Enhanced Open-Ci cui Vol age o Wide-Bandgap Pe o ski e
Pho o ol aics by Using Alloyed (FA1-xCsx)Pb(I1-xB x)3 Quan um Do s
Mokshin Su i,†,‡ Abhiji Haza ika,† B yon La son,† Qian Zhao,†,§ Ma a Vallés-Pela da, ||,† Timo hy
D. Siegle ,‡ Michael K. Abney,‡ And ew J. Fe guson,† B ian A. Ko gel,‡,* and Joseph M. Lu he †,*
† Na ional Renewable Ene gy Labo a o y, Golden, Colo ado 80401, USA
‡ McKe a Depa men o Chemical Enginee ing and Texas Ma e ials Ins i u e, The Uni e si y o
Texas a Aus in, Aus in, Texas 78712-1062, USA
§ College o Chemis y, Nankai Uni e si y, Tianjin 300071, China
|| Ins i u e o Ad anced Ma e ials (INAM), Uni e si a Jaume I, A enida de Vicen Sos Bayna , s/n,
12006 Cas elló de la Plana, Cas ellón, Spain
* Co esponding au ho s: [email p o ec ed] ; [email p o ec ed]
SUPPORTING INFORMATION
 Expe imen al Me hods
 Cha ac e iza ions
 Figu e S1. Compa ison o expe imen al PQD PV ol age ac ions o li e a u e
 Table S1. De ice me ics o PQD PVs used in Fig. 2 o main ex .
 Figu e S2. Radia i e li e ime es ima es o all colloidal PQD samples
 Figu e S3. TRPL ansien s o all PQD samples
 Table S2. Fi ing pa ame e s o ime- esol ed PL decays in Figu e S3.
 Table S3. De ice me ics o all PQD PVs, om Fig. 4 o main ex
 Figu e S4. Time- esol ed mic owa e conduc i i y (TRMC) o PQD ilms.
 Figu e S5. Yield-mobili y p oduc o PQD ilms
 Figu e S6. Abso bance and pho oluminescence o CsPb(I1-xB x)3 PQD samples used in
de ices and TRMC measu emen s.
 Figu e S7. Abso bance and pho oluminescence o FAPb(I1-xB x)3 PQD samples used in
de ices and TRMC measu emen s.
Expe imen al Me hods
Chemicals
All chemicals we e used as ecei ed wi hou u he pu i ica ion. Oleic acid (OA, echnical g ade
90%), oleylamine (OAm, echnical g ade 70%), 1-oc adecene (ODE, echnical g ade 90%),
oluene (anhyd ous, 99.8%), hexane ( eagen g ade ≥ 95%), oc ane (anhyd ous, ≥ 99%), 1-bu anol
(anhyd ous, 99.8%), me hyl ace a e (MeOAc, anhyd ous 99.5%), e hyl ace a e (E OAc,
anhyd ous, 99.8%), cesium ca bona e (Cs2CO3, 99.9%), lead (II) ni a e (Pb(NO3)2, 99.999%),
e hanol (E OH, 200 p oo ), i anium e hoxide (>97%), hyd ochlo ic acid (HCl; 37% in wa e ),
chlo obenzene (anhyd ous, 99.8%), 4- e -bu ylpy idine (4-TBP, 96%),
bis( i luo ome hane)sul onimide li hium sal (Li-TFSI, 99.95% ace me als basis), Fo mamidine
ace a e sale (FA-ace a e, 99%), and ace oni ile (anhyd ous, 99.8%) we e pu chased om Sigma-
Ald ich. Lead (II) iodide (PbI2 99.9985%) was pu chased om Al a Aesa . Fo mamidinium iodide
(FAI) was pu chased om G ea Cell Sola . 2,2’,7,7’-Te akis(N,N-di-p-me hoxyphenylamine)-9-
9’-spi obi luo ene (spi o-OMeTAD, ≥99.5%) was pu chased om Lum ech, Inc.
Syn heses o pe o ski e QDs
CsPb(I1-xB x)3 QD syn hesis
1.08 mmol o PbX2 powde (mix u e o PbI2 and PbB 2) was dissol ed in oc adecene in a 3-neck
lask. The mix u e was subjec ed o a acuum en i onmen and hea ed o 110 °C o 10 minu es.
2.5 mL o oleylamine and 2.5 mL oleic acid we e hea ed o 130 °C and injec ed in o he lask. This
allows o dissolu ion o he lead sal ; once he sal dissol es, he lask was subjec ed o a ni ogen
en i onmen and he solu ion was hea ed o 185 °C. As soon as he solu ion empe a u e eached
185 °C, a Cs-olea e p ecu so , a 130 °C, was injec ed all a once in o he lask. This p ocedu e is
adap ed om p e ious epo s.1,2
The Cs-olea e p ecu so was c ea ed by dissol ing 407 mg o Cs2CO3 in 20 mL o oc adecene and
1.25 mL o oleic acid. P ope dissolu ion o he Cs-olea e equi ed degassing a 120 °C ollowed
by hea ing o 150 °C.
Nuclea ion o CsPbX3 quan um do s occu s nea ly ins an aneously as he Cs-olea e is injec ed in o
he lead sal solu ion. In o de o main ain ela i e mono-dispe si y o he quan um do s, he lask
was cooled o 25-30 °C in an ice ba h immedia ely ollowing injec ion o he Cs-olea e.
Ex a ligands we e emo ed om he quan um do solu ion by cen i uging wi h anhyd ous me hyl
ace a e o 5 minu es a 7500 RPM. Mul iple washing s eps we e equi ed o p oduce high yield
p oduc .2
FAPb(I1-xB x)3 QD syn hesis
0.74 mmol o PbX2 powde (mix u e o PbI2 and PbB 2) we e mixed in 25 mL o oc adecene in a
3-neck lask. The mix u e was degassed o 20 minu es a 120 °C. Sepa a ely, 4mL o oleic acid
and 2mL o oleylamine we e mixed a 130 °C o 20 min. The oleic acid/oleylammine mix u e
was hen injec ed in o he Pb-sal lask o dissol e he Pb-sal . Once he sal s dissol ed, he lask
a mosphe e was changed o ni ogen and he empe a u e was adjus ed o a a ge ed eac ion
empe a u e depending on inpu halide a io o he lead-sal s.
Sepa a ely, FA-olea e p ecu so was p epa ed by mixing 521 mg o FA-ace a e in 10-20 mL oleic
acid in a 3-neck lask, yielding a FA concen a ion o 0.25-0.50 mM. The concen a ion o FA-
ace a e used o his syn hesis a ied linea ly om 0.25-0.50 mM based on inpu mola halide a io
o he PbX2 sal s. Fo FAPbI3, 0.50 mM o FA-ace a e was used, and o FAPbB 3, 0.25 mM o
FA-ace a e was used. This solu ion was hen degassed a 50 °C o 20 minu es, a e which, he
empe a u e was inc eased o 120 °C o induce comple e dissolu ion o he FA-olea e.3,4 Once
dissol ed, he a mosphe e o he 3-neck lask was changed o ni ogen be o e he injec ion p ocess.
The eac ion empe a u e o o m FAPb(I1-xB x)3 QDs a ied om linea ly 80 °C-135 °C based on
inpu mola halide composi ion, wi h FAPbB 3 syn hesis occu ing a 135 oC and FAPbI3 a 80 oC.
5-10 mL o he FA-olea e p ecu so was apidly injec ed in o he PbX2 solu ion a a a ge ed
empe a u e and he eac ion lask was quickly quenched in an ice ba h. (The concen a ion o FA-
olea e was di e en based on halide a io, howe e , an equal mola amoun o FA-olea e was
injec ed ac oss all halide a ios. Typically, he inpu mola halide a io o he PbX2 sal s a ied by
10-20% om he mola halide a io o he inal p oduc .)
To emo e excess ligands, he QDs we e aken in o 3 mL o oluene and hen subsequen ly c ashed
ou o solu ion by adding 5 mL o me hyl ace a e o he oluene suspension and cen i uging a
8000 RPM o 30 minu es. The supe na an was disca ded and he esul ing pelle was dispe sed
in 7 mL o oluene. The oluene based QD solu ion was mixed wi h 5mL o me hyl ace a e and
cen i uged a 8000 RPM o 10 minu es. The esul ing supe na an was disca ded and he pelle
was dispe sed in oc ane o use in cha ac e iza ion and de ice ab ica ion.
FA1-xCsxPb(I1-xB x)3 QD syn hesis
Mixed A-si e QDs we e o med ia pos -syn he ic mixing using me hods simila o hose shown
by Haza ika e .al.4 Fi s , FAPbI3 and CsPbB 3 QDs we e syn hesized using he me hods ou lined
abo e. Then, FAPbI3 and CsPbB 3 QD solu ions we e mixed a 70⁰C o 24 hou s in a ixed Cs:FA
mola a io. To con i m he exis ence o single phase FA1-xCsxPb(I1-xB x)3 QDs, he esul an
nanoc ys als we e cha ac e ized ia pho oluminescence emission and UV-Vis-NIR abso bance
spec oscopy o ensu e he con e gence o he luminescence peak and i s exci on.
Cha ac e iza ions
Abso bance and Pho oluminescence
UV-Vis abso p ion spec a we e measu ed using a Shimadzu UV-3600 UV-VIS-NIR abso p ion
spec opho ome e . S eady s a e PL emissions and PL exci a ion spec a we e measu ed in a
Ho iba’s Fluo omax-4 emission spec opho ome e .
QD ilm ab ica ion o de ices and TRMC measu emen s
QD ilms we e ab ica ed based on p e iously epo ed me hods.5 Sa u a ed solu ions o Pb(NO3)2
in MeOAc and FAI in E OAc we e p epa ed. Excess sal was emo ed by cen i uga ion a 3500
RPM o 5 min. To p epa e he QD ilm, concen a ed QD solu ions (~75 mg/mL) we e spin-cas
on o a TiO2 su ace a 1000 RPM o 20 s ollowed by 2000 RPM o 5 s. The esul ing ilms we e
dipped in o he Pb(NO3)2 solu ion o ~3 s ollowed by insing wi h nea MeOAc o ~3 s. This
p ocess was epea ed 3 imes o p oduce a hick QD ilm (100-400 nm). Du ing he ligand
exchange wi h he Pb(NO3)2 solu ion, he ambien ela i e humidi y (RH) was held a 15-25% RH
in a clima e con olled glo ebox. Once a hick QD ilm was deposi ed, ambien humidi y was
educed o 0% RH, and he ilms we e pos - ea ed wi h he FAI solu ion. The ilms we e dipped
in o he FAI solu ion o 10 s ollowed by insing wi h nea MeOAc.
De ice ab ica ion
A 50nm laye o TiO2 was deposi ed on o p e-pa e ned FTO coa ed glass subs a es (Thin Film
De ices Inc). Sol-gel TiO2 was p epa ed by mixing 5 mL o E OH, wo d ops o HCl, 125 mL o
deionized wa e , and 375 ml o i anium e hoxide, esul ing in a clea solu ion. The headspace o
he ial was illed wi h ni ogen, and he solu ion was s i ed o 48 hou s and hen kep in he
eeze un il use. The sol-gel was spin-cas a 3000 pm o 20 s and annealed a 115°C o 10 min
and 450°C o 30 min. The CsPbI3 QD ilm was deposi ed as no ed abo e. A spi o-OMeTAD hole-
anspo laye was spin-cas a 5000 RPM om a solu ion consis ing o 72.3 mg o spi o-
OMeTAD, 1mL o chlo obenzene, 28.8 μL o 4-TBP, and 17.5 μL o Li-TFSI solu ion (520 mg
Li-TFSI in 100 μL ace oni ile).6 A 15 nm laye o MoO3 was he mally e apo a ed a a a e o
0.1-0.5 Å/s a base p essu es o 2.7E-7 o . Finally, a 200 nm Al laye was he mally e apo a ed
a a a e o 0.5-2.0 Å/s. J/V cu es we e de eloped by es ing he de ices a 1 sun.
Time- esol ed pho oluminescence measu emen s
Time- esol ed pho oluminescence (TRPL) da a was measu ed ollowing exci a ion using a pulsed
exci a ion sou ce consis ing o a supe con inuum ibe lase (Fianium, SC-450-PP) ope a ing a 2
MHz coupled o an acous o-op ic uning il e (Fianium AOTF-Dual) o wa eleng h selec ion.
The exci a ion wa eleng h was chosen depending on he bandgap o he PQDs. The PQD emission
was ou ed o a isible s eak came a (Hamama su C10910-04) coupled o a spec og aph, and
ime- esol ed spec a we e collec ed o e a wa eleng h ange de e mined o co e he en i e PQD
emission spec um. In he TRPL s eak came a sys em, he ins umen esponse unc ion (IRF)
depends on he selec ed ime window, bu in all cases he IRF was signi ican ly sho e han he
measu ed PL decay.
Time- esol ed mic owa e conduc i i y measu emen s
Time- esol ed mic owa e conduc i i y (TRMC) is a pump-p obe echnique ha can be used o
measu e he pho oconduc ance o a ilm wi hou he need o cha ge collec ion a elec ical
con ac s.7,8
PQD ilms we e p epa ed on qua z subs a es p e-cu o ill he c oss-sec ion o an X-band
wa eguide (ca. 10.2 mm × 22.8 mm). This sample is placed in a mic owa e ca i y a he end o
he X-band wa eguide ope a ing a ca. 9 GHz, and is pho oexci ed h ough a g id wi h a ca. 5 ns
lase pulse om an op ical pa ame ic oscilla o (OPO) pumped by he hi d ha monic o an
Nd:YAG lase ope a ing a 10 Hz. The ela i e change o he mic owa e powe e lec ed om he
mic owa e ca i y, P, was eco ded and is due o abso p ion o he mic owa e p obe by
pho oinduced ee elec ons and holes in he sample, and can be ela ed o he pho oconduc i i y
by ΔP/P = −KΔG, whe e he calib a ion ac o K is expe imen ally de e mined indi idually o
each sample. Taking in o accoun ha pho oexci a ion esul s in pai s o elec ons and holes, he
peak pho oconduc ance can be exp essed as:
DG=
b
qeI0FA
S
m
( )
(S.E.1)
whe e qe is he elemen a y cha ge, β = 2.2 is he geome ic ac o o he X-band wa eguide used,
I0 is he inciden pho on lux, FA he ac ion o ligh abso bed a he exci a ion wa eleng h, ϕ is
he quan um e iciency o ee ca ie gene a ion pe pho on abso bed, and Σμ is he sum o he
mobili ies o elec ons and holes.
Eq. (S1) is used o e alua e he quan um e iciency o ee ca ie gene a ion pe pho on abso bed,
mul iplied by he local mobili y o ee ca ie s. These quan i ies can o en be co ela ed wi h
ma e ials p ope ies o p ocessing condi ions, o yield s uc u e- unc ion ela ionships ela ed o
ee ca ie gene a ion and anspo . Al hough he pho oconduc ance decay a e he end o he
lase pulse is also a use ul ool o he cha ac e iza ion o ee ca ie decay mechanisms by
ecombina ion and apping, his is beyond he scope o his s udy, He e, we employ a simple bi-
exponen ial i o he pho oconduc i i y decay ansien s, and he a e age ca ie li e ime was
calcula ed acco ding o he equa ion: τa g = (A0τ0 + A1τ1)/(A0 + A1).

Figu e S1. Compa ison o expe imen al PQD PV ol age ac ion o li e a u e. Ci a ions o his
igu e a e ound a he end o he Supplemen a y In o ma ion. 4,9–25
Table S1. De ice me ics o de ices shown in Figu e 2 o main ex
B comp
Voc
(V)
Jsc
(mA/cm2)
FF
PCE (%)
Re e se scan
0% B
1.18
16.27
0.73
14.17
8% B
1.13
14.99
0.60
10.39
13% B
1.08
10.36
0.47
5.32
1.6 1.8 2.0 2.2 2.4
101
102
103
Bandgap (eV)
Radia i e Li e ime (ns)
CsPb(I1-xB x)3
FAPb(I1-xB x)3
(FA1-xCsx)Pb(I1-xB x)3
x=0
x=0.16
x=0
x=0.42
x=0.19 x=0.45
x=0.12
x=0.74
x=0.70
x=0.88
x=0.95
Figu e S2. Radia i e li e ime o en i e PQD sample se .
𝜏𝑟𝑎𝑑 = 𝜑
𝜏 (S.E.2)
Equa ion S.E.2 shows how o calcula e adia i e li e ime (𝜏𝑟𝑎𝑑) using measu ed luo escence
li e ime (𝜏) and pho oluminescence quan um yield (𝜑). Rhodamine 6G was used o es ima e
ela i e quan um yield o he CsPb(I0.3B 0.7)3 sample because o he compa ibili y o he abso p ion
and emission spec a. The PLQY o he emainde o he samples we e es ima ed by compa ing
in eg a ed PL spec a. While ela i e PLQY measu emen s, such as his, ypically in ol e some
so o e o ange, we belie e he end o adia i e li e ime e sus bandgap and b omine con en
o be accu a e as shown in Figu e S4.
Figu e S3. TRPL ansien s o A) CsPb(I1-xB x)3, B) FAPb(I1-xB x)3, and C) FA1-xCsxPb(I1-xB x)3
colloidal PQDs used in de ices and o TRMC measu emen s.
Figu e S5. Yield-mobili y p oduc e sus bandgap o all PQD ilm samples

Figu e S6. A) abso bance o CsPb(I1-xB x)3 PQD samples used in de ices and TRMC
measu emen s, B) pho oluminescence spec a o CsPb(I1-xB x)3 PQD samples used in de ices and
TRMC measu emen s.
Figu e S7. A) abso bance o FAPb(I1-xB x)3 PQD samples used in de ices and TRMC
measu emen s, B) pho oluminescence spec a o FAPb(I1-xB x)3 PQD samples used in de ices and
TRMC measu emen s.
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