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Shinbum article. In addition to Applicants' remarks in regard to this rejection in 
Applicant's prior response, please consider the following: 

The date of the Asahi Shinbum article is November 28, 1986. As stated in Applicants' 
specification at page 6, lines 7-10: 

The basis for our invention has been described by us in the 
following previously published article: TG. Bednorz and 
K.A. Mueller, Zeitschrift for Physik B - Condensed Matter, 
64, pp. 189-193, Sept. (1986). 

The Examiner is using Asahi Shinbum as a reference under 35 USC § 102(a). 
Applicants respectfully disagree since to do so does not permit Applicants the one year 
period provided under 35 USC § 102(b) to file a U.S. application after their own 
publication which permitted Applicants to file the present application up to September 
1987. The date of the Asahi Shinbum article is after the date of Applicants' publication. 

In regard to the two-year grace period under a prior statute, the U.S. Supreme Court in 
Andrews v. Hovey, 123 US 267 (1887) states that: 

'The evident purpose of the section was to fix a period 
of limitation which should be certain, and require only a 
calculation of time, and should not depend upon the 
uncertain question of whether the Applicant had consented 
to or allowed the sale or use. Its object was to require the 
inventor to see to it that he filed his application within two 
years from the completion of his invention, so as to cut off 


all question of the defeat of his patent by a use or sale of it 
by others more than two years prior to his application, and 
thus leave open only the question of priority of invention. 
The evident intention of congress was to take away the right 
(which existed under the act of 1836) to obtain a patent after 
an invention had for a long period of time been in public use, 
without the consent or allowance of the inventor; it limited 
that period to two years, whether the inventor had or had 
not consented to or allowed the public use." 

From this quote from Andrews v. Hovey, it is evident that the use or sale by others prior 
to filing a patent application by the inventor docs not cut off the inventors right to 
obtain a patent so long as the inventor files the application within the statutory period 
which was 2 years at the time of the Andrews v. Hovey decision and is now 1 year under 
35 USC 102(b). 

The Patent Office Board of Appeals in Ex parte Powell and Davies, 37 USPQ 285 states 
in regard to the publication of Applicants foreign patent application before the filing of 
a U.S. application on October 5, 1936 on an invention described in the foreign patent 
application that: 

The Examiner has also rejected the claims on the printed 
specification of Applicants' own British application which 
appears from this record to have been published on August 
27, 1936. We know of no authority for such a rejection. 
Neither section 3886 nor section 4887 R.S. warrants the 
rejection. Obviously, the publication could not have a date 


- 3 - 

prior to Applicants' invention. There is no statute that 
requires an Applicant to make his invention in this country. 

Therefore, Applicants of the present invention can rely on their publication in Zeitschrift 
for Physik as evidence of their invention. 

The Patent Office Board of Appeals in Ex parte Powell and Davies, 37 USPQ 285, 286 
further states: 

The Commissioner indicates in Ex parte Grosselin that 
the Examiner should consider whether the German patent 
was derived from Applicant and was in effect nothing more 
than a printed publication of Grosselin's invention. 

The Asahi Shinbum article states in the first paragraph: 

A new ceramic with a very high T c of 30K of the 
superconducting transition has been found. The possibility 
of high T c - superconductivity has been reported by scientists 
in Switzerland this spring. The group of Prof. Shoji 
TANAKA, Dept. Appl. Phys. Faculty of Engineering at the 
University of Tokyo confirmed in November, that this is 

The ''scientists in Switzerland" are the inventors of the above-identified application. The 
Asahi Shinbum article only reports the work of Applicants and that it was reproduced 
by Prof. Tanaka. This article is a disclosure of Applicants' "own invention" and clearly 

YO987-074BY * - 4 - 

in the words of the Board in Ex parte Powell and Da vies, "was derived from 
[Applicants] and [is] in effect nothing more than a printed publication of 
[Applicants'] own invention and cannot be used as a reference. 

The Patent Office Board of Appeals in Ex parte Lcmicux 148, 140 states that: 

Finally, we believe that our holding is consistent with 
decisions in interference practice wherein, even though in the 
usual case a party may not establish a priority date of 
invention by reference to activity in a foreign country, yet in 
an originality case where a party is seeking to prove that the 
other party derived from him so that there is only a single 
original inventor, he may be permitted to prove derivation 
by reference to activity abroad. ... By analogy, in the 
present case appellant has demonstrated that he is the single 
original inventor, there being no adverse party. 

Following this decision it is clear from the Asahi Shinbum article that Applicants are the 
"single original inventor" and that the Asahi Shinbum article is "derived" from 
Applicants and that Professor Tanaka's work reported in the Asahi Shinbum article is 
"derived" from Applicants. 

Therefore, the Examiner is respectfully requested to withdraw the rejection of claims 
24-26, 86-90 and 96-108 under 35 USC § 102(a) as anticipated by Asahi Shinbum and 
under 35 USC § 103 as obvious over Asahi Shinbum. 

Attached are copies of the following decisions: 
YO987-073BY - 5 - 

Ex parte Powell and Davies 37 USPQ 285 
Ex parte Lemicux 115 USPQ 148 

Reg. No. 32,053 

IBM Corporation 

Intellectual Property Law Dept. 

P.O. Box 218 

Yorktown Heights, N.Y. 10598 
(914) 945-3217 




Ex parte Lemieux 

115 USPQ 

Patent Office Board of Appeals 
Ex parte Lemieux 
Patent issued Oct. 8, 1957 
Opinion dated July 31, 1957 


1 Interference — Reduction to practice — 
In general (§41.751) 
Patentability — Anticipation — In gen- 
eral (§ 51.201) 
Patentability — Anticipation — Pub- 
lications — In general (§51.2271) 
Act of August 8, 1946 (35 U.S.C. 104) 
was enacted to overrule Electric v. 
Shimadzu, 307 U.S. 5, 41 USPQ 155, and 
preclude applicant or patentee from rely- 
ing upon foreign activity to establish 
date of invention; it had no effect on Ex 
parte Powell, 37 USPQ 285; hence, in- 
ventor's foreign publication within year 
prior to filing United States application 
does not bar him from obtaining patent. 

2. Affidavits — Anticipating references 

(§ 12.3) 

Rule 131 does not apply where publica- 
tion is publication of applicant's own in- 
vention; domestic inventors are not 
distinguished from foreign inventors; all 
that is required is that identity of appli- 
cation inventor and publication author be 

3. Interference — Originality of inven- 

tion — In general (§ 41.551) 
Interference — Reduction to practice — 

In general (§ 41.751) 
Even though in usual case interference 
party may not establish priority date 
of invention by reference to activity in 
foreign country, in originality case, 
where party is seeking to prove that op- 
ponent derived from him so that there 
is only a single original inventor, he 
may be permitted to prove derivation by 
reference to activity abroad. 

Particular patents — Ustilic Acids 
2,809,205, Lemieux, Production of 
Ustilic Acids, claims 1 to 4 and 6 of ap- 
plication allowed. 

Appeal from Division 63- 
Application for patent of Raymond U. 

Lemieux, Serial No. 281,451, filed Apr. 

9, 1952. From decision rejecting claims 1 

to 4 and 6, applicant appeals. Reversed. 

Pierce, Scheffler & Parker, Washing- 
ton, D.C., and Alex E. MacRae for 

Before DuNCOMBE, Examiner in Chief, 
and Magil and Brewrink, Acting Ex- 
aminers in Chief. 

Magil, Acting Examiner in Chief. 

This is an appeal from the final rejec- 
tion of claims 1 through 4 and 6. Claims 
5 and 7, the remaining claims in the case, 
have been withdrawn from further con- 
sideration in accordance with Rule 142(b) 
and are not before us. 

Since the issue involved in this case 
is purely legal in nature, there is no 
reason for reproducing an illustrative 

The reference relied upon is: 

Lemieux, Canadian Journal of Chem- 
istry, Vol. 29, (May 1951), pages 415- 

We need not refer to the subject matter 
of the claims because, as previously in- 
dicated, the appeal involves only a legal 
point. The following facts are not in 

1. The appellant is the author of 
the cited publication. 

2. The subject matter of the ap- 
pealed claims is adequately disclosed 
in the cited publication. 

3. The cited article was published 
prior to appellant's filing date in this 
country, but not more than one year 
prior thereto. 

4. Appellant does not rely upon any 
earlier filing date to antedate the 
publication, nor does he assert that 
he completed the invention in this 
country prior to the date of the pub- 

The examiner holds that appellant is 
barred from obtaining a patent by the 
provision of 35 U.S.C. 102(a) and that 
he cannot avoid this bar because of the 
restriction of 35 U.S.C. 104 and the 
words "in this country" in Rule 131. 

Appellant contends that he filed his 
application within the one year period 
specified in 35 U.S.C. 102(b) and that 
Rule 131 is inapplicable. Appellant re- 
lies upon the case of Ex parte Powell 
and Davies, 489 O.G. 231, 1938 CD. 15, 
37 USPQ 285; he also refers to the 
International Convention for the Pro- . 
tection of Industrial Property and to | 
the effect of the examiner's rejection on ; 
Canadian inventors. 

We have carefully considered the ex- < 
aminer's rejection and the appellant's 
arguments and have studied the perti- 
ment cases on this subject. On its face, ; 
and disregarding subsequent statutory 
changes, the Powell and Davies case ap- ; 
pears to be most apposite. The examiner 
recognizes that the cited decision is rele- 
vant, but holds that it is no longer con- < 
trolling because of the Act of August 8, ] 
1946, which resulted in the enactment ol 
the statute presently corresponding to , 
35 U.S.C. 104. 


[1] We hp. 
U.S.C 104 an 
by the case 
Shimadzu et 
t;75t 83 Law 
5 04 O.G. 4,41 
in an infrmg. 
n0 t preclude 
invention by 
abroad. We 
the Shimadzu 
country" in 
to present Ri 
the case of It 
810, 1942 C. 
F.2d 169, 52 
the Shimadz 
anomalous si 
plying in int 
another rule 
ings. In ord« 
the Act of A 
nn d t as is e^ 
No. 1502, Jui 
2nd Session, ; 
January 28, 
Session, the } 
effect, to ovei 
tation of the 
elude an apr 
relying upon 
a date of invc 
rase is refen 
Senate and tl 

With the : 
be said that 
the Act of i 
to overrule t) 
it had no ef 
Davies decisi- 
Powell and 
affected, we 
trolling in th 
reversal of t> 
note that th 
was cited by 
In re Saurer, 
405, 529 O.G. 
78, but the C 
applicable oi 
failed to este 
person namec 
also state th; 
Kx parte Gr< 
CD. 248, cite 
decision, as 
Kx parte Gr 
CD. 163, to 

Aside fron 
104, there U 
section is no 
ease. Appell 
hsh a date o: 
argued that 1 
publication a 
the examiner 
°f invention 


ro the final rejec- 
1 4 and 6. Claims 
laims in the case, 
rom further con- 
with Rule 142(b) 

ved in this case 
are, there is no 
: an illustrative 

ipon is: 

Journal of Chem- 
951), pages 415- 

he subject matter 
as previously in- 
lves only a legal 
facts are not in 

5 the author of 

tter of the ap- 
juately disclosed 

3 was published 
ling date in this 
e than one year 

ot rely upon any 

0 antedate the 
he assert that 

vention in this 
late of the pub- 
hat ^pellant is 

1 patent by the 
102(a) and that 
r because of the 
\ 104 and the 

in Rule 131. 

nat he filed his 
one year period 
102(b) and that 
Appellant re- 
jX parte Powell 
1, 1938 CD. 15, 
> l refers to the 
n for the Pro- 
roperty and to 
er's rejection on 

nsidered the ex- 
the appellant's 
udied the perti- 
ct. On its face, 
quent statutory 
Davies case ap- 
:. The examiner 
decision is rele- 
; no longer con- 
.ct of August 8, 
he enactment of 
orresponding to 

115 USPQ 

Ex parte Lemieux 


[1] We have traced the history of 35 
U.S.C 104 and find that it was prompted 
by the case of Electric Storage Co v 
Shimadzu et al., 307 U.S. 5, 59 SupCt* 
675, 83 Law. Ed. 1071, 1939 CD. 870* 
504 O.G. 4, 41 USPQ 155, which held that 
in an infringement action the patentee is 
not precluded from proving his date of 
invention by reference to his activity 
abroad. We note that, on the basis of 
the Shimadzu decision, the words "in this 
country" in old Rule 75, corresponding 
to present Rule 131, were held invalid in 
the case of In re McFarlane, 29 CC P A 
810, 1942 CD. 254, 540 O.G. 237, 125 
F.2d 169, 52 USPQ 335. The decision in 
the Shimadzu et al. case created an 
anomalous situation, with one rule ap- 
plying in interference proceedings and 
another rule applying in other proceed- 
ings. In order to remedy this situation 
the Act of August 8, 1946 was enacted 
^ nd »asis evident fr0m Senate Report 
No. 1502, June 14, 1946, 79th Congress, 
2nd Session, and House Report No. 1498 
January 28, 1946, 79th Congress, 2nd 
Session, the purpose of the law was, in 
effect, to overrule the statutory interpre- 
tation of the Shimadzu decision and pre- 
clude an applicant or a patentee from 
relying upon foreign activity to establish 
a date of invention. The Shimadzu et al 
case is referred to by name in both the 
Senate and the House Reports. 

With the foregoing analysis, it may 
be said that the purpose and effect of 
the Act of August 8, 1946 was solely 
to overrule the Shimadzu et al. case and 
it had no effect upon the Powell and 
Davies decision cited by appellant. The 
rowell and Davies decision being un- 
affected, we should hold that it is con- 
trolling in the present case and dictates 
reversal of the examiner's decision. We 
note that the Powell and Davies case 
was cited by the appellant in the case of 
in re Saurer, 28 C.C.P.A. 1021 1941 C n 
«9 O.C: 802, 118 Fid t 719. 49 USPQ 
78, but the Court found the decision in- 
? n ll , becaus e the appellant 
failed to establish his identity with the 
Person named in the reference. We may 
also state that we consider the case of 
parte Grosselin, 97 O.G. 2977, 1901 
UO. 248, cited in the Powell and Davies 
decision as well as the earlier case of 

pn P ?^ e Grosseli n> 84 O.G. 1284, 1898 
v^-u. 163, to be pertinent. 

1n £ sid , e from the history of 35 U.S.G. 

there is another reason why this 
IT t,0 V s not applicable to the present 
case. Appellant is not seeking to "estab- 
»sn a date of invention" but has merely 
argued that he is the author of the cited 
Publication and this is not disputed by 
examiner. There being no evidence 
invention by anyone else prior to 

appellant's filing date, the date of ap- 
pellant's invention is immaterial. In 
the present case, we are not concerned 
with appellant's "date of invention" vis- 
a-vis the publication of another, an in- 
terferant, or other adverse party. 

[2] Insofar as the requirements of 
Rule 131 are concerned, we need do noth- 
ing more than refer to and state our 
agreement with the holdings in the first 
Grosselin decision (84 O.G. 1284. 1898 
CD. 163) and in the Powell and Davies 
case concerning old Rule 75, correspond- 
ing to present Rule 131. In the former 
decision it was held that "this rule pre- 
supposes that the printed publication is 
the publication by some one other than 
the applicant whose application is re- 
jected-by some one who asserts inventor- 
ship therein either in himself or some 
other person than the applicant." In the 
later case it was held that the rule is 
not "intended to apply to a case where 
the publication appears without question 
to be a publication of the applicant's own 

We also take cognizance of several de- 
cisions (Ex parte Ensign, 2 USPQ 214- 
Ex parte Layne, 63 USPQ 17; Ex parte 
Hirschler, 110 USPQ 384) which have 
held that, apparently in the case of a 
domestic inventor, a publication dated 
less than a year prior to the filing date 
of an application is not an effective bar 
if the applicant makes a satisfactory 
showing that the publication is his own 
invention or that he is, in effect, the 
author of the publication. In none of 
these cases is there any indication that 
the applicant made the usual showing 
under Rule 131, that is, reduction to 
practice prior to the date of the publica- 
tion or conception prior to the date of the 
publication coupled with the necessary 
diligence. We find no reason for dis- 
tinguishing between a domestic inventor 
and a foreign inventor in situations of 
this type and all that is required is that 
the identity of the application inventor 
and the publication author be established 
There is no dispute on this point in the 
present case. 

m [3] Finally, we believe that our hold- 
ing is consistent with decisions in inter- 
ference practice wherein, even though in 
the usual case a party may not establish 
a priority date of invention by reference 
to activity in a foreign country, yet in 
an originality case where a party is 
seeking to prove that the other party 
derived from him so that there is only 
a single original inventor, he may be 
permitted to prove derivation by refer- 
ence to activity abroad. Shiels v. Law- 
rence and Kennedy, 81 O.G. 2085, 1897 
CD. 184; Stiff v. Galbraith, 108 O.G. 
290, 1904 CD. 10. By analogy, in the 
present case appellant has demonstrated 



Ex parte Bergmann 

115 USPQ 


that he is the single original inventor, 
there being no adverse party. 

In accordance with the foregoing rea- 
soning, we conclude that the examiner's 
rejection cannot be sustained. We do not 
consider it necessary to discuss appel- 
lant's arguments concerning the Inter- 
national Convention for the Protection 
of Industrial Property or the effect of 
the examiner's rejection on Canadian in- 

The decision of the examiner is re- 

Patent Office Board of Appeals 
Ex parte Bergmann 
Patent issued Oct 8, 1957 
Opinion dated Jan. 22, 1957 



1. Patentability — Change 
(§ 51.257) 

Claims are allowed where applicant 
did not merely indulge in routine exper- 
imentation with material having prop- 
erties which would be expected to produce 
results desired, but utilized to advantage 
a material whose properties appeared to 
be unfavorable. 

Particular patents — Sound Recording 
2,809,237, Bergmann, Magnetic Sound 
Recording Head, claims 1 and 3 to 7 of 
application allowed. 

Appeal from Division 16. 

Application for patent of Friedrich 
Bergmann, Serial No. 209,250, filed Feb. 
3, 1951. From decision rejecting claims 
1 and 3 to 7, applicant appeals. Reversed. 
Marzaia, Johnston, Cook & Root, 

Chicago, 111., for applicant. 

Before Taylor and Kreek, Examiners 
in Chief, and NiLSON, Acting Ex- 
miner in Chief. 

Kreek, Examiner in Chief. 

This is an appeal from the final re- 
jection of claims 1 and 3 to 7 inclusive. 
No claims have been allowed. 

Claim 1 is illustrative: 

1. Magnetic sound recording head 
having a core consisting exclusively of 
magnetic ferrite. 

The references relied on are: 

Burns 2,536,260 Jan. 2,1951 

Buhrendorf 2,592,652 Apr. 16, 1952 

As is apparent from the illustrative 
claim, the subject matter here on appeal 
relates to a recording head for a mag- 
netic sound recorder in which the core 
consists exclusively of magnetic ferrite. 
Numerous advantages are claimed for 
this construction among which are re- 
duction of wear on the core as a result 
of the magnetic record medium passing 
thereover, as compared to the wear of 
conventional iron cores under similar 
circumstances; and reduction in electrical 
losses especially at high frequencies. 

Claims 1 and 3 to 7 were rejected as 
being unpatentable over Buhrendorf or 
Burns in view of the general knowledge 
of the art, the examiner's position being 
"The routine examination of any known 
substance for a particular use is ex- 
pected where the known basic require- 
ments of the use are compatible with 
some characteristics of the substance. 1 * 
It is his opinion "that the mere knowl- 
edge that 'ferrites' are magnetic is 
enough to warrant investigation by 
workers in magnetic recording. The 
knowledge of their high frequency losses 
and avowed utility in electo-acoustic de- 
vices practically demands investigation." 

Appellant contends that the references 
relied on do not suggest making cores 
exclusively of ferrite, and that the known 
permeability, saturation and abrasive 
characteristics of ferrite would point 
away from its use in sound recording 
heads rather than suggest it. He asserts 
that recording heads heretofore used are 
made with cores of highly permeable 
material to secure proper operation, but 
that satisfactory operation is secured 
with ferrite cores even though the perme- 
ability thereof is considerably less than 
the magnetic materials previously used. 
He asserts that the smaller magnetic 
saturation of ferrite as compared with 
metallic magnetic material would tend 
to indicate its unsuitability in erasinf 
heads where high magnetic saturation It 
required He further asserts that the f«t 
ferrite would not abrade the surface w 
the sound band was surprising sinci 
sintered ferrite behaves somewhat uM 
sintered porcelain. This characterise 
which would have been expected to be dev 
rimental is alleged to provide a gre» 
advantage resulting in heads having • 
life at least ten times longer than thy* 
of metal heads heretofore used. ApP«* 
lant has made of record a publication W 
Rolf Cruel in Technische HausmitteUufl- 
gen des Nordwestdeutschen Rundiun*j 
which compares magnetic heads nia** 
with ferrite with previously used la^T 
nated, high permeability iron alloy, ^ Dl ? 
publication demonstrates important tecjj 
nical advantages possessed by * eT F& 
over previously used magnetic materiAJ 
These are summarized as greater d**^ 

115 USPQ 

ness resulting in ^ 
sistance to wear sc 
used for much Ion 
without adjustment 
high frequency and 
for erasing. 

We have careful^ 
in view of appellan 
various publication 
show the suitability 
material for record ii 
of which we are of 
rejection cannot be 
The patent to E 
magnetic recording 
netic materials such 
ing high percneabilit 
tions are made extr 
0.001 of an inch th 
reduce eddy current 
value as is feasible 
ability to work wit! 
tions. Obviously 1 
anticipatory value, bi 
the problems confro 
this field as of the t 
Buhrendorf applicati 
Burns shows a maj 
for magnetic recor 
utilize a central yol 
either side of which 
Iron pole pieces 11 an 
contact the surface o 
used in the recorder 
forms a part of the c 
tor, the frequency of 
a result of the variati 
flow through the fe 
noted, however, that 
pieces are necessary ( 
netic tape from bein 
frequency currents fi 
wound in the ferrite ; 
no suggestion in Bui 
core may be made of 
ik * 1 Til e examiner 
jnat low permeability 
£ctor as he states "s 
^ undesirable perme: 
undesigned results." 
"J teachings of the 
Wnt away from th* 
£»tenai having low 
** ferrite as the sol 

w£L!° r * sound recc 

^eabihty of ferrit( 
fo7£ pro P er ties are 
a satlsf actorily a: 

S fl f ^rrite have 

to ten tim- 

"■Portant factor in r * 

37 USPQ 


ice is 
n for 

to the 
of re- 
ith the 

and an 

of the 
ised 11 

3usse In 
d to dis- 

has no 
d Busse 

nted the 

ich peti- 

t the pri- 
onfined his 
he motions 

to rewrite 
h this con- 
f appeal- 

the extent 


Patent Office Board of Appeals 
Ex parte Powell and Davies 
Appl No. 23985 Patent issued Apr. 5, 1938-Opinion dated Mar. 1, 

Patents-Patentability-Anticipation-Foreign patents; Affidavits-Anticipating ref- 

erences (Rule 75)— ... v..- opolpH s a there is no reason for 

Applicants' own British patent ha S not been sealed, sa tnere ^ 

registry under Rule 29; the British aPP^ 10 " ,^L5 sut es Application filed less 
thfre is y no authority for basing on it reject.on of United States «PP £x rte 

than two years after such publication Rule 75. "as >nte nae v > 

^JS&JfSS^^ ° f SUver » da5mS 1 ' 2 ' At ° 7 ' 10 

and 11 of application allowed. 

Patent No. 2113517 for electrodeposition 
of silver issued on application tiled 
Oct. 5, 1936. 

Appeal from Division 56. 

HowsoN & HOWSON for applicants. 

Before Van Arsdale, Assistant Commis- 
sioner, and Redrow and Porter, Ex- 
aminers in Chief. 

Porter, Examiner in Chief. — This is 
an appeal from the final rejection of 
claims 1, 2 t 4 to 7, 10 and 11. 

Claim 7 is illustrative. 

7. A plating bath comprising a potas- 
sium argento-cyanide, an excess of free 
potassium cyanide, carbon disulphide and 
Turkey red oil. 

The references relied upon are as iol- 


Schlotter (British) 443,428, Feb. 27, 

Powell et al (British) 450,979, Aug. 
27, 1936. n . . . . 

Blum & Hogaboom, Principles of 
Electroplating (2nd Ed.) 1930, pages 
350, 355 to 357. 

It appears from Blum and Hogaboom 
that the silver plating solution of the 
claims is old except for the addition of 
alkali metal soaps or their equivalents. 
Blum et al describe an excess of free 
alkali metal cyanide but the British pat- 
ent indicates that this excess should be 
very large and describes the use of 
Turkey red oil to which applicants refer 
at the bottom of page 3 of their specifi- 
cation. The British patent does not sug- 
gest the use of carbon bisulphide but 
rather suggests a substitute therefor. 
Blum et al does not suggest the use of 
soap. It is the combined use of carbon 
bisulphide and soap in the silver plating 
which applicants describe as their inven- 
tion. The gist of the examiner's position 
with respect to the references referred 

to appears to be that there is no inven- 
tion in the combined use of the carbon 
bisulphide and soap in the silver plating 
bath. The trouble with this position is 
that it is not warranted by the record 
which does not show carbon bisulphide 
combined with a dispersing agent of the 
nature of the one employed by appli- 

The examiner has also rejected the 
claims on the printed specification of 
applicants' own British application which 
appears from this record to have been 
published on August 27, 1936. We know 
of no authority for such a rejection. 
Neither section 4886 nor section 4887 
R S warrants the rejection. Obviously, 
the publication could not have a. date 
prior to applicants' invention. There is 
no statute that requires an applicant to 
make his invention in this country. 

It does not appear that the British 
patent has been sealed which sealing 
would be necessary in the case of a 
British patent in a rejection under Rule 
29 and it appears from the decision ot 
the Supervisory Examiner (Paper No. 
7) that the examiner's real position is 
not that applicants are barred by the 
provisions of Rule 29 as appears from 
his statement, but that applicants have 
failed to overcome their own publication 
by affidavits filed under Rule 75. 

Applicants filed a petition to the Com- 
missioner asking that the examiner be 
instructed to withdraw the citation of 
their own British specification as a ref- 
erence against the claims. This the 
Commissioner refused to do indicating 
that an adverse decision on the point by 
him might act to preclude a favorable 
decision by the Board of Appeals. 

The examiner holds the affidavits in- 
sufficient as the nature of the contents 
of i;he notes referred to in the affidavit 
of Coussmaker does not appear and there 
is no such showing as to facts as is 


Ex parte Powell avd Davies 

necessary in affidavits filed under Rule 
75. The affidavits have been reexamined 
but we find nothing therein except the 
mere inference that the subject matter in 
issue here was disclosed to Stones by 

The case of Ex parte Grosselin 1901 
C. D. 248, is analyzed by applicants in 
such a way as to contend that this de- 
cision never was intended to apply to 
a case where the printed publication in 
question was cne's own publication 
There are, however, certain obiter state- 
ments made in the Grosselin decision 
which might be taken to indicate that 
the provisions of Rule 75 requiring the 
applicants to show completion of the in- 
vention in this country apply to a case 
wherein the applicant is required to over- 
come the filing date of his own publica- 
tion. It is our opinion, however, that 
these obiter statements are not definite 
and any such construction of Rule 75 
as contended for by the examiner is 
clearly refuted by the general tenor and 
intent of the decision. Rule 75 was in- 
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It is our opinion that this record does 
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^_ CondGnssd 

Z. Phys. B - Condensed Matter 64, r«<^<1986) W Zeit^ B MatS^ 

© Springer-Verlag 1986 

Possible High T c Superconductivity 
in the Ba-La-Cu-O System 

J.G. Bednorz and K.A- Muller 

IBM Zurich Research Laboratory, Ruschlikon, Switzerland 
Received April 17, 1986 

Metallic oxygen-deficient compounds in the Ba - La -Cu-O system, with the composi- 
tion BaLa 5 _ Cu 5 0 5(3 _ y) have been prepared in polycrystallme form. Samples with 
x - 1 and 0 15 j»0, annealed below 900 °C under reducing conditions, consist of three 
phases one of them a perovskite-like mixed-valent copper compound. Upon cooling, 
the samples show a linear decrease in resistivity, then an approximately logarithmic 
increase, interpreted as a beginning of localization. Finally an abrupt decrease by up 
to three orders of magnitude occurs, reminiscent of the onset of percolauve superconduc- 
tivity The highest onset temperature is observed in the 30 K range. It is markedly 
reduced by high current densities. Thus, it results partially from the percolative nature, 
bute possibly also from 2D superconducting fluctuations of double perovskite layers 
of one of the phases present. 

L Introduction 

"At the extreme forefront of research in supercon- 
ductivity is the empirical search for new materials" 
[1]. Transition-metal alloy compounds of ,4 15 
(Nb 3 Sn) and B 1 (NbN) structure have so far shown 
the highest superconducting transition temperatures. 
Among many A 15 compounds, careful optimization 
of Nb-Ge thin films near the stoichiometric compo- 
sition of Nb 3 Ge by Gavalev et al. and Testardi et al. 
a decade ago allowed them to reach the highest T c = 
23.3 K reported until now [2, 3]. The heavy Fermion 
systems with low Fermi energy, newly discovered, are 
not expected to reach very high TVs [4]. 

Only a small number of oxides is known to exhibit 
superconductivity. High -temperature superconduc- 
tivity in the Li-Ti-O system with onsets as high 
as 13.7 K was reported by Johnston et al. [5]. Their 
x-ray analysis revealed the presence of three different 
crystallographic phases, one of them, with a spinel 
structure, showing the high T c [5]. Other oxides like 
perovskites exhibit superconductivity despite their 
small carrier concentrations, n. In Nb-doped SrTi0 3 , 
with n = 2 x 10 20 cm" 3 , the plasma edge is below the 
highest optical phonon. which is therefore unshielded 

[6], This large electron-phonon coupling allows a T c 
of 0.7 K [7] with Cooper pairing. The occurrence of 
high electron-phonon coupling in another metallic 
oxide, also a perovskite, became evident with the dis- 
covery of superconductivity in the mixed-valent com- 
pound BaPb! _ x Bi x Os by Sleight et al., also a decade 
ago [8]. The highest T c in homogeneous oxygen-defi- 
cient mixed crystals is 1 3 K with a comparatively low 
concentration of carries n -2-4 x 10 21 cm 3 [9]. Flat 
electronic bands and a strong breathing mode with 
a phonon feature near 100 cm -1 , whose intensity is 
proportional to T c , exist [10]. This last example indi- 
cates that within the BCS mechanism, one may find 
still higher T/s in perovskite-type or related metallic 
oxides, if the electron-phonon interactions and the 
carrier densities at the Fermi level can be enhanced 

Strong electron-phonon interactions in oxides 
can occur owing to polaron formation as well as m 
mixed-valent systems. A superconductivity (metallic) 
to bipolaronic (insulator) transition phase diagram 
was proposed theoretically by Chakraverty [11]. A 
mechanism for polaron formation is the Jahn-TeHer 
effect, as studied by Hock et al. [12]. Isolated Fe , 
Ni 34 and Cu" in octahedral oxygen environment 


show strong Jahn-Tellcr (J.T.) effects [13]. While 
SrFe(VI)C>3 is distorted perovskite insulator, 
LaNi(III)03 is a JT. undistorted metal in which the 
transfer energy b n of the J.T. e g electrons is sufficiently 
large [14] to quench the J.T. distortion. In analogy 
to Chakraverty's phase diagram, a J.T.-type polaron 
formation may therefore be expected at the border- 
line of the metal-insulator transition in mixed perovs- 
kites, a subject on which we have recently carried 
out a series of investigations [15J. Here, we report 
on the synthesis and electrical measurements of com- 
pounds within the Ba - La - Cu - O system. This sys- 
tem exhibits a number of oxygen-deficient phases 
with mixed-valent copper constituents [16], i.e., with 
itinerant electronic states between the non-J.T. Cu 3 + 
and the J.T. Cu 2+ ions, and thus was expected to 
have considerable electron-phonon coupling and me- 
tallic conductivity. 

II. Experimental 

1. Sample Preparation and Characterization 

Samples were prepared by a coprecipitation method 
from aqueous solutions [17] of Ba-, La- and Cu-ni- 
trate (SPECPURE JMC) in their appropriate ratios. 
When added to an aqueous solution of oxalic acid 
as the precipitant, an intimate mixture of the corre- 
sponding oxalates was formed. The decomposition 
of the precipitate and the solid-state reaction were 
performed by heating at 900 °C for 5 h. The product 
was pressed into pellets at 4 kbar, and reheated to 
900 °C for sintering. 

2. X-Ray Analysis 

X-ray powder diffractograms (System D500 SIE- 
MENS) revealed three individual crystallographic 
phases. Within a range of 10° to 80° (20), 17 lines 
could be identified to correspond to a layer-type per- 
ovskite-like phase, related to the K 2 NiF 4 structure 
(a-3.79 A and c=13.21 A) [16]. The second phase 
is most probably a cubic one, whose presence depends 
on the Ba concentration, as the line intensity de- 
creases for smaller x(Ba). The amount of the third 
phase (volume fraction > 30% from the x-ray intensi- 
ties) seems to be independent of the starting composi- 
tion, and shows thermal stability up to 1,000 °C. For 
higher temperatures, this phase disappears progres- 
sively, giving rise to the formation of an oxygen-defi- 
cient perovskite (La 3 Ba 3 Cu 6 0 14 ) as described by Mi- 
chel and Raveau [16]. 

J.G. Bcdnorz and K.A, Muller: Ba-La-Cu-O System 







' ■ 1 


** * 


• • « 

y yy 

— g • . 


<J - ♦*••„•••* 

_ *•* 



- *e 



• m 

• 0.25 A/cm 2 

• 0.50 A/cm 2 
- 0.50 A/cm 2 

* w 


1 1 








T (K> 



Fig. 1. Temperature dependence of resistivity in Ba^La^ _ *Cu 5 0 5 , 3 _ , 
for samples with jr(Ba)=l (upper curves, left scale) and x(Ba) = 
0.75 (lower curve, right scale). The first two cases also show the 
influence of current density 

3. Conductivity Measurements 

The dc conductivity was measured by the four-point 
method. Rectangular-shaped samples, cut from the 
sintered pellets, were provided with gold electrodes 
and contacted by In wires. Our measurements be- 
tween 300 and 4.2 K were performed in a continuous- 
flow cryostat (Leybold-Hereaus) incorporated in a 
computer-controlled (IBM-PC) fully-automatic sys- 
tem for temperature variation, data acquisition and 

For samples with x(Ba)<1.0, the conductivity 
measurements, involving typical current densities of 

0. 5 A/cm 2 , generally exhibit a high-temperature me- 
tallic behaviour with an increase in resistivity at low 
temperatures (Fig. 1). At still lower temperatures, a 
sharp drop in resistivity (>90%) occurs, which for 
higher currents becomes partially suppressed (Fig. 1 : 
upper curves, left scale). This characteristic drop has 
been studied as a function of annealing conditions, 

1. e., temperature and 0 2 partial pressure (Fig. 2). For 
samples annealed in air, the transition from itinerant 
to localized behaviour, as indicated by the minimum 
in resistivity in the 80 K range, is not very pro- 
nounced. Annealing in a slightly reducing atmo- 
sphere, however, leads to an increase in resistivity 
and a more pronounced localization effect. At the 
same time, the onset of the resistivity drop is shifted 

tern . 

J.G. Bednorzand KA Mullcr: Ba-I 

*u— O System 









0.05 - 

0 04 

003 — 






30 40 

T 00 

Fig- 2. Low-temperature resistivity of samples with x(Ba) = 1.0, an- 
nealed at 0 2 partial pressure of 0.2 bar (curve ©) and 
0.2 x 10" 4 bar (curves ® to CD) 

towards the 30 K region. Curves © and ®, recorded 
for samples treated at 900 °C, show the occurrence 
of a shoulder at still lower temperature, more pro- 
nounced in curve ®. At annealing temperatures of 
1,040 °C, the highly conducting phase has almost 
vanished. As mentioned in the Introduction, the 
mixed-valent state of copper is of importance for elec- 
tron-phonon coupling. Therefore, the concentration 
of electrons was varied by the Ba/La ratio. A typical 
curve for a sample with a lower Ba concentration 
of 0.75 is shown in Fig. 1 (right scale). Its resistivity 
decreases by at least three orders of magnitude, giving 
evidence for the bulk being superconducting below 
13 K with an onset around 35 K, as shown in Fig. 3, 
on an expanded temperature scale. The latter figure 
also shows the influence of the current density, typical 
for granular compounds. 

III. Discussion 

The resistivity behaviour of our samples, Fig. 1, 
is qualitatively very similar to the one reported in 
the Li-Ti-O svstem. and in superconducting 








© 7.5 A /cm 2 
- 2.5 A/cm 2 
• 0.5 A /cm 2 



30 40 
T (K) 


Fig. 3. Low-temperature resistivity of a sample with jr(Ba) = 0.75, 
recorded for different current densities 

BaPbj -^B^Oa polycrystalhne thin films [5, 18]. 
Upon cooling from room temperature, the latter ex- 
hibit a nearly linear metallic decrease of p(T\ then 
a logarithmic type of increase, before undergoing the 
transition to superconductivity. One could, of course, 
speculate that in our samples a metai-to-metal struc- 
tural phase transition occurs in one of the phases. 
The shift in the drop in p(T) with increasing current 
density (Fig. 3), however, would be hard to explain 
with such an assumption, while it supports our inter- 
pretation that we observe the onset of superconducti- 
vity of percolative nature, as discussed below. In 
BaPbi-^Bi^Oa, the onset of superconductivity has 
been taken at the resistivity peak [18]. This assump- 
tion appears to be valid in percolative systems, i.e., 
in the thin films [18] consisting of polycrystals with 
grain boundaries, or when different crystalline phases 
with interpenetrating grains are present, as found in 
the Li-Ti-O [5] or in our Ba - La -Cu-O system. 
The onset can also be due to fluctuations in the super- 
conducting wave functions. We assume one of the 
Ba- La -Cu-0 phases exhibits this behaviour. 
Therefore, under the above premises, the peak m p(T) 
at 35 K. observed for an v(Ba) = 0.75 (Fig. 1). has 


to be identified as the start to superconductive coop- 
erative phenomena in the isolated grains. It should 
be noted that in granular AI, Cooper pairs in coupled 
grains have been shown to exist already at a point 
where p(T) upon cooling has decreased by only 20% 
of its highest value. This has been proven qualitative- 
ly [19] and more recently also quantitatively [20] by 
the negative frequency shift occurring in a microwave 
cavity. In 100 A films, a shoulder in the frequency 
shift owing to 2D fluctuations was observed above 
the T c of the grains. In our Ba-La-Cu-O system, 
a series of layer-like phases with considerable variety 
in compositions are known to exist [16, 21], and 
therefore 2D correlations can be present. 

The granularity of our system can be justified 
from the structural information, and more quantita- 
tively from the normal conductivity behaviour. From 
the former, we know that more than one phase is 
present and the question arises how large are the 
grains. This can be inferred from the logarithmic 
fingerprint in resistivity. Such logarithmic increases 
are usually associated with beginning of localization. 
A most recent example is the Anderson transition 
in granular Sn films [22]. Common for the granular 
Sn and our samples is also the resistivity at 300 K, 
lying in the range of 0.06 to 0.02 Qcm, which is near 
the microscopic critical resistivity of p c ^i0L o ft/e 2 
for localization. From the latter formula, an inter- 
atomic distance L 0 in the range oflOO A is computed, 
thus a size of superconducting grains of this order 
of magnitude must be present. Upon cooling below 
r f , Josephson junctions between the grains phase- 
lock progressively [23] and the bulk resistivity gradu- 
ally drops to zero by three orders of magnitude, for 
sample 2 (Fig. 1). At larger current densities,' the 
weaker Josephson junctions switch to normal resistiv- 
ity, resulting in a temperature shift of the drop, as 
shown in Fig. 3. The plateau in resistivity occurring 
below the 80% drop (Fig. 1) for the higher current 
density of 0.5 A/cm 2 , and Fig. 2 curve ®) may be 
ascribed to switching of junctions to the normal state. 

The way the samples have been prepared seems 
to be of crucial importance: Michel et aL [21] ob- 
tained a single-phase perovskite by mixing the oxides 
of La and Cu and BaC0 3 in an appropriate ratio 
and subsequent annealing at 1,000 °C in air. We also 
applied this annealing condition to one of our sam- 
ples, obtained by the decomposition of the corre- 
sponding oxalates, and found no superconductivity. 
Thus, the preparation from the oxalates and anneal- 
ing below 950 °C are necessary to obtain a non-per- 
ovskite-type phase with a limited temperature range 
of stability exhibiting this new behaviour. The forma- 
tion of this phase at comparatively low temperatures 
is favoured by the intimate mixture of the compo- 

J.G. Bcdnor* and K.A. MQllcr: Ba-La-Cu-O System 

nents and the high reactivity of the oxalates owW 
to the evolution of large amounts of H 2 0 and CO 
during decomposition. 2 

IV. Conclusion 

In the concentration range investigated, compounds 
ol the Ba-La-Cu-O system are metallic at high 
temperatures, and exhibit a tendency towards local- 
ization upon cooling. Samples annealed near 900 °C 
under reducing conditions show features associated 
with an onset of granular superconductivity near 
30 K. The system consists of three phases, one of 
them having a metallic perovskite-type layer-like 
structure. The characterization of the new, apparently 
superconducting, phase is in progress. An identifica- 
tion of that phase may allow growing of single crys- 
tals for studying the Meissner effect, and collecting 
specific-heat data to prove the presence of high T 
bulk superconductivity. ' 

The authors would like to thank H.E. Weibel for his help in getting 
familiar with the conductivity measurement system, E. Courtens 
and H. Thomas for discussions and a critical reading of the manu- 


1. Tinkham, M„ Beasley, M.R., Larbalestier, D.C, Clark A F 
Finnemore. D.K.: Workshop on Problems in Superconductiv- 
ity, Copper Mountain, Colorado, August 1983, p 12 

2. Beasley, M.R., Geballe, T.H. : Phys. Today 36 (10), 60 (1984) 

3. MuUer, : Rep. Prog. Phys. 43, 663 (1980) 

4. Ott, H.R.; Unconventional Superconductivity. Zurich Phys. 
Soc. Seminar, Zurich, February 13, 1986 

5. Johnston, D.C., Prakash, H., Zachariasen, W.H., Viswanathan 
R.: Mat. Res. Bull. 8, 777 (1973) 

6. BaratofT, A., Binnig, G.: Physics 108 B, 1335 (1981) 
BaratofT, A., Binnig, G., Bednorz, J.G., Gervais, F,, Servoin, 
J.L.: In: Superconductivity in d- and /-Band Metals, Proceed- 
ings IV Conference in 'Superconductivity in d- and /-Band Met- 
als'. Buckel, W. and Weber, W. (eds), p. 419, Kernforschungs- 
zentrum Karlsruhe 1982 

7. Binnig, G., BaratofT A., Honig, H.E., Bednorz, J.G.: Phys. Rev. 
Lett. 45, 1352 (1980) 

8. Sleight, A.W., Gillson, J.L., Bierstedt, F.E.: Solid State Com- 
mun. 17, 27 (1975) 

Batlogg. B. : Physica 126 B, 275 (1984) 

9. Thanh, T.D., Koma. A., Tanaka, S. : AppJ. Phys. 22, 205 (1980) 

10. Mattheis, F., Hamann, D R.; Phys. Rev. B 26, 2682 (1982); 
ibid. 28. 4227 (1983) 

11. Chakraverty, B.K.: J. Phvs. Leu. 40. L99 (1979); J. Phvs. 42, 
1351 (19S1) 

12. Hock. K.-H.. Nickisch, H., Thomas. H Helv Phvs Acta 56. 
237 (1983) 

13. Englmann. R. : In: The Jahn-Tellcr Effect in Molecules and 
Crystals. London, New York: Wiley Intcrsciencc 1972 

14 Goodenoueh. J.B., Longo. M : Magnetic and other properties 
of oxide and related compounds. In: Landoh-Boernstem New 


co 2 

J.G. Bcdnorz and K.A. Muller: Ba^a-Cu-O System 

Series. VoIIII/4a: Crystal and solid state physics. Hcllwege, 
K.H., Hcllwege, A.M. (eds). p. 262, Fig. 73. Berlin, Heidelberg, 
New York: Springer- Verlag 1970 

15. Bednorz, J.G., Mullcr, K.A.: (in preparation) 

16. Michel, C. f Raveau, B.: Chim. Min. 21, 407 (1984) 

17. Bcdnorz, J.G., Muller, K.A., Arend, H., Granicher, H.: Mat 
Res. Bull. 18(2), 181 (1983) 

18. Suzuki, M., Murakami, T., Inamura, T.: Shinku 24, 67 (1981) 
(in Japanese) 

Enomoto, Y., Suzuki, M., Murakami, T., Inukai, T., Inamura, 
T.: Jpn. J. Appl. Phys. 20, L661 (1981) 

19. Mullcr, K.A., Pomeranlz, M., Knoedler, CM.. Abraham, D.: 
Phys. Rev. Lett. 45, 832 (1980) 

20. Stocker, E., Buttat, J.: Solid State Commun. 53, 915 (1985) 


21. Michel, C, Er-Rakho, L-, Raveau, B.: Mat. Res. Bull 20 667 
(1985) ' 

22. Van Haesendonck, C, Bruynseraede, Y.: Phys. Rev B 33 J684 

23. Dcuischer, G., Entin-Wohlman, O., Fishman, S., Shapira Y • 
Phys. Rev. B 21, 5041 (1980) 

J.G. Bcdnorz 
K.A. Muller 

IBM Zurich Research Laboratory 
Saumerstrassc 4 
CH-8803 Ruschlikon 

Note Added in Proof 

Chemical analysis of the bulk composition of our samples revealed 
a deviation from the ideal La/Ba ratios of 4 and 5.66. The actual 
ratios are 16 and 18. respectively. This is in agreement with an 
identification of the third phase as CuO.