Investigation of Interfacial Charge Transfer in

Solution Processed Cs2SnI6 Thin Films

Gaurav Kapil, * Takeshi Ohta, Tsuguo Koyanagi, Murugan Vigneshwaran, Yaohong Zhang,

Yuhei Ogomi, Shyam S Pandey, Kenji Yoshino, Qing Shen, Taro Toyoda, Md. Mijanur

Rahman, Takashi Minemoto, Takurou N. Murakami, Hiroshi Segawa, Shuzi Hayase

The University of Tokyo, Research Center for Advanced Science and Technology, 4-6-1,

Komaba, Meguro-ku, Tokyo 153-8904, Japan

Kyushu Institute of Technology, Graduate School of Life Science and Systems Engineering, 2-4

Hibikino, Wakamatsu-ku, Kitakyushu 808-0196 Japan

University of Miyazaki, Faculty of Engineering, Gakuen-kibanadai-nishi-1-1, Miyazaki, 889-

2192, Japan

University of Electro Communication, Graduate school of Informatics and Engineering, 1-5-1

Chofugaoka, Chofu, Tokyo, 182-8585, Japan

Ritsumeikan University, Department of Electrical and Electronic Engineering , 1-1-1

Nojihigashi, Kusatsu, Shiga 525-8577, Japan

The National Institute of Advanced Industrial Science and Technology, 1-1-1 Higashi,

Tsukuba, Ibaraki 305-8565, Japan

E-mail: [email protected]

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 1.2
Cs2SnI6
P3HT/Cs2SnI6
1 P3HT
PCBM
Absorption (a.u.)

PCBM/Cs2SnI6
0.8

0.6

0.4

0.2

0
310 410 510 610 710 810
Wavelength (nm)
Figure S1. Absorption spectrum of thin films fabricated.

L=(0.9* Wavlength(X-ray source))/(FWHM)*(Cos 26.42)

90000
=(0.9* 0.15405 nm)/(26.74-26.16)* (3.14/180)*(Cos 26.42)
= 15 nm
80000

70000

60000 Cs2SnI6
Intensity (a.u)

50000

40000

30000

20000

10000 26.42

25.5 26.0 26.5 27.0 27.5

2

Figure S2. Crystallite size calculated using Scherrers formula using peak (222)

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Figure S3. TEM image showing particle size less than 10 nm.

Figure S4. Photoelectron yield spectroscopy (PYS) for HOMO measurement

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 Figure S5. Cross sectional SEM image for spray deposited film

0.02 -0.5 ps 0.020

-0.5
0.5 ps 0.015 0.5 ps
0.01
2 ps 0.010 2 ps
10 ps 10 ps
0.005
A

0.00 0.000

-0.005

-0.01 -0.010

-0.015

-0.02 -0.020
700 750 850 900 700 750 850 900
Wavelength (nm) Wavelength (nm)

(a) (b)

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 0 ps
1 ps 0.2
3 ps
0.04 10 ps 0.0

Normalized
100 ps
900 ps -0.2 0.71 mW
0.02 0.4 mW
-0.4
A

0.28 mW
0.15 m
0.00 -0.6

-0.8
-0.02
-1.0

-0.04 700 750 850 900 1 10 100 1000

Wavelength (nm) Time (ps)

(c) (d)

0.04
0.04
0.02
0.02
0.00
A

0.00 0 ps
0 ps -0.02 1 ps
1 ps 3 ps
-0.02 3 ps
10 ps
10 ps -0.04
100 ps 100 ps
-0.04 900 ps 900 ps

700 750 850 900 -0.06 700 750 850 900

Wavelength (nm) Wavelength (nm)
(e) (f)

Figure S6. fs-TA spectra (a) PCBM only (b) P3HT only (c) Cs2SnI6 only (d) Cs2SnI6 at different
pump power (e) Cs2SnI6 with PCBM and (f) Cs2SnI6 with P3HT pumped at 650 nm.

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 Figure S7. Absorption and PL spectra showing less possibility of energy transfer from
Cs2SnI6 to P3HT and PCBM

1.0 1.0 Cs2SnI6

With P3HT
0.8 Cs2SnI6 0.8 With PCBM
0.6 With P3HT 0.6
With PCBM
A

0.4 0.4

0.2 0.2

0.0 0.0

-0.2 -0.2
0 10 20 30 40 50 1 10 100 1000
time (ps) time (ps)
(a) (b)

Figure S8. fs-TA decay for different samples pumped at 650 nm and probed at 900 nm from
glass side

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 0.4 0.4
0.2 0.2
0.0 0.0
-0.2 -0.2
A(a.u.)

A(a.u.)
Cs2SnI6
-0.4 With P3HT -0.4 Cs2SnI6
-0.6 With PCBM -0.6 With P3HT
With PCBM
-0.8 -0.8
-1.0 -1.0
0 5 10 15 20 0 5 10 15 20 25 30
time(ps) time(ps)

(a) (b)

Figure S9. fs-TA decay for different samples pumped at 650 nm and probed at 710 nm from (a)
glass side (b) film side

-1 1.0
Cs2SnI6/P3HT (10 mg ml )
1.0 -1 Cs2SnI6/PCBM(10 mg ml )
-1

Cs2SnI6/P3HT (15 mg ml ) -1
Cs2SnI6/PCBM(40 mg ml )
Normalized A

Normalized A

0.5
0.5

0.0

0.0
-0.5

-0.5 -1.0
1E-6 1E-5 1E-4
1E-6 1E-5 1E-4
Time (s)
Time (s)
(a) (b)

Figure S10. ns-TAS of (a) Cs2SnI6/P3HT (b) Cs2SnI6/PCBM at different concentration.

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