Lead-free double-halide perovskite Cs 3 BiBr 6 with well-defined crystal structure and high thermal stability for optoelectronics
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1 Electronic Supplementary Material (ESI) for Journal of Materials Chemistry C. This journal is The Royal Society of Chemistry 2019 Electronic Supplementary Information (ESI) Lead-free double-halide perovskite Cs 3 BiBr 6 with well-defined crystal structure and high thermal stability for optoelectronics Yingying Tang, a Mingli Liang, a Bingdong Chang, b Hongyu Sun, c Kaibo Zheng, a,d Tönu Pullerits, d Qijin Chi* a a. Department of Chemistry, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark b. DTU Danchip, Technical University of Denmark, 2800 Kongens Lyngby, Denmark c. Department of Micro- and Nanotechnology, Technical University of Denmark, 2800 Kongens Lyngby, Denmark d. Department of Chemical Physics and NanoLund, Lund University, Box 124, 22100, Lund, Sweden * To whom correspondence should be addressed. cq@kemi.dtu.dk; Phone:
2 Contents: Table S1. Crystal data and structure refinements for the Cs 3 BiBr 6. Table S2. Atomic coordinates and equivalent isotropic displacement parameters for Cs 3 BiBr 6. Table S3. Bond lengths (A) and angles (deg) for Cs 3 BiBr 6. Table S4. Anisotropic displacement parameters for Cs 3 BiBr 6. Table S5. Crystallographic and electronic parameters for the known perovskites. Fig. S1 View of the structures constructed by (a) Bi1 and (b) Bi2, respectively. Fig. S2 Comparison of XRD pattern for Cs 3 BiBr 6, Rb 3 BiBr 6, Cs 3 BiCl 6. Fig. S3 TGA curves of Cs 3 BiBr 6 and CH 3 NH 3 PbBr 3. Fig. S4 (a) Electron micrograph of the microstructure for the photodetector. (b)-(d) Energy dispersive X-ray (EDX) mapping of the element distribution: (b) Br, (c) Cs, (d) Bi. Fig. S5 EQE versus voltage under light illumiantion of 4 mw/cm 2 and 25 mw/cm 2. Fig. S6 The high-resolution I-t curve of Cs 3 BiBr 6 devices towards 400 nm illumination with a powder intensity of 25 mw/cm 2. Fig. S7 Photoresponse of Cs 3 BiBr 6 under white light illumination with power density of 350 mw/cm 2. Fig. S8 EQE versus voltage under light illumination of 4 mw/cm 2 and 25 mw/cm 2. Fig. S9 The high-resolution I-t curve of Cs3BiBr 6 devices towards 400 nm illumination with a powder intensity of 25 mw/cm 2. Fig. S10 Photoresponse of Cs 3 BiBr 6 under white light illumination with power density of 350 mw/cm 2. Fig. S11 The stability for the photodetector under light illumination. 2
3 Table S1. Crystal data and structure refinements for the Cs 3 BiBr 6. formula Cs 3 BiBr 6 fw T, K room temp λ, Å space group Pbcm a, Å 8.689(2) b, Å (1) c, Å (9) α, deg 90 β, deg 90 γ, deg 90 V, Å (6) Z 8 D calcd, g cm µ, mm GOF on F R1,wR2 [I >2σ(I)] a , R1,wR2(all data) , a R1 = F o - F c / F o, wr2 = { w[(f o ) 2 (F c ) 2 ] 2 / w[(f o ) 2 ] 2 } 1/2 Table S2. Atomic coordinates ( 10 4 ) and equivalent isotropic displacement parameters (Å ) for Cs 3 BiBr 6. U(eq) is defined as one third of the trace of the orthogonalized Uij tensor. Atom x y z U(eq) Bi(1) 7451(1) 806(1) (1) Bi(2) -2141(1) (1) Cs(3) 3140(1) -939(1) 1546(1) 35(1) Cs(2) 8180(1) -2461(1) 1615(1) 37(1) Br(5) 6001(1) -1075(1) (1) Br(6) 8801(1) 2722(1) (1) Br(7) -2221(2) -4191(1) 588(1) 57(1) Br(4) 294(1) -1717(1) 582(1) 47(1) Br(3) 9470(1) 202(1) 1752(1) 48(1) Br(2) 5486(1) 1392(1) 1720(1) 46(1) Br(1) -4459(1) -3387(1) -581(1) 51(1) Cs(1) -2566(1) -5855(1) -493(1) 70(1) 3
4 Table S3. Bond lengths (Å) and angles (deg) for Cs 3 BiBr 6. Bi(1)-Br(3) (9) Bi(1)-Br(3)# (8) Bi(1)-Br(5) (11) Bi(1)-Br(6) (11) Bi(1)-Br(2) (8) Bi(1)-Br(2)# (8) Bi(2)-Br(7) (8) Bi(2)-Br(7)# (8) Bi(2)-Br(1) (9) Bi(2)-Br(1)# (9) Bi(2)-Br(4) (9) Bi(2)-Br(4)# (9) Cs(3)-Br(1)# (10) Cs(3)-Br(3)# (11) Cs(3)-Br(6)# (9) Cs(3)-Br(5) (10) Cs(3)-Br(7)# (11) Cs(3)-Br(4) (10) Cs(3)-Br(2) (11) Cs(3)-Br(2)# (11) Cs(2)-Br(4)# (10) Cs(2)-Br(2)# (11) Cs(2)-Br(6)# (10) Cs(2)-Br(5) (10) Cs(2)-Br(7)# (11) Cs(2)-Br(3)# (11) Cs(2)-Br(3) (10) Cs(2)-Br(1)# (12) Cs(2)-Bi(2)# (5) Cs(1)-Br(4)# (11) Cs(1)-Br(4)# (13) Cs(1)-Br(2)# (13) Cs(1)-Br(3)# (15) Cs(1)-Br(1)# (15) Cs(1)-Br(7)# (17) Cs(1)-Cs(1)# (15) Cs(1)-Cs(3)# (9) Cs(1)-Cs(3)# (9) Cs(1)-Cs(2)# (10) Br(3)-Bi(1)-Br(3)# (5) Br(3)-Bi(1)-Br(5) 90.73(3) Br(3)-Bi(1)-Br(6) 90.63(3) Br(5)-Bi(1)-Br(6) (3) Br(3)-Bi(1)-Br(2) 84.22(3) Br(3)#1-Bi(1)-Br(2) (3) Br(5)-Bi(1)-Br(2) 89.28(3) Br(6)-Bi(1)-Br(2) 89.42(3) Br(3)-Bi(1)-Br(2)# (3) Br(3)#1-Bi(1)-Br(2)# (3) Br(5)-Bi(1)-Br(2)# (3) Br(6)-Bi(1)-Br(2)# (3) Br(2)-Bi(1)-Br(2)# (4) Br(7)-Bi(2)-Br(7)# (6) Br(7)-Bi(2)-Br(1) 87.83(3) Br(7)#2-Bi(2)-Br(1) 90.18(3) Br(1)-Bi(2)-Br(1)# (5) Br(7)-Bi(2)-Br(4) 89.87(3) Br(7)#2-Bi(2)-Br(4) 92.21(3) Br(1)-Bi(2)-Br(4) (3) Br(1)#2-Bi(2)-Br(4) 92.66(3) Br(4)-Bi(2)-Br(4)# (4) Br(7)-Bi(2)-Cs(2)# (2) Br(7)#2-Bi(2)-Cs(2)# (2) Br(1)-Bi(2)-Cs(2)# (2) Br(1)#2-Bi(2)-Cs(2)# (2) Br(4)-Bi(2)-Cs(2)# (2) Br(4)#2-Bi(2)-Cs(2)# (19) Br(7)#2-Bi(2)-Cs(2)# (2) Br(1)-Bi(2)-Cs(2)# (2) Cs(2)#3-Bi(2)-Cs(2)# (17) Br(1)#5-Cs(3)-Br(3)# (3) Br(1)#5-Cs(3)-Br(6)# (3) Br(3)#4-Cs(3)-Br(6)# (2) Br(1)#5-Cs(3)-Br(5) 97.66(3) Br(3)#4-Cs(3)-Br(5) (3) Br(6)#6-Cs(3)-Br(5) 76.27(2) Br(1)#5-Cs(3)-Br(7)# (3) Br(3)#4-Cs(3)-Br(7)# (3) Br(6)#6-Cs(3)-Br(7)# (3) Br(5)-Cs(3)-Br(7)# (3) Br(1)#5-Cs(3)-Br(4) 77.20(3) Br(3)#4-Cs(3)-Br(4) 69.78(2) Br(6)#6-Cs(3)-Br(4) 93.95(2) Br(5)-Cs(3)-Br(4) (3) Br(7)#7-Cs(3)-Br(4) 61.86(2) Br(1)#5-Cs(3)-Br(2) 89.80(3) Br(3)#4-Cs(3)-Br(2) 95.41(3) Br(6)#6-Cs(3)-Br(2) (2) Br(5)-Cs(3)-Br(2) 65.41(2) Br(7)#7-Cs(3)-Br(2) 70.43(2) Br(4)-Cs(3)-Br(2) (2) Br(1)#5-Cs(3)-Br(2)# (2) Br(3)#4-Cs(3)-Br(2)# (3) Br(6)#6-Cs(3)-Br(2)# (2) Br(5)-Cs(3)-Br(2)# (2) Br(7)#7-Cs(3)-Br(2)# (3) Br(4)-Cs(3)-Br(2)# (3) Br(2)-Cs(3)-Br(2)# (16) 4
5 Br(1)#5-Cs(3)-Cs(2)# (2) Br(3)#4-Cs(3)-Cs(2)# (17) Br(6)#6-Cs(3)-Cs(2)# (17) Br(5)-Cs(3)-Cs(2)# (2) Br(7)#7-Cs(3)-Cs(2)# (2) Br(4)-Cs(3)-Cs(2)# (16) Br(2)-Cs(3)-Cs(2)# (2) Br(2)#6-Cs(3)-Cs(2)# (19) Br(1)#5-Cs(3)-Cs(2) 51.81(2) Br(3)#4-Cs(3)-Cs(2) (2) Br(6)#6-Cs(3)-Cs(2) (2) Br(5)-Cs(3)-Cs(2) (16) Br(7)#7-Cs(3)-Cs(2) (2) Br(4)-Cs(3)-Cs(2) (2) Br(2)-Cs(3)-Cs(2) (18) Br(2)#6-Cs(3)-Cs(2) (17) Cs(2)#4-Cs(3)-Cs(2) (18) Br(1)#5-Cs(3)-Cs(2)# (2) Br(3)#4-Cs(3)-Cs(2)# (17) Br(6)#6-Cs(3)-Cs(2)# (2) Br(5)-Cs(3)-Cs(2)# (2) Br(7)#7-Cs(3)-Cs(2)# (18) Br(4)-Cs(3)-Cs(2)# (2) Br(2)-Cs(3)-Cs(2)# (17) Br(2)#6-Cs(3)-Cs(2)# (2) Cs(2)#4-Cs(3)-Cs(2)# (12) Cs(2)-Cs(3)-Cs(2)# (15) Br(1)#5-Cs(3)-Cs(1)# (2) Br(3)#4-Cs(3)-Cs(1)# (2) Br(6)#6-Cs(3)-Cs(1)# (19) Br(5)-Cs(3)-Cs(1)# (2) Br(7)#7-Cs(3)-Cs(1)# (2) Br(4)-Cs(3)-Cs(1)# (19) Br(2)-Cs(3)-Cs(1)# (2) Br(2)#6-Cs(3)-Cs(1)# (19) Br(4)#10-Cs(2)-Br(2)# (3) Br(4)#10-Cs(2)-Br(6)# (2) Br(2)#6-Cs(2)-Br(6)# (3) Br(4)#10-Cs(2)-Br(5) (3) Br(2)#6-Cs(2)-Br(5) 72.94(2) Br(6)#11-Cs(2)-Br(5) 83.38(2) Br(4)#10-Cs(2)-Br(7)# (2) Br(2)#6-Cs(2)-Br(7)# (3) Br(6)#11-Cs(2)-Br(7)# (3) Br(5)-Cs(2)-Br(7)# (3) Br(4)#10-Cs(2)-Br(3)# (3) Br(2)#6-Cs(2)-Br(3)# (3) Br(6)#11-Cs(2)-Br(3)# (2) Br(5)-Cs(2)-Br(3)# (3) Br(7)#10-Cs(2)-Br(3)# (2) Br(4)#10-Cs(2)-Br(3) 69.92(2) Br(2)#6-Cs(2)-Br(3) (3) Br(6)#11-Cs(2)-Br(3) 69.66(3) Br(5)-Cs(2)-Br(3) 65.87(2) Br(7)#10-Cs(2)-Br(3) (3) Br(3)#11-Cs(2)-Br(3) (17) Br(4)#10-Cs(2)-Br(1)# (2) Br(2)#6-Cs(2)-Br(1)# (2) Br(6)#11-Cs(2)-Br(1)# (3) Br(5)-Cs(2)-Br(1)# (2) Br(7)#10-Cs(2)-Br(1)# (2) Br(3)#11-Cs(2)-Br(1)# (2) Br(3)-Cs(2)-Br(1)# (3) Br(4)#10-Cs(2)-Bi(2)# (15) Br(2)#6-Cs(2)-Bi(2)# (2) Br(6)#11-Cs(2)-Bi(2)# (2) Br(5)-Cs(2)-Bi(2)# (19) Br(7)#10-Cs(2)-Bi(2)# (14) Br(3)#11-Cs(2)-Bi(2)# (19) Br(3)-Cs(2)-Bi(2)# (2) Br(1)#5-Cs(2)-Bi(2)# (14) Br(4)#10-Cs(2)-Cs(3)# (16) Br(2)#6-Cs(2)-Cs(3)# (2) Br(6)#11-Cs(2)-Cs(3)# (16) Br(5)-Cs(2)-Cs(3)# (2) Br(7)#10-Cs(2)-Cs(3)# (2) Br(3)#11-Cs(2)-Cs(3)# (19) Br(3)-Cs(2)-Cs(3)# (17) Br(1)#5-Cs(2)-Cs(3)# (2) Bi(2)#10-Cs(2)-Cs(3)# (13) Br(4)#10-Cs(2)-Cs(3) (2) Br(2)#6-Cs(2)-Cs(3) (18) Br(6)#11-Cs(2)-Cs(3) (2) Br(5)-Cs(2)-Cs(3) (17) Br(7)#10-Cs(2)-Cs(3) 99.02(2) Br(3)#11-Cs(2)-Cs(3) (2) Br(3)-Cs(2)-Cs(3) 82.11(2) Br(1)#5-Cs(2)-Cs(3) (15) Br(4)#10-Cs(2)-Cs(3)# (2) Br(2)#6-Cs(2)-Cs(3)# (18) Br(6)#11-Cs(2)-Cs(3)# (2) Br(5)-Cs(2)-Cs(3)# (2) Br(7)#10-Cs(2)-Cs(3)# (16) Br(3)#11-Cs(2)-Cs(3)# (17) Br(3)-Cs(2)-Cs(3)# (2) Br(1)#5-Cs(2)-Cs(3)# (2) Br(1)-Cs(1)-Br(4)# (3) Br(1)-Cs(1)-Br(7) 63.09(2) Br(4)#15-Cs(1)-Br(7) 61.13(2) Br(1)-Cs(1)-Br(4)# (4) Br(4)#15-Cs(1)-Br(4)# (2) Br(7)-Cs(1)-Br(4)# (3) 5
6 Br(1)-Cs(1)-Br(2)# (2) Br(4)#15-Cs(1)-Br(2)# (3) Br(7)-Cs(1)-Br(2)# (3) Br(4)#9-Cs(1)-Br(2)# (2) Br(1)-Cs(1)-Br(3)# (3) Br(4)#15-Cs(1)-Br(3)# (3) Br(7)-Cs(1)-Br(3)# (3) Br(4)#9-Cs(1)-Br(3)# (2) Br(2)#3-Cs(1)-Br(3)# (2) Br(1)-Cs(1)-Br(1)# (3) Br(4)#15-Cs(1)-Br(1)# (2) Br(7)-Cs(1)-Br(1)# (3) Br(4)#9-Cs(1)-Br(1)# (3) Br(2)#3-Cs(1)-Br(1)# (3) Br(3)#3-Cs(1)-Br(1)# (3) Br(1)-Cs(1)-Br(7)# (3) Br(4)#15-Cs(1)-Br(7)# (2) Br(7)-Cs(1)-Br(7)# (3) Br(4)#9-Cs(1)-Br(7)# (2) Br(2)#3-Cs(1)-Br(7)# (3) Br(3)#3-Cs(1)-Br(7)# (2) Br(1)#16-Cs(1)-Br(7)# (3) Symmetry transformations used to generate equivalent atoms: #1 x,y,-z+1/2; #2 x,-y-1/2,-z; #3 x- 1,-y-1/2,-z ; #4 x-1,y,z; #5 x+1,-y-1/2,-z; #6 -x+1,y-1/2,z ; #7 -x,y+1/2,z; #8 -x+1,y+1/2,z; #9 -x,- y-1,-z; #10 x+1,y,z; #11 -x+2,y-1/2,z; #12 -x+2,y+1/2,-z+1/2 ; #13 -x+2,y+1/2,z ; #14 - x+1,y+1/2,-z+1/2; #15 -x,y-1/2,z; #16 -x-1,-y-1,-z; #17 x,-y-3/2,-z; #18 -x+1,-y-1,-z. Table S4. Anisotropic displacement parameters (Å ) for Cs 3 BiBr 6. The anisotropic displacement factor exponent takes the form: -2 π 2 [h 2 a* 2 U h k a*b*u12 ]. atom U11 U22 U33 U23 U13 U12 Bi(1) 19(1) 22(1) 25(1) 0 0 2(1) Bi(2) 25(1) 20(1) 19(1) 0(1) 0 0 Cs(3) 28(1) 46(1) 32(1) 6(1) 2(1) 2(1) Cs(2) 32(1) 47(1) 30(1) -3(1) 1(1) 0(1) Br(5) 33(1) 28(1) 33(1) 0 0-4(1) Br(6) 32(1) 26(1) 32(1) 0 0-2(1) Br(7) 114(1) 25(1) 32(1) 9(1) -6(1) -2(1) Br(4) 45(1) 65(1) 31(1) -9(1) -1(1) -27(1) Br(3) 50(1) 40(1) 55(1) -6(1) 29(1) 5(1) Br(2) 50(1) 41(1) 47(1) 4(1) -24(1) 8(1) Br(1) 48(1) 60(1) 46(1) -2(1) -21(1) -17(1) Cs(1) 103(1) 58(1) 47(1) -9(1) -19(1) 29(1) Table S5. Crystallographic and electronic parameters for the known perovskites. Space group a b c Cs 3 BiCl 6 C2/c Rb 3 BiBr 6 Pnma Cs 2 SnCl 6 Fm-3m Cs 2 SnBr 6 Fm-3m Cs 2 SnI 6 Fm-3m Cs 2 AgInCl 6 Fm-3m Cs 3 BiBr 6 Pbcm
7 Fig. S1 View of the structures constructed by (a) Bi1, Cs3; and (b) Bi1, Bi2, Cs3 on the mirror plane, respectively. (c) A basic unit constructed from the Bi1, Bi2, Cs3. Color code: Bi1, red; Bi2, purple; Cs1, green; Cs2, orange; Cs3, blue; Br, Brown. Fig. S2 Comparison of XRD pattern for Cs 3 BiBr 6,Rb 3 BiBr 6, Cs 3 BiCl 6. 7
8 Fig. S3 The bandgap calculated from the DFT. Fig. S4 The PL spectra for the Cs 3 BiBr 6. Fig. S5 TGA curves of Cs 3 BiBr 6 and CH 3 NH 3 PbBr 3. 8
9 Fig. S6 (a) Electron micrograph of the microstructure for the photodetector. (b)-(d) Energy dispersive X-ray (EDX) mapping of the element distribution: (b) Br, (c) Cs, (d) Bi. 9
10 Fig. S7 (a) I-V characteristics under different power density. (b) Photocurrent responses under various light densities at bias voltage of 0-6 V. (c) Comparison of the detectivity at two different light densities. Fig. S8 EQE versus voltage under light illumiantion of 4 mw/cm 2 and 25 mw/cm 2. 10
11 Fig. S9 The high-resolution I-t curve of Cs3BiBr 6 devices towards 400 nm illumination with a powder intensity of 25 mw/cm 2. Fig. S10 Photoresponse of Cs 3 BiBr 6 under white light illumination with power density of 350 mw/cm 2. 11
12 Fig. S11 The stability for the photodetector under light illumination. 12
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