US005449419A
`
`
`
`United States Patent
`
`
`
`5,449,419
`[11] Patent Number:
`
`
`
`
`
`Sep. 12, 1995
`[45] Date of Patent:
`Suzuki et al.
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`
`NAOAT
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`4,918,555 4/1990 Yoshizawaetal...sso 360/125
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`
`..
`1/1991 Yoshizawaet al.
`. 148/311
`4,985,089
`
`
`
`
`
`
`
`7/1991 Ihara et al.
`............
`.. 148/310
`5,028,280
`5,069,731 12/1991 Yoshizawaetal. ..
`.. 148/306
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`9/1992 Makinoetal. ........
`w- 164/423
`5,144,999
`9/1992 AShOK .rescccscoeecsecseesesseneeeees 164/479
`5,148,855
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`
`
`
`
`FOREIGN PATENT DOCUMENTS
`
`
`
`242063 9/1960 Australia .
`
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`
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`6/1988 European Pat. Off.
`0271657
`W084/03852 10/1984 WIPO .
`
`
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`WO87/00462
`1/1987 WIPO .
`
`
`
`
`
`
`Primary Examiner—John Sheehan
`
`
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`
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`Attorney, Agent, or Firm—Guy W. Shoup; Patrick T.
`Bever
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`
`............ 148/305
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`[75]
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`[56]
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`[54] FE BASED SOFT MAGNETIC ALLOY,
`MAGNETIC MATERIALS CONTAINING
`
`
`
`AND
`NETI
`ARA
`aN THE MAGNETIC aeALS
`
`
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`
`
`
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`
`:
`ira
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`Inventors: Kiyonori Suzuki, Sendai; Akihiro
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`Makino, Nagaoka; Tsuyoshi
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`Masumoto, 8-22 3 chome, Uesugi,
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`Aoba-ku, Sendai-shi, Miyagi-ken;
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`Akihisa Inoue; Noriyuki Kataoka,
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`both of Sendai, all of Japan
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`[73] Assignees: Alps Electric Co., Ltd., Tokyo;
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`Tsuyoshi Masumoto, Sendai, both of
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`Japan
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`
`[21] Appl. No.: 201,135
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`[22] Filed:
`Feb. 24, 1994
`
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`
`
`Related U.S. Application Data
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`Continuation of Ser. No. 690,201, Apr. 23, 1991, aban-
`[63]
`doned.
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`Foreign Application Priority Data
`[30]
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`Apt. 24, 1990 [JP]
`Sapam cercsssssssssseessssseesesnsee 2-108308
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`wherein Q represents at least one element selected from
`Aug. 31, 1990 [JP]
`Japa «....essssssecceseeseneesrsesnets 2-230135
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`the group consisting of Co and Ni; T represents at least
`Sep. 7; 1990 [JP]
`Sapam csesceccsesssssesesssseesessee 2-237752
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`one element selected from the group consisting of Ti,
`Sep. 7, 1990 [JP]
`Japan .....secrescsecseonessessesensees 2-237753
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` Japan ....---.scessesesecersessesreees 2-237754
`Zr, Hf, V, Nb, Ta, Mo and W,with Zr and/or Hfbeing
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`Sep. 7, 1990 [JP]
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`always included; T’ represents at least one element
`Sep. 7, 1990 [JP]
`Japan .....ssessessesesreeseeeereeseenes 2-237755
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`selected from the group consisting of Cu, Ag, Au, Ni,
`Sep. 7, 1990 [JP]
`Sapam eseesccsssssesssssseeeesssseee 2-237757
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`Pd and Pt; a, b, x, y and z are real numberssatisfying
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`Sep. 7, 1990 [JP]|Japan ..... .. 2-237758
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`relationships below:
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`Sep. 13, 1990 [JP]
`Japan .....
`. 2-243589
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`0SaX0.05 atomic %,
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`Sep. 13, 1990 [JP]
`Japan ....
`.. 2-243590
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`0<b=93 atomic %,
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`Nov. 27, 1990 [JP]
`Japan ....
`.. 2-324518
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`0.52x=16 atomic %,
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`Nov.27, 1990 [JP]—Japatt .......sessssesessrerseeeeoneeee 2-324519
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`4Sy310 atomic %,
`[SE]
`Tint, C16 onceesteeeneeneeneeteneteneees HOIF 1/147
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`0%z=45 atomic %
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`[52] US. CL. oeseeeesseeceecersceeenenenenes 148/306; 148/310;
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`provided that when 0<z=4.5 atomic %, Q represents
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`148/311; 148/305; 420/121; 420/125; 75/244
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`Co and 0<b=92 atomic %; and when z=0, 0.5=x=8
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`[58] Field of Search............... 148/305, 306, 310, 311;
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`atomic % and 4Sy=9 atomic %. Also disclosed are
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`420/121, 125; 75/244
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`soft magnetic materials such as thin films, ribbons, and
`
`
`References Cited
`
`
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`
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`powder magnetic transducers such as low frequency
`
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`
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`U.S. PATENT DOCUMENTS
`
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`transformers and magnetic heads using the material.
`
`
`
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`
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`Finally, processes and apparatuses for producing rib-
`cecscsssereecees 148/112
`
`
`
`
`
`4,257,830
`on...
`3/1981 Tsuya et al.
`
`
`
`
`
`
`
`bons formed from thealloy are disclosed.
`
`
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`
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`
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`4,718,475
`ws 164/415
`2/1988 Das etal. ....
`
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`
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`4,735,865 4/1988 Nago etal......
`a. 428/610
`
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`
`
`4 Claims, 19 Drawing Sheets
`
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`
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`6/1988 Makinoet al. ..........ee 148/304
`4,750,951
`
`
`
`ABSTRACT
`[57]
`
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`An Fe-based soft magnetic alloy having a high satu-
`
`
`
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`
`
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`rated magnetic flux density and having a composition
`
`
`
`represented by formula {1) below:
`
`
`
`(Fey-cQa)pBxTyT’z
`
`@
`
`
`
`
`
`
`
`
`
`* FeasCu1B3Zrs
`
`
`
`° FesiZr782
`
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`
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`
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`PERMEABILITY (1KHz)
`
`100
`10
`
`
`RATE OF COOLING (‘C/min)
`
`
`
`
`
`
`WATER
`QUENCHING
`
`
`
`Petitioner Samsung and Google
`Ex-1018, 0001
`
`Petitioner Samsung and Google
`Ex-1018, 0001
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 1 of 19
`
`5,449,419
`
`FIG 1
`PRIOR ART
`
`FIG. 2
`
`Petitioner Samsung and Google
`Ex-1018, 0002
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 2 of 19
`
`5,449,419
`
`FIG. 3
`
`FIG. 4
`
`10
`
`Petitioner Samsung and Google
`Ex-1018, 0003
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 3 of 19
`
`5,449,419
`
`•
`
`0
`
`\()
`l:j
`Lt:
`
`•
`
`\ • l • . /
`
`✓
`
`0
`N
`
`0 -
`
`( W 77 ) Z tf ' X't'W tf
`
`0
`
`o!
`
`0 t 0
`
`0
`~
`
`E
`E
`a..
`<(
`l!J
`UJ w
`U"'I z
`ci~
`V) -Cl
`
`0
`
`o (cid:173)
`U"'I O'I
`QJ
`"'O
`
`~Q:>
`z
`0
`1-
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`w z
`o (cid:173)
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`
`<(
`
`l!J - z
`
`0
`
`0
`
`-
`
`0
`
`C0
`0
`
`Petitioner Samsung and Google
`Ex-1018, 0004
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 4 of 19
`
`5,449,419
`
`0 \ I
`
`I
`)
`;.
`I
`'y
`I
`
`N -
`
`N m
`
`m m
`
`-N
`
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`
`m
`N
`
`'° N
`
`0
`-
`
`10
`
`0 -
`
`m
`N
`
`cc -
`
`Petitioner Samsung and Google
`Ex-1018, 0005
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 5 of 19
`
`5,449,419
`
`FIG. 8
`
`E "'\
`
`{}
`
`I ,--7 f PU
`A'®~-~r@B
`
`PL
`
`FIG. 9A
`
`FIG 98
`
`FIG9C
`
`73
`72 /70
`
`7
`
`72 ;70
`
`-·i.·::-. .
`. ::i,-•• :.;--... (
`
`1··
`~
`
`B
`
`71
`
`B
`
`71
`
`F
`
`71
`
`(
`
`(
`
`Petitioner Samsung and Google
`Ex-1018, 0006
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 6 of 19
`
`5,449,419
`
`FIG 10
`
`84 82
`
`~a1
`
`87
`90(70)
`
`86
`
`FIG. 11
`
`73
`
`Petitioner Samsung and Google
`Ex-1018, 0007
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 7 of 19
`
`5,449,419
`
`FIG. 12
`
`FIG. 13
`
`D
`
`FIG. 14
`
`FIG. 15
`
`/
`/;:
`
`V
`
`~
`
`:\.:
`
`101
`
`~
`
`- ~ 00
`
`I/
`
`"~
`
`Petitioner Samsung and Google
`Ex-1018, 0008
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 8 of 19
`
`5,449,419
`
`FIG. 16
`
`111
`
`112
`
`111a
`112
`~ 1 1 6
`1 1 2~
`
`FIG. 17A
`
`FIG. 178
`
`112
`
`I
`
`112
`
`Petitioner Samsung and Google
`Ex-1018, 0009
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 9 of 19
`
`5,449,419
`
`....--120
`D
`
`124 122
`
`121
`
`FIG. 18
`
`(cid:143)
`
`123
`
`FIG. 19
`
`131
`
`D1
`
`D\
`_ -"' 142
`
`°2
`FIG. 20 ~
`
`140
`
`Petitioner Samsung and Google
`Ex-1018, 0010
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 10 of 19
`
`5,449,419
`
`FIG. 21
`
`N
`:c: 1E+OS
`
`~
`
`cu
`::t. 10000
`>-
`I-
`....J
`co
`;
`a::
`UJ a..
`
`1000
`
`,,
`
`,,
`
`/
`
`/
`
`/
`
`,,
`
`/
`
`/
`
`/
`
`/
`
`Fes6Zr186(u1
`100'---'--~~---L-------1-------'-----_J
`550
`60 0
`RQ
`500
`660
`Trc
`
`FIG. 22
`
`CuKa
`
`QUENCHED STATE
`
`1 tltl 11111111 llfll I IU llt 1111 ftll tlfl lt\lJIIJ I I llrl 1111 Ill If I It Ill t I It II tt 'I u JII 1111 t 111 I JI IC 11111111 Ill ttl 111 tlll If Ir fl
`so
`30
`40
`60
`7 0
`80
`90
`
`AFTER HEAT TREATMENT
`AT 600-C FOR 1 HOUR
`
`10111111111 t 111111 IIJ I Pltl 111111111 ltl I 1J 1111 U llltl 11111titfII1111!11111111111 11111111 llSJ 111111111fIIJf11111 tltllll I l
`so
`30
`40
`60
`70
`80
`90
`ANGLE OF DIFFRACTION 28 (0
`
`)
`
`Petitioner Samsung and Google
`Ex-1018, 0011
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 11 of 19
`
`5,449,419
`
`FIG. 23
`
`1----1
`0
`
`1000A
`
`FIG. 24
`
`- - µe H=10m(cid:143) e. 1KHz
`----- Bs (G)
`
`500~600•c 1h
`
`Cu 1at%
`
`/
`
`/
`13000/
`14000// 2
`10000
`"
`15000 /
`
`,,
`
`AMORPHOUS
`2 o,__ _ _ _ _ .....__"""'-"------"-....__.....,..__,_..,___,,,~....__"-1..J.~~~-..L.-',.l,o
`85
`95
`80
`90
`100
`Fe+ Cu at%
`
`Petitioner Samsung and Google
`Ex-1018, 0012
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 12 of 19
`
`5,449,419
`
`FIG 25
`
`Fe93-aB6Cu1
`500~600°( 1h
`
`N 1E+05
`:c:
`
`:x:: -
`
`QJ
`
`::t 10000
`>-
`~
`.....J
`co
`<(
`UJ
`L
`a::
`UJ a..
`
`1000
`
`100
`
`4
`
`5
`
`6
`
`7
`a /atom%
`
`8
`
`9
`
`10
`
`FIG 27
`600~ 1oo·c 1h
`
`N :c: 1E+05
`
`:x:: -QJ
`
`~
`
`::t
`>-
`.....J 10000
`CD
`<(
`UJ
`L
`a::
`UJ a.
`
`1000
`
`0
`
`1
`
`Fes1-xZr4 Nb3B6 Cux
`2
`3
`Cu/atom%
`X
`
`4
`
`5
`
`Petitioner Samsung and Google
`Ex-1018, 0013
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 13 of 19
`
`5,449,419
`
`FIG 26
`
`-
`µ.e 1 KHz , 10m0e
`----- Bs (G)
`
`650°( 1h
`
`Nb 3at %
`Cu 1 at%
`
`20~~~....,___"'---L....LL..____,__-L-C---C..-"'-....£-...£"---L--..L---L--~-L..-".-~"--L.......L._~~o
`
`80
`
`85
`
`90
`Fe+Cu at%
`
`95
`
`100
`
`Petitioner Samsung and Google
`Ex-1018, 0014
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 14 of 19
`
`5,449,419
`
`FIG. 28
`
`( Fe1-aCoa)s6Zr4Nb3B6Cu1
`600~650°C 1 h
`
`1E+05
`
`N ::c
`~ ...-
`QJ 10000
`::t
`>-I-
`
`1000
`
`.....I
`a:)
`<(
`w
`:E
`a::
`w a..
`
`100
`
`0
`
`0.1
`
`0.2
`Co/ Fe+ Co
`
`0.3
`( a)
`
`0.4
`
`0.5
`
`FIG. 29
`
`(b)
`
`f = 1 KHz
`Hm=10mQe
`
`Fe91 Zr1B2
`
`Ta FOR 1hr
`
`OJ
`
`N 30000
`::c
`~ ...-
`
`25000
`::t 20000
`>-I-
`.....I
`co
`<( 10000
`w
`L a:
`LIJ a..
`
`300
`0
`QUENCHED STATE
`
`400 450 500
`
`5so
`
`600 650 100 re 1
`
`Petitioner Samsung and Google
`Ex-1018, 0015
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 15 of 19
`
`5,449,419
`
`FIG. 30
`µ.1K 600°( 1HOUR
`10
`5
`
`15
`
`20
`
`5
`
`BO
`
`85
`
`90
`
`95
`
`Fe--
`
`FIG. 31
`1 HOUR
`
`5
`
`20
`
`1000
`
`80
`
`as
`
`90
`
`95
`
`Fe--+-
`
`Petitioner Samsung and Google
`Ex-1018, 0016
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 16 of 19
`
`5,449,419
`
`Bs(G)
`
`FIG. 32
`
`5
`
`15
`
`\
`Zr
`
`20
`
`80
`
`85
`
`90
`
`95
`
`Os
`
`B
`I
`
`Fe__.
`
`FIG. 33
`5
`
`15
`
`\
`Zr
`0
`u
`\
`fa
`
`7j+
`
`5
`
`80
`
`85
`
`90
`
`95
`
`Fe
`
`....
`
`Petitioner Samsung and Google
`Ex-1018, 0017
`
`

`

`U.S. Patent
`
`
`
`
`Sep. 12, 1995
`
`
`
`
`
`Sheet 17 of 19
`
`
`5,449,419
`
`
`
`
`FIG. 34
`
`
`
`600~650°C th
`
`
`
`
`10000
`
`
`
`< 2
`
`
`
`
`
`
`
`
`> z
`
`pa| 1
`
`(Fei-aQa)9iZr7b2 nm 1E+05
`° Fe9iZr7B2 PERMEABILITYys(1KHz)
`
`000
`
`
`
`
`100
`
`0
`
`01
`
`
`
`
`03
`0.2
`
`Q/Fe+Q(a)
`
`
`
`04
`
`
`
`05
`
`
`
`
`
`
`¢ FessCuiB3Zrs
`
`
`
`
`
`
`
`
`
`10
`400
`
`
`RATE OF COOLING (*C/min)
`
`
`
`WATER
`QUENCHING
`
`
`
`Petitioner Samsung and Google
`Ex-1018, 0018
`
`uJ
`
`
`=~t
`
`
`.
`
`
`Ja
`
`
`
`Petitioner Samsung and Google
`Ex-1018, 0018
`
`

`

`FIG 36
`
`FIG. 37
`
`~ •
`00
`•
`
`THICKNESS OF RIBBON: 20~30 µm
`
`• Fea1Zr3Nb3B6Cu1
`0 SENDUST HEAD
`6 Nb-PEARMALLOY HEAD
`2o·c.S0%R.H.
`r-Fe2O3 TAPE
`
`15
`
`o • SURFACE OF FREE
`SOLIDIFICATION
`(cid:143) (cid:127) SURFACE OF ROLL
`CONTACT
`
`_ 10
`E
`::l
`
`N
`
`c::: ..
`X -c:
`& 5
`
`0 -
`
`-
`
`-
`
`0
`-
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`-
`
`(cid:143)-/--
`0
`0
`/
`. - - - - - - - - 0
`- - (cid:127)
`
`-
`
`-
`
`• •
`
`.--(cid:173)
`
`.---
`
`RMAX
`
`r
`
`,,,.o---
`
`- - ' - 0
`
`/
`
`/
`I
`
`;/
`
`•
`
`s~
`
`E
`::l
`
`(/)
`(/)
`0
`_J
`
`z
`0
`(/)
`<( c:::
`co
`<(
`
`I
`I
`I
`I
`I
`I
`I
`I
`I
`I
`I
`0
`/
`I
`(cid:143)---
`I
`•
`
`(cid:127)-----
`
`R MAX
`I
`f
`- - - (cid:143)----(cid:143)
`• - - •
`Rz
`
`1400
`1000
`600
`200
`SURFACE ROUGHNESS OF ROLL
`(GRAIN NUMBER OF POLISHING PAPER)
`
`mirror
`
`0
`
`I
`500
`t (hr)
`
`l
`
`I
`
`1000
`
`Petitioner Samsung and Google
`Ex-1018, 0019
`
`

`

`U.S. Patent
`
`Sep. 12, 1995
`
`Sheet 19 of 19
`
`5,449,419
`
`A L
`I
`
`·I·:
`)
`15
`8
`
`150
`
`Im'
`
`FIG. 38
`
`4l
`
`;--+t
`
`154
`l
`
`l 156
`
`FIG. 39
`
`~52
`
`Petitioner Samsung and Google
`Ex-1018, 0020
`
`

`

`FE BASED SOFf MAGNETIC ALLOY, MAGNETIC
`MATERIALS CONTAINING SAME, AND
`MAGNETIC APPARATUS USING THE MAGNETIC
`MATERIALS
`
`This application is a continuation of application Ser.
`No. 07/690,201, filed Apr. 23, 1991 now abandoned.
`
`BACKGROUND OF THE INVENTION
`1. Field of the Invention
`The present invention relates to an Fe based soft
`magnetic alloy. Further, the present invention relates to
`magnetic materials containing such a soft magnetic
`alloy, for example, ribbons, compressed powders and 15
`the like as well as to a process and apparatus for produc(cid:173)
`ing such magnetic materials. Also, the present invention
`relates to magnetic transducers such as a magnetic head,
`a transformer and a choke coil. However, the present
`invention is also useful in other applications.
`2. Description of Related Arts
`Soft magnetic alloys used in magnetic heads, trans(cid:173)
`formers. choke coils and the like must generally have
`the following characteristics:
`(1) They have a high saturated magnetic flux density. 25
`(2) They have a high permeability.
`(3) They have a low coercive force.
`(4) They can be shaped into a thin material.
`On the other hand, magnetic heads must have the
`following characteristics in addition to (1) to (4) above 30
`from a point of view of abrasion resistance:
`(5) They have a high hardness.
`Accordingly, when producing soft magnetic alloys or
`magnetic heads, extensive investigations on the physical
`properties of various alloy compositions have been 35
`made taking into consideration the above-described
`points.
`Heretofore, for the aforementioned purposes, there
`have been used crystalline alloys such as Sendust, Perm(cid:173)
`alloy (50% Ni-Fe Permalloy, 80% Ni-Fe Permalloy, 40
`etc.), and silicon steel (see for example, Japanese Patent
`Publication Nos. 37688/1987 and 45285/1987). Re(cid:173)
`cently, Fe-based or Co-based amorphous alloys have
`also been used.
`In the case of magnetic heads, however, their has 45
`been a growing demand for magnetic materials suitable
`for high performance magnetic heads in order to cope
`with a recent trend toward magnetic recording media
`having a higher coercive force thereby keeping pace
`with a recent shift toward higher density recording. As 50
`for transformers and choke coils, high performance
`magnetic materials are desired because further miniatur(cid:173)
`ization thereof is required to meet with miniaturization
`of various electronic devices.
`However, the aforementioned Sendust has a defect in 55
`that its saturated magnetic flux density is as low as about
`11 kG while it has an excellent soft magnetic character(cid:173)
`istics. Similarly, Permalloy has a defect in that it has a
`low saturated magnetic flux density as low as about 8
`kG when it has an alloy composition which exhibits 60
`excellent soft magnetic characteristics. More particu(cid:173)
`larly, when it is applied to magnetic cores, core loss at
`high frequencies is large and the temperature of the core
`increases drastically at a frequency of no less than sev(cid:173)
`eral tens kHz, resulting in that it is difficult to use as a 65
`material for magnetic cores. Silicon steel has a high
`saturated magnetic flux density but it has a poor soft
`magnetic characteristics. Also it is disadvantageous in
`
`1
`
`5,449,419
`
`5
`
`2
`that its iron loss is not low enough and thus it is unsatis(cid:173)
`factory from a point of view of energy saving and has a
`problem with heat generation when used in transform(cid:173)
`ers.
`On the other hand, as for the amorphous alloy, Co-
`based amorphous magnetic cores have been increas(cid:173)
`ingly used as cores for controlling switching power
`source, making the most of their features of having a
`low core loss at high frequencies and having a high
`10 squareness.
`However, the Co-based amorphous alloys have prob(cid:173)
`lems in that not only they are costly because their con(cid:173)
`stituent raw materials are expensive but also they have
`a low saturated magnetic flux density at a frequencies in
`zone of several tens kHz to 100 kHz and therefore they
`suffer from limited working magnetic flux density, thus
`making it difficult to sufficiently miniaturize magnetic
`cores.
`Fe-Based alloys generally have a high saturated mag-
`20 netic flux density and those having a saturated magnetic
`flux density of 15 kG or higher can be obtained but they
`have insufficient soft magnetic characteristics. It is
`known that Fe-based amorphous alloys give rise to
`magnetic cores having a high squareness ratio of a di(cid:173)
`rect current B-H curve and a high maximum permeabil(cid:173)
`ity can be obtained as described in Japanese Patent
`Publication No. 1183/1983.
`However, magnetic cores made of the above(cid:173)
`described Fe-based amorphous alloys have a large iron
`loss and efforts have been made to improve the iron loss
`by adjusting additive elements. However, in spite of
`these efforts, Fe-based amorphous alloys still have a
`large iron loss as compared with Co-based amorphous
`alloys. In addition, Fe-based amorphous alloys have an
`extremely large magnetic strain and are sensitive to
`stress. Therefore, they have a problem that their mag-
`netic characteristics tend to deteriorate due to deforma(cid:173)
`tions as a result of mechanical vibration or by the
`weight of the alloys themselves.
`Turning to an apparatus for producing magnetic ma(cid:173)
`terials, FIG. 1 shows a conventional apparatus for con(cid:173)
`tinuously producing a ribbon made of an amorphous
`alloy according to a so-called single roll method. The
`apparatus has a cooling roll 1 made of Cu Which is
`rotated at a high speed and a nozzle 2 arranged in the
`vicinity of a top portion of the roll 1 which sprays a
`molten metal 3 onto the roll 1 thereby quickly cooling
`the molten metal 3 on the surface of the cooling roll 1
`and solidifying it so that a ribbon can be formed, ribbon
`is drawn in a direction in which the cooling roll 1 ro(cid:173)
`tates.
`In the apparatus shown in FIG. 1, the surface of the
`cooling roll 1 is mirror surface-finished, the nozzle 2 is
`provided substantially vertically at a top portion of the
`cooling roll 1, with the distance between the tip of the
`nozzle and the surface of the cooling roll 1 being set to
`about 1 mm or less. The molten metal 3 discharged from
`the nozzle 2 forms a puddle 4 which is substantially
`stationary between the tip of the nozzle 2 and the sur(cid:173)
`face of the cooling roll 1. As the cooling roll 1 rotates,
`the molten metal 3 is drawn out from the puddle 4 and
`cooled on the surface of the cooling roll 1 to be solidi(cid:173)
`fied in the form of a belt or ribbon, thus continuously
`forming a ribbon 5.
`In this case, soft magnetic alloys generally used as a
`material for making magnetic heads are required to
`have a sufficiently smooth surface, that is, their surface
`roughness must be sufficiently small. However, ribbons
`
`Petitioner Samsung and Google
`Ex-1018, 0021
`
`

`

`5,449,419
`
`3
`produced by the conventional apparatus fail to always
`have a surface roughness small enough to be useful for
`acoustic magnetic heads and accordingly it has been
`strenuously demanded to develop an apparatus for pro(cid:173)
`ducing an alloy ribbon which can give rise to smooth 5
`surfaces.
`A further problem of the conventional apparatus is
`that ribbons produced thereby have a surface rough(cid:173)
`nesses which fluctuates between both surfaces. More
`specifically, in comparison with the roll contacting 10
`surface, which is formed while the molten metal is being
`solidified in contact with the cooling roll, the free solid(cid:173)
`ification surface, which is formed by solidification of
`the molten metal without contact with the roll, has a
`relatively large surface roughness. Because of this de- 15
`feet, it is difficult to use the ribbons as a material for
`making magnetic heads.
`Furthermore, in the case where ribbons are produced
`from a soft magnetic alloy mainly composed of Fe,
`there is a fear that the ribbons tend to be oxidized after 20
`quenching. Accordingly, there has also been a demand
`to produce Fe-based soft magnetic alloy ribbons with(cid:173)
`out being oxidized.
`
`4
`wherein Q represents at least one element selected from
`the group consisting of Co and Ni; T represents at tez.st
`one element selected from the group consisting of Ti,
`Zr, Hf, V, Nb, Ta, Mo and W, with Zr and/or Hf being
`always included; T' represents at least one element
`selected from the group consisting of Cu, Ag, Au, Pi,
`Pd and Pt; a, b, x, y and z are real numbers satisfying
`relationships below:
`0;:§a;:§0.05 atomic %,
`0<b;:§93 atomic %,
`0.5;:§x;:§ 16 atomic %,
`4;:§y;:§ 10 atomic %,
`0;:§z;:§4.5 atomic %
`provided that when 0<z;:§4.5 atomic%, Q represents
`Co and 0<b;:§92 atomic%; and when z=0, 0.5;:§:;;;:§8
`atomic % and 4;:§y;:§9 atomic%.
`According to the second aspect of the present inven(cid:173)
`tion, there is provided a process for heat treating a high
`magnetic flux density alloy, comprising the steps of:
`heating an Fe-based soft magnetic alloy having a high
`saturated magnetic flux density and having a com(cid:173)
`position represented by formula (I) as defined
`above at a temperature no lower than a crystaHiza(cid:173)
`tion temperature, and
`cooling the alloy at a cooling rate of no lower than
`100° C./minute.
`According to the third aspect of the present inven(cid:173)
`tion, there is provided a soft magnetic thin film com(cid:173)
`posed of an Fe-based soft magnetic alloy having a high
`saturated magnetic flux density and having a composi(cid:173)
`tion represented by formula (I) as defined above.
`According to the fourth aspect of the present inven(cid:173)
`tion, there is provided an Fe-based soft magnetic pov1-
`der compact, comprising powder of an Fe-based soft
`magnetic alloy having a high saturated magnetic fiu;:
`density and having a composition represented by for(cid:173)
`mula (I) as defined above, the powder being com(cid:173)
`pressed.
`According to the fifth aspect of the present invention,
`there is provided a process for preparing an Fe-baseri
`soft magnetic alloy powder having a high saturated
`magnetic flux density, comprising the steps of:
`heating an Fe-based soft magnetic alloy having a high
`saturated magnetic flux density and having a com(cid:173)
`position represented by formula (I) as defmed
`above at a temperature no lower than a crystaliiz2-
`tion temperature to render it brittle, and
`pulverizing the alloy.
`According to the sixth aspect of the present inven(cid:173)
`tion, there is provided an apparatus for producing 2.n
`Fe-based soft magnetic alloy ribbon, having a cooling
`roll for cooling a molten metal of an Fe-based soft mag••
`netic alloy, the cooling roll being rotatable and a nozzle
`having a tip, the nozzle being associated with the cool(cid:173)
`ing roll with the tip thereof being arranged in the vici:.7.(cid:173)
`ity of a surface of the cooling roll at a predeterminec;
`distance therefrom and being adapted to spray the mol(cid:173)
`ten metal onto the surface of the cooling roll while the
`cooling roll is rotated in a predetermined direction so
`that the molten metal on the surface of the cooling roil
`can be molded in the form of a ribbon while it is being
`cooled and withdrawn in the direction in which the
`cooling roll is rotated, wherein the cooling roll has aE
`outer peripheral surface portion and an inner portion, at
`least one of the outer peripheral surface portion and the
`inner portion being made of an Fe-based alloy, 2I1ci
`wherein the nozzle is arranged in a slanted state with its
`
`25
`
`40
`
`SUMMARY OF THE INVENTION
`The present invention is intended to provide Fe(cid:173)
`based soft magnetic alloys free of the above-described
`problems, magnetic materials containing such alloys, a
`process and apparatus for producing the magnetic mate(cid:173)
`rials, as well as magnetic transducers using the magnetic 30
`materials.
`An object of the present invention is to provide a soft
`magnetic alloy having a high saturated magnetic flux
`density and a high permeability and at the same time
`having a high mechanical strength and a high thermal 35
`stability.
`Another object of the present invention is to provide
`a process for heat treatment of an Fe-based soft mag(cid:173)
`netic alloy in order to improve the magnetic character-
`istics thereof.
`Still another object of the present invention is to
`provide a soft magnetic thin film having a high satu(cid:173)
`rated magnetic flux density and a high permeability and
`at the same time having a high mechanical strength and
`a high thermal stability.
`Yet another object of the present invention is to pro(cid:173)
`vide a process and apparatus for producing an Fe-based
`soft magnetic alloy ribbon having a high saturated mag(cid:173)
`netic flux density and a high permeability and at the
`same time having a high mechanical strength and a high 50
`thermal stability and also with improved physical(cid:173)
`chemical properties such as surface roughness or extent
`of oxidation.
`Further, an object of the present invention is to pro(cid:173)
`vide magnetic transducers, such as a magnetic cores, a 55
`magnetic heads or a low frequency transformer, to
`which are applied an Fe-based soft magnetic alloy hav(cid:173)
`ing a high saturated magnetic flux density and a high
`permeability and at the same time having a high me(cid:173)
`chanical strength and a high thermal stability as well as 60
`showing a small iron loss.
`According to the first aspect of the present invention,
`there is provided an Fe-based soft magnetic alloy hav(cid:173)
`ing a high saturated magnetic flux density and having a
`composition represented by formula (I) below:
`
`45
`
`65
`
`(I)
`
`Petitioner Samsung and Google
`Ex-1018, 0022
`
`

`

`5,449,419
`
`25
`
`5
`axis being slanted at a predetermined angle with respect
`to an imaginary vertical axis.
`According to the seventh aspect of the present inven(cid:173)
`tion, there is provided an apparatus for producing an
`Fe-based soft magnetic alloy ribbon, having a cooling 5
`roll for cooling a molten metal of an Fe-based soft mag(cid:173)
`netic alloy ribbon, the cooling roll being rotatable and a
`nozzle having a tip, the nozzle being associated with the
`cooling roll with the tip thereof being arranged in the
`vicinity of a surface of the cooling roll at a predeter- 10
`mined distance therefrom and being adapted to spray
`the molten metal onto the surface of the cooling roll
`while the cooling roll is rotated in a predetermined
`direction so that the molten metal on the surface of the
`cooling roll can be molded in the form of a ribbon while 15
`it is being cooled and withdrawn in the direction in
`which the cooling roll is rotated, wherein the cooling
`roll has an outer peripheral surface portion and an inner
`portion, at least one of the outer peripheral portion and
`the inner portion being made of an Fe-based alloy, and 20
`wherein the outer peripheral surface portion has a sur(cid:173)
`face roughness corresponding to that obtainable by
`polishing with a polishing paper having a grain number
`of 100 to 1,000.
`According to the eighth aspect of the present inven(cid:173)
`tion, there is provided a process for producing an Fe(cid:173)
`based soft magnetic alloy ribbon by providing a molten
`metal of an Fe-based soft magnetic alloy, ejecting the
`alloy through a nozzle onto a surface of a cooling roll 30
`being rotated in a predetermined direction, the nozzle
`being associated with the cooling roll with a tip of the
`nozzle being arranged in the vicinity of the surface of
`the cooling roll at a predetermined distance therefrom,
`and withdrawing the ribbon in the same direction as 35
`that in which the cooling roll is rotated, wherein the
`cooling roll has an outer peripheral portion and an inner
`portion, at least one of the outer peripheral portion and
`the inner portion being made of an Fe-based alloy, and
`wherein the nozzle is arranged in a slanted state with its 40
`axis being slanted at a predetermined angle with respect
`to an imaginary vertical axis in the same direction as the
`direction in which the cooling roll is rotated so that the
`molten metal from the tip of the nozzle can be ejected
`onto the surface of the cooling roll which is coming up 45
`to the tip of the nozzle.
`According to the ninth aspect of the present inven(cid:173)
`tion, there is provided a process for producing an Fe(cid:173)
`based soft magnetic alloy ribbon by providing a molten
`metal of an Fe-based soft magnetic alloy, ejecting the 50
`alloy through a nozzle onto a surface of a cooling roll
`being rotated in a predetermined direction, the nozzle
`being associated with the cooling roll with a tip of the
`nozzle being arranged in the vicinity of the surface of
`the cooling roll at a predetermined distance therefrom, 55
`and withdrawing the ribbon in the same direction as
`that in which the cooling roll is rotated, wherein the
`cooling roll has an outer peripheral portion and an inner
`portion, at least one of the outer peripheral portion and
`the inner portion being made of an Fe-based alloy, and 60
`wherein the outer peripheral surface portion has a sur(cid:173)
`face roughness corresponding to that obtainable by
`polishing with a polishing paper having a grain number
`of 100 to 1,000.
`According to the tenth aspect of the present inven- 65
`tion, there is provided a process for producing an Fe(cid:173)
`based soft magnetic alloy ribbon, comprising the steps
`of:
`
`6
`providing a molten metal of an Fe-based soft mag(cid:173)
`netic alloy having a composition represented by
`formula (I) as defined above,
`providing an evacuatable chamber,
`housing a nozzle for ejecting the molten metal and a
`cooling roll in the evacuatable chamber,
`establishing vacuum in the evacuatable chamber,
`ejecting the alloy through the nozzle onto a surface of
`the cooling roll while the roll is being rotated in a
`predetermined direction, the nozzle being associ(cid:173)
`ated with the cooling roll with a tip of the nozzle
`being arranged in the vicinity of the surface of the
`cooling roll at a predetermined distance therefrom,
`to form a ribbon of the alloy, and
`withdrawing the ribbon in the same direction as that
`in which the cooling roll is rotated.
`According to the eleventh aspect of the present in(cid:173)
`vention, there is provided a magnetic core made of an
`Fe-based soft magnetic alloy, wherein said Fe-based
`soft magnetic alloy is composed of a high saturated
`magnetic flux density Fe-based soft magnetic alloy hav(cid:173)
`ing having a composition represented by formula (I) as
`defined above.
`According to the twelfth aspect of the present inven(cid:173)
`tion, there is provided a low frequency transformer
`having an Fe-based soft magnetic alloy and a conductor
`wire, wherein said Fe-based soft magnetic alloy is com(cid:173)
`posed of a high saturated magnetic flux density Fe(cid:173)
`based soft magnetic alloy having a composition repre(cid:173)
`sented by formula (I) as defined above.
`According to the thirteenth aspect of the present
`invention, there is provided a magnetic head having a
`core made of an Fe-based soft magnetic alloy, wherein
`said Fe-based soft magnetic alloy is composed of a high
`saturated magnetic flux density Fe-based soft magnetic
`alloy having a composition represented by formula (I)
`as defined above.
`According to the present invention, there can be
`provided an Fe-based soft magnetic alloy not only hav(cid:173)
`ing soft magnetic characteristics equal to or superior to
`the conventional alloys put into practical use but also
`having a higher saturated magnetic flux density. In
`addition, the soft magnetic alloy of the invention has a
`high mechanical strength and a high thermal stability
`simultaneously.
`From this it follows that the Fe-based soft magnetic
`alloy of the present invention is suitable for magnetic
`transducers such as transformers and choke coils of
`which further reduction in size is demanded, and when
`it is used in these applications i can effectively increase
`performance of the magnetic transducers and reduce
`their size and weight.
`Further, according to the present invention, ribbons
`made of Fe-based soft magnetic alloys can be produced
`continuously in a state in which their physical chemical
`properties such as surface roughness or extent of oxida(cid:173)
`tion are improved.
`Other objects, constructions and effects of the present
`invention will be obvious to one skilled in the art from
`the following detailed explanation with reference to
`accompanying drawings.
`
`BRIEF DESCRIPTION OF THE
`ACCOMPANYING DRAWINGS
`FIG. 1 is a schematic cross-sectional view of a con(cid:173)
`ventional apparatus for producing an amorphous alloy
`ribbon;
`
`Petitioner Samsung and Google
`Ex-1018, 0023
`
`

`

`5,449,419
`
`20
`
`25
`
`7
`FIG. 2 is a schematic cross-sectional view of the
`apparatus for continuously producing an Fe-based soft
`magnetic alloy ribbon according to one embodiment of
`the present invention;
`FIG. 3 is a schematic cross-sectional view of the 5
`apparatus for continuously producing an Fe-based soft
`magnetic alloy ribbon according to another embodi(cid:173)
`ment of the present invention, illustrating the positional
`relationship between the cooling roll and the nozzle;
`FIG. 4 is a schematic fragmentary cross-sectional 10
`view of the apparatus shown in FIG. 3, illustrating the
`angle of slanting of the nozzle