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 .
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 1-28 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.
Regarding Claim 1, Applicant recites, “wherein the perovskite material comprises three or more different cations in addition to the B cation(s)”. Its unclear if the recitation of “B cation(s)” corresponds to the divalent metal cation or a different plurality of B cations. Its also unclear if there is a singular cation or multiple cations present. Appropriate action is required.
Regarding Claim 1, Applicant recites, “wherein the perovskite material comprises three or more different cations in addition to the B cation(s)”. Its unclear if the three or more different cations in addition to the B cation(s) is corresponding to the cations already recited or if these are additional cations. Appropriate action is required.
Regarding Claim 6, Applicant recites, “three or more different monovalent cations”. Its unclear if this recitation also includes the cations already recited in preceding Claim 1. Appropriate action is required.
Regarding Claim 7, Applicant recites, “which comprises 3 or 4 evaporation sources”. Its unclear if this recitation also includes the evaporation sources already recited in preceding claim 1 or if this is in addition to those evaporation sources. Appropriate action is required.
Regarding Claim 10, Applicant recites, “a preceding step of forming a compound of formula (I) B(XyX’1-y)2”. Its unclear if these corresponds to the same compound already recited in preceding claim 1 or is further limiting how this compound is being formed. Appropriate action is required.
Regarding Claim 11, Applicant recites, “such that formula (I) is BxB’1-x(XyX’1-y)2”. In preceding claim 1, B is associated to be equal to one and a divalent metal cation. Its unclear how B already limited is now two separate cations with ratios outside of B’s original value. Appropriate action is required.
Regarding Claim 12, Applicant recites, “which comprises a step (iv)”. Step (iv) has already been positively recited in preceding claim 1, thus its unclear if this claim is further limiting step (iv) or if this is a different distinct inorganic halide than what was introduced in claim 1. Appropriate action is required.
Regarding Claim 13, Applicant recites, “which comprises 4 evaporation sources”. Its unclear if this recitation also includes the evaporation sources already recited in preceding claim 1 or if this is in addition to those evaporation sources. Appropriate action is required.
Regarding Claim 13, Applicant recites, “and in step (iii) an organic halide is provided in a third evaporation source”. Its unclear if this organic halide in a third evaporation source is the same or different than the one or more further organic halides from one or more further evaporation sources already recited in preceding claim 1 in step (iii). Appropriate action is required.
Regarding Claim 14, Applicant recites, “to give the single precursor phase Pb(IyBr1-y)z”. Its unclear if this passage is further limiting formula 1 in claim 1 step (ii) or if a different precursor is being introduced. Appropriate action is required.
Regarding Claim 15, Applicant recites, “which comprises 4 evaporation sources”. Its unclear if this recitation also includes the evaporation sources already recited in preceding claim 1 or if this is in addition to those evaporation sources. Appropriate action is required.
Regarding Claim 15, Applicant recites, “such that only one halide component”. Its unclear if this passage is further limiting the one or more metal halides reciting in step (ii) or claim 1 or limiting the entirety of the perovskite material which lends ambiguity as claim 1 recites that step (i) comprises organic halides. Appropriate action is required.
Regarding Claim 15, Applicant recites, “and in step (iii) an organic halide is provided in a third evaporation source”. Its unclear if this organic halide in a third evaporation source is the same or different than the one or more further organic halides from one or more further evaporation sources already recited in preceding claim 1 in step (iii). Appropriate action is required.
Regarding Claim 16, Applicant recites, “which comprises 4 evaporation sources”. Its unclear if this recitation also includes the evaporation sources already recited in preceding claim 1 or if this is in addition to those evaporation sources. Appropriate action is required.
Regarding Claim 16, Applicant recites, “such that only one halide component”. Its unclear if this passage is further limiting the one or more metal halides reciting in step (ii) or claim 1 or limiting the entirety of the perovskite material which lends ambiguity as claim 1 recites that step (i) comprises organic halides. Appropriate action is required.
Regarding Claim 16, Applicant recites, “and in step (iii) an organic halide is provided in a third evaporation source”. Its unclear if this organic halide in a third evaporation source is the same or different than the one or more further organic halides from one or more further evaporation sources already recited in preceding claim 1 in step (iii). Appropriate action is required.
Regarding Claim 16, Applicant recites, “the two inorganic halides”. This phrase lacks antecedent basis. Its unclear if this passage is further limiting the one or more inorganic halides or if different organic halides are being introduced. Appropriate action is required.
Regarding Claim 22, Applicant recites, “and wherein the one or more inorganic halides, when present”. Its unclear if the one or more inorganic halides are present or not. Appropriate action is required.
Regarding Claim 23, Applicant recites, “FA”, “EA”, “MA”, “GA”, “DMA”, “BzA”, “Ac”, “Bz”, “IM”, “PEA”. Its unclear what these acronyms correspond to. Appropriate action is required.
Regarding Claim 25, Applicant recites, “MA” and “FA”. Its unclear what these acronyms correspond to. Appropriate action is required.
Regarding Claim 26, Applicant recites, “GA”. Its unclear what this acronym corresponds to. Appropriate action is required.
Regarding Claim 27, Applicant recites, “which comprises a step (iv)”. Step (iv) has already been positively recited in preceding claim 1, thus its unclear if this claim is further limiting step (iv) or if this is a different distinct inorganic halide than what was introduced in claim 1. Appropriate action is required.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
Claims 1, 3-10, 12, 15, 17, 20-22, 24-25, and 27 are rejected under 35 U.S.C. 103 as being unpatentable over Zhu et al. (US 2020/0239499 A1) in view of Qi et al. (US 2017/0226641 A1).
In view of Claim 1, Zhu et al. discloses a method of forming perovskite material from a plurality of evaporation sources comprising co-subliming (Fig. 2, #212-#216 are a plurality of evaporation sources co-sublimed to produce a final perovskite material – Paragraph 0057);
a first source comprising a mixture of organic halides wherein the organic halides comprises:
a first organic halide comprising a first organic cation A (Paragraph 0053 – first precursor AX – Paragraph 0006 can be methylammonium);
a second organic halide comprising an organic cation A’ which is different to the first organic cation A and has a larger ionic radius that the first organic cation A (Paragraph 0053 – second precursor A’X – Paragraph 0006 can be formamidinium which has a larger ionic radius than methylammonium);
a second source comping one or more metal halides having the formula BX2 (Paragraph 0005 & 0053 – fourth precursor BX2);
wherein B is a divalent metal cation and X is a halide when y = 0 (Paragraph 0057);
one or more further organic halides from one or more further sources (Paragraph 0005 & 0053 – third precursor A’’X);
one or more inorganic halides from one or more further sources (Paragraph 0005, 0007 & 0053 – B’X2 – fifth precursor);
to form the perovskite material, wherein the perovskite material comprises three or more different cations in addition to the B cations (Paragraph 0053 – AxA’yA’’(1-x-y)B(XaX’bX’’(1-a-b))3, where x, y, a, and be are each greater than or equal to zero and less than or equal to one).
Zhu et al. does not disclose that these precursor materials are in the form of evaporation sources wherein the sources are co-sublimed together to form the perovskite material.
Qi et al. discloses that precursor materials identical to Zhu et al. precursor materials, such as the AX form (Paragraph 0054 – MACl, MABr, MAI, FACl, FABR, FAI and the like) and the BX2 form (Paragraph 0029) can be deposited in the form of evaporation units coupled to side sections of a chamber, one source can be configured to evaporate a MACl vapor and another can deposit a FABr vapor, indicating multiple sources of AX can be co-sublimably deposited via one or more evaporation sources (Fig. 2, #216 & Paragraph 0031), while also disclosing multiple sources of BX2 can be co-sublimably deposited via one or more evaporation sources (Fig. 2, #220 & Paragraph 0032, 0040 & 0046 – SN evaporation units). Qi et al. teaches that this method of depositing perovskite material effectuates a substantially uniform chemical reaction on a large area of a substrate surface, which results in large-scale uniform perovskite films with high crystallinity (Paragraph 0040) and that the present system can be configured for bandgap engineering such as mixed-halide perovskites and that implementation of multiple sources and independent control of a wide variety of growth parameters, offers suitable means for bandgap engineering such as in situ tuning, precise thickness control and concentration profile design and so no (Paragraph 0060). Accordingly, it would have been obvious to one of ordinary skill in the art at the time the invention was filed to use Qi et al. method of depositing perovskite material via precursors that are in the form of evaporation sources as Zhu et al. deposition method for the advantage of utilizing a method that results in large-scale uniform perovskite films with high crystallinity while also offering in situ tuning, precise thickness control and concentration profile design.
In view of Claim 3, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. discloses that the halides in the organic and inorganic halides are selected from iodine and bromine (Paragraph 0007).
In view of Claim 4, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that the one or more further organic halides in step (iii) can be different than the first organic halide (Paragraph 0005 & 0053 – third precursor A’’X).
In view of Claim 5, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 5. Zhu et al. teaches that the perovskite material comprises a mixed halide (Paragraph 0053 – AxA’yA’’(1-x-y)B(XaX’bX’’(1-a-b))3, where x, y, a, and be are each greater than or equal to zero and less than or equal to one).
In view of Claim 6, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that the perovskite material comprises three or more different monovalent cations (Paragraph 0053 – AxA’yA’’(1-x-y)B(XaX’bX’’(1-a-b))3, where x, y, a, and be are each greater than or equal to zero and less than or equal to on – Paragraph 0006 – A, A’, A’’ are selected from methylammonium, formamidinium, ethylammonium, butylammonium).
In view of Claim 7, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that the method comprises three or four sources (See above rejection of claim 1). While Qi et al. was relied upon to disclose that it would be obvious that the sources are in the form of evaporated sources.
In view of Claim 8, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that the first organic halide comprises an organic cation A which is a monovalent organic cation (Paragraph 0006 – A, A’, A’’ are selected from methylammonium, formamidinium, ethylammonium, butylammonium).
In view of Claim 9, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that the A’ is selected from ethylammonium (Paragraph 0006 – A, A’, A’’ are selected from methylammonium, formamidinium, ethylammonium, butylammonium).
In view of Claim 10, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Qi et al. discloses that BX2 sources are heated prior to deposition in an inert chamber (Paragraph 0065).
In view of Claim 12, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches that step (iv) comprise an inorganic halide that’s Vs based (Paragraph 0003).
In view of Claim 15, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. discloses that the method can comprise four sources (See above rejection of claim 1), and that an organic halide is provided as the third source and an inorganic halide is provided as a fourth source (Paragraph 0005, 0007 & 0053). Zhu et al. teaches that y=0 such that only halide can be provided in the perovskite material (Paragraph 0057).
In view of Claim 17, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. discloses a thin film of perovskite material (Paragraph 0065).
In view of Claim 20, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. discloses that the method is directed towards multi-junction photovoltaic devices comprising two or more sub-cells comprising a photovoltaic device wherein the photovoltaic device comprises a photoactive region comprising a perovskite material and further sub-cells that comprise photoactive regions (Paragraph 0069). Qi et al. was relied upon to disclose that the precursors Zhu et al. utilizes can be used in evaporated form. Qi et al. discloses that the evaporated sources can also be used to construct multi-junction photovoltaic cells (Paragraph 0005).
In view of Claim 21, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Zhu et al. teaches a perovskite material (Paragraph 0065).
In view of Claim 22, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 21. Zhu et al. teaches that B is selected from Pb and Sn (Paragraph 0007) and that the one or more further organic halides are different that the first organic halide (Paragraph 0005, 0007 & 0053) and the one or more inorganic halides can be Cs (Paragraph 0003).
In view of Claim 24, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 21. Zhu et al. teaches a semiconductor device comprising a perovskite material as claimed in claim 21 (Paragraph 0065 & 0069).
In view of Claim 25, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 8. Zhu et al. teaches that the first organic halide can comprise an organic cation A which is MA or FA (Paragraph 0048).
In view of Claim 27, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 12. Zhu et al. teaches that the inorganic halide is CsI (Paragraph 0057).
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Zhu et al. (US 2020/0239499 A1) in view of Qi et al. (US 2017/0226641 A1) in view of Alberti et al. (US 2024/0117524 A1).
In view of Claim 2, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 1. Modified Zhu et al. does not disclose that the precursors in the first and second evaporation sources are congruently or non-congruently sublimed, wherein the different in sublimation temperatures of the precursors for congruent sublimation is up to 20 °C and the difference in sublimation temperatures of the precursors for non-congruent sublimation is between 50-150 °C.
Alberti et al. teaches that MAI and PbI2 (precursors used in modified Zhu et al.) can be congruently deposited via sublimation together within 20 °C and that this temperature is required for sublimation of the precursor (Paragraph 0125). Accordingly, it would have been obvious to one of ordinary skill in the art have the precursor temps that are congruent sublimed being substantially the same (thus within up to 20 °C) as this is a required temperature for sublimation.
Claim 26 is rejected under 35 U.S.C. 103 as being unpatentable over Zhu et al. (US 2020/0239499 A1) in view of Qi et al. (US 2017/0226641 A1) in view of Leitjens et al. (US 2020/0148711 A1).
In view of Claim 26, Zhu et al. and Qi et al. are relied upon for the reasons given above in addressing Claim 9. Modified Zhu et al. does not disclose that the second organic halide comprises an organic monocation A’ which is GA.
Leitjens et al. discloses that an “A” cation can be selected from GA as well as any of the cations disclosed by Zhu (Paragraph 0079 – GA, MA, FA etc. are listed as suitable cations in the organic cation position). Leitjens et al. discloses that guanidium can be used to increase the band gap of the perovskite material (Paragraph 0092). Accordingly, it would have been obvious to one of ordinary skill in the art at the time the invention was filed to incorporate guanidium as the A cation in modified Zhu et al. for the advantage of being able to increase the band gap of the perovskite material. Additionally, the substituted component GA, MA, FA, and their functions are known in the art and one of ordinary skill in the art could have substituted one known element for another and the results of the substitution would have been predictable. See MPEP 2143, I, B.
Allowable Subject Matter
Claims 11, 13-14, 16, and 18 would be allowable if rewritten to overcome the rejection(s) under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), 2nd paragraph, set forth in this Office action and to include all of the limitations of the base claim and any intervening claims.
Claims 23 and 28 would be allowable if rewritten or amended to overcome the rejection(s) under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), 2nd paragraph, set forth in this Office action.
Conclusion
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/DANIEL P MALLEY JR./Primary Examiner, Art Unit 1726