state “golden fleece””, Materials Letters, vol. 65, No. 15-16, Aug. 1, 2011, pp. 2514-2517. cited by applicant
Robertson et al., Gap states in silicon nitride, Applied Physics Letters, 1984, 44, 415-417. cited by applicant
Nychyporuk et al., Electroless deposition of Ag nanoparticles on the surface of SiNx : H dielectric layers, Solar Energy Materials and Solar Cells, vol. 94, Issue 12, Dec. 2010, pp. 2314-2317. cited by applicant
Mo et al, Luminescence of nanometer-sized amorphous silicon nitride solids, Journal of Applied Physics Letters, 1993, 73, 5185-5188. cited by applicant
Yamaguchi et al, Short lifetime photoluminescence of amorphous-SiNx films, Applied Physics Letters, 2000, vol. 77, No. 23, 3773-3775. cited by applicant
Kang et al, White photoluminescence from SiNx films prepared by plasma enhanced chemical vapor deposition, Proc. of SPIE, vol. 6337, 633710, (2006). cited by applicant

edspgr.09746460