DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 3/9/2026 and 3/18/2026 has been entered.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 12-22 and 27-30 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
As amended, claim 12 recites “wherein the perovskite material of the absorber layer has a halide atomic percent in a range of 5.0% to 9.0% bromine” (emphasis added) in lines 14-15. A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). In the present instance, claim 12 recites the broad recitation “halide” genus, and the claim also recites “bromide” species, which is the narrower statement of the range/limitation. The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
Claims 13-19, 22, and 27-30 are rejected on the same ground as claim 12.
For the purpose of this office action, the limitation is construed as the atomic percent of bromide in the halides.
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claims 19 and 29 are rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends.
Claim 19 and 29 depend on claim 12 and recites “the perovskite material having a composition Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3, wherein 0.02≤ x ≤ 0.08, 0.82≤y≤0.92, and 0.07≤z≤0.09 in claim 19, and Cs0.05MA0.08FA0.87Pb(I0.92Br0.08)3 in claim 29. As such, claim 19 recite the atomic percent of bromide to be 0.21 (or 0.07x3) to 0.27 (or0.09x3) which is different from the claimed range of 5.0% to 9.0% bromide recited in claim 12. Similarly, claim 29 recites the atomic percent of bromide to be 0.24 which is not in the claimed range of 5.0% to 9.0% bromide recited in claim 12.
Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 12, 15-16 and 22 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al. (“In situ induced core/shell stabilized hybrid perovskites via gallium (III) acetylacetonate intermediate towards highly efficient and stable solar cells”) in view of Wang et al. (CN 109768168A, see machine translation).
Regarding claim 12, Li et al. discloses method of making a photovoltaic device (see “Solar cell fabrication”):
depositing a first charge transport layer (NiOx) over a first contact layer (FTO-coated glass substrate described in “Solar cell fabrication”);
applying a precursor solution (or perovskite precursor solution) to a surface of a first charge transport layer (NiOx) resulting in a liquid layer of the precursor solution on the surface of the first charge transport layer (see “Solar cell fabrication”), wherein the precursor solution comprises a perovskite precursor, an additive and a solvent (GBL:DMSO); wherein:
the perovskite precursor comprises formamidinium iodide (FAI), cesium iodide (CsI) and lead iodide (PbI2, see “Solar cell fabrication”);
the additive comprises gallium acetylacetonate (Ga(AcAc)3, see “Solar cell fabrication”);
treating the liquid layer to remove at least a portion of the solvent (see annealing step), thereby forming an absorber layer comprising a perovskite material which is solid.
Li et al. does not teach comprising solution further comprises lead bromide such that the perovskite material of the absorber layer having an atomic percent of bromine in the halides in a range of 5.0% to 9.0%.
Wang et al. discloses using FAI, CsI, PbBr2, and PbI2 to form a perovskite material of FA0.7Cs0.1MA0.2Cs0.1Pb(Br0.05I0.95)3 (see [0077], [0099], [0116] of the translation) having the atomic percent of bromine (Br) in the mixed halides to be 5.0% (or 0.05). 5.0% is right within the claimed range of 5.0% to 9.0%.
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Li et al. by further including lead bromide (PbBr2) in the perovskite precursor to form a perovskite material FA0.7Cs0.1MA0.2Cs0.1Pb(Br0.05I0.95)3 having the atomic percent of bromine in the mixed halides to be 5.0% as taught by Wang et al., because Wang et al. such perovskite material is preferable to achieve perovskite solar cell with high energy conversion efficiency and fill factor (see [0010], [0077], [0099], [0116]). Furthermore, such modification would involve nothing more than forming known material for its intended use in a known environment to accomplish entirely expected result. International Co. v. Teleflex Inc. (KSR), 550 U.S. 398, 82 USPQ2d 1385 (2007)
Regarding claim 15, modified Li et al. discloses a method as in claim 12 above, wherein Li et al. teaches providing a second contact layer (Ag electrode) over the absorber layer (see “Solar cell fabrication” and using gallium acetylacetonate (Ga(AcAc)3) to passivate the surface of the perovskite material and protect the perovskite material for enhancing the long-term stability while maintaining high power conversion efficiency (see abstract-broader context and conclusion).
Li et al. does not explicitly teach treating the absorber layer with a surface modifier comprising Ga(AcAc)3, after the step of forming an absorber layer comprising the perovskite material, and prior to providing the second contact layer.
However, it would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Li et al. by treating the absorber layer with a surface modifier of Ga(AcAc)3 after the step of forming an absorber layer comprising the perovskite material and prior to providing the second contact layer to further passivate and protect the perovskite absorber layer for enhancing the long-term stability while maintaining high power conversion efficiency, because Li et al. teaches using Ga(AcAc)3 to passivate and protect the surface of the perovskite material.
Regarding claim 16, modified Li et al. discloses a method as in claim 12 above, wherein Li et al. teaches the additive comprises gallium acetylacetonate (Ga(AcAc)3, see claim 12 above or the whole document of Li et al.).
Regarding claim 22, modified Li et al. discloses all the steps of the claimed method as in claim 12 above, the method will result the same product as claimed in the instant claim, or the additive is present in the absorber layer with a concentration gradient. In re Best, 562 F.2d 1252, 1255, 195 USPQ 430, 433 (CCPA 1977). Furthermore, Li et al. also shows the gallium acetylacetonate presents in the absorber in different shadings (see HRTEM images in figs. 2d-f), or in a concentrating gradient.
Claim(s) 12, 14, 16, 19 and 29 are rejected under 35 U.S.C. 103 as being unpatentable over Snaith et al. (WO 2020/109787) in view of Li et al. (“In situ induced core/shell stabilized hybrid perovskites via gallium (III) acetylacetonate intermediate towards highly efficient and stable solar cells”).
Regarding claims 12, 14 and 16, Snaith et al. discloses method of making a photovoltaic device (see pages 78-79, claims 32-50 and also see pages 54-77) comprising:
depositing a first charge transport layer (NiO) over a first contact layer (FTO-coated glass, see page 78);
applying a precursor solution (or perovskite precursor solution) to a surface of a first charge transport layer (NiO) resulting in a liquid layer of the precursor solution on the surface of the first charge transport layer (see page 79), wherein the precursor solution comprises a perovskite precursor comprising formamidinium iodide (FAI), cesium iodide (CsI), lead bromide (PbBr2), and lead iodide (PbI2), an additive (or ionic liquid such as BMIMBF4), and a solvent (DMF/DMSO, see paragraph bridging pages 78 and 79);
treating the liquid layer to remove at least a portion of the solvent (see annealing step on pre-heated hot plate described in page 79; also see page 63), thereby forming an absorber layer comprising a solid perovskite material (or crystalline A/M/X, see the entire document of Snaith et al., and more specifically claims 320), and crystalline perovskite material is solid.
Snaith et al. teaches using the precursor to form a perovskite material of (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 in the example described in the paragraph bridging pages 78 and 79, or the perovskite having 10% atomic percent of bromine in the halides.
Snaith et al. teaches the does not teach forming a perovskite material having an atomic percent of bromine in the halides in the range of 5.0% to 9.0% as claimed in claim 12, 6.0% to 8.0% as claimed in claim 1in the example described in the paragraph bridging pages 78 and 79.
However, Snaith et al. teaches the atomic percent (y) of bromine (Br) in the halides in the perovskite material (or A/M/X material) of APb[BryI1-y]3 to be greater than 0 and less than 1, or 0.01 to 0.99 or from 1% to 99% (see page 42).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method in the example (described in paragraph bridging pages 78-79) by forming the perovskite material having atomic percent of bromine in the halides in the perovskite material selectively to be 5.0% to 9.0% or 6.0% to 8.0% in the range of greater than 0 and less than 1, or 0.01 to 0.99 or from 1% to 99% described in page 42, because Snaith et al. explicitly suggests doing so and selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Snaith et al. discloses using BMIMBF4 in the example. Snaith et al. does not teaches using additives as claimed in claim 12.
Li et al. teaches using gallium (III) acetylacetonate (GaAA3 or Ga(AcAc)3) to protect the perovskite against water ingress from ambient atmosphere and passivate its defect states, and thereby enhance the long-term stability while maintaining high PCE (see abstract, “Broader context” and conclusion).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified by incorporating an additive of gallium (III) acetylacetonate (GaAA3 or Ga(AcAc)3) to the perovskite precursor solution to protect the perovskite against water ingress from ambient atmosphere and passivate its defect states, and thereby enhance the long-term stability while maintaining high PCE as taught by Li et al.
Regarding claim 19, modified Snaith et al. discloses a method as in claim 12 above, wherein Snaith et al. discloses forming (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 in the method described in pages 78 and 79, the additive comprises BMIM:BF4 (see claim 12 above or pages 78-79 of Snaith et al.), and the first charge transport layer (NiO) is a hole transport layer (or p-type, see pages 78-79). (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 has a composition of Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3 with x is 0.17, y is 0.83, and x+y is 0.95. 0.17 is right within the range of greater than 0 and less than 1, 0.83 is right within the range of greater than 0 and less than 1, and 0.95 is right within the claimed range of less than 1.
Snaith et al. also teaches the atomic percent (y) of bromine (Br) in the perovskite material (or A/M/X material) of APb[BryI1-y]3 to be 0.01 to 0.99 (see page 42).
Snaith discloses the perovskite obtained from the method in pages 78-79 having the atomic percent (z) of the bromine (Br) is 0.1, but does not disclose the perovskite obtained from the method in pages 78-79 having the atomic percent (z) of the bromine (Br) to be in the range of greater than 0.06 and less than 0.09.
However, it would have been obvious to it would have been obvious to one skilled in the art to modify the method of Snaith et al. in pages 78-79 by forming a perovskite material of the absorber layer has a halide (or Br) atomic percent selected to be 6.0% (or 0.06) to 9.0% (or 0.09) in the range 0.0.1 to 0.99 disclosed by Snaith et al., because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Regarding claim 29, Snaith et al. discloses a method as in claim 12 above, and discloses the perovskite composition is (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 or Cs0.05MA0.1445 FA0.7885Pb(I0.9Br0.1)3 which is approximately equal (or close enough) to Cs0.05MA0.08FA0.87Pb(I0.92Br0.08)3 .
Snaith et al. does not disclose obtaining the exact composition Cs0.05MA0.08FA0.87Pb(I0.92Br0.08)3 with the atomic percent of bromine to be 0.08 and the atomic percent of and the MA to be 0.08, or (FA0.9158MA0.0842)0.95Cs0.05Pb(I0.92Br0.08)3 in the method described in pages 78-79.
However, Snaith et al. discloses the atomic percent (y) of bromine (Br) in the perovskite material (or A/M/X material) of APb[BryI1-y]3 to be 0.01 to 0.99 (see page 42) and the combining of MA (CH3NH3+) and FA (H2N-C(H)=NH2+) has a combination of formula (CH3NH3)x(H2N-C(H)-NH2)1-x with x being from 0.01 to 0.99 or from 0.05 to 0.95 or 0.1 to 0.9 (see paragraph bridging pages 41-42).
Therefore, it would have been obvious to one skilled in the art to have used the method disclosed in pages 78-29 to form the perovskite having formula (FA0.9158MA0.0842)0.95Cs0.05Pb(I0.92Br0.08)3 with the atomic percent (y) of bromine of 0.08 to be selected in the ranges 0.01 to 0.99 disclosed by Snaith et al., and the atomic percent of MA of 0.0842 to be selected in the ranges 0.01 to 0.99 or from 0.05 to 0.95 or 0.1 to 0.9 disclosed by Snaith et al., because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Claim(s) 13 is rejected under 35 U.S.C. 103 as being unpatentable over modified Li et al. (“In situ induced core/shell stabilized hybrid perovskites via gallium (III) acetylacetonate intermediate towards highly efficient and stable solar cells”) or modified Snaith et al. (WO 2020/109787) as applied to claim 12 above, and further in view of Jung et al. (US 20180075979).
Regarding claim 13, modified Li et al. or modified Snaith et al. discloses a method as in claim 12 above.
Modified Li et al. nor modified Snaith et al. does not disclose the step of treating the liquid layer (or the annealing step) comprises directing nitrogen gas to contact a surface of the liquid layer.
Jung et al. disclose annealing the perovskite solution including subjecting the perovskite material solution to blowing nitrogen or the like to complete drying of the solvent before the coating solution is repelled (see [0030] and [0050]). In other words, Jung et al. discloses the step of treating the liquid layer comprising directing nitrogen gas to contact a surface of the liquid layer, or subjecting the solution to blowing nitrogen.
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Li et al. by subjecting the liquid layer to blowing nitrogen, or directing nitrogen gas to contact a surface of the liquid layer, to complete drying of the solvent before the coating solution is repelled as taught by Jung et al.
Claim(s) 15 is rejected under 35 U.S.C. 103 as being unpatentable over modified Li et al. or modified Snaith et al. as applied to claim 12 above, and further in view of Zhou et al. (“Reduced defects and enhanced Vbi in perovskite absorbers through synergetic passivating effect using 4-methoxypheylacetic acid”).
Regarding claim 15, modified Li et al. or modified Snaith et al. discloses a method as in claim 12 above, wherein Li et al. teaches providing a second contact layer (Ag electrode) over the absorber layer (see “Solar cell fabrication” and using gallium acetylacetonate (Ga(AcAc)3) to passivate the surface of the perovskite material and protect the perovskite material for enhancing the long-term stability while maintaining high power conversion efficiency (see abstract-broader context and conclusion).
Modified Li et al. or modified Snaith et al. does not explicitly teach treating the absorber layer with a surface modifier comprising Ga(AcAc)3, or performing the passivating step after the step of forming an absorber layer comprising the perovskite material, and prior to providing the second contact layer.
Zhou et al. teaches treating or performing the passivating step after the step of forming an absorber layer comprising the solid perovskite material, and prior to providing the second contact layer (or Au top electrode, see “device fabrication” in the Supplementary Information).
However, it would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Li et al. or modified Snaith et al. by treating the perovskite absorber layer with a surface modifier of Ga(AcAc)3 to passivate and protect the perovskite absorber layer for enhancing the long-term stability while maintaining high power conversion efficiency, because Li et al. teaches using Ga(AcAc)3 to passivate and protect the surface of the perovskite material.
In addition, it would have been obvious to one skilled in the art to have performed the treating step after the step of forming an absorber layer comprising the solid perovskite material, and prior to providing the second contact layer as taught by Zhou et al.; because Li et al. teaches using Ga(AcAc)3 to passivate and protect the perovskite material and Zhou et al. teaches such treating would passivate the perovskite absorber layer to enhance the built-in potential to accelerate the separation of the photogenerated charges within perovskite absorbers to achieve a higher efficiency (see abstract, conclusion and table S1).
Claim(s) 17-18 are rejected under 35 U.S.C. 103 as being unpatentable over modified Li et al. or modified Snaith et al. as applied to claim 12 above, and further in view of Du et al. (“Polymer Surface Modification of NiOx-Based Inverted Planar Perovskite Solar Cells with Enhanced Performance”).
Regarding claims 17-18, modified Li et al. and modified Snaith et al. disclose a method as in claim 12 above.
Modified Li et al. nor modified Snaith et al. does not explicitly disclose the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer, wherein the second sublayer is adjacent to and in direct contact with both the absorber layer and the first sublayer as claimed in claim 17; nor do they teach the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer; the first sublayer comprises nickel oxide; the second sublayer comprises PTAA; and depositing the first charge transport layer comprises: forming a layer of nickel oxide over the first contact and forming a layer of PTAA over the layer of nickel oxide as claimed in claim 18.
Du et al. disclose a transport layer comprises a first sublayer (NiOx) and a second sublayer (PTAA) such that the second sublayer (PTAA) is adjacent to and in direct contact with both the absorber layer (PVK) and the first sublayer (NiOx, see NiOx/PTAA/PVK shown in fig. 1f, and described throughout the document, also see the Experimental section in page 16807) such that the nickel oxide layer is deposited on the first contact (or FTO-coated glass substrate) and the PTAA layer is deposited over the layer of nickel oxide (NiOx, see Experimental section in page 16807)
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Li et al. or modified Snaith et al. by forming the transport layer of bilayer of NiOx and PTAA, or adding PTAA layer on top of the NiOx layer of Li et al., as taught by Du et al.; because Du et al. teaches the bilayer of NiOx/PTAA would enhance the performance of the device (see abstract, figs. 5-6, table 1 and conclusion).
Claim(s) 20-21 rejected under 35 U.S.C. 103 as being unpatentable over Snaith et al. in view of as applied to claim 12 above, and further in view of Du et al. (“Polymer Surface Modification of NiOx-Based Inverted Planar Perovskite Solar Cells with Enhanced Performance”).
Regarding claim 20, Snaith et al. discloses method of making a photovoltaic device (see pages 78-79, claims 32-50 and also see pages 54-77) comprising:
depositing a first charge transport layer (NiO) over a first contact layer (FTO-coated glass, see page 78);
applying a precursor solution (or perovskite precursor solution) to a surface of a first charge transport layer (NiO) resulting in a liquid layer of the precursor solution on the surface of the first charge transport layer (see page 79), wherein the precursor solution comprises a perovskite precursor comprising formamidinium iodide (FAI), cesium iodide (CsI), lead bromide (PbBr2), and lead iodide (PbI2), an additive (or ionic liquid such as BMIMBF4), and a solvent (DMF/DMSO, see paragraph bridging pages 78 and 79);
treating the liquid layer to remove at least a portion of the solvent (see annealing step on pre-heated hot plate described in page 79; also see page 63), thereby forming an absorber layer comprising a solid perovskite material (or crystalline A/M/X, see the entire document of Snaith et al., and more specifically claims 320), and crystalline perovskite material is solid.
Snaith et al. teaches using the precursor to form a perovskite material of (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 in the example described in the paragraph bridging pages 78 and 79). Snaith et al. also teaches using perovskite having formula (ID, see page 42) and more specifically [(CH3NH3)x(H2N-C(H)=NH2)1-x]Pb[BryI1-y]3 – or MAxFA1-xPb(BryI1-y)3 with x and y are both greater than 0 and less than 1 or 0.01-0.99 or 0.05-0.95 (see page 43).
Snaith et al. does not explicitly discloses the perovskite having a composition Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3 with 0.02≤ x ≤0.08, 0.82≤ y ≤0.92, and 0.07≤ z ≤0.09.
However, it would have been obvious to one of ordinary skill in the art at the time of invention to used perovskite having formula MAxFA1-xPb(BryI1-y)3 with x and y are both greater than 0 and less than 1 or 0.01-0.99 or 0.05-0.95 for the method in the example, because Snaith et al. explicitly suggests doing so. In addition, it would have been obvious to one skilled in the art to have selected the overlapping portion of 0.08 in the ranges of greater than 0 and less than 1, 0.01-0.99 or 0.05-0.95 for x (or amount of MA) and 0.07-0.09 in the ranges greater than 0 and less than 1, 0.01-0.99 or 0.05-0.95 for y (or amount of Br) in the perovskite MAxFA1-xPb(BryI1-y)3 disclosed by Snaith et al., because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549. In such modification, the perovskite MAxFA1-xPb(BryI1-y)3 of Snaith et al. is MA0.08FA0.92Pb(BrzI1-z)3 with 0.07≤ z (or y of Snaith et al.) ≤0.09 that is read on the claimed perovskite having formula Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3 with x =0.08, y=0.92, and 0.07≤ z ≤0.09.
Snaith et al. teaches including one or more additional of charge transport layer between the electrode and charge transport layer (see page 33).
Snaith et al. does not explicitly disclose the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer, wherein the first sublayer comprises an inorganic hole transport material, the second sublayer comprises an organic hole transport material, the second sublayer is position between the absorber layer and the first layer and the second sublayer is adjacent to and in direct contact with both the absorber layer and the first sublayer.
Du et al. disclose a transport layer comprises a first sublayer of inorganic hole transport layer (NiOx) and a second sublayer of organic hole transport layer (PTAA) such that the second sublayer (PTAA) is adjacent to and in direct contact with both the absorber layer (PVK) and the first sublayer (NiOx, see NiOx/PTAA/PVK shown in fig. 1f, and described throughout the document, also see the Experimental section in page 16807).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Snaith et al. by forming the transport layer comprising a first sublayer of inorganic hole transport material of NiOx and the second sublayer of organic hole transport material of PTAA as taught by Du et al., because Snaith et al. explicitly suggest adding additional charge transport layer, and Du et al. teaches the bilayer of NiOx/PTAA would enhance the performance of the device (see abstract, figs. 5-6, table 1 and conclusion).
Regarding claim 21, modified Snaith et al. discloses a method as in claim 20 above, wherein the first sublayer is of nickel oxide (or NiOx) and the second sublayer is of PTAA (see claim 20 above). Snaith et al. discloses a charge transport layer having a thickness from 1 to 500nm, for instant from 5 to 250nm or from 10 to 75nm (see 4th paragraph of page 26 of Snaith et al.), wherein the range 10-75nm is right within the claimed range of 1.5nm to 100.0nm for the charge transport layer of NiO. Du et al. teaches the PTAA is very thin (see Experimental section of Du et al.).
Modified Snaith et al. does not explicitly disclose the second sublayer of charge transport layer of PTAA having a thickness in a range from 0.2 nm to 15.0 nm.
However, it would have been obvious to one of ordinary skill in the art at the time of invention to have selected the overlapping portions of 1-15nm in the range 1-500nm disclosed by Snaith et al., or 5-15nm in the range 5-250nm disclosed by Snaith et al., or 10-15nm in the range 10-75nm disclosed by Snaith et al., because Du et al. explicitly teaches the PTAA is very thin and selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Claim(s) 22, 27 and 28 are rejected under 35 U.S.C. 103 as being unpatentable over modified Snaith et al. as applied to claim 12 above, in view of Degani et al. (“23.7% Efficient inverted perovskite solar cells by dual interfacial modification).
Regarding claims 22 and 27-28, modified Snaith et al. discloses a method as in claim 12 above, wherein the additive is Ga(AcAc)3 (see claim 12 above).
Modified Snaith et al. does not disclose the additive comprises PEAI as claimed in claim 27, nor do they teach the additive comprises at least two of BMIM:BF4, TAH, CC, Ga(AcAc)3 Pb(SCN)2, OAM, PbCl2, D4TBP, PEAI, or 4F-PEAI as claimed in claim 28 such that the additive is present in the absorber layer with a concentration gradient as claimed in claim 22.
Degani et al. discloses adding PEAI such as PEAI or 4F-PEAI in addition to an ionic liquid ([BMP]+[BF4]-) (see fig. 1B and “perovskite film preparation and device fabrication”) to improve both open-circuit voltage and fill factor thereby improving the device efficiency (see abstract, table 1).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by further incorporating PEAI in addition to the Ga(AcAc)3 to improve the efficiency of the device as taught by Degani et al.. In such modification, the additive comprises Ga(AcAc)3 and PEAI or Ga(AcAc)3 and 4F-PEAI and the additive of PEAI is present in the absorber layer with a concentration gradient as it is added late (or no or little PEAI in the early formed portion of the absorbing layer and substantial in the later formed portion of the absorbing layer).
Claim 30 is rejected under 35 U.S.C. 103 as being unpatentable over modified Li et al. or modified Snaith et al. as applied to claim 12 above, in view of Zheng et al. (“Defect passivation in hybrid perovskite solar cells using quarternary ammonium halide anions and cations”)
Regarding claim 30, modified Li et al. or modified Snaith et al. discloses a method as in claim 12 above, wherein Li et al. discloses the additive comprises Ga(AcAc)3 (see claim 12 above). Li et al. teaches passivating the perovskite would effectively protect the perovskite and passivate the defect states of the perovskite thereby enhance the long-term stability while maintain high power conversion efficiency (see abstract – broader context and conclusion of Li et al.)
Li et al. does not teach the additive comprises at least two of TAH, CC, Ga(AcAc)3 or D4TBP.
Zheng et al. teaches passivating the perovskite with choline chloride (CC) to effectively passivate the perovskite to further improve both the efficiency and stability of solar cells (see abstract, table 1, and conclusion).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Li et al. or modified Snaith et al. by incorporating CC as taught by Zheng et al. in addition to gallium acetylacetonate (Ga(AcAc)3) such that the additive comprises Ga(AcAc)3 and CC, because Zheng et al. teaches including choline chloride (CC) would further improve both the efficiency and stability of solar cells. Furthermore, one of ordinary skill in the art at the time the invention was made would have been led by the applied references to forgo use of separate additive materials and to combine them into a single additive, along with their function and benefit, where doing so is technically feasible. See In re Thompson, 545 F.2d 1290, 1229, 188 USPQ 365, 367 (CCPA 1976).
Response to Arguments
Applicant’s arguments with respect to claim(s) 12-22 and 27-30 have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
Applicant argues previous cited references do not teach the claimed method. However, Applicant’s arguments are moot in view of the new ground of rejection. See the rejection above.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to THANH-TRUC TRINH whose telephone number is (571)272-6594. The examiner can normally be reached 9:00am - 6:00pm.
Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Jeffrey T. Barton can be reached on 5712721307. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, visit: https://patentcenter.uspto.gov. Visit https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
THANH-TRUC TRINH
Primary Examiner
Art Unit 1726
/THANH TRUC TRINH/Primary Examiner, Art Unit 1726