Engineered Magnetization and Exchange Stiffness in Direct-Write Co-Fe Nanoelements

Appl. Phys. Le . 118, 022408 (2021); h ps://doi.o g/10.1063/5.0036361 118, 022408
© 2021 Au ho (s).
Enginee ed magne iza ion and exchange
s i ness in di ec -w i e Co–Fe nanoelemen s
Ci e as: Appl. Phys. Le . 118, 022408 (2021); h ps://doi.o g/10.1063/5.0036361
Submi ed: 04 No embe 2020 . Accep ed: 21 Decembe 2020 . Published Online: 15 Janua y 2021
S. A. Bunyae , B. Budinska, R. Sachse , Q. Wang, K. Le chenko, S. Knaue , A. V. Bonda enko, M.
U bánek, K. Y. Guslienko, A. V. Chumak, M. Hu h, G. N. Kakazei, and O. V. Dob o olskiy
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Enginee ed magne iza ion and exchange s i ness
in di ec -w i e Co–Fe nanoelemen s
Ci e as: Appl. Phys. Le . 118, 022408 (2021); doi: 10.1063/5.0036361
Submi ed: 4 No embe 2020 .Accep ed: 21 Decembe 2020 .
Published Online: 15 Janua y 2021
S. A. Bunyae ,
1
B. Budinska,
2
R. Sachse ,
3
Q. Wang,
2
K. Le chenko,
2
S. Knaue ,
2
A. V. Bonda enko,
1
M. U b
anek,
4
K. Y. Guslienko,
5,6
A. V. Chumak,
2
M. Hu h,
3
G. N. Kakazei,
1
and O. V. Dob o olskiy
2,a)
AFFILIATIONS
1
Ins i u e o Physics o Ad anced Ma e ials, Nano echnology and Pho onics (IFIMUP)/Depa amen o de F
ısica e As onomia,
Uni e sidade do Po o, 4169-007 Po o, Po ugal
2
Facul y o Physics, Uni e si y o Vienna, 1090 Vienna, Aus ia
3
Physikalisches Ins i u , Goe he Uni e si y, 60438 F ank u am Main, Ge many
4
CEITEC BUT, B no Uni e si y o Technology, 61200 B no, Czech Republic
5
Di ision de Fisica de Ma e iales, Dep o. Polime os y Ma e iales A anzados: Fisica, Quimica y Tecnologia,
Uni e sidad del Pais Vasco, UPV/EHU, 20018 San Sebas ian, Spain
6
IKERBASQUE, The Basque Founda ion o Science, 48009 Bilbao, Spain
a)
Au ho o whom co espondence should be add essed: oleksand .dob o olskiy@uni ie.ac.a
ABSTRACT
Media wi h enginee ed magne iza ion a e essen ial building blocks in magnonics, spin onics, and supe conduc i i y. Howe e , he
es ablished hin film and li hog aphic echniques insu ficien ly sui he ealiza ion o plana componen s wi h on-demand- ailo ed
magne iza ion in he la e al dimension. He e, we demons a e he enginee ing o he magne ic p ope ies o CoFe-based nanodisks ab ica ed
by he mask-less echnique o ocused elec on beam-induced deposi ion (FEBID). The ma e ial composi ion in he nanodisks is uned in
si u ia he e-beam wai ing ime in he FEBID p ocess and hei pos -g ow h i adia ion wi h Ga ions. The sa u a ion magne iza ion M
s
and
exchange s i ness Ao he disks a e deduced om pe pendicula spin-wa e esonance measu emen s. The achie ed M
s
a ia ion in he
b oad ange om 720 emu/cm
3
o 1430 emu/cm
3
con inuously b idges he gap be ween he M
s
alues o widely used magnonic ma e ials
such as Pe malloy and CoFeB. The p esen ed app oach pa es he way owa d nanoscale 2D and 3D sys ems wi h con ollable space- a ied
magne ic p ope ies.
V
C2021 Au ho (s). All a icle con en , excep whe e o he wise no ed, is licensed unde a C ea i e Commons A ibu ion (CC BY) license (h p://
c ea i ecommons.o g/licenses/by/4.0/).h ps://doi.o g/10.1063/5.0036361
Magnonics— he s udy o spin wa es and hei use in in o ma ion
p ocessing sys ems—has eme ged as one o he mos apidly
de eloping esea ch fields o mode n magne ism.
1–10
Now, i s key
challenges a e guiding and con ol o spin wa es in 1D (e.g., magnonic
c ys als
11–14
), 2D (e.g., magnonic ci cui s
8,9
), and eme ging 3D
sys ems.
7,15,16
Fo s ee ing o spin wa es, one should change an ex e -
nal pa ame e such as magne ic field
5,17–19
and empe a u e
20–22
o
al e he condui shape
11,23,24
and magne iza ion.
22,25–29
Among hese
app oaches, magne iza ion a ia ion has an ad an age i being passi e
(no cu en o hea in ol ed) and i can be s ongly localized o
g adien - ailo ed on pu pose. Thus, in si u app oaches o uning mag-
ne iza ion in a b oad ange a e s ongly demanded. In his ega d, ion
i adia ion-induced e olu ion o he magne ic pa ame e s o hin films
and nanos uc u es has been a ma e o ex ensi e esea ch.
29–35
Focused elec on beam-induced deposi ion (FEBID) can o e
unique ea u es, which go beyond he s a e-o - he-a ab ica ion ech-
nologies o magnonics.
36
Fi s , he down o 10 nm la e al esolu ion
( o selec ed ma e ials, such as Co–Fe alloys
37
discussed in wha
ollows) makes FEBID sui able o he ab ica ion o nanos uc u es
wi h ea u e sizes compa able o mode n complemen a y me al-oxide
semiconduc ing (CMOS) echnology. Second, he composi ion and
magne ic p ope ies o FEBID nanos uc u es can be uned ia pos -
g ow h i adia ion o s uc u es wi h ions
24,38
and elec ons.
39,40
In
addi ion, FEBID is capable o ab ica ing complex-shaped 3D nano-
a chi ec u es,
41,42
which make i he echnique o choice o s udies in
supe conduc i i y,
43–45
magne ism,
46–48
and magnonics.
7,15,16
In a p e ious s udy, we obse ed he dec ease in he magne iza-
ion M
s
and he exchange s i ness Awi h educ ion o he diame e o
Appl. Phys. Le . 118, 022408 (2021); doi: 10.1063/5.0036361 118, 022408-1
V
CAu ho (s) 2021
Applied Physics Le e s ARTICLE sci a ion.o g/jou nal/apl
indi idual Co–Fe nanodisks.
49
The e ec was a ibu ed o he w i ing
o smalle disks in a deple ed-p ecu so egime, which esul s in a
lowe me al con en . He e, we in oduce a beam wai ing ime ou side
o w i en s uc u es o demons a e on-demand enginee ing o he
magne iza ion and exchange s i ness in indi idual Co–Fe nanodisks
wi h a hickness o 40 nm and a la ge fixed adius R¼500 nm. In ou
s udies, one se ies o nanodisks was ab ica ed using di e en e-beam
wai ing imes in he FEBID p ocess and ano he se ies o nanodisks
was i adia ed wi h di e en doses o Ga ions. The magne iza ion M
s
and exchange s i ness Ao he disks we e deduced om spin-wa e
esonance (SWR) measu emen s, employing a ecen ly de eloped spa-
ially esol ed app oach.
49
We demons a e ha wi h an inc ease in
he e-beam wai ing ime, M
s
o he disks eaches 1430 emu/cm
3
,which
is by a ac o o wo la ge han M
s
o he disks i adia ed wi h Ga
ions. Thus, he combina ion o hese wo app oaches p o ides access
o he ab ica ion o geome ically uni o m magnonic condui s wi h a
d as ic a ia ion o sa u a ion magne iza ion.
The ci cula Co–Fe disks we e ab ica ed by FEBID in a high-
esolu ion dual-beam scanning elec on mic oscope (SEM: FEI No a
NanoLab 600) employing HCo
3
Fe(CO)
12
as p ecu so gas.
37,50
FEBID
was done wi h 5 kV/1.6 nA, 20 nm pi ch, and 1 ls dwell ime, using a
se pen ine scanning s a egy, see Fig. 1(a). All disks we e w i en wi h
1632 beam passes, deduced om a hickness calib a ion by a omic
o ce mic oscopy (AFM). Two se ies o samples used in ou s udies
a e desc ibed nex .
The fi s se ies o samples is a se o ou disks deposi ed on o a
Si/SiO
2
(200 nm) subs a e, w i en wi h di e en beam wai ing imes.
A e each pass o he elec on beam o e he disk su ace, he beam
was “pa ked” o he ime s a ied om s0¼0 os3¼50 ms ou side
o he disk. The essen ial s eps o he w i ing p ocess a e illus a ed in
Fig. 1(a). All disks om he fi s se ies exhibi a fla mo phology,
Fig. 1(d). The hickness a ia ion o he disks w i en wi h di e en s
i
did no exceed 0.5 nm.
The subs a e was moun ed on o a ansla ional s age o hei
ace- o- ace posi ioning unde he 2-lm-wide and 6-lm-long ac i e
pa o an Au coplana wa eguide (CPW), Fig. 1(c).TheCPWwas
p epa ed by e-beam li hog aphy om a 55-nm- hick Au film dc-mag-
ne on-spu e ed on o a Si/SiO
2
(200 nm) subs a e wi h a 5-nm- hick
C bu e laye . The CPW was co e ed wi h a 5-nm- hick TiO
2
laye
o elec ical insula ion om he disks. SWR measu emen s on bo h
sample se ies we e aken a he fixed equency o 9.85 GHz wi h he
magne ic field o ien ed pe pendicula ly o he disk plane, Fig. 1(c).
The second se ies o samples e e s o ou s a es o a disk w i en
wi h s0¼0 on he CPW and i adia ed wi h 30 keV Ga ions up o a
cumula i e dose D
3
o 15 pC/lm
2
in s eps o 5 pC/lm
2
,Fig. 1(b).
SRIM simula ions o he dis ibu ion o 30 keV Ga ions implan ed in
he Co-Fe disks indica e ha i has a gen le-dome shape sp eading
h ough he en i e disk hickness, wi h he la ges numbe o s opped
Ga ions in he dep h ange om 13 nm o 28 nm, see he inse in
Fig. 1(b). In consequence o he ion i adia ion, he disk hickness
dec eased o 36.8 60.5 nm o D3¼15 pC/lm
2
,Fig. 1(d),whichwas
accompanied by an inc ease in he su ace oughness.
Fo he analy ical desc ip ion o he field alues o esonance
peaks, we conside ed azimu hally symme ic spin-wa e modes in a hin
cylind ical disk sa u a ed in he ou -o -plane di ec ion by he biasing
magne ic field H. In his case, he exci ed spin-wa e eigenmodes can be
desc ibed by Bessel unc ions o he ze o h o de because o he axial
symme y o he samples. The de ails o he analy ical heo y can be
ound elsewhe e.
51
This app oach allows o he deduc ion o M
s
and A
wi h high p ecision.
Figu e 2 p esen s he expe imen ally measu ed SWR spec a
as a unc ion o he ou -o -plane magne ic field H o he disks
i adia ed wi h di e en doses o Ga ions and he disks deposi ed
wi h di e en elec on beam wai ing imes. In all cases, he mos
in ense esonance peak is obse ed a he la ges field ha co e-
sponds o he lowes spin-wa e mode numbe n¼1. On he low-
field side, he main esonance is accompanied by a se ies o peaks
wi h a mono onously dec easing ampli ude. Such a spin-wa e
spec um is ypical o confined ci cula nanodo s.
51
We obse e
ha he wo used app oaches lead o shi s o he SWR fields in
opposi e di ec ions wi h espec o he e e ence s a e (D0¼0;
s0¼0). A he same ime, he shape and he in e modal dis ance
pa e n e ol e consis en ly, which is indica i e o composi ional
uni o mi y and magne ic homogenei y o he samples. A e in e-
g a ion and sub ac ion o he backg ound, he expe imen al spec-
a we e fi ed o mul ipeak Lo en zian unc ions o ob ain he
esonance fields o each mode.
FIG. 1. (a) Illus a ion o he FEBID p ocess o he fi s se ies o disks: a e each
pass o e he sample su ace (1), he beam is pa ked ou side o he disk o he
gi en ime s
i
(2). The w i ing p ocess is con inued un il he desi ed disk hickness is
achie ed (3). (b) In he second se ies o measu emen s, a Co–Fe disk is i adia ed
by 30 keV Ga ions wi h di e en doses D
i
. Inse : simula ed dis ibu ion o s opped
Ga ions ac oss he disk hickness. (c) Expe imen al geome y (no o scale). A sub-
s a e wi h a se ies o Co–Fe nanodisks is placed ace- o- ace o a gold coplana
wa eguide o spin-wa e exci a ion in he ou -o -plane bias magne ic field H. (d)
A omic o ce mic oscopy image o he e e ence disk (s0¼0;D0¼0) and i s su -
ace mo phology in compa ison wi h he ion-i adia ed disk wi h D3¼15 pC/lm
2
.
Applied Physics Le e s ARTICLE sci a ion.o g/jou nal/apl
Appl. Phys. Le . 118, 022408 (2021); doi: 10.1063/5.0036361 118, 022408-2
V
CAu ho (s) 2021
A heo e ical model
51
was applied o fi he expe imen al da a
using M
s
and Aas wo fi ing pa ame e s and assuming he gy omag-
ne ic a io o c=2p¼3:05 MHz/Oe.
52
In he supplemen a y ma e ial,
we demons a e ha a a ia ion o he gy omagne ic a io by 3% in
he fi s is equi alen o a a ia ion o M
s
and Aby less han 1% so ha
he gy omagne ic a io is assumed o be cons an o all samples. In
consequence o he ion-i adia ion e ching o he disks om he
second se ies, we used 39, 38, and 37 nm o hei hicknesses a e he
i adia ion s eps D
1
–D
3
, espec i ely. The applica ion o a leas -
squa es algo i hm allowed us o deduce he magne ic pa ame e s o
all indi idual nanodisks wi h a p ecision o abou 5%. Figu e 3 illus-
a es ha he bes heo e ical fi s (solid lines) nicely desc ibe he
expe imen al da a (symbols). We no e ha he loca ion o he main
esonance peak is p ima ily de e mined by M
s
. The alue o Aonly
weakly a ec s he posi ion o he main esonance peak; howe e , i
s ongly a ec s he posi ions o he highe -o de peaks.
The deduced M
s
and A alues a e epo ed in Figs. 4(a) and 4(b).
The field-sweep esonance linewid h, de e mined as he peak- o-peak
dis ance in Fig. 2(b),isp esen edinFig. 4(c). We nex analyze hei
e olu ionincompa isonwi h hecomposi iono hedisksin e ed
om ene gy-dispe si e x- ay (EDX) spec oscopy. The EDX was
done a 3 kV/1.6 nA, co esponding o a disk hickness emi ing x
ays o abou 35 nm, as es ima ed by Mon e Ca lo simula ions
(Casino). While he p obed laye hickness should be smalle han
he disk hickness in all cases, he open symbols in Fig. 4(d) ep e-
sen he co ec ed da a whe e he po en ial oxygen loss om he
subs a e (þ3 a . % a e each i adia ion s ep) is aken in o
FIG. 2. Expe imen ally measu ed SWR spec a a 9.85 GHz o a se ies o 40-nm-
hick Co-Fe disks wi h adius R¼500 nm i adia ed wi h Ga ions a di e en doses,
as indica ed (a) and deposi ed wi h di e en elec on beam pa king imes (b). The
esonance mode numbe nand he peak- o-peak esonance linewid h a e
indica ed.
FIG. 3. Dependences o he esonance field H es on he spin-wa e mode numbe n
o he disks i adia ed wi h Ga ions a di e en doses and disks deposi ed wi h di -
e en pa king imes o he elec on beam a e each pass. Symbols: expe imen .
Solid lines: fi s o he analy ical heo y
51
wi h he magne iza ion Msand he
exchange cons an A a ied as fi ing pa ame e s, as epo ed in Fig. 4, and he
gy omagne ic a io c=2p¼3:05 MHz/Oe.
FIG. 4. E olu ion o he magne iza ion M
s
(a), he exchange cons an A(b), he line-
wid h (c), and he disk composi ion (d) wi h he inc ease in he elec on beam wai -
ing ime (s
1
–s
3
, ligh blue backg ound) and he Ga ion i adia ion dose (D
1
–D
3
, ligh
magen a backg ound). In (d), open symbols a e he da a co ec ion accoun ing o
a possible oxygen loss om he subs a e by þ3 a . % a e each i adia ion s ep.
Dashed lines a e guides o he eye.
Applied Physics Le e s ARTICLE sci a ion.o g/jou nal/apl
Appl. Phys. Le . 118, 022408 (2021); doi: 10.1063/5.0036361 118, 022408-3
V
CAu ho (s) 2021
accoun . The EDX da a in Fig. 4(d) e eal an inc ease in he
[CoþFe] con en om abou 75 a . % in he e e ence sample
(s0¼0) o abou 87 a . % o he sample w i en wi h he beam
pa king ime s3¼50 ms, Fig. 4(d). The inc ease in he me al con en
co ela es well wi h he inc ease in M
s
and Aand he dec ease in he
linewid h in Fig. 4. In con as , i adia ion wi h Ga ions causes a deg a-
da ion o he magne ic p ope ies o he nanodisks, leading o a educ-
ion o M
s
and A, and an inc ease in he linewid h.
The pa icula alues o sand Dwe e chosen as a scale ac o in
Fig. 4 o demons a e in one plo he opposi e cha ac e o he used
app oaches and he whole uning ange o M
s
and A o Co-Fe nano-
s uc u es. The da a in Fig. 4(a) sugges ha M
s
can be a ied by a ac-
o o abou wo, which o e s su ficien flexibili y, e.g., o he design
o g aded-index magnonic condui s
23,26,27
and magnonic c ys-
als.
11,13,14
The da a in Figs. 4(c) and 4(d) indica e ha a dec ease in
he me al con en in he disks by abou 35 a . % is accompanied by a
ac o -o - wo linewid h b oadening. Ye , we no e ha he linewid h
(90 Oe a 9.85 GHz) in he mos CoFe- ich disk is a ac o o abou
wo la ge han in spu e ed Py films.
53
Rega ding he physical eason o he la ge M
s
and Ain he disks
w i en wi h longe e-beam wai ing ime, we need o se in o pe spec-
i e he equen obse a ion ha he me al con en ends o inc ease
wi h inc easing beam cu en in he deple ed egime,
54
and ou obse -
a ion ha he me al con en —and hus M
s
and A—inc eases wi h
inc easing beam wai ing ime. F om ou ecen s udy on he a e age
p ecu so esidence ime o HCo
3
Fe(CO)
12
,
55
we can calcula e ha he
s a iona y p ecu so co e age unde he g ow h condi ions used he e
is only abou 0.0065 monolaye s, which is deple ed in a beam dwell
e en by abou 40%. Wi h a calcula ed a e age esidence ime a oom
empe a u e o abou 17 ls and a loop ime o 490 ls, p ecu so
eplenishmen is al eady comple ed wi hin one loop. We hus con-
clude ha he e ec o he addi ional wai ing ime o he disks s udies
he e is no ha o p ecu so eplenishmen . We a he specula e ha
he wai ing ime allows o a mo e comple e he mally induced
ca bonyl ligand deso p ion, esul ing in an inc eased me al con en .
As o he smalle M
s
and Ain he i adia ed disks, deg ada ion
o e omagne ic p ope ies in consequence o ion i adia ion is a well-
known e ec .
29–35
We no e ha ion i adia ion can lead o a di e en
mic os uc u e om he o iginal ma e ial, such as, e.g., changes in he
la ice pa ame e , g ain sizes, and new phase o ma ion.
31
While an
i adia ion-induced inc ease in he su ace oughness has been
e ealed by AFM, a comp ehensi e mic os uc u al cha ac e iza ion o
ion-i adia ed Co–Fe has o emain o u he in es iga ions.
To summa ize, we ha e demons a ed a me hodology o he
magne iza ion and exchange s i ness enginee ing in Co–Fe nanodisks.
The disks we e ab ica ed by he di ec -w i e nano ab ica ion echnol-
ogy o ocused elec on beam-induced deposi ion. The analysis o he
pe pendicula SWR measu emen da a e ealed an inc ease in he
magne iza ion M
s
and he exchange s i ness Ain he disks w i en
wi h longe e-beam wai ing ime and a educ ion o M
s
and Ain disks
i adia ed wi h Ga ions. The dec ease in M
s
and Ain conjunc ion wi h
he linewid h inc ease eflec s a deg ada ion o he magne ic p ope ies
and a highe inhomogenei y o he disks i adia ed wi h Ga ions.
Specifically, he achie ed a ia ion o M
s
om abou 720 emu/cm
3
o
abou 1430 emu/cm
3
allows o i s enginee ing in a b oad ange,
con inuously b idging he gap be ween he M
s
alues o widely used
magnonic ma e ials such as Py and CoFeB.
13
In conjunc ion wi h a
spin-wa e decay leng h in he ange o 5–7 lm,
24
his makes Co–Fe an
in e es ing ma e ial o nanomagnonics. The M
s
uning is accompa-
nied by a a ia ion o he exchange s i ness in he ange o
1:35 106e g/cm o 2:07 106e g/cm and he field-sweep FMR
linewid h be ween 190 Oe and 90 Oe. The epo ed app oach opens a
way owa d nanoscale 2D and 3D sys ems wi h ully con ollable and
space- a ying magne ic p ope ies.
See he supplemen a y ma e ial o Fig. S1, which illus a es he
accu acy o he de e mina ion o M
s
and Aupon a ia ion o he gy o-
magne ic a io and he disk hickness.
The au ho s a e e y g a e ul o S en Ba h (Goe he Uni e si y
F ank u ) o p o iding he p ecu so . O.V.D. acknowledges he
Aus ian Science Fund (FWF) o suppo h ough G an No. I
4889 (Cu iMag). The Po uguese eam acknowledges he Ne wo k
o Ex eme Condi ions Labo a o ies-NECL and Po uguese
Founda ion o Science and Technology (FCT) suppo h ough
P ojec Nos. NORTE-01-0145-FEDER-022096, POCI-0145-
FEDER-030085 (NOVAMAG), PTDC/FIS-MAC/31302/2017, and
EXPL/IF/00541/2015. B.B. acknowledges financial suppo om he
Vienna Doc o al School in Physics (VDSP). K.L. and A.V.C.
acknowledge he Aus ian Science Fund (FWF) o suppo h ough
G an No. I 4696. K.Y.G. acknowledges suppo om IKERBASQUE
( he Basque Founda ion o Science). The wo k o K.Y.G. was
suppo ed by he Spanish Minis e io de Ciencia, Inno acion y
Uni e sidades G an No. FIS2016-78591-C3-3-R. A.V.C. and Q.W.
acknowledge suppo wi hin he ERC S a ing G an No. 678309
MagnonCi cui s. Suppo h ough he F ank u Cen e o Elec on
Mic oscopy (FCEM) is g a e ully acknowledged. Fu he mo e,
suppo om he Eu opean Coope a ion in Science and Technology
ia COST Ac ion No. CA16218 (NANOCOHYBRI) is acknowledged.
DATA AVAILABILITY
The da a ha suppo he findings o his s udy a e a ailable
wi hin he a icle and i s supplemen a y ma e ial.
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