Journal
ADVANCED MATERIALS
Volume 34, Issue 7, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202104782
Keywords
inorganic 2D perovskites; low exciton binding energy; photodetectors; photoresponse; pseudohalide; reversible phase transformation; single crystals
Categories
Funding
- John Hooke Chair of Nanoscience Postgraduate Research Scholarships
- Ministry of Education [110L9006]
- Ministry of Science and Technology in Taiwan [MOST 110-2634-F-002-043, 108-2638-E-002-003-MY2, 109-2628-E-002-008-MY3, 110-2923-E-002-007-MY3]
- Top University Project from the National Taiwan University [110L7836, 110L7726]
- MOST [110-2731-M-002-001, XRD000200]
- Australian Government through an Australian Research Council (ARC) Future Fellowship [FT210100210]
- ARC Centre of Excellence in Exciton Science [CE 170100026]
- Australian Renewable Energy Agency (ARENA) [2020/RND001, 2020/RND003]
- Australian Research Council [FT210100210] Funding Source: Australian Research Council
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The first inorganic-cation pseudohalide 2D phase perovskite single crystal Cs2Pb(SCN)(2)Br-2 is reported in this study, synthesized by the antisolvent vapor-assisted crystallization method at room temperature. This 2D single crystal exhibits a low exciton binding energy and demonstrates respectable responsivity and detectivity at low bias voltage.
Most of the reported 2D Ruddlesden-Popper (RP) lead halide perovskites with the general formula of A(n)(+1)B(n)X(3)(n)(+1) (n = 1, 2, horizontal ellipsis ) comprise layered perovskites separated by A-site-substituted organic spacers. To date, only a small number of X-site-substituted RP perovskites have been reported. Herein, the first inorganic-cation pseudohalide 2D phase perovskite single crystal, Cs2Pb(SCN)(2)Br-2, is reported. It is synthesized by the antisolvent vapor-assisted crystallization (AVC) method at room temperature. It exhibits a standard single-layer (n = 1) Ruddlesden-Popper structure described in space group of Pmmn (#59) and has a small separation (d = 1.69 angstrom) between the perovskite layers. The SCN- anions are found to bend the 2D Pb(SCN)(2)Br-2 framework slightly into a kite-shaped octahedron, limiting the formation of a quasi-2D perovskite structure (n > 1). This 2D single crystal exhibits a reversible first-order phase transformation to 3D CsPbBr3 (Pm3m #221) at 450 K. It has a low exciton binding energy of 160 meV-one of the lowest for 2D perovskites (n = 1). A Cs2Pb(SCN)(2)Br-2-single-crystal photodetector is demonstrated with respectable responsivity of 8.46 mA W-1 and detectivity of approximate to 1.2 x 10(10) Jones at a low bias voltage of 0.5 V.
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