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Supporting Information

1

Discussion on Electron Transport in BHJs with Different Acceptors

1. Evaluating Electron Mobilities with AS and SCLC Techniques

The structure of electron-only devices is ITO/Al/BHJ/LiF/Al, where an Al thin film between ITO

and BHJ acts as the hole blocking layer. Under a forward DC voltage biased with a small AC

perturbation, BHJ films show significant frequency dependent capacitances. A maximum in the

negative differential susceptance (−∆ B) can be extracted from a plot of −∆ B as a function of

frequency (f), and the corresponding frequency (f r ≡1/τ r) is defined to characterize the charge

carrier mobility from the follow relation

τ1 /2=0.56 τ r (S1a)

μave=d

τ1 /2 ∙ F= d2

0.56 τ r ∙V (S1b)

where τ r is the corresponding time, of which the maximum in −∆ B appears, τ1 /2 is the average

transit time of carriers, μave is the average carrier mobility, F is the applied electric field, V is the

applied voltage, and d is the BHJ thickness.

We study thefrequency-dependent capacitances of fullerene-based PTB7:PC71BM, PTB7-

Th:PC71BM, and non-fullerene-based PTB7-Th:ITIC BHJ films. First, effects of applied electric

fields were investigated. Figure S1displays AS signals of BHJs under various electric fields and

temperatures. AS signals of fullerene-based BHJs exhibit significant shifts of f r. For

PTB7:PC71BM BHJs, f r shifts towards to high frequency regions, when F increases gradually.

Correspondingly, under 240 and 300 (V/cm)1/2, calculated μe are 9.5×10-5 and 1.6×10-4 cm2V-1s-1,

respectively. However, there is no obvious shifts of f r in non-fullerene PTB7-Th:ITIC BHJs, and

2

f r maintains around 2×104 Hz, when the applied electric field increases from 300 to 450

(V/cm)1/2. Interestingly, unlike fullerene-based BHJs where f r mainly shifts in the frequency

domain, the PTB7-Th:ITIC film achieves lower minimum capacitances under relatively higher

fields, indicating enhanced dispersity of electron transports in highfields. Besides F, temperature

is another factor for electron transport in BHJs. As shown in Figure S1(d-f), f r moves to low

frequency region, when temperature decreases in both fullerene- and non-fullerene-based BHJ

films.

Space-charge-limited current (SCLC) was performed to evaluate the property of electron

transport in all-polymer-based PTB7-Th:N2200 BHJs.(Figure S2) The structure of electron-only

devices is the same with samples for AS measurements. Compared with PTB7:PC71BM, μ0 , e of

PTB7-Th:N2200 film exhibit reduced variations when we tune the D:A compositions. μ0 , eof the

[98:02] BHJ is 1.7×10-7 cm2V-1s-1, and increases gradually to 2.2×10-4 cm2V-1s-1 in the [67:33]

BHJ, which is the optimized D:A composition for OPV device fabrication. As different tools for

mobility measurements, results of carrier transports extracted from AS and SCLC are compared,

and the temperature dependent electron mobilities of fullerene-based PTB7:PC71BM, PTB7-

Th:PC71BM, and non-fullerene-based PTB7-Th:ITIC BHJs from AS and SCLC measurements

are summarized in Figure S3. μe , SCLC is typically half to one order larger than μe , AS, and one

possible explanation is the hole carrier leakage in the electron-only devices.[S1] At room

temperature, μe ,0 , SCLC of the [40:60] PTB7:PC71BM and [43:57] PTB7-Th:ITIC BHJs are 2.3×10-

4and 1.6×10-4cm2V-1s-1, whereas μe ,0 from AS for the same devices are 9.6×10-6and 1.3×10-

5cm2V-1s-1, respectively. However, each BHJ shows similar energetic disorders σ from both

measurements. σ decreases gradually from ~90meV in the PTB7:PC71BM BHJ to ~67meV in the

PTB7-Th:ITIC BHJ.3

　　Three popular BHJs are under investigation, involving fullerene-based PTB7:PC71BM, NF

small molecule-based PTB7-Th:ITIC, and all-polymer PTB7-Th:N2200. Figure S4 shows the

field dependent electron mobilities of BHJs with their BHJs before electron percolation (a-c);

BHJs during electron percolation (d-f); and optimized D:A compositions in solar cells at room

temperature (g-i). The field dependent electron mobilities can be well-expressed by the Poole-

Frenkel (PF) equation i.e.

μe (F )=μ0 ,e exp ( βe F1 /2 ) (S2)

where μ0 , e is the zero-field electron mobility, βe is the associated PF slope, and F is the applied

electric field.[S7,S8] The PF slope βe is used to describe the electric field dependence of charge

transport properties in solid-state films.[S9,S10] We observe distinct differences in βe for

acceptors with different topologies. As shown in Figure S7(g), the optimized PTB7:PC71BM BHJ

exhibits highly field-dependent electron mobilities with βe of 4.1×10-3(V /cm )

12. In contrast, Non-

fullerene BHJs exhibit suppressed PF effects. The electron mobilities in the optimized PTB7-

Th:ITIC BHJ slightly fluctuate around 10-5 cm2V-1s-1. Interestingly, the optimized PTB7-

Th:N2200 BHJ displays negative PF effects of the electron transport, and the all-polymer BHJ

achieves higher electron mobilities under low applied field. The different PF effects of fullerene-

based BHJs, NF small molecular BHJs, and all-polymer BHJs are attributed to film topologies.

4

Figure S1. Capactiance-frequency signals of devices for AS measurements. The electron-only devices

had a structure of ITO/Al/BHJ/LiF/Al. The Al layer next to ITO was to block holes. (a-c) BHJs under

various applied electric field; (d-f) BHJs in RT and low temperatures; and (h-g) PTB7-Th:ITIC and

PTB7:PC71BM films with different D:A weight compositions of which electron transport are in the

conditions of (h) before percolation; (i) near critical point; and (g) PCE-optimized BHJs.

5

Figure S2. JV characteristics of electron-only PTB7-Th:N2200 BHJ devices with various D:A

compositions at room temperature.

6

0 100 200 300 400 50010-6

10-5

10-4

10-3

PTB7:PC71BM PTB7-Th:PC71BM PTB7-Th:ITIC

Carr

ier M

obili

t(cm

2 V-1s-1

)

F1/2[(V/cm)1/2]

0 3 6 9 12 15 1810-7

10-5

10-3

10-1

From SCLC PTB7:PC71BM PTB7-Th:PC71BM PTB7-Th:ITIC

From AS PTB7:PC71BM PTB7-Th:PC71BM PTB7-Th:ITICZe

ro F

ield

Mob

ility

(cm

2 V-1s-1

)

(1000/T)2(K-2)

Figure S3 (a) Electron mobilities of PTB7:PC71BM, PTB7-Th:PC71BM, and PTB7-Th:ITIC

BHJs as a function of applied electric field from AS measurements at room temperature; (b)

zero-field electron mobilities of PTB7:PC71BM, PTB7-Th:PC71BM, and PTB7-Th:ITIC BHJs at

different temperatures extracted from AS and SCLC measurements.

7

Figure S4. Field dependent electron mobilities of PTB7:PC71BM, PTB7-Th:ITIC and PTB7-

Th:N2200 BHJs (a-c) before electron percolation; (d-f) near critical points of electron

percolation; and (g-i) optimized D:A compositions in BHJ solar cells.

8

Figure S5. Logarithm of electron mobilities of PTB7:PC71BM, PTB7-Th:ITIC, and PTB7-

Th:N2200 BHJs as a function of the acceptor weight fraction. Circular symbols are data and solid

curves are fits to the data using Eq. 3.

9

Figure S6. JV characteristics of (a) binary PTB7:PC71BM and (b) PTB7-Th:N2200 and ternary

devices with different polystyrene weight fractions under 100mW/cm2 of AM 1.5G condition.

10

Figure S7. JV characteristics of PTB7-Th:PC71BM; and PTB7-Th:N2200 BHJ solar cells before

and after moisture treatments (RH ~75-85%) for different exposure times (a) fresh cells; (b) 30

mins; (c) 60 mins; and (d) 120 mins. BHJ films with PC71BM acceptor degrade severely after

moisture exposure. In contrast, BHJ films with polymer acceptor N2200 remain almost

immuned.

11

Figure S8. JV characteristics of (a) PTB7:PC71BM (1:1.5), PTB7:PC71BM:PS (1:1.35:0.15) and

(b) PTB7-Th:N2200 (1:1.5), PTB7-Th:N2200:PS (1:0.45:0.05) electron-only devices.

12

Figure S9. AFM height images of PTB7:PC71BM, PBDB-T-SF:IT-4F, and PTB7-Th:N2200

BHJs in fresh and after a 180-min high humidity treatment.

13

Table S1. Fitting parameters of Eq. 3 for electron acceptors of N2200, ITIC, and PC71BM. The hopping distance ξ of the electron in BHJs is adopted from the reference 25. The saturation mobilities of N2200, ITIC, and PC71BM are adopted from the magnitude of the references S24, S25,S11-S14 and our data. b/a is estimated using the approximate dimensions of the acceptors. For the polymer acceptor N2200, the average repeatable NDI units is calculated from the molecular weight reported by 1-Material.

N2200 ITIC PC71BM

D /ξ 150 15 9

b /a 13 0.16 1

μ0 (cm2V-1s-1) 10-4 10-5 10-4

Chemical List

PTB7: Poly({4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b]dithiophene-2,6-diyl}{3-fluoro-2-[(2-ethylhexyl)carbonyl] thieno[3,4-b]thiophenediyl})

PTB7-Th: Poly[4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b;4,5-b']dithiophene-2,6-diyl-alt-(4-(2-ethylhexyl)-3-fluorothieno[3,4-b]thiophene-)-2-carboxylate-2-6-diyl)]

PBDB-T: Poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)-benzo[1,2-b:4,5-b’]dithiophene))-alt-(5,5-(1’,3’-di-2-thienyl-5’,7’-bis(2-ethylhexyl)benzo[1’,2’-c:4’,5’-c’]dithiophene-4,8-dione)]

PBDB-T-SF: Poly[(2,6-(4,8-bis(5-(2-ethylhexylthio)-4-fluorothiophen-2-yl)-benzo[1,2-b:4,5-b’]dithiophene))-alt-(5,5-(1’,3’-di-2-thienyl-5’,7’-bis(2-ethylhexyl)benzo[1’,2’-c:4’,5’-c’]dithiophene-4,8-dione)]

N2200: Poly{[N,N'-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)}

ITIC: 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2’,3’-d’]-s-indaceno[1,2-b:5,6-b’]dithiophene

ITM: 3,9-bis(2-methylene-((3-(1,1-dicyanomethylene)-6/7-methyl)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2’,3’-d’]-s-indaceno[1,2-b:5,6-b’]dithiophene

ITIC-Th: 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(5-hexylthienyl)-dithieno[2,3-d:2’,3’-d’]-s-indaceno[1,2-b:5,6-b’]dithiophene

14

IT-4F: 3,9-bis(2-methylene-((3-(1,1-dicyanomethylene)-6,7-difluoro)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2’,3’-d’]-s-indaceno[1,2-b:5,6-b’]dithiophene

IEICO-4F: sindaceno[1,2-b:5,6-b'] dithiophene-2,7-diyl)bis(4-((2-ethylhexyl)oxy)thiophene-5,2-diyl))bis (methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1diylidene))dimalononitrile

PCBM: [6,6]-Phenyl-C61-butyric acid methyl ester

PC71BM: [6,6]-Phenyl-C71-butyric acid methyl ester

ICBA: 1′,1′′,4′,4′′-Tetrahydro-di[1,4]methanonaphthaleno[1,2:2′,3′,56,60:2′′,3′′][5,6]fullerene-C60

15

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