High-pe o mance la ge-a ea blade-coa ed pe o ski e sola cells wi h
low ohmic loss o low ligh ing indoo applica ions
Zhuoneng Bi,1,2 Xueqing Xu,1,2* Xia Chen,1 Yanqing Zhu,1 Chang Liu, 3 Hua Yu,
3* Yupeng Zheng,1,2 Pa el A. T oshin,4,5 An onio Gue e o, 6 Gang Xu1,2
1
Key Labo a o y o Renewable Ene gy, Guangdong Key Labo a o y o New and
Renewable Ene gy Resea ch and De elopmen , Guangzhou Ins i u e o Ene gy
Con e sion, Chinese Academy o Sciences, Guangzhou 510640, China
2 Cen e o Ma e ials Science and Op oelec onics Enginee ing, Uni e si y o Chinese
Academy o Sciences, Beijing 100049, China
3 Ins i u e o Pho o ol aics, Sou hwes Pe oleum Uni e si y, Chengdu 610500, P. R.
China
4 Silesian Uni e si y o Technology, Akademicka 2A, 44-100 Gliwice, Poland
5 Ins i u e o P oblems o Chemical Physics o he Russian Academy o Sciences
(IPCP RAS), Academician Semeno a enue 1, Che nogolo ka, Moscow egion,
142432 Russian Fede a ion
6 Ins i u e o Ad anced Ma e ials (INAM), Uni e si a Jaume I, 12006 Cas elló, Spain
* Co esponding au ho
email: [email protected], [email p o ec ed]m
Abs ac
Eme ging hyb id o ganic-ino ganic pe o ski es wi h supe io op oelec onic
p ope y demons a e p omising p ospec o pho o ol aic applica ions, in pa icula o
low-ligh ing indoo applica ions e.g. wi hin in e ne o hings (IoT) ne wo ks o low-
ene gy wi eless communica ion de ices. In o de o p epa e de ices wi h high powe
ou pu unde low-illumina ion condi ions, scalable ab ica ion echniques a e p e e ed
o la ge-a ea pe o ski e sola cells. In addi ion, one o he key pa ame e s o achie e
high-e iciency la ge-a ea pe o ski e sola cells is o minimize he ohmic loss o u he
boos he sola cell e iciency. He ein, a one-s ep blade-coa ing me hod assis ed by
hexa luo obenzene (HFB) was de eloped o deposi la ge-a ea smoo h and de ec - ee
pe o ski e ilms wi h low ohmic loss. The as- ab ica ed de ices demons a ed powe
con e sion e iciency (PCE) o 20.7% (a ea o 0.2 cm2) and 16.5% (1 cm2),
espec i ely, unde s anda d 1000 mW/cm2 (AM1.5G) illumina ion condi ions.
Besides, he la ge-a ea (1 cm2) de ices demons a ed a ema kable PCE o ~32% unde
0.1 mW/cm2 (~285 lux) illumina ion p o ided by whi e ligh -emi ing diode (LED)
lamp o indoo ligh ing which s ongly indica e ha he ab ica ed la ge-a ea de ices
exhibi ed p ac ical applica ions o be used in he as majo i y o low-ligh ing indoo
condi ions (≥100 lux). The analysis using a single diode model sugges s ha he high
pe o mance o he la ge-a ea de ices unde low-ligh ing indoo condi ions is highly
associa ed wi h he la gely educed ohmic losses o he pe o ski e ilms by a acile and
scalable blade-coa ing me hod. The ohmic loss o he 1 cm2 de ice was es ima ed as
low as 1.66% a ~285 lux. The p esen ed scalable app oach pa es he way o designing
high-pe o mance pe o ski e sola cells o a a ie y o eme ging indoo PV
applica ions.
Keywo ds: pe o ski e sola cells, blade-coa ing, la ge a ea, low-ligh ing indoo
applica ions, ohmic loss
In oduc ion
Hyb id o ganic-ino ganic pe o ski e sola cells (PSCs) ha e been demons a ed o
be one o he mos p omising candida es o he nex gene a ion pho o ol aics due o
hei high powe con e sion e iciency (PCE) and low ma e ials and ab ica ion cos 1,
2. PSCs ha e e sa ile p omising applica ions in po able elec onics, such as emo e
ene gy-independen senso s o he in e ne o hings ne wo ks, o low-ene gy wi eless
communica ion de ices 3-5. Mos o hese de ices need o wo k con inuously unde low
indoo illumina ion condi ions (100 ~ 1000 lux) 5. Low-ligh ing indoo pho o ol aics
has a e y high demand in he cu en and u u e powe -supply ma ke 4. Hence, he
low-ligh ing indoo pe o ski e pho o ol aics ha e ecen ly eme ged as one o he
p omising and p ac ical echnology o indoo powe supply 6-11.
O ganic-ino ganic pe o ski e abso be ma e ials is one o he ideal candida es o
indoo pho o ol aics since hei abso p ion spec a pe ec ly ma ch he emission spec a
o LED o luo escen lamps (400 - 800 nm) 12. Recen ly, Liu e al. achie ed an
imp essi e PCE o 40.1% unde indoo illumina ion condi ions (824.5 lux) o he
pe o ski e sola cell wi h a small ac i e a ea o 0.08 cm2 12. The e a e also mul iple
o he epo s on small-a ea PSCs deli e ing PCEs o 30 – 40% unde indoo condi ions.
Howe e , he small a ea de ice is no p ac ically o comme cializa ion use and he
de elopmen o la ge-a ea indoo PSCs is impeded by la ge ohmic loss. Feng e al. ha e
epo ed one o he highes eco ds o da e o la ge-a ea de ices (2.25 cm2)
demons a ing excellen PCE o 30.6% unde indoo condi ion (1000 lux)13.
Gene ally, he e a e wo popula app oaches o imp o e PCE o PSCs unde indoo
illumina ion condi ions. The i s app oach equi es he de ices achie ing high shun
esis ance (Rsh), which can e ec i ely minimize ohmic losses unde low-ligh
condi ions 14-16. In e ace modi ica ion is a common s a egy o ob ain high shun
esis ance de ices 6, 14. The o he app oach is based on supp essing he cha ge ca ie
ecombina ion losses, which is mani es ed in he diode ideali y ac o s (n) close o 1 10.
The ideali y ac n can be es ima ed om he dependence o he open-ci cui ol age
(VOC) on he inciden ligh in ensi y 13. Achie ing good ideali y ac o s equi es
supp essing ap-assis ed ecombina ion wi hin he de ice. The passi a ion o aps and
de ec s in he pe o ski e ilms is an e ec i e way o educe VOC losses 12.
Fo po en ial p ac ical applica ions, low-ligh ing pe o ski e sola cells should be
p oduced using scalable echniques compa ible wi h he oll- o- oll p ocess. Howe e ,
mos o he pe o ski e ilms epo ed so a p epa ed by non-scalable me hods such as
spin-coa ing. To da e, la ge-a ea deposi ion me hods emain insu icien ly in es iga ed.
The i s epo s on blade-coa ing we e published in 2015, and p esen ed PSCs wi h he
PCEs o 11-15% p oduced using DMF as a sol en 17, 18. Mo e ecen ly, meniscus-
assis ed echnique p oduced la ge-g ain pe o ski e ilms, which boos ed he de ice
e iciency up o 20% (using DMSO as a sol en ) 19. Sol en mix u es o DMSO and
gamma-bu y olac one (GBL) we e p e iously used o ab ica e PSCs wi h he PCE o
abou 18% 20, 21. Fu he de elopmen o he blade-coa ing echniques o PSCs
ab ica ion is commonly conside ed as one o he mos p omising s eps owa ds la ge-
scale comme cial applica ions o PSCs 2, 22-25.
In his wo k, we p esen a one-s ep blade-coa ing assis ed by HFB app oach o
deposi high-quali y de ec - ee pe o ski e ilms o indoo pe o ski e pho o ol aics.
The p oposed me hod p oduces highly c ys alline pe o ski e ilms in a single s ep by
using enginee ed inks based on a low inhala ion oxic sol en mix u e o DMSO, GBL
and HFB. The p ehea ing o he p ecu so ink enables comple e dissolu ion o PbI2 and
MAI in he mixed sol en close o he solubili y limi . I is ound ha he HFB addi i e
e ec i ely smoo hs down he pe o ski e ilms and passi a e he de ec s, hus, he as-
ab ica ed de ices demons a e high powe con e sion e iciency (PCE) o 20.7% on a
small a ea o 0.2 cm2 and 16.5% on he a ea o 1 cm2 unde s anda d 1 sun (AM1.5G)
illumina ion condi ions. Fu he mo e, he la ge-a ea (1 cm2) de ices deli e a
ema kable PCE o ~32% unde 0.1 mW/cm2 (~285 lux) illumina ion p o ided by ligh -
emi ing diode (LED) lamp.
Resul s and discussion
Figu e 1. a) Schema ic diag am o he HFB-assis ed one-s ep blade-coa ing me hod o
p oduce high-quali y de ec - ee MAPbI3 ilm. b) Pho og aphs o MAPbI3 p ecu so
solu ions wi h and wi hou HFB a oom empe a u e and a 70 oC.
Figu e 1a shows he schema ic diag am o he blade-coa ing se up o p oduce
MAPbI3 pe o ski e ilms. In he expe imen al p ocess he subs a e is ixed on a
ho pla e wi h a blade se abo e he subs a e o ming he sli o a ound 100 m. The
pe o ski e p ecu so ink is injec ed in o he sli and he p e-hea ing blade immedia ely
mo es ho izon ally on he hea ing subs a e. Wi h he sol en e apo a ing, he black
pe o ski e ilm o ms in a couple o seconds. The one-s ep blade coa ing p ocess is e y
simple and adap s o di e en p ocess a ia ions. In addi ion, o u he imp o e he
quali y o pe o ski e ilms on his one-s ep blade coa ing app oach he sol en may
be easily modi ied. In pa icula we obse e ha he use o a co-sol en HFB in he
pe o ski e p ecu so is bene icial o he ilm quali y. Fu he de ails o he one-s ep
blade-coa ing p ocess a e gi en in he expe imen al sec ion.
Figu e 2. a, d) AFM images o he Con ol and HFB 15% MAPbI3 ilms. b, e) Top-
iew and c, ) c oss-sec ion SEM images o he Con ol HFB 15% samples.
Figu e 1b shows a image o he e e ence p ecu so solu ion and he modi ied ink
loaded wi h HFB addi i e. HFB is a low inhala ion oxic o ganic sol en ha is
commonly used in medicine 26. HFB is immiscible wi h wa e , bu i can be miscible
wi h DMSO in a ce ain p opo ion 27. A oom empe a u e, pe o ski e inks wi h HFB
addi i e a e non- anspa en , which indica es incomple e ma e ial solubiliza ion bu o
he p esence o a bad sol en (o an i-sol en ) such as HFB. Howe e , p ehea ing he

p ecu so solu ion a 70 oC esul s in comple e solubiliza ion o PbI2 and MAI and
o ma ion o anspa en solu ion wi h ma e ial concen a ions close o he solubili y
limi leading o sa u a ed solu ions.
Figu e S1 shows he scanning elec on mic oscopy (SEM) images o he MAPbI3
ilms p epa ed om he inks wi h di e en HFB loadings and ma ked as Con ol
(co esponds o HFB 0%), HFB 5%, HFB 10%, and HFB 15%. All samples exhibi
sphe uli ic g ow h and la ge gain size wi h no oids o pinholes. The Con ol and HFB
15% samples display ob ious di e ence be ween as illus a ed by he SEM images
shown in Figu es 2b and 2e. The HFB 15% sample exhibi s a la and uni o m
c ys alline g ain su ace, whe eas he Con ol sample has wa y su ace mo phology.
The su ace opog aphy o he ilms was u he s udied by a omic o ce mic oscopy
(AFM) as shown in Figu e 2a and 2d. The oo -mean-squa e oughness alues o he
Con ol and HFB 15% samples we e de e mined as 28.1 and 20.5 nm, espec i ely,
which is consis en wi h he SEM images. The c oss-sec ion SEM images (Figu es 2c,
2 and S2) e eal he a e age hickness o pe o ski e ilms as ~415 nm and ~438 nm
o Con ol and HFB 15% samples, espec i ely. I is wo h no ing ha he HFB 15%
sample shows a mo e uni o m s uc u e and hickness o he pe o ski e ilm.
Figu e 3. Cha ac e iza ion o he MAPbI3 ilms wi h di e en HFB loadings on he
glass/FTO/SnO2-PbO/SnO2 subs a es. a) XRD di ac ion pa e ns. b) UV- is
abso p ion spec a. c) S eady-s a e PL spec a. d) Time- esol ed PL (TRPL) p o iles.
The e ec o he HFB addi i e on he s uc u al and op ical p ope ies o pe o ski e
ilms is illus a ed in Figu e 3a and Figu e 3b, espec i ely. All samples show simila
peaks on he x- ay di ac ion (XRD) pa e ns, indica ing a high phase pu i y o he
pe o ski es. The di ac ion peaks a 14.12˚ 20.02˚ 28.46˚ 31.90˚ and 40.70˚ can be
assigned o (110), (112), (220), (310), and (224) c ys al planes o he e agonal MAPbI3
pe o ski e la ice, espec i ely 18. The sha p and in ense (112) di ac ion peaks indica e
a highly o ien ed c ys al s uc u e o he ilms. In e es ingly, he addi ion o HFB
inc eases he in ensi y o (110) peaks, sugges ing imp o ed ilm c ys alliza ion.
The abso p ion spec a become signi ican ly s onge wi h inc easing he HFB
loading om 0% o 15%. We belie e ha he uni o m hickness o HFB-p ocessed ilms
helps o a oid abso p ion losses, while in he case o Con ol samples some ligh passes
h ough he oids o deep alleys in he ilms. Thus, he ob ained esul s e eal ha
HFB can no only make he pe o ski e ilms mo e uni o m bu also al e he c ys al
g ow h and enhance ilm abso bance.
Figu es 3c and 3d show s eady-s a e pho oluminescence (PL) and ime- esol ed
pho oluminescence (TRPL) spec a. The PL peaks o he HFB p ocessed sample a e
ed-shi ed compa ed o ha o he Con ol sample and he magni ude o he ed-shi
is p opo ional o he HFB loading wi h a ~7 nm peak shi o he HFB 15% sample.
Fu he mo e, a ed-shi o he low-ene gy abso p ion onse was obse ed, which in
combina ion wi h PL da a implies ha he HFB-p ocessed samples ha e a sligh ly lowe
bandgap as compa ed o he Con ol, which could be a consequence o he enhanced
ma e ial c ys allini y. The cha ge ca ie li e imes in he HFB-p ocessed samples we e
conside ably longe han ha o he Con ol (

1= 36.0 ns and

2= 73.7 ns) sample and
he li e ime inc ease was p opo ional wi h he HFB loading. In pa icula , he HFB 15%
sample showed almos wice longe li e imes (

1 = 52.7 ns and

2= 122.8 ns) as
compa ed o he Con ol sample, which e idences ha HFB addi i e e ec i ely
supp esses ap-assis ed ca ie ecombina ion due o he o ma ion o high-quali y
pe o ski e g ains wi h a low densi y o de ec s.
Fab ica ion and cha ac e iza ion o pho o ol aic de ices
Figu e 4. a) J-V cu es measu ed unde s anda d 100 mW cm-2 AM1.5G simula ed
illumina ion condi ions. b) EQE spec a o he de ices. c) S a is ics o 20 Con ol and
20 HFB 15% de ices. d) S abilized ou pu measu emen s in he maximum powe poin
acking egime unde he s anda d illumina ion condi ions.
Pho o ol aic de ices we e ab ica ed wi h de ice a chi ec u e o Glass/FTO/SnO2-
PbO/SnO2/MAPbI3/Spi o-OMeTAD/Au. The MAPbI3 ilms we e p epa ed wi h
di e en HFB loadings in he p ecu so ink, which a e ma ked as Con ol, HFB 5%,
HFB 10%, and HFB 15% samples. Fu he de ails on he de ice ab ica ion can be
ound in he Expe imen al sec ion. I is wo h men ioning ha he deposi ion o MAPbI3
by he de eloped one-s ep blade coa ing me hod does no equi e any addi ional s eps
such as sol en annealing o an i-sol en ba h, e c. The ep esen a i e J-V cu es
measu ed unde he simula ed 1 sun illumina ion condi ions a e p esen ed in Figu e 4a,
whe eas he co esponding de ice pa ame e s a e summa ized in Table S1.
The Con ol de ices show PCE exceeding 17%, which is in good ag eemen wi h he
p e iously epo ed cha ac e is ics o he MAPbI3 de ices ab ica ed in d y box
condi ions wi h a ela i e humidi y be ween 10% o 20%. Howe e , inc easing o HFB
amoun in he ink imp o es he pho o ol aic pe o mance o he de ices p ocessed
unde he same condi ions. Using he op imal amoun o HFB (15%), he champion
cells wi h a PCE o 20.7%, open-ci cui ol age VOC o 1.13 V, sho -ci cui cu en
densi y JSC o 23.4 mA/cm2, and ill ac o FF o 78.4% was achie ed. The s abilized
ou pu measu emen s o he PCE and pho ocu en densi y o he champion cell
deli e ed he alues o 19.8% and 21.9 mA/cm2, espec i ely (Figu e 4d). The ob ained
pho ocu en densi y is in good ag eemen wi h he in eg a ed JSC ex ac ed om he
EQE spec um by i s in eg a ion o e he e e ence sola AM1.5G spec um (Figu e 4b).
The s a is ics o 20 de ices o each ype (Figu e 4c) show a ema kable imp o emen
in a e age PCE om 16.6% o 19.1% when HFB is inco po a ed in o he p ecu so inks.
Fu he mo e, i was su p ising ha HFB addi i e also imp o es he en i onmen al
s abili y o he de ices as shown in Figu e S4. Thus, HFB could be conside ed as a
highly p omising co-sol en o pe o ski e inks and p ocessing addi i e imp o ing
simul aneously he e iciency and s abili y o PSCs.
Design and cha ac e iza ion o la ge-a ea PSCs o low ligh ing indoo
applica ions
Figu e 5. a) J-V cu e o he ab ica ed de ice wi h an ac i e a ea o 1 cm2 measu ed
unde simula ed 1 sun illumina ion condi ions. b) The linea dependences o -dV/dJ s.
(JSC-J)-1 o de ices wi h di e en ac i e a ea sizes c) J-V cu es o 1 cm2 cell measu ed
unde di e en illumina ion in ensi ies p o ided by whi e-ligh LED. C) J-V cu e
unde 0.1 mW/cm2 (~285 lux) whi e LED. e) J-V cu es measu ed in he da k o
de ices wi h di e en ac i e a ea sizes; inse shows he es ima ion o Rsh alues. ) VOC
plo as a unc ion o illuminance o he calcula ion o ideali y ac o .
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