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 .
Information Disclosure Statement
The information disclosure statement (IDS) submitted on May 15, 2026, was filed after the mailing date of the non-final Office Action on February 19, 2026. The submission is in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statement is being considered by the examiner.
Specification
The objections to the specification are withdrawn in view of applicants’ amendments to the specification.
Claim Objections
Claim 1 is objected to because of the following informalities:
The status identifier for claim 1 indicates it is “(Currently Amended),” but there do not appear to be any actual claim amendments. As such, it should have been identified as “(Previously Presented).”
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The 35 U.S.C. 112(b) rejection of claims 11, 13, and 19 is withdrawn in view of applicants’ claim amendments.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 1-14 and 17-22 is/are rejected under 35 U.S.C. 103 as being unpatentable over U.S. Patent Appl. Publ. No. 2017/0229647 to Qi, et al. (hereinafter “Qi”) in view of U.S. Patent No. 6,117,498 to Chondroudis, et al. (“Chondroudis”) and further in view of U.S. Patent Appl. Publ. No. 2020/0328077 to Bush, et al. (“Bush”).
Regarding claim 1, Qi teaches a method of deposition of at least one layer of at least one precursor of Perovskite on at least one substrate, through use of at least one deposition chamber (see the Abstract, Figs. 1-18, and entire reference which teach a method of depositing a perovskite thin film onto a substrate (116) located within a housing (100)), wherein:
in said at least one deposition chamber at least one inlet mouth and at least one outlet mouth are obtained, configured to be selectively opened-closed so as to allow the entrance-exit of at least one process control gas in-out of said at least one deposition chamber (see Fig. 1 and ¶[0030] which teach that the housing (100) includes an outlet attached to a gate valve (108) and a pumping unit (104) as well as Figs. 11A-D and ¶¶[0050]-[0052] which teach that the housing (100) or (1100) is connected to a load-lock chamber (1160) via an inlet in the form of gate valve (1172) in order to facilitate insertion and removal of the substrate; furthermore, gate valves (1172) and (108) control the entrance and exit of gases to and from the housing (100) which necessarily permits one or more gases that may be broadly considered as process gases to enter the housing (100) when gate valve (1172) is opened);
said at least one deposition chamber at said at least one outlet mouth thereof, is operatively connected to at least one vacuum pump (see Fig. 1 and ¶[0030] which teach that the housing (100) is attached to a pumping unit (104) via the gate valve (108));
said at least one deposition chamber houses at least one source, said at least one source being configured to receive at least one precursor of said Perovskite without using a carrier gas, and said at least one source having at least one delivery mouth, configured to let one gas of said at least one precursor of said Perovskite, when it is sublimated into said source, pass directly from said at least one source, into said at least one deposition chamber without using a carrier gas (see Fig. 1 and ¶[0030] which teach that a first evaporator unit (120) having a delivery mouth is provided in a bottom section of the housing (100) to generate a vapor of the metal halide material BX2 without the use of a carrier gas); and
said at least one deposition chamber houses at least one supporting device for said at least one substrate, said supporting device being configured to support said substrate between at least one working position, wherein said at least one substrate is aligned with said at least one delivery mouth of said at least one source, at a preset deposition distance dw therefrom, and one resting position, wherein it is spaced apart from said at least one delivery mouth of said at least one source, at a distance greater than said preset deposition distance dw (see Fig. 1 and ¶[0030] which teach that a substrate stage (112) for supporting a substrate (116) a predetermined distance from the first evaporator unit (120) is provided in the housing (100); see also Figs. 11-12 and ¶¶[0050]-[0053] which teach that the substrate (116) is transferred from the housing (100) or (1100) to the load lock (1160) via a transfer system (1180) which necessarily means that the stage (112) is able to be raised to a second position which is a greater distance from the first evaporator unit (120) or, alternatively, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to move the stage (112) to a second position which is a greater distance from the evaporator unit (120) in order to facilitate transfer of the substrate (116) and permit uninterrupted movement of the transfer rod (1185) towards the load lock (1160)); and
wherein said at least one substrate is supported in said at least one deposition chamber and said at least one precursor of said Perovskite is charged into said at least one source of said at least one deposition chamber without using a carrier gas (see Fig. 1 and ¶[0030] which teach that the substrate (116) is supported in the housing (100) and a BX2 precursor is charged into the first evaporator unit (120) without using a carrier gas);
said method comprising the following operational steps in sequence (see Fig. 9 and ¶¶[0042]-[0049] which teach a process for depositing a perovskite thin film):
A. reducing pressure into said at least one deposition chamber, through activation of said vacuum pump, until one pressure value Pc comprised within a preset operational pressure interval DPc is obtained, into said at least one deposition chamber (see Fig. 1, ¶[0030], and ¶[0042] which teach that the housing (100) is pumped down to a base pressure from 105 to 10-7 Pa);
B. sublimating said at least one precursor in said at least one source, until one gas of said at least one sublimated precursor is obtained (see Fig. 9, ¶¶[0042]-[0049], and step (916) which teach heating the first evaporator unit (120) to sublimate the BX2 precursor);
C. if not yet in said working position, bringing said at least one substrate in said working position and said at least one substrate to one preset working temperature Tw (see Fig. 1 and ¶[0030] as well as Figs. 11A-D and ¶¶[0050]-[0053] which teach that the substrate stage (112) is brought into a position for film growth; see also Fig. 9, ¶¶[0042]-[0049], and step (916) which teach that the substrate stage is heated to a predetermined temperature);
D. depositing said at least one gas of said at least one precursor thereby sublimated, said gas exiting said at least one source through said at least one delivery mouth, directly on said substrate without using a carrier gas (see Fig. 9, ¶¶[0042]-[0049], and steps (928), (932), and (936) which teach that the first shutter (136) is moved to expose the substrate and deposit the BX2 precursor onto the substrate (116) without using a carrier gas); and
E. cooling said at least one source (see Fig. 9, ¶¶[0042]-[0049], and step (940) which teaches stopping heating of the first evaporator unit (120) which necessarily causes it to cool);
wherein said preset operational pressure interval DPc is between 0.1x10⁻³ mbar and 100x10⁻³ mbar, optionally between 1x10⁻² mbar and 5x10⁻² mbar, more optionally between 2x10⁻² mbar and 4x10-2 mbar (see Fig. 1, ¶[0030], and ¶[0042] which teach that the pressure in the housing (100) is in from 105 to 10-7 Pa during film growth).
Even if it is assumed arguendo that Qi does not teach an inlet mouth configured to be selectively opened-closed so as to allow the entrance of at least one process control gas, this would have been obvious in view of the teachings of Chondroudis. In at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of inert gas through the housing (100) and then out through the gate valve (108) and pump unit (104) prior to or during pump-down in the system and method of Qi and Bush in order to purge the housing (100) and maintain an inert environment suitable for the growth of a higher quality perovskite layer with a reduced quantity of contaminants.
Qi and Chondroudis do not teach that the preset deposition distance dw is between 0.5 cm and 5 cm, optionally between 1 cm and 3 cm, more optionally comprised between 1.5 cm and 2.5 cm. However, in Figs. 2-5, ¶¶[0036]-[0044], and ¶¶[0053]-[0096] as well as elsewhere throughout the entire reference Bush teaches an analogous system and method for delivering one or more precursors to a deposition chamber (130) from a vaporizer source (150) or (250). As explained specifically in ¶[0042]-[0043] and ¶[0096] Bush teaches that depending on the substrate temperature and the pressure utilized during film growth the vapor source exit to substrate (140) distance should be < 4 cm in order to facilitate laminar flow, increase materials utilization, and to minimize rapid cooling of the vapor exiting the outlet due to interaction with cooler gas molecules. Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to utilize a source-to-substrate deposition distance of 4 cm or less which is squarely within the claimed range of 0.5 to 5 cm in order to facilitate laminar flow, increase materials utilization, and minimize rapid cooling of the precursor vapors during film growth. The combination of prior art elements according to known methods to yield predictable results has been held to support a prima facie determination of obviousness. All the claimed elements are known in the prior art and one skilled in the art could combine the elements as claimed by known methods with no change in their respective functions, with the combination yielding nothing more than predictable results to one of ordinary skill in the art. KSR International Co. v. Teleflex Inc., 550 U.S. 398, __, 82 USPQ2d 1385, 1395 (2007). See also, MPEP 2143(A).
Regarding claim 2, Qi teaches that said at least one delivery mouth is configured to be selectively opened-closed, wherein said step A occurs with said at least one delivery mouth closed and wherein said step D occurs with said at least one delivery mouth open (see Figs. 1 & 3, ¶[0036], step (908) in Fig. 4, and ¶[0043] which teach that a second shutter (140) is positioned over the mouth of the first evaporator unit (120) during pump-down and the shutter (140) is removed during film growth such that the mouth of the first evaporator unit (120) is open).
Regarding claim 3, Qi and Bush do not teach that said step A further comprises feeding at least said process control gas into said at least one deposition chamber through said at least one inlet mouth. However, in at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of inert gas through the housing (100) and then out through the gate valve (108) and pump unit (104) prior to or during pump-down in the system and method of Qi and Bush in order to purge the housing (100) and maintain an inert environment suitable for the growth of a higher quality perovskite layer with a reduced quantity of contaminants.
Regarding claim 4, Qi and Chondroudis teach that said at least one pressure value Pc within said preset operational pressure interval DPc, in said at least one deposition chamber is obtained at said step A by one or more between: adjusting one feeding flux of said at least one process control gas into said at least one deposition chamber through a constant feeding flux of said at least one process control gas into said at least one deposition chamber, adjusting of one flow rate of at least one valve, through which said at least one deposition chamber is operatively connected with said at least one vacuum pump; through a constant feeding flux of said at least one process control gas into said at least one deposition chamber, adjusting suction speed of said at least one vacuum pump (see Fig. 1 and ¶[0030] of Qi which teach that the pressure within the housing (100) may be controlled by adjusting the position of the gate valve (108); see also col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 of Chondroudis which teach that the pressure within the growth chamber (1) may be controlled by the flow rate of an inert gas from an inlet (7) to an outlet (8)).
Regarding claim 5, Qi teaches comprising in said step B, one or more between:
heating up said at least one source to a source temperature Tₛ comprised between 70°C and 800°C, optionally between 80°C and 700°C, more optionally comprised between 100°C and 600°C (see ¶¶[0043]-[0044] which teach that the first evaporator unit (120) is heated to a first temperature in the range of 250 °C);
heating up at least one deposition chamber to a temperature comprised between 40°C and 120°C, optionally between 50°C and 100°C, more optionally between 60°C and 80°C (see ¶[0031] which teaches that the body of the housing (100) is heated to 70 °C).
Regarding claim 6, Qi teaches that in said step C said at least one substrate (4) is heated up to one working temperature Tw comprised between 30°C and 300°C, optionally comprised between 50°C and 200°C, more optionally comprised between 60°C and 150°C (see ¶[0043] and ¶[0056] which teaches that the substrate stage (112) and, hence, the substrate (116) is heated to a temperature of up to 200 °C).
Regarding claim 7, Qi teaches that wherein if in said step A said at least one substrate is in said working position, said method comprises cooling said at least one substrate, during said steps A and B, down to a temperature lower than one temperature that is required in said step B to sublimate said at least one precursor in said at least one source (see ¶[0043] and ¶[0056] which teaches that the substrate stage (112) and, hence, the substrate (116) is heated to a temperature of up to 200 °C and, in one embodiment, is cooled to room temperature (25 °C) during film growth, both of which are lower than the first temperature of 250 °C for the first evaporator unit as taught in ¶¶[0043]-[0044]).
Regarding claim 8, Qi teaches that before said step D there is a pressure difference DPsc between said at least one source and said at least one deposition chamber (see Fig. 1 and ¶[0043] which teach that the pressure within the housing (100) and, consequently, the pressure difference between the source and the housing (100) may be adjusted by changing the position of the gate valve (108) and the temperature of the first evaporator unit (120)), but does not explicitly teach that the pressure difference DPsc is equal to or greater than 1×10⁻² mbar. However, since ¶[0029] and ¶¶[0043]-[0044] of Qi teach that the first evaporator unit (120) is comprised of a metal halide BX2 heated to an overlapping first temperature in the range of 250 °C, ¶[0043] and ¶[0056] teach that the substrate (116) is heated to a temperature of up to 200 °C, ¶[0031] teaches that the body of the housing (100) is heated to 70 °C, and ¶[0030] and ¶[0042] teach that the pressure in the housing (100) is in from 105 to 10-7 Pa during film growth, Qi therefore utilizes the exact same process conditions as disclosed in the instant application which, consequently, must necessarily produce the same results, namely a pressure difference DPsc of equal to or greater than 1×10⁻² mbar as claimed. Alternatively, since the pressure difference DPsc between the source material within the first evaporator unit (120) and the chamber (100) is determined by, inter alia, the typer of source material utilized, the temperature of the first evaporator unit, the pumping speed of the pump (104) and the position of the gate valve (108), it is considered to be a result-effective variable, i.e., a variable which achieves a recognized result. See, e.g., In re Antonie, 559 F.2d 618, 195 USPQ 6 (CCPA 1977). See also MPEP 2144.05(II)(B). It therefore would have been within the capabilities of a person of ordinary skill in the art prior to the effective filing date of the invention to utilize routine experimentation to determine the optimal pressure difference DPsc between the source material within the first evaporator unit (120) and the chamber (100), including within the claimed range of equal to or greater than 1×10⁻² mbar necessary to produce the desired growth rate and materials properties of the resulting perovskite thin film.
Regarding claim 9, Qi does not teach that before said step A, said method comprises letting said at least one process control gas flow through said at least one deposition chamber, from said at least one inlet mouth thereof to said at least one outlet mouth thereof. However, as noted supra with respect to the rejection of claim 3, in at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of inert gas through the housing (100) and then out through the gate valve (108) and pump unit (104) prior to or during pump-down in the system and method of Qi and Bush in order to purge the housing (100) and maintain an inert environment suitable for the growth of a higher quality perovskite layer with a reduced quantity of contaminants.
Regarding claim 10, Qi teaches a method of deposition of at least one Perovskite layer on at least one substrate (see the Abstract, Figs. 1-18, and entire reference which teach a method of depositing a perovskite thin film onto a substrate (116) located within a housing (100)), comprising the following operational steps in sequence:
F. arranging at least one deposition chamber (see Fig. 1 and ¶[0030] which teach providing a housing (100)), wherein:
in said at least one deposition chamber at least one inlet mouth and at least one outlet mouth are obtained, configured to be selectively opened-closed so as to allow the entrance-exit of at least one process control gas in-out of said at least one deposition chamber (see Fig. 1 and ¶[0030] which teach that the housing (100) includes an outlet attached to a gate valve (108) and a pumping unit (104) as well as Figs. 11A-D and ¶¶[0050]-[0052] which teach that the housing (100) or (1100) is connected to a load-lock chamber (1160) via an inlet in the form of gate valve (1172) in order to facilitate insertion and removal of the substrate; furthermore, gate valves (1172) and (108) control the entrance and exit of gases to and from the housing (100) which necessarily permit one or more gases that may be broadly considered as process gases to enter the housing (100) when gate valve (1172) is opened);
said at least one deposition chamber at said at least one outlet mouth thereof, is operatively connected to one vacuum pump (see Fig. 1 and ¶[0030] which teach that the housing (100) is attached to a pumping unit (104) via the gate valve (108));
said at least one deposition chamber houses at least one source, said at least one source being configured to receive at least one precursor of said Perovskite without using a carrier gas and said at least one source having at least one delivery mouth, to let one gas of said at least one precursor of said Perovskite, when it is sublimated into said source pass directly from said at least one source into said at least one deposition chamber without using a carrier gas (see Fig. 1 and ¶[0030] which teach that a first evaporator unit (120) having a delivery mouth is provided in a bottom section of the housing (100) to generate a vapor of the metal halide material BX2 without the use of a carrier gas); and
said at least one deposition chamber houses at least one supporting device for said at least one substrate, said supporting device being configured to support at least one substrate between at least one working position, wherein said at least one substrate is aligned with said at least one delivery mouth of said at least one source at a preset deposition distance dw therefrom, and one resting position, wherein it is spaced apart from said at least one delivery mouth, of said at least one source, at a distance greater than said preset deposition distance dw (see Fig. 1 and ¶[0030] which teach that a substrate stage (112) for supporting a substrate (116) a predetermined distance from the first evaporator unit (120) is provided in the housing (100); see also Figs. 11-12 and ¶¶[0050]-[0053] which teach that the substrate (116) is transferred from the housing (100) or (1100) to the load lock (1160) via a transfer system (1180) which necessarily means that the stage (112) is able to be raised to a second position which is a greater distance from the first evaporator unit (120) or, alternatively, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to move the stage (112) to a second position which is a greater distance from the evaporator unit (120) in order to facilitate transfer of the substrate (116) and permit uninterrupted movement of the transfer rod (1185) towards the load lock (1160)); and
wherein said substrate is supported in said at least one deposition chamber and said at least one precursor of said Perovskite is charged into said at least one source of said at least one deposition chamber without using a carrier gas (see Fig. 1 and ¶[0030] which teach that the substrate (116) is supported in the housing (100) and a BX2 precursor is charged into the first evaporator unit (120) without using a carrier gas);
G. depositing at least one layer of said at least one precursor of said Perovskite on said at least one substrate, through a method comprising the following operational steps in sequence (see Fig. 9 and ¶¶[0042]-[0049] which teach a process for depositing a layer of a perovskite thin film using a first evaporator unit (120)):
A. reducing pressure into said at least one deposition chamber, through activation of said vacuum pump, until one pressure value Pc comprised within a preset operational pressure interval Рc is obtained, into said at least one deposition chamber (see Fig. 1, ¶[0030], and ¶[0042] which teach that the housing (100) is pumped down to a base pressure from 105 to 10-7 Pa);
B. sublimating said at least one precursor in said at least one source, until one gas of said at least one sublimated precursor is obtained (see Fig. 9, ¶¶[0042]-[0049], and step (916) which teach heating the first evaporator unit (120) to sublimate the BX2 precursor);
C. if not yet in said working position, bringing said at least one substrate in said working position and said at least one substrate to one preset working temperature Tw (see Fig. 1 and ¶[0030] as well as Figs. 11A-D and ¶¶[0050]-[0053] which teach that the substrate stage (112) is brought into a position for film growth; see also Fig. 9, ¶¶[0042]-[0049], and step (916) which teach that the substrate stage is heated to a predetermined temperature);
D. depositing said at least one gas of said at least one precursor thereby sublimated, said gas exiting said at least one source through said at least one delivery mouth, directly on said substrate without using a carrier gas (see Fig. 9, ¶¶[0042]-[0049], and steps (928), (932), and (936) which teach that the first shutter (136) is moved to expose the substrate and deposit the BX2 precursor onto the substrate (116) without using a carrier gas); and
E. cooling said at least one source (see Fig. 9, ¶¶[0042]-[0049], and step (940) which teaches stopping heating of the first evaporator unit (120) which necessarily causes it to cool);
wherein said preset operational pressure interval DРc is between 0.1 x10³ mbar and 100x10³ mbar, optionally between 1x10² mbar and 5x10² mbar, more optionally between 2x10² mbar and 4x10² mbar wherein said preset operational pressure interval DPc is between 0.1x10⁻³ mbar and 100x10⁻³ mbar, optionally between 1x10⁻² mbar and 5x10⁻² mbar, more optionally between 2x10⁻² mbar and 4x10-2 mbar (see Fig. 1, ¶[0030], and ¶[0042] which teach that the pressure in the housing (100) is in from 105 to 10-7 Pa during film growth) and
H. depositing at least one layer of said at least another precursor of said Perovskite on said at least one substrate (see Fig. 9 and ¶¶[0042]-[0049] which teach a process for depositing a layer of a perovskite thin film using a second evaporator unit (124)), through said method comprising the following operational steps in sequence:
A. reducing pressure into said at least one deposition chamber, through activation of said vacuum pump, until one pressure value Pc comprised within a preset operational pressure interval Pc is obtained, into said at least one deposition chamber (see Fig. 1, ¶[0030], and ¶[0042] which teach that the housing (100) is pumped down to a base pressure from 105 to 10-7 Pa);
B. sublimating said at least another precursor, until one gas of said at least another sublimated precursor is obtained (see Figs. 1 & 9, ¶¶[0031]-[0034], ¶¶[0042]-[0049], and step (920) which teach heating the second evaporator unit (124) to sublimate an AX precursor);
C. if not yet in said working position, bringing said at least one substrate in said working position and said at least one substrate to one preset working temperature Tw (see Fig. 1 and ¶[0030] as well as Figs. 11A-D and ¶¶[0050]-[0053] which teach that the substrate stage (112) is brought into a position for film growth; see also Fig. 9, ¶¶[0042]-[0049], and step (916) which teach that the substrate stage is heated to a predetermined temperature);
D. depositing said at least one gas of said at least another precursor thereby sublimated, said gas forming directly on said substrate without using a carrier gas (see Figs. 1, 4A, & 9, ¶[0037], ¶¶[0042]-[0049], and steps (928), (932), and (936) which teach that the first shutter (136) and the shutter (420) covering the cell (404) which constitutes the second evaporator unit (124) is moved to expose the substrate and deposit the AX precursor onto the substrate (116) without using a carrier gas); and
E. cooling said at least one source (see Fig. 9, ¶¶[0042]-[0049], and step (940) which teaches stopping heating of the second evaporator unit (124) which necessarily causes it to cool);
wherein said preset operational pressure interval Pc is between 0.1 x10³ mbar and 100x10³ mbar, optionally between 1x10² mbar and 5x10² mbar, more optionally between 2x10² mbar and 4x10² mbar (see Fig. 1, ¶[0030], and ¶[0042] which teach that the pressure in the housing (100) is in from 105 to 10-7 Pa during film growth) and
I. if on said substrate, due to a chemical reaction between said at least one precursor and said at least another precursor of said Perovskite, the growth of said at least one layer of said Perovskite is obtained, interrupting the method; otherwise J. going back to step H (see Fig. 9 and ¶¶[0042]-[0049], and steps (936), (940), and (940) which teach that once a perovskite film of a predetermined thickness is attained, heating of the first and second evaporation units is stopped and the gate valve (108) is opened in order to pump out the remaining vapor in the housing (100)).
Even if it is assumed arguendo that Qi does not teach an inlet mouth configured to be selectively opened-closed so as to allow the entrance of at least one process control gas, this would have been obvious in view of the teachings of Chondroudis. In at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of inert gas through the housing (100) and then out through the gate valve (108) and pump unit (104) prior to or during pump-down in the system and method of Qi and Bush in order to purge the housing (100) and maintain an inert environment suitable for the growth of a higher quality perovskite layer with a reduced quantity of contaminants.
Qi and Chondroudis do not explicitly teach that the preset deposition distance dw is between 0.5 cm and 5 cm, optionally between 1 cm and 3 cm, more optionally comprised between 1.5 cm and 2.5 cm for each deposition sequence. However, in Figs. 2-5, ¶¶[0036]-[0044], and ¶¶[0053]-[0096] as well as elsewhere throughout the entire reference Bush teaches an analogous system and method for delivering one or more precursors to a deposition chamber (130) from a vaporizer source (150) or (250). As explained specifically in ¶[0042]-[0043] and ¶[0096] Bush teaches that depending on the substrate temperature and the pressure utilized during film growth the vapor source exit to substrate (140) distance should be < 4 cm in order to facilitate laminar flow, increase materials utilization, and to minimize rapid cooling of the vapor exiting the outlet due to interaction with cooler gas molecules. Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to utilize a source-to-substrate deposition distance of 4 cm or less which is squarely within the claimed range of 0.5 to 5 cm in order to facilitate laminar flow, increase materials utilization, and minimize rapid cooling of the precursor vapors during film growth. The combination of prior art elements according to known methods to yield predictable results has been held to support a prima facie determination of obviousness. All the claimed elements are known in the prior art and one skilled in the art could combine the elements as claimed by known methods with no change in their respective functions, with the combination yielding nothing more than predictable results to one of ordinary skill in the art. KSR International Co. v. Teleflex Inc., 550 U.S. 398, __, 82 USPQ2d 1385, 1395 (2007). See also, MPEP 2143(A).
Qi, Bush, and Chondroudis do not teach that the at least another precursor is sublimated from the same source container with the same delivery mouth. However, if only one crystal growth system is available it is self-evident that if all of the BX2 source material (508) contained in the crucible (504) in Figs. 5(A)-(C) and ¶[0038] that constitutes the first evaporator unit (120) in Fig. 1 of Qi is evaporated or sublimed or, alternatively, if it is desirable to utilize a different metal halide BX2 such as PbBr2 instead of PbCl2 to form a multilayer film with different compositions then it would be necessary to refill or replace the BX2 source material (508) located in crucible (504) with the same or a different metal halide after completion of film growth. This is necessarily the case because the desired perovskite thin film cannot be deposited from a precursor if the precursor is not present in the crucible. Similarly, if it is desirable to utilize a PBr2 source powder instead of PCl2 then PBr2 cannot be used unless the PCl2 contained within the crucible (504) is replaced or supplemented with PBr2. Accordingly, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to refill, replace, or supplement the original BX2 powder (508) in the crucible (504) of Qi with at least another precursor after performing an initial deposition sequence in order to deposit a thicker perovskite thin film and/or to deposit a multilayer comprised of a second layer of perovskite formed upon the first layer as part of a process for forming one or more electronic devices thereupon. Prior art is not limited just to the references being applied, but includes the understanding of one of ordinary skill in the art. The “mere existence of differences between the prior art and an invention does not establish the invention’s nonobviousness.” Dann v. Johnston, 425 U.S. 219, 230, 189 USPQ 257, 261 (1976). See also MPEP 2141(III).
Regarding claim 11, Qi does not explicitly teach that the method comprises:
(b) if in said at least on deposition chamber only one source is housed: substituting, in said source, said at least one precursor with said at least another precursor, between said step G and said step H and, if applicable, between each step H and a next step; and
(c) if in said at least one deposition chamber two or more sources are housed: charging said at least one precursor and said at least another precursor in a respective source and moving said substrate between one source and the other, between said step G and said step H and, if applicable, between each step H and the next step; and
(d) if said method is carried out in two or more deposition chambers, said method comprises moving said substrate between one deposition chamber and at least another deposition chamber, between said step G and said step H and, if applicable, between each step H and the next step.
As noted supra with respect to the rejection of claim 10, from among the available options (b)-(d) recited in claim 11, it is the Examiner’s position that option (b) would have been obvious to a person of ordinary skill in the art prior to the effective filing date of the invention for reasons which are reiterated below. If only one crystal growth system is available it is self-evident that if all of the BX2 source material (508) contained in the crucible (504) in Figs. 5(A)-(C) and ¶[0038] that constitutes the first evaporator unit (120) in Fig. 1 of Qi is evaporated or sublimed or, alternatively, if it is desirable to utilize a different metal halide BX2 such as PbBr2 instead of PbCl2 to form a multilayer film with different compositions then it would be necessary to refill or replace the BX2 source material (508) with the same or a different metal halide after completion of film growth. This is necessarily the case because a perovskite thin film cannot be deposited from a precursor if the precursor is not present. Similarly, if it is desirable to utilize a PBr2 source powder instead of PCl2 then PBr2 cannot be used unless the PCl2 contained within the crucible (504) is replaced or supplemented with PBr2. Accordingly, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to refill, replace, or supplement the original BX2 powder (508) in the crucible (504) of Qi with at least another precursor after performing an initial deposition sequence in order to deposit a thicker perovskite thin film and/or to deposit a multilayer comprised of a second layer of perovskite formed upon the first layer as part of a process for forming one or more electronic devices thereupon. Prior art is not limited just to the references being applied, but includes the understanding of one of ordinary skill in the art. The “mere existence of differences between the prior art and an invention does not establish the invention’s nonobviousness.” Dann v. Johnston, 425 U.S. 219, 230, 189 USPQ 257, 261 (1976). See also MPEP 2141(III).
Regarding claim 12, Qi teaches that said pressure value (Pc) of said at least one deposition chamber, one pressure value (Pₛ) of said at least one source, said temperature value of said substrate Tw and said deposition distance dw, within each step G and H, are adjusted in advance or continuously or at preset intervals during execution of said method (see Fig. 9 and ¶¶[0042]-[0049] as well as the rejection of claim 10 and elsewhere throughout the entire reference which teach that a predetermined chamber pressure, temperature and, hence, partial pressure of the BX2 and AX source materials, temperature of the substrate (116), and source-to-substrate distance are necessarily set in advance in order to deposit a perovskite thin film having the desired thickness and materials properties.
Regarding claim 13, Qi does not teach that after the execution of the last executed step H, said method comprises feeding into said at least one deposition chamber at least one gas selected among the group comprising nitrogen, argon, neon, helium, and hydrogen. However, in at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of an ultrapure inert gas such as nitrogen through the housing (100) and then out through the gate valve (108) and pump unit (104) before, during, and/or after film growth has completed in the system and method of Qi and Bush in order to purge the housing (100) prior to being vented and/or prior to removing the substrate (116) from the housing (100) in order to maintain a clean environment for subsequent film growth and minimize the transfer of potentially hazardous gases out of the housing (100).
Regarding claim 14, Qi teaches that said at least one precursor and said at least another precursor are selected from the group comprising: Pbl₂, MAI, FAI, Csl, Snl₂, PbCl₂, EuCl₃, Eul₂, in the form of powder or granules or tablets (see ¶[0029 which teach the use of precursors such as PbI2, PbCl2, and MAI in powder form).
Regarding claim 17, Qi teaches that said substrate is made of one material selected from the group comprising glass, Silicon, PEN, PET or said substrate is made of Aluminum, Titanium or Silicon Carbide (see Figs. 15-16, ¶¶[0025]-[0026], and ¶¶[0057]-[0058] which teach the use of glass substrate with a surface layer of ITO).
Regarding claim 18, Qi teaches that said substrate comprising glass, Silicon, PEN, PET, is provided with one surface layer of a material selected among: ITO, PTAA, FTO, TiO2, ZnO (see Figs. 15-16, ¶¶[0025]-[0026], and ¶¶[0057]-[0058] which teach the use of glass substrate with a surface layer of ITO).
Regarding claim 19, Qi does not teach that said process control gas includes one or more gases selected among the group comprising nitrogen, argon, neon, helium and hydrogen. However, as noted supra with respect to the rejection of claim 3, in at least Fig. 4 and col. 3, l. 50 to col. 6, l. 4 Chondroudis teaches an analogous embodiment of a system and method for the deposition of hybrid organic-inorganic perovskites onto a substrate (3) by evaporation of a predetermined quantity of an organic-inorganic hybrid material (6) provided on a heated sheet (4). In col. 2, l. 66 to col. 3, l. 5 and col. 5, ll. 32-34 Chondroudis specifically teaches that film growth may be performed in an inert atmosphere in which an inert gas such as nitrogen is supplied to a growth chamber (1) through an inlet (7) and then is evacuated through an outlet (8). When used in conjunction with one or more valves the inert gas flow rate necessarily facilitates control of the pressure within the chamber (1) via the gas flow and pumping rates and has the effect of purging the chamber (1) by flushing potential contaminants out through the outlet (8). Thus, a person of ordinary skill in the art prior to the effective filing date of the invention would be motivated to include a gas inlet (7) for the flow of an inert gas such as nitrogen through the housing (100) and then out through the gate valve (108) and pump unit (104) prior to or during pump-down in the system and method of Qi and Bush in order to purge the housing (100) and maintain an inert environment suitable for the growth of a higher quality perovskite layer with a reduced quantity of contaminants.
Regarding claim 20, Qi teaches that said at least one precursor is selected from the group comprising: Pbl2, MAI, FAI, Csl, SnI2, PbCl2, EuCl3, Eul2, in the form of powder or granules or tablets (see ¶[0029 which teach the use of precursors such as PbI2, PbCl2, and MAI in powder form)..
Regarding claim 21, Qi teaches that said substrate is made of one material selected from the group comprising glass, Silicon, PEN, PET or said substrate is made of Aluminum, Titanium or Silicon Carbide (see Figs. 15-16, ¶¶[0025]-[0026], and ¶¶[0057]-[0058] which teach the use of glass substrate with a surface layer of ITO).
Regarding claim 22, Qi teaches that said substrate comprising glass, Silicon, PEN, PET, is provided with one surface layer of a material selected among: ITO, PTAA, FTO, TiO2, ZnO (see Figs. 15-16, ¶¶[0025]-[0026], and ¶¶[0057]-[0058] which teach the use of glass substrate with a surface layer of ITO).
Response to Arguments
Applicants’ arguments filed May 15, 2026, have been fully considered, but they are not persuasive.
Applicants initially argue in Point 1 that there is no motivation to combine the teachings of Qi with Chondroudis and Bush because the latter two references rely on a carrier gas to transport material. See applicants’ 5/15/2026 reply, pp. 15-16. Applicants’ argument is noted, but is unpersuasive. As an initial matter it is pointed out that the system utilized for perovskite deposition in Fig. 1 of Qi does not utilize a carrier gas and, hence, it is Qi rather than Chondroudis and Bush that is relied to teach this aspect of the claims. Choudroudis is merely relied upon to teach that film growth may be performed in an inert atmosphere which is controlled via the use of a gas inlet (7) and outlet (8) to adjust the amount of gas entering and leaving the chamber (1). There is no teaching or suggestion that the use of a carrier gas is critical. In fact, Fig. 1 of Choudroudis shows an embodiment of a system in which film growth is performed in a vacuum rather than an inert gas atmosphere. Then Bush is relied upon to teach that the source-to-substrate distance conventionally is in the range of < 4 cm depending on the substrate temperature and pressure utilized during film growth in order to facilitate laminar flow, to increase source material utilization, and to minimize rapid cooling of the precursor vapor exiting the source outlet. Then in at least ¶[0039] Bush teaches that flow of the precursor vapors may be aided by the use of a carrier gas which clearly indicates that the use of a carrier gas is not explicitly required. Even if Bush does utilize a carrier gas for film growth, the teachings of Bush remain relevant to the problem to be solved, which is facilitating the efficient transfer of precursor species to the substrate. Even in the absence of a carrier gas in the method of Qi the pressure and temperature utilized during film growth will still influence the transport of gaseous precursors and to this end a PHOSITA would look to the teachings of Bush for this purpose and would be motivated to utilize a substrate-to-source distance of < 4 cm to facilitate laminar flow, to increase the efficiency by which the source material is utilized, and to minimize rapid cooling of the precursor vapor during transport.
Applicants subsequently argue in Point 2 that since the deposition distance in Bush is optimized for a laminar flow regime driven by a carrier gas which utilizes a completely different physics for particle transport and deposition it therefore is not applicable to a distinct collisional effusion process as recited in claim 1. Id. at pp. 16-17. Applicants’ argument is noted, but it is pointed out that in at least ¶[0030] and ¶[0042] Qi specifically teaches that the pressure within the housing (100) during film growth may be controlled over the range of 105 to 10-7 Pa which overlaps the entirety of the claimed range. In ¶[0043] Qi specifically teaches the use of a pressure of 0.3 Pa which is equal to 3×10-3 mbar and, hence, is fully within the range of 0.1×10-3 to 100×10-3 mbar as recited in claim 1. Then in ¶[0039] Bush specifically teaches that the vaporizers in the VPT system may be operated at a pressure of 10-4 to 1 Torr which is equivalent to 1.3×10-3 to 1.3 mbar which also substantially overlaps both the pressure range recited in claim 1 and the ranges disclosed in the teachings of Qi. Then, as noted supra, in at least ¶[0039] Bush teaches that flow of the precursor vapors may be aided by the use of a carrier gas which clearly indicates that the use of a carrier gas is not explicitly required. Since both Qi and Bush teach the use of overlapping pressure ranges it therefore is the Examiner’s position that the teachings of Bush with respect to the source-to-substrate distance are applicable to the method of Qi.
Finally, in Part 3 applicants argue that since ¶[0041] of Qi teaches avoiding directional deposition of the organic precursor (AX) onto the substrate, a PHOSITA following the teachings of Qi would be discouraged from pursuing a method that involves the direct, high-flux deposition of an organic precursor as recited in the method of claim 10. Id. at p. 17. Applicants’ argument is noted, but it is unclear as to which specific aspect of claim 10 is not taught or suggested by Qi. Each and every element of claim 10 which is taught by Qi is clearly outlined in the rejection of claim 10 while any deficiencies present are remedied via the introduction of Chondroudis and Bush. With respect to ¶[0041] of Qi it is assumed applicants are referring to the last sentence which states that “[t]he evaporator shutter 820 can be adjusted to cover the opening of the crucible 804 to avoid the high flux of the AX vapor exiting from the second evaporator unit 724 hitting directly the substrate 716.” Here Qi is not specifically teaching that it is essential to avoid direct deposition of the AX precursor onto the substrate, but instead is merely showing that a shutter can be used for this purpose if so desired. This is exemplified by at least Figs. 1 and 7 of Qi which teaches another embodiment in which a shutter is not utilized directly above the second evaporator unit (124) or (724), respectively. Since it is the Examiner’s position that the combination of Qi, Chondroudis, and Bush teach each and every element recited in claims 1 and 10, the rejection is therefore maintained.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/KENNETH A BRATLAND JR/Primary Examiner, Art Unit 1714
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