A icle h ps://doi.o g/10.1038/s41467-024-49838-1
S ong angula and spec al na owing o
elec oluminescence in an in eg a ed Tamm-
plasmon-d i en halide pe o ski e LED
Zhe Ying Ooi
1
, Albe o Jiménez-Solano
2,3
,K zysz o Gałkowski
4,5,6
,
Yuqi Sun
4
, Jo di Fe e O i
4,7
, Kyle F ohna
4
, Hayden Salway
1
,
Simon Kahmann
1,4
, Shenyu Nie
1
, Guadalupe Vega
3,8
,ShaoniKa
4
,
MichałP. Nowak
9
, Sebas ian Maćkowski
5
,Pio Nyga
9
, Ca e ina Duca i
7
,
Neil C. G eenham
4
, Be ina V. Lo sch
2,10,11
,MiguelAnaya
1,8
&
Samuel D. S anks
1,4
Nex -gene a ion ligh -emi ing applica ions such as displays and op ical
communica ions equi e judicious con ol o e emi ed ligh , including
in ensi y and angula dispe sion. To da e, his emains a challenge as con-
en ional me hods equi e cumbe some op ics. He e, we epo highly di ec-
ional and enhanced elec oluminescence om a solu ion-p ocessed quasi-2-
dimensional halide pe o ski e ligh -emi ing diode by building a de ice
a chi ec u e o exploi hyb id plasmonic-pho onic Tamm plasmon modes. By
exploi ing he p ocessing and bandgap unabili y o he halide pe o ski e
de ice laye s, we cons uc he de ice s ack o op imise bo h op ical and
cha ge-injec ion p ope ies, leading o na ow o wa d elec oluminescence
wi h an angula ull-wid h hal -maximum o 36.6° compa ed wi h he con-
en ional iso opic con ol de ice o 143.9°, and na ow elec oluminescence
spec al ull-wid h hal -maximum o 12.1 nm. The de ice design is e sa ile and
unable o wo k wi h emission lines co e ing he isible spec um wi h desi ed
di ec ionali y, hus p o iding a p omising ou e o modula , inexpensi e, and
di ec ional ope a ing ligh -emi ing de ices.
In he pas decade, ligh -emi ing diodes (LEDs) ha e domina ed he
ligh emission ma ke in applica ions such as ligh ing, indica o s
and displays hanks o hei ou s anding pe o mance including
long li e imes, low ene gy consump ion, as swi ching, small size
and high obus ness1,2. Whe eas c ys alline epi axially g own III-V
semiconduc o s3,4a e s ill domina ing he ligh ing ma ke , new gen-
e a ion emi ing ma e ials such as solu ion-p ocessed quan um do s5,
o ganics6and polyme s7a e now finding ac ion pa icula ly in he
display ma ke . Mo e ecen ly, solu ion-p ocessible halide pe o ski es
ha e eme ged as popula op oelec onic ma e ials wi h ema kable
Recei ed: 11 Ap il 2023
Accep ed: 21 June 2024
Check o upda es
1
Depa men o Chemical Enginee ing and Bio echnology, Uni e si y o Camb idge, Camb idge, UK.
2
Max Planck Ins i u e o Solid S a e Resea ch, Hei-
senbe gs asse 1, 70569 S u ga , Ge many.
3
Depa amen o de Física, Uni e sidad de Có doba, EdificioEins ein(C2),CampusdeRabanales,14071
Có doba, Spain.
4
Ca endish Labo a o y, Uni e si y o Camb idge, Camb idge, UK.
5
Ins i u e o Physics, Facul y o Physics, As onomy and In o ma ics, Nicolaus
Cope nicus Uni e si y, To uń,Poland.
6
Depa men o Expe imen al Physics, Facul y o Fundamen al P oblems o Technology, W oclaw Uni e si y o Science
and Technology, W oclaw, Poland.
7
Depa men o Ma e ials Science and Me allu gy, Uni e si y o Camb idge, Camb idge, UK.
8
Depa amen o Física de la
Ma e ia Condensada, Ins i u o de Ciencia de Ma e iales de Se illa, Uni e sidad de Se illa−CSIC, Calle Amé ico Vespucio 49, Se illa 41012, Spain.
9
Ins i u e o
Op oelec onics, Mili a y Uni e si y o Technology, Wa saw, Poland.
10
Depa men o Chemis y, Ludwig-Maximilians-Uni e si ä (LMU), Bu enand s asse 5-13,
81377 Munich, Ge many.
11
e-con e sion, Lich enbe gs asse 4a, 85748 Ga ching, Ge many. e-mail: [email p o ec ed];[email p o ec ed]
Na u e Communica ions | (2024) 15:5802 1
1234567890():,;
1234567890():,;
p ope ies, including bandgap unabili y, high ca ie mobili y and
high luminescence e ficiency8,9, which makes hem p omising candi-
da es o he nex gene a ion ligh ing echnologies. To ully exploi he
p ope ies o hese ma e ials in a ange o ligh applica ions, absolu e
con ol o he emission p ope ies ia he implemen a ion o efined
ligh managemen me hods will be c ucial.
Con en ional pho on managemen s a egies include imple-
men a ion o plasmonic wa eguides10–16, pho onic ca i ies17–21,and
hyb id ca i ies22. Plasmonic wa eguides ha e s ong ligh confinemen
o s ong enhancemen o op ical field and op ical o ce bu he
plasmonic me al a enua es elec omagne ic fields hus o ming sho -
anged plasmonic e ec s23,24. Pho onic sys ems ha e longe ange,
howe e , he confinemen ac oss he emi ing laye is ypically lowe
han he plasmonic analogues22,25. A long- anged and s ongly confined
hyb id plasmonic-pho onic s uc u e is an a ac i e solu ion. Tamm
plasmons a e localised su ace s a es ha a e confined a he me al
(plasmonic)-pho onic-c ys al in e ace, wi h me al deposi ed di ec ly
on he high e ac i e index laye o he pho onic c ys al26,27.The
Tamm plasmon esonance can be uned ac oss he pho onic s opband
o he pho onic c ys al by a ying he hickness o he op high
e ac i e index laye a he in e ace27. Unlike con en ional su ace
plasmons, Tamm plasmons o m bo h ans e se elec ic and mag-
ne ic mode pola isa ions wi h dispe sion wi hin he ligh cone, and
hus can be op ically exci ed wi hou addi ional op ical p isms o
g a ings27. The Tamm plasmon modes a e ound in simple plana
s uc u es which a e ela i ely easy o ab ica e, easy o design and
une, and could easily ans o m in o a de ice a chi ec u e. These
ema kable p ope ies o Tamm plasmon modes ha e p omp ed hei
de elopmen o a a ie y o op ical applica ions such as op ical
coa ings wi h dye-doped nanosphe es28, III-V semiconduc o lase s29,
o ganic sola cells30 and quan um do -based single pho on sou ces31.
In his wo k, we employ a halide pe o ski e ligh -emi ing diode
(PeLED) de ice d i en by Tamm plasmon modes o p ecise angula
and colou con ol. Wi h ca e ul con ol o he s uc u e, we une he
Tamm plasmon esonance wa eleng h o ma ch he pe o ski e elec-
oluminescence (EL) peak and hus confine he Tamm plasmon modes
wi hin he en i e pe o ski e laye . The Tamm plasmon esonance
modes enhance he pe o ski e EL in o wa d di ec ion by a ac o o 1.8
compa ed o he e e ence, and ou couple ligh modes e ficien ly wi h
na ow and con ollable angula dispe sion wi h angula ull-wid h
hal -maximum (FWHM) o 36.6° compa ed o 143.9° o he con ol. As
a plasmonic sys em, he Tamm plasmon modes show s onge con-
finemen o he elec omagne ic field han he ull pho onic mic o-
ca i ies, hus a ac i e o PeLEDs as he pe o ski e film is ypically
hin. The app oach is e sa ile and uneable ac oss di e en emi ing
ene gies and angles, hus opening a enues o wide applica ions in
display and ligh sou ces which equi e fine con ol o he angula
dispe sion and in ensi y o emi ed ligh .
Resul s
De elopmen o pe o ski e-based Tamm plasmon s uc u e
We fi s employ a ans e ma ix model powe ed by a gene ic algo-
i hm (see Me hods o u he de ails) o es ablish he op imum
combina ion o ma e ials and hickness o each laye o achie e a s ong
Tamm plasmon esonance confined ac oss he en i e quasi-2-
dimensional (2D) pe o ski e laye (Supplemen a y Fig. 1). A quasi-2D
(PEA)
2
(CsPbB
3
)
n−1
PbB
4
pe o ski e (PEA: 2-phenyle hylamine, Cs: cae-
sium, Pb: lead, B : b omide) is employed and op imised o ealise a
smoo h hin film wi h pho oluminescence (PL) peak wa eleng h a ound
510 nm (Supplemen a y Fig. 1). This ma e ial o e s high b igh ness,
pho oluminescence quan um yield and ex e nal quan um e ficiency
(EQE) when inco po a ed in LEDs due o dielec ic and quan um con-
finemen e ec s go e ned by he o ma ion o lowe dimensional
halide pe o ski e s uc u es32,33 (Supplemen a y Fig. 2). We show using
simula ions ha using sil e (Ag) as he Tamm plasmon me al laye
achie es he highes enhancemen o elec ic field wi hin he pe o ski e
laye compa ed wi h aluminium (Al) and gold (Au) (Supplemen a y
Fig. 3). This is due o small ohmic loss o Ag (low imagina y pe mi i i y
o dielec ic cons an ) ac oss he isible spec um34.
Acco ding o he op imised simula ion design, we hen expe i-
men ally ab ica ed he pe o ski e-based Tamm-plasmon s uc u e. As
shown in he c oss-sec ional high-angle annula da k field scanning
ansmission elec on mic oscopy (HAADF-STEM) image (Fig. 1a) and
ene gy dispe si e X- ay (EDX) spec oscopy chemical composi ion
map (Fig. 1b), he op imised Tamm-plasmon-based pe o ski e s uc-
u e has smoo h and uni o m in e aces ac oss each laye and he
hickness o each laye closely ma ches he op imised design om
simula ion (Fig. 1c). The pe o ski e-based Tamm-plasmon s uc u e
employed he e is made up o a 1-dimensional pho onic c ys al com-
p ising 3 pai s o al e na ing i anium dioxide (TiO
2
)andsilicondiox-
ide (SiO
2
) laye s, a hin ( oughly 10 nm o minimise op ical e ec s)
laye o poly inylca bazole (PVK), a quasi-2D pe o ski e film and a
sil e laye . The hin PVK laye is added o ensu e consis ency o pe -
o ski e g ow h on di e en subs a es and will ac as he e en ual hole
anspo laye wi hin he PeLEDs. The quasi-2D pe o ski e film wi h a
e ac i e index o n= 2.05 (a 510 nm) eplaces he TiO
2
laye (n=2.35
a 510 nm) as he bo om pho onic c ys al laye a he me al-pho onic-
c ys al in e ace (see Supplemen a y No e 1 o de ails o pho onic
c ys al). The quasi-2D pe o ski e film is placed a he me al-pho onic-
c ys al in e ace as he Tamm plasmon modes a e s ongly confined a
he me al-pho onic-c ys al in e ace. F om he simula ion shown in
Fig. 1c, we obse e ha he Tamm plasmon esonance enhances and
confines elec ic field in ensi y a he me al-pho onic-c ys al in e ace,
and he enhancemen spans he en i e pe o ski e laye when con-
side ing he emission wa eleng h o 510 nm.
Fine uning o he Tamm plasmon esonance is ealised by a ying
he hickness o he final high e ac i e index laye a he me al-
pho onic-c ys al in e ace26,27,34.Wefinely manipula e he pe o ski e
hicknesses be ween 20 nm o 54 nm by uning he concen a ion o
pe o ski e p ecu so s (Fig. 1d). The esul ing pe o ski e hicknesses
a e es ima ed wi h a omic o ce mic oscopy (AFM) (Supplemen a y
Fig. 4). The AFM hickness measu emen s a e in excellen ag eemen
wi h he HAADF-STEM imaging and he fi ed simula ion esul s om
he Tamm plasmon esonance wa eleng h, wi h esul ing e o wi hin
±3 nm (Fig. 1e). We no e ha he Tamm plasmon esonance wa e-
leng hs om Fig. 1d, e a e measu ed using an in eg a ing sphe e whe e
he sample is il ed a 8° (see Me hods o de ails); he Tamm plasmon
esonance a 0° is es ima ed o be ca. 3 nm ed-shi ed om his alue.
In Fig. 1e, i is seen ha he expe imen ally measu ed Tamm plasmon
esonance linea ly ed shi s om 485 nm o 565 nm as he pe o ski e
hickness inc eases om 20 nm o 54 nm. F om hese samples, we
ound ha a pe o ski e hickness o 26 nm in he pe o ski e-based
Tamm plasmon s ack gi es a ma ching Tamm plasmon esonance wi h
he pe o ski e film PL wa eleng h (dashed black line).
Di ec ionali y o he pe o ski e-based Tamm plasmon s uc u e
To con ex ualise he p ope ies o ou pe o ski e-based Tamm plas-
mon s uc u e, we fi s define a e e ence pe o ski e s uc u e as he
glass/PVK/quasi-2D pe o ski e/Ag s ack which has iden ical laye s o
he Tamm-plasmon s uc u e discussed abo e bu elimina ing he
TiO
2
/SiO
2
laye s ha comp omise he pho onic c ys al. We obse e a
sho ened PL li e ime ac oss a ange o fluences in he e e ence-
pe o ski e s ack (li e ime o 1.5 ns) compa ed o he e e ence-
pe o ski e s uc u e wi hou Ag (li e ime o 3.7 ns) (Supplemen a y
Fig. 5), indica ing he di ec deposi ion o Ag on pe o ski e quenches
he PL h ough inc eased non- adia i e ecombina ion a he
in e ace35,36. By he e e ence pe o ski e defini ion,we uleou he
e ec o he Tamm plasmon esonance in ou e e ence-pe o ski e
s ack while e aining he quenching e ec o Ag on he pe o ski e. As
showninFig.2a, b, he PL o ou e e ence-pe o ski e s uc u e ollows
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 2
a Lambe ian emission p ofile, which is compa able o he fini e-
di e ence ime-domain simula ion (Fig. 2c) and is ypical o iso opic
emi e s37. The PL maximum o he e e ence-pe o ski e s uc u e is
cons an a 510 nm ac oss all angles.
Compa ing Fig. 2a, d, he PL linewid h o he pe o ski e-based
Tamm plasmon s uc u e wi h pe o ski e hickness o 26 nm (FWHM
o 16.9 nm) is significan ly na owe han he e e ence-pe o ski e
sample (FWHM o 29.1 nm). We obse e ha he PL in ensi y o he
pe o ski e-based Tamm plasmon s uc u e wi h pe o ski e hickness
o 26nm is enhanced and peaks a 510 nm in he o wa d di ec ion (0°
o no mal) (Fig. 2d). Thus, we e e o his sample as he na ow-angle-
Tamm-plasmon-pe o ski e s ack because he Tamm plasmon eso-
nance ma ches he pe o ski e PL a na ow angles. As he angle
inc eases, he PL in ensi y is supp essed and sligh ly blue-shi ed. This
obse a ion is concomi an wi h he blue-shi ing o he Tamm plas-
mon esonance a inc easing angles in a Tamm plasmon sys em27.As
showninFig.2e, he na ow-angle-Tamm-plasmon-pe o ski e exhibi s
sha p emission di ec ionali y wi h angula FWHM o 44.7° compa ed
o 124.5° o he e e ence pe o ski e wi h he same exci a ion powe
densi y (exci ed wi h a 405 nm lase ). While all samples we e exci ed a
he same exci a ion in ensi y, he na ow-angle-Tamm-plasmon-pe -
o ski e shows s ong enhancemen by a ac o o 2.6 in o wa d
emission wi hin a solid angle o ±15° pe pendicula o he sample
su ace (calcula ions in Me hods), which is c ucial in applica ions ha
equi e o wa d emission.
In Supplemen a y Fig. 5, we obse e no significan changes in PL
li e ime o he na ow-angle-Tamm-plasmon-pe o ski e compa ed
wi h he e e ence pe o ski e s uc u e conside ing small sample- o-
sample a ia ion, which is consis en wi h o he plana confined sys-
ems ope a ing unde weak confinemen egime and epo ed e y
small <10% changes38–41. The simula ed abso p ion ac oss he en i e
pe o ski e laye a he exci a ion wa eleng h o 405 nm wi hin bo h
he e e ence-pe o ski e s uc u e and he na ow-angle-Tamm-plas-
mon-pe o ski e s uc u e a e compa able (Supplemen a y Fig. 6), hus
showing he o wa d enhancemen in PL is p ima ily due o he Tamm
plasmon modes esona ing a he emission wa eleng h o 510 nm
a he han pho on ecycling by e-abso p ion- e-emission e en s. We
also no e ha bo h samples ha e uni o m spa ial uni o mi y o PL
(Supplemen a y Fig. 7). Indeed, he enhanced di ec ional emission o
he na ow-angle-Tamm-plasmon-pe o ski e s uc u e obse ed
expe imen ally is also compa able o he simula ion shown in Fig. 2 .
Thus, we epo s ongly di ec ional emission wi h ou na ow-angle-
Tamm-plasmon-pe o ski e s uc u e.
We demons a e ha he pe o ski e-based Tamm plasmon
s uc u e o e s e sa ile adjus men o he emission di ec ionali y
be ween 0° o 40° by uning he quasi-2D pe o ski e hickness
be ween 26 nm and 54 nm (Supplemen a y Fig. 8). Taking he
pe o ski e-based Tamm plasmon sample wi h pe o ski e hickness o
50 nm as an example, we obse e a significan ly ed-shi ed PL a small
angles (Fig. 2g), which ma ches he Tamm plasmon esonance mode
Fig. 1 | De elopmen o he pe o ski e-based Tamm plasmon s uc u e. a C oss-
sec ional HAADF-STEM image o he pe o ski e-based Tamm plasmon s uc u e.
Le : Magnified image o he me al-quasi-2D pe o ski e in e ace. The scale ba
shows 50 nm. A simila s uc u e is ab ica ed as he e e ence-pe o ski e s uc u e
(wi hou TiO
2
/SiO
2
laye pai s) o ensu e esul s a e no a ec ed by unwan ed
e ec s, e.g., PL quenching due o me al deposi ion. The hickness o each laye is
TiO
2
= (70 ± 2) nm, SiO
2
= (90 ± 2) nm, quasi-2D pe o ski e + PVK = (34 ± 5) nm, Ag =
(100 ± 5) nm. bEDX chemical map o pe o ski e-based Tamm plasmon s uc u e.
A eas ich in Ag, Cs, Pb, B , C, Si and Ti a e ma ked in he legend. The scale ba
shows 200 nm. The obse ed halo ea u es a he i anium (Ti)- ich in e ace a e
ound o be a sligh composi ional g adien o Ti, while he oxygen composi ion
emains cons an a he in e ace. cSimula ed elec ic field enhancemen , Ejj
2
E0
jj
2o
he na ow-angle-Tamm-plasmon-pe o ski e s uc u e. dExpe imen al op imisa-
ion o pe o ski e-based Tamm-plasmon s uc u e by a ying he pe o ski e
hicknesses be ween 20 nm o 54 nm (Tamm plasmon esonance wa eleng h bes
fi ed wi h ans e ma ix model o es ima e hickness o pe o ski e). Tamm
plasmon esonance dip acqui ed om eflec ance measu emen s a 8°. PL o quasi-
2D pe o ski e hin film on glass is shown as dashed line. eTamm plasmon eso-
nance wa eleng h a 8° e sus pe o ski e film hickness. Pe o ski e hickness is
measu ed unde AFM (solid line) and es ima ed om Tamm plasmon esonance
wa eleng h bes fi ed wi h simula ion (dashed line). Inse : schema ic o he
pe o ski e-basedTamm-plasmon s uc u ewi h a g een a ow indica ing he quasi-
2D pe o ski e laye .
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 3
measu ed a small angles (dashed line). As he angle o emission
inc eases, he PL blue-shi s in esponse o he dispe sion ela ion o
he Tamm plasmon mode27. The highes PL in ensi y is achie ed when
he blue shi ing o he Tamm plasmon esonance ma ches he pe -
o ski e PL posi ion, which is obse ed a a collec ion angle o 40° o
his sample (Fig. 2h). We he ea e e e o hese samples wi h wide-
angled di ec ionali y as he wide-angle-Tamm-plasmon-pe o ski e
s uc u e. The inc ease o emission di ec ionali y angle is dependen
on he inc ease o pe o ski e hickness, which leads o an inc ease in
Tamm plasmon esonance wa eleng h a 0°. The la ge angle emission
di ec ionali y o he wide-angle-Tamm-plasmon-pe o ski e s uc u e
shown expe imen ally in Fig. 2h ma ches he simula ion shown in
Fig. 2i. Resul s o he angle-dependen PL spec a o all wide-angle-
Tamm-plasmon-pe o ski e s uc u es can be ound in Supplemen a y
Fig. 9, demons a ing he e sa ili y o his pho onic pla o m.
Tamm-plasmon-d i en pe o ski e LEDs
To demons a e he e ec in elec oluminescence om ull de ices,
we ab ica e PeLEDs wi h he s uc u e o subs a e/indium in oxide
(ITO)/ poly(4-bu yl iphenylamine) (poly-TPD)/PVK/quasi-2D pe -
o ski e/2,2’,2”-(1,3,5-benzine iyl)- is(1-phenyl-1-H-benzimidazole)
(TPBi)/8-quinolinola o li hium (LiQ)/Ag. He e, he subs a e o e e -
ence PeLEDs and Tamm-plasmon-d i en PeLEDs e e s o glass and
glass/pho onic c ys al subs a e espec i ely. The hole injec ion laye s
we e o med by spin-coa ing laye s o poly-TPD and PVK wi h hick-
ness o ~10 nm and ~5 nm espec i ely. A 40-nm laye o he mally
e apo a ed TPBi ac s as he elec on injec ing laye , ollowed by e a-
po a ed LiQ (3 nm)/Ag (100 nm) as elec odes. Each o he de ice s ack
laye s a e op imised o be ac i e pa s o he pho onic c ys al/me al
combina ions o ealise he Tamm plasmon e ec s (see Supplemen-
a y Fig. 10).
We obse e s ong EL spec al na owing om FWHM o 22.4 nm
in he e e ence PeLEDs o FWHM o 12.1 nm in he na ow-angle-
Tamm-plasmon-d i en PeLEDs (pe o ski e hickness ~26 nm) due o
he sha p Tamm plasmon esonance ma ching he EL peak, as shown
by hedashedlineinFig.3a. The cu en densi y– ol age cu es o he
e e encePeLEDs and na ow-angle-Tamm-plasmon-d i en PeLEDs a e
simila (Fig. 3b), which is consis en wi h he pho onic c ys al laye s
being smoo h and uni o m, and lying below he ITO con ac , hus no
elec ically modi ying he PeLED de ice. The highes o wa d lumi-
nance o he na ow-angle-Tamm-plasmon-d i en PeLEDs eached
21,800 cd m−2which is significan ly highe han he e e ence PeLEDs
Fig. 2 | Pe o ski e-based Tamm plasmon s uc u es show unabili y o he
emission angula dis ibu ion. Expe imen al angula pho oluminescence (PL)
esul s and simula ions o (a–c) e e ence pe o ski e s ack, (d– ) na ow-angle-
Tamm-plasmon-pe o ski e s uc u e wi h quasi-2D pe o ski e hickness o 26 nm
and (g–i) wide-angle-Tamm-plasmon-pe o ski e s uc u e wi h quasi-2D pe o ski e
hickness o 50 nm. a,d,gPL in ensi y o each samples collec ed a inc easing angle
o 0°, 5°, 10°, 20°, 30°, 40°, 50° and 80°. Reflec ance is shown as a dashed line.
b,eDe ec ion angle agains PL o e e ence-pe o ski e s ack and na ow-band-
Tamm-plasmon-based pe o ski e s uc u e wi h PL spec a in eg a ed om
480 nm o 540 nm. hDe ec ion angle agains PL o wide-angle-Tamm-plasmon-
pe o ski e s uc u e wi h PL spec a in eg a ed be ween 505 nm o 565 nm. Lam-
be ian cu e in dashed line. Inse : schema ic o each s uc u e. Since all samples
a e exci ed a he same powe densi y, he in eg a ed PL a e compa able among he
h ee samples. c, ,iFini e-di e ence ime-domain simula ion o angula ou pu
powe o each s uc u e. PL in ensi y o all configu a ions no malised o he PL
in ensi y o na ow-angle-Tamm-plasmon-pe o ski e s uc u e (see colou ba s).
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 4
wi h a maximum o 14,500 cd m-2. Fo applica ions such as displays
whe e o wa d di ec ional emission is c ucial, cu en e ficiency
defined as he a io be ween o wa d luminance and cu en is a mo e
ele an pa ame e o conside 42. Figu e 3c shows ha he maximum
cu en e ficiency o ou Tamm-plasmon-d i en PeLEDs a 61.8 cd A−1is
much highe han he e e ence PeLEDs a 29.6 cd A−1.Weno e ha
whils he e is an enhancemen in he EL in he o wa d di ec ion o
he Tamm plasmon PeLED, he e is a educ ion in o al EQE as ha
quan i y conside s emission in all di ec ions (inse Fig. 3c), which
ma ches he d op in pho oluminescence quan um e ficiency (PLQE) in
he Tamm plasmon PeLED compa ed wi h he e e ence PeLED (see
Supplemen a y No e 2). This obse a ion may ela e o op ical losses
which a e common in coupling sys ems bu could be imp o ed wi h
mo e ca e ul design and imp o ed pe o ski e quali y. Unlike he bulk
pe o ski e coun e pa s, he quasi-2D PeLED shows s onge oll-on
and oll-o in EQE agains cu en densi y (mo e discussion in Sup-
plemen a y No e 3). The PL li e ime o e e ence PeLED and na ow-
angle-Tamm-plasmon-d i en PeLEDs s uc u es shows no significan
changes (mo e discussion in Supplemen a y No e 4 and Supplemen-
a y Fig. 11).
The EL spec a as a unc ion o angle a e plo ed in image maps in
Fig. 3d– . The EL o he e e ence PeLED consis en ly peaks a 513 nm
ac oss all angles and shows a Lambe ian emission p ofile wi h angula
FWHM o 143.9° (whi e dashed line, Fig. 3d). In Fig. 3e, he na ow-
angle-Tamm-plasmon-d i en PeLED shows enhancemen by a ac o o
1.8 in o wa d di ec ional EL wi h na owed angula FWHM o 36.6°
(whi e dashed line) compa ed o he e e ence PeLED. The e is a small
blue shi in he EL spec um om 0° o 30° due o blue shi ing o he
Tamm plasmon modes a inc easing angle. Fu he inc ease in collec-
ion angle leads o s ong supp ession o EL in ensi y as he Tamm
plasmon modes decouple om he o iginal EL o he quasi-2D pe -
o ski e. In Fig. 3 (whi e dashed line), we show wide-angled EL in he
wide-angle-Tamm-plasmon-d i en PeLED by employing hicke
(~54 nm) pe o ski e films. The pe o mance o he wide-angle-Tamm-
plasmon-d i en PeLED is shown in Supplemen a y Fig. 12. The ed-
shi ed EL spec um a small angles g adually blue-shi s wi h
inc easing collec ion angle due o shi ing in Tamm plasmon eso-
nance modes and he EL in ensi y peaks when Tamm plasmon modes
esona e a he pe o ski e EL. This esul again demons a es he e -
sa ili y o he emission pla o m.
Discussion
The EL angula esponse o bo h he na ow-angle and wide-angle-
Tamm-plasmon-d i en PeLEDs esemble he PL angula esponse o
he na ow-angle and wide-angle-Tamm-plasmon-d i en s uc u es,
espec i ely. Thus, we ha e demons a ed he ansla ion o he PL
di ec ional enhancemen in he pe o ski e-based Tamm plasmon
s uc u e in o di ec ional emission om an ope a ing Tamm-plasmon-
d i en PeLED. Besides, simula ions also show he adap abili y o he
Tamm-plasmon-d i en PeLEDs in he ed and blue egimes (Supple-
men a y Fig. 13) by fine uning he hicknesses o each laye . This wo k
demons a es he emi ing ma e ial as he bo om laye o he
Fig. 3 | Tamm-plasmon-d i en PeLEDs wi h con olled di ec ionali y and
elec oluminescence in ensi y. a No malised elec oluminescence (EL) spec-
um o e e ence PeLEDs and na ow-angle-Tamm-plasmon-d i en PeLED.
Tamm plasmon esonance o he na ow-angle-Tamm-plasmon-d i en PeLED
shown wi h a eflec ance measu emen (black dashed line). bCu en
densi y– ol age–luminance pe o mance o e e ence PeLED and na ow-angle-
Tamm-plasmon-d i en PeLED. Inse : schema ic o Tamm-plasmon-d i en PeLED.
cCu en e ficiency–cu en densi y cu e. Inse : EQE–cu en densi y cu e
conside ing emission o e all angles. Angle-dependen EL spec um o (d)
e e ence PeLED, (e) na ow-angle-Tamm-plasmon-d i en PeLED and ( ) wide-
angle-Tamm-plasmon-d i en PeLED collec ed ac oss he PeLED su ace mac o-
scopically. Whi e dashed line: EL as a unc ion o angle in eg a ed om 490 nm o
540 nm (d,e). No malised EL in eg a ed om 490 nm o 540 nm in ( ). EL
in ensi y o all configu a ions each no malised o he EL in ensi y o na ow-
angle-Tamm-plasmon-d i en PeLED (see colou ba ).
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 5
pho onic c ys al a he me al-pho onic-c ys al in e ace in a plana
Tamm plasmon sys em enhances di ec ional pho o-exci ed emission
and can be in eg a ed in o an LED o show di ec ional elec o-
luminescence amplifica ion. Impo an ly, he PeLED de ice s ack and
o he pho oniclaye s a e all op ically and/o elec ically ac i e laye s in
he Tamm plasmon s uc u e in a monoli hic ashion wi hou use o
u he complica ed op ics.
In Supplemen a y Fig. 14, we compa e ou design wi h simula ed
and op imised me al-me al and dis ibu ed B agg eflec o (DBR)-DBR
mic oca i ies, showing a significan ly s onge elec ic field enhance-
men (no malised o he Tamm plasmon enhancemen ) in he Tamm
plasmon pe o ski e s uc u e (a 515 nm: 1.00; a 533 nm: 1.00) com-
pa ed wi h DBR-DBR mic oca i ies (a 515 nm: 0.60; a 533 nm: 0.56)
and me al-me al mic oca i ies (a 515 nm: 0.93; a 533 nm: 0.80). To
compa e he e sa ili y o Tamm plasmon and me al-me al ca i ies in
he highes e ficiency blue43, g een8and ed44 pe o ski e LED de ices,
bo h Tamm plasmon and me al-me al ca i ies a e simula ed based on
he epo ed de ice s uc u es (Supplemen a y Fig. 15). Fo all h ee
examples, he Tamm plasmon s uc u e shows be e spec al na -
owing (sha pe esonance) and highe no malised in eg a ed elec ic
field in ensi y wi hin he pe o ski e laye o all blue (1.0 in Tamm
plasmon, 0.41 in me al-me al), g een (1.0 in Tamm plasmon, 0.61 in
me al-me al) and ed (1.0 in Tamm plasmon, 0.92 in me al-me al)
PeLEDs. Fu he mo e, he Tamm plasmon s uc u e employs he exac
de ice s uc u e as epo ed, wi h only he elec ically inac i e pho-
onic c ys al lying below ITO; p ac ical eplacemen o ITO wi h me al
in me al-me al ca i ies is challenging due o we abili y and sensi i i y
issues when solu ion-p ocessing he pe o ski e de ice laye s on a
me al, and e y ew expe imen al demons a ions o wo king PeLEDs
a e epo ed in his a chi ec u e. Thus, he Tamm plasmon s uc u e
has mo e deg ees o eedom o design conside a ions - he pho onic
c ys al can be mo e ca e ully designed o achie e a s onge elec ic
field enhancemen o a gi en LED de ice by uning he elec ically
inac i e pho onic c ys al, o example by adding ex a me al oxide
laye s again. By con as , he elec ic field in ensi y alues o he
me al-me al ca i ies a e nea hei uppe limi s due o limi a ions on
de ice pe o mance, me al choice and abso p ion loss o he me al.
Compa ed wi h he DBR-DBR ca i ies, he me al in he Tamm plasmon
s uc u e is easie o ab ica e compa ed wi h deposi ing DBR on op
o pe o ski e films and can eadily ac as he elec ode o he LED
de ice, hus is easie o implemen .
As Ag has he lowes ohmic loss in he isible egime compa ed o
o he common me als, u he imp o emen s migh be achie ed by
alloying he Ag me al, adding passi a ion laye s o spacing in e laye s,
o u he sup ess quenching and inhibi ionic eac ions o he pe -
o ski ewi h heAgelec ode
35,45. We expec u he imp o emen s by
inc easing he pho onic c ys al laye pai s o inc ease he coupling
s eng h (Supplemen a y Fig. 3d), by adding an i- eflec i e coa ing on
he ai /glass in e ace o imp o e ou coupling e ficiency a wide
angles, as well as h ough in es iga ion on he in e ac ion be ween
wa eguiding modes and emission modes ha can u he enhance he
emission o he Tamm-plasmon-d i en PeLEDs. In his p oo -o -
concep demons a ion, we balanced he numbe o laye s (complex-
i y in manu ac u ing) wi h he final pe o mance o ou emi e and
de ice.
We demons a ed Tamm-plasmon-d i en PeLEDs wi h s ong
di ec ional and enhanced emission. The bo om pho onic c ys al laye
a he me al-pho onic-c ys al in e ace in a Tamm plasmon sys em is
eplaced wi h an emi ing quasi-2D halide pe o ski e laye o s ongly
confine he Tamm plasmon modes ac oss he en i e pe o ski e laye .
As a esul , he na ow-angle-Tamm-plasmon-d i en PeLED shows
good di ec ionali y (angula FWHM o 36.6° compa ed o e e ence
143.9°), EL enhancemen by 1.8 imes a small angles, and EL spec al
na owing om 22.4 nm o 12.1 nm. The excellen adap abili y o
Tamm-plasmon-d i en PeLEDs co e ing he isible spec um, s ong
enhancemen in o wa d di ec ion, enhanced di ec ional emission
(wi h na ow-angle Tamm plasmon esonance), uneabili y o la ge
angle di ec ional emission (wi h wide-angle Tamm plasmon eso-
nance), EL spec al na owing, small hickness o ac i e s uc u e and
ela i ely simple scalabili y o ab ica ion me hods makes Tamm-
plasmon-d i en PeLEDs desi able. The Tamm-plasmon-d i en PeLEDs
show po en ial in applica ions whe e angula con ol, emission in en-
si y and colou pu i y a e c ucial, including displays, op ical commu-
nica ions, i ual eali y headse s, di ec ional ligh sou ces, op ical
aligne s and measu ing sys ems.
Me hods
Op ical simula ions
Op ical simula ions we e conduc ed using a cus om code based on he
ans e ma ix me hod46 and a gene ic algo i hm o he Tamm plas-
mon s uc u al design. A e esol ing he sample s uc u e, he
emission p ope ies we e analysed using a comme cial fini e-
di e ence ime-domain so wa e (3D Elec omagne ic Simula o
om Lume ical Inc.)47. The e ac i e indices o all ma e ials used in he
simula ions a e de ailed in Supplemen a y Fig. 16. This me hodology
in ol ed iso opically embedding emi ing dipoles (a e aged o e
h ee pe pendicula o ien a ions) h oughou he pe o ski e laye o
examine he luminous powe emi ed om he s uc u e’ssu ace.
Single-wa eleng h simula ions we e pe o med a wa eleng h,
λ=514nm wi hin a simula ion box sized 2x2x1 µm3, wi h pe ec ly
ma ched laye s applied o all bounda ies. The mesh g id dimensions
we e se o 10 nm o he x- and y-axis and 1 nm o he z-axis. A
2-dimensional equency-domain field moni o was employed o cap-
u e he a -field p ojec ion ia Fou ie ans o m, cap u ing ou going
adia ion ac oss a hemisphe e48.
Fab ica ion o 1-dimensional pho onic c ys al
One-dimen ional pho onic c ys al made o 3 pai s o al e na ing i a-
nium dioxide (TiO
2
) and silicon dioxide (SiO
2
) we e deposi ed on glass
subs a es in he Ins i u e o Op oelec onics, Mili a y Uni e si y o
Technology. Thickness o each laye was TiO
2
:(70±2)nmandSiO
2
:
(90 ± 2) nm. The pho onic c ys al we e deposi ed in an e-beam e a-
po a ion sys em wi h a plasma sou ce assis ance (Sy us 710 P o, Bühle
Leybold Op ics, Alzenau, Ge many). The base p essu e o he sys em
was 2 × 10−6mba . TiO
2
and SiO
2
we e deposi ed a 0.25 nm s−1and
0.6 nm s−1 a e, espec i ely.
ITO spu e ing
ITO elec odes we e spu e ed on glass subs a es ( o e e ence
PeLEDs) and pho onic c ys al subs a es ( o Tamm-plasmon-d i en
PeLEDs) using a cus om se up loca ed in he Class 10,000 clean oom
in he Elec ical Enginee ing Di ision, Depa men o Enginee ing,
Uni e si y o Camb idge. The ITO elec odes we e pa e ned using a
me al mask. The ITO spu e ing u ilised an In
2
O
3
/SnO
2
90/10 w % a -
ge , ope a ed a a gon flow o 20 sccm, wi h he p essu e o 5 mTo
and powe o 40 W. The spu e ing a e achie ed was 3.7 nm minu e−1,
esul ing in ITO conduc i i y o 1800 S cm−1as measu ed by a 4-poin -
p obe, wi h an ITO hickness o 83 nm de e mined by AFM.
Ma e ials
Lead (II) b omide (PbB
2
, 99.999%), phenyle hylammonium b omide
(PEAB , >99.5%), 1,4,7,10,13,16-hexaoxacyclooc adecane (18-c own-6,
≥99%), poly(4-bu yl iphenylamine) (poly-TPD, Mw ≥20,000 g mol−1),
poly(9- inylca bazole) (PVK, MW:25,000-50,000 mg mol−1), dime hyl
sul oxide (DMSO, anhyd ous, 99.9%), chlo obenzene (CB, anhyd ous,
99.8%) we e pu chased om Sigma-Ald ich. Cesium b omide
(CsB , 99.999%) was pu chased om Al a Aesa . 2,2’,2”-(1,3,5-
Benzine iyl)- is(1-phenyl-1-H-benzimidazole) (TPBi, >99.5%),
8-Hyd oxyquinolinola o-li hium (LiQ, >99%) we e pu chased om
Ossila. All chemicals we e used wi hou any u he pu ifica ion.
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 6
P epa a ion o pe o ski e p ecu so solu ion
Pe o ski e p ecu so was p epa ed by dissol ing PbB
2
,CsB and
PEAB (mola a io o 1: 1.05: 0.4) in DMSO a 0.25 M ini ially and hen
u he dilu ed down o concen a ions be ween 0.13 and 0.23 M o
hickness a ia ion. 18-c own-6 was added as addi i e (mola a io o
1.7% o PbB
2
) in pe o ski e p ecu so s o PeLEDs o imp o e he
PeLED pe o mance49.
Fab ica ion pe o ski e s uc u es
Glass subs a es and glass/pho onic c ys al subs a es we e cleaned
using de e gen , deionised wa e , ace one and isop opanol unde
ul asonica ion o 10 minu es each, ollowed by a 15-min UV ozone
ea men . A solu ion o PVK (6 mg ml−1in CB) was spin-coa ed
on o he subs a e a 4000 pm o 30 s, hen immedia ely annealed
a 100 °C o 10 min. I is wo h no ing ha o he common hole
injec ion laye such as Poly(3,4-e hylenedioxy hiophene)-poly(-
s y enesul ona e) (PEDOT:PSS), Poly(4-bu yl iphenylamine) (poly-
TPD), Poly[(9,9-dioc ylfluo enyl-2,7-diyl)-co-(4,4′-(N-(4-sec-bu ylphe-
nyl)diphenylamine)] (TFB) posses simila e ac i e indices, making
hem compa ible wi h such op ical s uc u es. Pe o ski e p ecu so s,
wi h concen a ion anging om 0.13 M o 0.25 M, we e spin-coa ed a
6000 pm o 90 s and immedia ely annealed a 70 °C o 5 min. A
100 nm hick Ag film was subsequen ly he mally e apo a ed on o he
pe o ski e film a a a e o 0.1 nm s−1.
Fab ica ion pe o ski e LEDs
Glass/ITO subs a es and glass/pho onic c ys al/ITO subs a es we e
cleaned in de e gen , deionised wa e , ace one and isop opanol unde
ul asonica ion o 10 minu es each, hen ea ed wi h UV Ozone o
15 min. Poly-TPD (10 mg ml−1in CB) and PVK (6 mg ml−1in CB) is
sequen ially spin-coa ed on o he subs a e a 4000 pm o 30 s and
immedia ely annealed a 100 °C o 10 min and 140 °C o 20 min,
espec i ely. The pe o ski e p ecu so o concen a ion 0.16 M (na -
ow-angle-Tamm-plasmon PeLED) and 0.25 M (wide-angle-Tamm-
plasmon PeLED) was spin coa ed a 1000 pm o 5 s and 4000 pm o
55 seconds and hen immedia ely annealed a 90 °C o 10 minu es.
TPBi (40 nm), LiQ (3 nm) and Ag (100 nm) we e hen sequen ially
he mal e apo a ed on he pe o ski e film.
Film hickness measu emen
Film hicknesses we e assessed by scanning ac oss he dep h o a
sc a ch made on he film wi h a azo blade (Supplemen a y Fig. 4).
The scan was pe o med on B uke Dimension Icon a omic o ce
mic oscope (AFM) wi h a silicon ip on Ni ide le e (B uke Scanasys -
Ai can ile e , sp ing cons an 0.4 N m−1) unning on peak o ce ap-
ping mode. Da a we e analysed wi h WSxM 5.0 so wa e50.
Reflec ance measu emen
Tamm plasmon esonance ( eflec ance) was cha ac e ised by
UV– isible spec ome e (Shimadzu UV-3600Plus) wi h an in eg a ing
sphe e a achmen (Shimadzu ISR-603). The o al eflec ance was
measu ed a 8° o se o keep he specula eflec ed ligh wi hin he
in eg a ing sphe e. Gi en ha he eflec ance o he Tamm-plasmon-
pe o ski e s uc u e shown in Fig. 1d was measu ed a 8°, he ac ual
Tamm plasmon esonance wa eleng h a 0° should be ca. 3 nm ed-
shi ed. The baseline measu emen was done wi h a 100 nm hick
e apo a ed sil e mi o as a e e ence due o high eflec i i y o ou
samples.
Reflec ance measu emen was c oss-checked wi h he Agilen
Ca y7000 Uni e sal Measu emen Spec ome e using he Uni e sal
Measu emen Accesso y. The sample is il ed a 6° and he de ec o a
12° o collec he specula eflec ance wi hou blocking he exci a ion
lamp. The baseline measu emen is done a 100% ansmi ance
wi hou any e e ence, hus elimina ing any inaccu acy due o he
e e ence de ec s.
Mic oscale eflec ance o pho onic c ys al subs a es was mea-
su ed wi h hype spec al mic oscope (Pho on E c. IMA). A lamp ligh
was ocussed on he sample h ough a condense om below he
sample and was collec ed by he objec i e lens (Olympus MPLFLN20x
wi h NA o 0.45) and measu ed by a CCD came a. The measu ed
eflec ance o pho onic c ys al was calib a ed wi h eflec ance o a
calib a ion mi o .
Pho oluminescence quan um e ficiency
PLQE o pe o ski e films, e e ence s uc u es and Tamm plasmon
s uc u es a e measu ed wi h a 405 nm con inuous wa e lase unde
exci a ion be ween 3 o 167 mW cm−2in an in eg a ing sphe e and he
spec um collec ed wi h Ando iDus Si de ec o . Calcula ions a e based
on 3 configu a ions o he sphe e—emp y sphe e, sample placed in he
sphe e bu lase beam di ec ed on he sphe e wall and lase beam
di ec ed on o he sample51.
Cha ac e isa ion o pe o ski e LED pe o mance
All PeLEDs we e encapsula ed in a N
2
-filled glo ebox wi h UV-cu ed
esin and glass. The PeLEDs we e measu ed unde ambien condi ion
wi h he LED measu emen se up om he Op oelec onics g oup in
Ca endish Labo a o y. The PeLEDs we e powe ed by a Kei hley
2400 sou ce me e as a ol age sou ce o measu ing he cu en
densi y– ol age cha ac e is ics. The pho on flux was simul aneously
measu ed using a calib a ed ci cula silicon pho odiode cen ed o e
he ligh -emi ing pixel. The luminance o he PeLEDs we e calcula ed
based on he emission unc ion o he PeLEDs and on he known
spec al esponse o he silicon pho odiode. The EL spec a o he
de ices we e measu ed using a Labsphe e CDS 610 spec ome e . The
cu en e ficiency was calcula ed as he a io be ween o wa d lumi-
nance and cu en . The esul ing EQE was calcula ed conside ing he
angula esol ed emission using equa ion om A che e al.42.
ηEQEðVÞ=1002π 2
APD
VPDðVÞ
RPD
q
hc
1
IPeLED VðÞRSλ,0ðÞλdλ
RSλ,0ðÞRλðÞdλZπ
2
0RSλ,θðÞλdλ
RSλ,0ðÞλdλsin θdθð1Þ
whe e VPD,RPD,APD a e ol age, esis ance and a ea o pho odiode
espec i ely. is he dis ance be ween pho odiode and PeLED. Sλ,θðÞis
he measu ed spec al adian in ensi y a angle θ.RλðÞis he pho o-
diode esponsi i y. IPeLED is he cu en ac oss he PeLED. q,h,andca e
uni cha ge, Planck cons an and speed o ligh espec i ely.
Angula luminescence measu emen
The mac oscale angula PL and EL was measu ed on a home-buil
se up (Supplemen a y Fig. 17). Fo PL, a 405 nm con inuous wa e
lase and he sample we e fixed on he op ical able wi h he exci-
a ion angle no mal o sample su ace in x–y di ec ion and 20° abo e
in he z-di ec ion. The lase beam was ocussed on he sample wi h a
lens ( = 1000 mm, powe densi y o 0.5 W cm−2). Fo EL, he PeLEDs
we e powe ed by he Kei hley 2400 sou ce me e a a cons an
cu en densi y o 0.44 mA cm−2. Bo h PL and EL spec a was cap-
u ed by a spec oscopy came a (Ando iDus DU420A Si de ec o )
connec ed o a fib e collima o (Tho labs F220SMA-532) h ough an
op ical fib e. The fib e collima o was fixed on an au oma ed o a ing
s age (Tho labs PRMTZ8 Mo o ised con inuous o a ion s age,
Tho labs K-Cube DC se o mo o con olle ). The fib e collima ed
was fixed a 10 cm away om he sample o maximise he angula
esolu ion while ensu ing a high collec ion o fluo escence. The PL
and EL spec a we e collec ed a 1° in e al wi h a scan a e o 3° s−1
and 5° s−1, espec i ely. In Supplemen a y Fig. 18, we showed he PL
and EL s abili y a e sui ably s able o e he o al angula PL and EL
measu emen ime scales o 60 s and 36 s, espec i ely, unde he
same con inuous exci a ion and d i ing cu en o 0.5 W cm−2 o
angula PL and 0.44 mA cm−2 o angula EL. In addi ion o he PL and
EL s abili y, he PL and EL a e always collec ed om one end o he
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 7
o he end, e.g. om −90° o 90°. Thus, we make su e ha he angula
measu emen s a e no a ec ed by deg ada ion by checking ha he
cu es a e symme ical (see Figs. 2b, d, h and 3d– ). Fo bo h PL and
EL measu emen s, all 4 edges o he samples we e masked wi h black
ape o elimina e emission om he sample edge.
The emission ac oss he solid angle is calcula ed om he angula
PL and EL measu emen s based on he equa ion shown below, which is
de i ed om A che e al.42.
Isolid angle =I0×Zα
αRSλ,θðÞλdλ
RSλ,0ðÞλdλsin θdθð2Þ
whe e αis he solid angle o in e es , Isolid angle is hePLo ELin ensi y,
I0is he o wa d in ensi y, Sλ,θðÞis he spec al adian in ensi y.
Mic oscale PL was measu ed wi h hype spec al mic oscope
(Pho on E c. IMA), exci ed wi h a 405 nm con inuous lase . The
hype spec al mic oscopy measu emen s we e collec ed wi h objec-
i e lenses (Olympus MPLFLN) o 20x and NA o 0.45 (equi alen o
collec ion angle o 26.7°).
T ansien pho oluminescence
Time- esol ed pho oluminescence was measu ed a fluences be ween
1and370nJcm
−2pulse−1wi h con ocal mic oscope (PicoQuan
Mic oTime 200). The samples we e exci ed wi h 405 nm pulsed lase
(pulse wid h ~100 ps, epe i ion a e 5 MHz) ha was ocussed wi h an
10x ai objec i e lens.
Time- esol ed pho oluminescence a lowe fluence be ween 0.01
and 5 nJ cm−2pulse−1we e measu ed wi h pho oluminescence spec-
ome e (Edinbu gh Ins umen s FLS1000). A 405 nm pulsed lase
(pulse wid h ~50 ps, epe i ion a e 2 MHz) was ocussed on he sam-
ples a 45° and 60° and he emission was collec ed be ween 45° and
30° espec i ely a 1 nm bandwid h. Time esol ed emission scans
we e done by sweeping he emission collec ion wa eleng hs be ween
490-520 nm wi h 5 nm s ep. Measu emen s a e done wi h bo h unen-
capsula ed and encapsula ed samples in ai and bo h shows simila
esul s.
C oss-sec ion o Tamm-Plasmon-pe o ski e s uc u e
The TEM lamella c oss-sec ion was p epa ed wi h an FEI Helios
Nanolab Dualbeam FIB/SEM ollowing a s anda d p o ocol52.The
lamella was ans e ed minimising ai exposu e in o an FEI Osi is TEM
ope a ing a 200 kV and ~140 pA beam cu en . HAADF images we e
acqui ed using a Fischione de ec o a a came a leng h o 115 mm, wi h
a dwell ime o 1.9 µs and a spa ial sampling o 0.7 nm pixel−1.STEM-
EDX maps we e acqui ed using a B uke Supe -X silicon d i de ec o
wi h a collec ion solid angle o ≈0.9 s , a dwell ime o 50 ms, a spa ial
sampling o 5 nm pixel−1, and a spec al esolu ion o 5 eV channel−1.
STEM-EDX composi ional maps we e spec ally ebinned o 10 eV pe
channel, and denoised using PCA/NMF aking he fi s 8 componen s.
Da a p ocessing was done using Hype Spy 1.6.1, a Py hon-based
analysis sui e o hype spec al da a53.
Da a a ailabili y
The da a ha suppo he findings o his s udy a e openly a ailable in
Apollo—Uni e si y o Camb idge Reposi o y a h ps://doi.o g/10.
17863/CAM.109169.
Code a ailabili y
De ails on he code ha suppo s he findings o his s udy can be
sha ed unde eques .
Re e ences
1. Be gesen, J. D., Tähkämö, L., Gibon, T. & Suh, S. Po en ial long- e m
global en i onmen al implica ions o e ficien ligh -sou ce ech-
nologies. J. Ind. Ecol. 20,263–275 (2016).
2. Risi,I.,Omubo-Pepple,V.&Alab aba,M.Compa a i es udyo ligh
emi ing diode (LED), compac fluo escen (CF) and incandescen
lamps. J. Sci. Eng. Res. 5,197–203 (2018).
3. Holonyak, N. & Be acqua, S. F. Cohe en ( isible) ligh emission
om Ga(As1−xPx) junc ions. Appl. Phys. Le . 1,82–83 (1962).
4. Nakamu a, S., Mukai, T. & Senoh, M. Candela‐class high‐b igh ness
InGaN/AlGaN double‐he e os uc u e blue‐ligh ‐emi ing diodes.
Appl. Phys. Le . 64,1687–1689 (1994).
5. Col in, V., Schlamp, M. & Ali isa os, A. Ligh -emi ing diodes made
om cadmium selenide nanoc ys als and a semiconduc ing poly-
me . Na u e 370,354–357 (1994).
6. Tang,C.W.&VanSlyke,S.A.O ganicelec oluminescen diodes.
Appl. Phys. Le . 51,913–915 (1987).
7. Kim, S. T. e al. E ficien g een elec oluminescen diodes based on
poly (2-dime hyloc ylsilyl-1,4-phenylene inylene). Ad . Ma e . 8,
979–982 (1996).
8. Kim, J. S. e al. Ul a-b igh , e ficien and s able pe o ski e ligh -
emi ing diodes. Na u e 611,688–694 (2022).
9. Zhu, L. e al. Un eiling he addi i e-assis ed o ien ed g ow h o
pe o ski e c ys alli e o high pe o mance ligh -emi ing diodes.
Na . Commun. 12,5081(2021).
10. K ess, S. J. P. e al. Wedge wa eguides and esona o s o quan um
plasmonics. Nano Le . 15,6267–6275 (2015).
11. Kel , T. A. e al. Localized and delocalized plasmons in me allic
nano oids. Phys.Re .B74, 245415 (2006).
12. Pe ney, N. M. B. e al. Tuning localized plasmon ca i ies o op imized
su ace-enhanced Raman sca e ing. Phys.Re .B76, 035426 (2007).
13. Di lbache , H. e al. Sil e nanowi es as su ace plasmon esona o s.
Phys.Re .Le .95,257403(2005).
14. Bo o iks, S. e al. Ex emely confined gap plasmon modes: when
nonlocali y ma e s. Na . Commun. 13, 3105 (2022).
15. Bozhe olnyi, S. I. & Sønde gaa d, T. Gene al p ope ies o slow-
plasmon esonan nanos uc u es: nano-an ennas and esona o s.
Op . Exp ess 15,10869–10877 (2007).
16. Po s, A. & Bozhe olnyi, S. I. Plasmonic me asu aces o e ficien
phase con ol in eflec ion. Op . Exp ess 21,27438–27451 (2013).
17. Chen,S.,Zhang,C.,Lee,J.,Han,J.&Nu mikko,A.High-Q,low-
h eshold monoli hic pe o ski e hin-film e ical-ca i y lase s. Ad .
Ma e . 29, 1604781 (2017).
18. Wang, Y., Li, X., Nalla, V., Zeng, H. & Sun, H. Solu ion-p ocessed low
h eshold e ical ca i y su ace emi ing lase s om all-ino ganic
pe o ski e nanoc ys als. Ad . Func . Ma e . 27,1605088(2017).
19. Zhang, S. e al. S ong exci on–pho on coupling in hyb id
ino ganic–o ganic pe o ski e mic o/nanowi es. Ad . Op . Ma e . 6,
1701032 (2018).
20. Liu, P. e al. O ganic–ino ganic hyb id pe o ski e nanowi e lase
a ays. ACS Nano 11,5766–5773 (2017).
21. Zhang,Q.,Ha,S.T.,Liu,X.,Sum,T.C.&Xiong,Q.Room-
empe a u e nea -in a ed high-q pe o ski e whispe ing-galle y
plana nanolase s. Nano Le . 14,5995–6001 (2014).
22. Deschle , F. e al. High pho oluminescence e ficiency and op ically
pumped lasing in solu ion-p ocessed mixed halide pe o ski e
semiconduc o s. J. Phys. Chem. Le . 5,1421–1426 (2014).
23. Bo iskina, S. V. e al. Losses in plasmonics: om mi iga ing ene gy
dissipa ion o emb acing loss-enabled unc ionali ies. Ad . Op .
Pho on. 9, 775–827 (2017).
24. Wang,H.,Ma,R.,Liu,G.,Wang,L.&Lin,Q.S ongligh confinemen
and op ical o ce enhancemen in phospho ene wi h acous ic
plasmons. Appl. Phys. Exp ess 15, 072010 (2022).
25. Liu, T. e al. Spec al na owing and enhancemen o di ec ional
emission o pe o ski e ligh emi ing diode by mic oca i y. Lase
Pho onics Re . 16, 2200091 (2022).
26. Kali ee ski, M. e al. Tamm plasmon-pola i ons: Possible elec o-
magne ic s a es a he in e ace o a me al and a dielec ic B agg
mi o . Phys. Re . B 76,165415(2007).
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 8
27. Sasin, M. E. e al. Tamm plasmon pola i ons: slow and spa ially
compac ligh . Appl. Phys. Le . 92, 251112 (2008).
28. Jiménez-Solano, A., Galis eo-López, J. F. & Míguez, H. Flexible and
adap able ligh -emi ing coa ings o a bi a y me al su aces based
on op ical amm mode coupling. Ad . Op . Ma e . 6,1700560
(2018).
29. Symonds, C. e al. Confined Tamm plasmon lase s. Nano Le . 13,
3179–3184 (2013).
30. Zhang, X.-L., Song, J.-F., Li, X.-B., Feng, J. & Sun, H.-B. Op ical Tamm
s a es enhanced b oad-band abso p ion o o ganic sola cells.
Appl. Phys. Le . 101, 243901 (2012).
31. Gazzano, O. e al. Single pho on sou ce using confined Tamm
plasmon modes. Appl. Phys. Le . 100, 232111 (2012).
32. Zhao, B. e al. E ficien ligh -emi ing diodes om mixed-
dimensional pe o ski es on a fluo ide in e ace. Na . Elec on. 3,
704–710 (2020).
33. Ban, X. e al. Highly e ficien quasi-2D pe o ski e ligh -emi ing
diodes inco po a ing a TADF dend ime as an exci on- e ie ing
addi i e. ACS Appl. Ma e . In e aces 13,44585–44595 (2021).
34. Chang, C.-Y., Chen, Y.-H., Tsai, Y.-L., Kuo, H.-C. & Chen, K.-P. Tun-
abili y and op imiza ion o coupling e ficiency in Tamm plasmon
modes. IEEE J. Sel. Top. Quan um Elec on. 21,262–267 (2015).
35. S ans öm, S. e al. Deg ada ion mechanism o sil e me al
deposi ed on lead halide pe o ski es. ACS Appl. Ma e . In e aces
12,7212–7221 (2020).
36. K an hi aja, K. e al. S abili y and deg ada ion in iple ca ion and
me hyl ammonium lead iodide pe o ski e sola cells media ed ia
Au and Ag elec odes. Sci. Rep. 12, 18574 (2022).
37. Ma, D. e al. Dis ibu ion con ol enables e ficien educed-
dimensional pe o ski e LEDs. Na u e 599,594–598 (2021).
38. V edenbe g, A. M. e al. Con olled a omic spon aneous emission
om ER3+ in a anspa en Si/SiO
2
mic oca i y. Phys.Re .Le .71,
517–520 (1993).
39. Lo a, P. e al. All-polyme pho onic mic oca i ies doped wi h
pe ylene bisimide J-agg ega es. Ad . Op . Ma e . 5, 1700523
(2017).
40. Megahd, H. e al. Con ol o nea -in a ed dye fluo escence li e ime
in all-polyme mic oca i ies. Ma e . Chem. F on . 6,2413–2421
(2022).
41. Jo dan, R. H., Dodabalapu , A. & Slushe , R. E. E ficiency enhance-
men o mic oca i y o ganic ligh emi ing diodes. Appl. Phys. Le .
69, 1997–1999 (1996).
42. A che , E. e al. Accu a e e ficiency measu emen s o o ganic ligh -
emi ing diodes ia angle- esol ed spec oscopy. Ad . Op . Ma e .
9, 2000838 (2021).
43. Yuan, S. e al. E ficien blue elec oluminescence om educed-
dimensional pe o ski es. Na . Pho on. 18,1–7 (2024).
44. Jiang, J. e al. Red pe o ski e ligh -emi ing diodes wi h e ficiency
exceeding 25% ealized by co-space ca ions. Ad . Ma e . 34,
2204460 (2022).
45. Na h, B., Ramamu hy, P. C., Hegde, G. & Roy Mahapa a, D. Role o
elec odes on pe o ski e sola cells pe o mance: a e iew. ISSS J.
Mic o Sma Sys . 11,61–79 (2022).
46. Oh a, K. & Ishida, H. Ma ix o malism o calcula ion o elec ic field
in ensi y o ligh in s a ified mul ilaye ed films. Appl. Op . 29,
1952–1959 (1990).
47. Lume ical Inc. h ps://www.lume ical.com/.
48. Taflo e, A. & Hagness, S. Compu a ional Elec odynamics: The
Fini e-Di e ence Time-Domain Me hod 3 d edn. Vol. 2062 (A ech
House, Inc., 2005).
49. Ban, M. e al. Solu ion-p ocessed pe o ski e ligh emi ing diodes
wi h e ficiency exceeding 15% h ough addi i e-con olled nanos-
uc u e ailo ing. Na . Commun. 9,3892(2018).
50. WSXM: A so wa e o scanning p obe mic oscopy and a ool o
nano echnology. Re . Sci. Ins um. 78,013705.
51. Mello, J. C., de Wi mann, H. F. & F iend, R. H. An imp o ed
expe imen al de e mina ion o ex e nal pho oluminescence quan-
um e ficiency. Ad . Ma e . 9,230–232 (1997).
52. Kosasih, F. U. e al. Op ical emission om ocused ion beam milled
halide pe o ski e de ice c oss-sec ions. Mic osc. Res. Tech. 85,
2351–2355 (2022).
53. Peña, F. de la e al. Hype spy/Hype spy 1.4.1. (Zenodo, 2018).
h ps://doi.o g/10.5281/zenodo.1469364.
Acknowledgemen s
The au ho s acknowledge he Eu opean Resea ch Council (ERC) unde
he Eu opean Union’s Ho izon 2020 esea ch and inno a ion p og am
(HYPERION, g an ag eemen No. 756962), Camb idge Royce acili ies
g an EP/P024947/1, Si Hen y Royce Ins i u e— ecu en g an EP/
R00661X/1 and he Enginee ing and Physical Sciences Resea ch Council
(EPSRC) (g an ag eemen Nos. EP/R023980/1, EP/T02030X/1 and EP/
S030638/1). This wo k was co-financed by Mili a y Uni e si y o Tech-
nology unde esea ch p ojec UGB 502-6700-23-759. Z.Y.O. acknowl-
edges schola ship om S John’s College, Uni e si y o Camb idge. A.J.-
S. g a e ully acknowledges a pos doc o al schola ship om he Max
Planck Socie y and he Spanish Minis y o Uni e si ies o unding
h ough a Bea iz Galindo Resea ch ellowship BG20/00015. K.G.
app ecia es suppo om he Polish Minis y o Science and Highe
Educa ion wi hin he Mobilnosc Plus p og am (g an no.1603/MOB/V/
2017/0) and he Na ional Science Cen e (2022/47/D/ST5/03332). Y.S.
acknowledges CSC Camb idge Schola ship. J.F.O and C.D. acknowl-
edge unding om he Enginee ing and Physical Sciences Resea ch
Council (EPSRC) Nano Doc o al T aining Cen e (EP/L015978/1). K.F.
acknowledges a Geo ge and Lilian Schi S uden ship, Win on Sus ain-
abili y Fund S uden ship, he Enginee ing and Physical Sciences
Resea ch Council (EPSRC) s uden ship. H.S. hanks he UK Enginee ing
and Physical Sciences Resea ch Council (EPSRC) g an EP/S023046/1
o he EPSRC Cen e o Doc o al T aining in Senso Technologies o a
Heal hy and Sus ainable Fu u e. S.Kahmann is g a e ul o unding om
he Ge man Academic Exchange Se ice (DAAD) (91793256) o a sho -
e m esea ch ellowship, and om he Le e hulme Ea ly Ca ee Fel-
lowship unded by he Le e hulme T us (ECF-2022-593) and he Isaac
New on T us (22.08(i)). G.V. acknowledges he suppo o he Spanish
Minis y o Educa ion, Voca ional T aining and Spo s h ough a Beca de
Colabo ación (G an No. 23CO1/000162). M.A. acknowledges unding
om he Le e hulme Ea ly Ca ee Fellowship (g an ag eemen No. ECF-
2019-224) unded by he Le e hulme T us and he Isaac New on T us
and om he Royal Academy o Enginee ing unde he Resea ch Fel-
lowshipp og amme.M.A.andG.V.acknowledge suppo om MICIU/
AEI/10.13039/501100011033 and he Eu opean Union Nex Gene -
a ionEU/PRTR h ough a PID2022-142525OA-I00 g an and a Ramón y
Cajal Fellowship (RYC2021-034941-I). S.D.S. acknowledges he Royal
Socie y and Ta a G oup (g an no. UF150033). We hank Youcheng
Zhang (Ca endish labo a o y, Uni e si y o Camb idge) o ITO con-
duc i i y checks. Fo he pu pose o open access, he au ho s ha e
applied a C ea i e Commons A ibu ion (CC BY) licence o any Au ho
Accep ed Manusc ip e sion a ising om his submission.
Au ho con ibu ions
Z.Y.O., A.J.-S., K.G., M.A. and S.D.S. concei ed and de eloped he
Tamm-plasmon-d i en PeLEDs. A.J.-S. and G.V. modelled and op imised
he Tamm-plasmon-d i en PeLEDs wi h inpu om M.A. Z.Y.O. and Y.S.
ab ica ed and op imised he pe o ski e-based Tamm plasmon s uc-
u e. Z.Y.O ab ica ed and op imised he Tamm-plasmon-d i en PeLEDs
including ITO spu e ing. Z.Y.O collec ed and analysed he AFM da a,
UV- isible spec oscopy da a, angula PL and EL da a. J.F.O. collec ed
andanalysed heHAADF-STEMandEDXda a.K.F.pe o med he
hype spec al mic oscopy. H.S., S.Kahmann and Z.Y.O collec ed and
analysed he PL decay da a. Z.Y.O measu ed and analysed he PeLEDs
pe o mance. P.N. and M.P.N. p epa ed he pho onic c ys al. S.N.
A icle h ps://doi.o g/10.1038/s41467-024-49838-1
Na u e Communica ions | (2024) 15:5802 9