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Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Synthesis and Optical Properties of One Year Air-Stable Chiral Sb(III) Halide Semiconductors
AU - Azmy, Ali
AU - Konovalova, Daria M
AU - Lepore, Leah
AU - Fyffe, Alexander
AU - Kim, Doyun
AU - Wojtas, Lukasz
AU - Tu, Qing
AU - Trinh, Minh Tuan
AU - Zibouche, Nourdine
AU - Spanopoulos, Ioannis
PY - 2023/12/11
Y1 - 2023/12/11
N2 - Chiral hybrid metal-halide semiconductors (MHS) pose as ideal candidates for spintronic applications owing to their strong spin-orbit coupling (SOC), and long spin relaxation times. Shedding light on the underlying structure-property relationships is of paramount importance for the targeted synthesis of materials with an optimum performance. Herein, we report the synthesis and optical properties of 1D chiral ( -/ -THBTD)SbBr (THBTD = 4,5,6,7-tetrahydro-benzothiazole-2,6-diamine) semiconductors using a multifunctional ligand as a countercation and a structure directing agent. ( -/ -THBTD)SbBr feature direct and indirect band gap characteristics, exhibiting photoluminescence (PL) light emission at RT that is accompanied by a lifetime of a few ns. Circular dichroism (CD), second harmonic generation (SHG), and piezoresponse force microscopy (PFM) studies validate the chiral nature of the synthesized materials. Density functional theory (DFT) calculations revealed a Rashba/Dresselhaus (R/D) spin splitting, supported by an energy splitting ( ) of 23 and 25 meV, and a Rashba parameter (α ) of 0.23 and 0.32 eV·Å for the and analogs, respectively. These values are comparable to those of the 3D and 2D perovskite materials. Notably, ( -THBTD)SbBr has been air-stable for a year, a record performance among chiral lead-free MHS. This work demonstrates that low-dimensional, lead-free, chiral semiconductors with exceptional air stability can be acquired, without compromising spin splitting and manipulation performance.
AB - Chiral hybrid metal-halide semiconductors (MHS) pose as ideal candidates for spintronic applications owing to their strong spin-orbit coupling (SOC), and long spin relaxation times. Shedding light on the underlying structure-property relationships is of paramount importance for the targeted synthesis of materials with an optimum performance. Herein, we report the synthesis and optical properties of 1D chiral ( -/ -THBTD)SbBr (THBTD = 4,5,6,7-tetrahydro-benzothiazole-2,6-diamine) semiconductors using a multifunctional ligand as a countercation and a structure directing agent. ( -/ -THBTD)SbBr feature direct and indirect band gap characteristics, exhibiting photoluminescence (PL) light emission at RT that is accompanied by a lifetime of a few ns. Circular dichroism (CD), second harmonic generation (SHG), and piezoresponse force microscopy (PFM) studies validate the chiral nature of the synthesized materials. Density functional theory (DFT) calculations revealed a Rashba/Dresselhaus (R/D) spin splitting, supported by an energy splitting ( ) of 23 and 25 meV, and a Rashba parameter (α ) of 0.23 and 0.32 eV·Å for the and analogs, respectively. These values are comparable to those of the 3D and 2D perovskite materials. Notably, ( -THBTD)SbBr has been air-stable for a year, a record performance among chiral lead-free MHS. This work demonstrates that low-dimensional, lead-free, chiral semiconductors with exceptional air stability can be acquired, without compromising spin splitting and manipulation performance.
U2 - 10.1021/acs.inorgchem.3c03098
DO - 10.1021/acs.inorgchem.3c03098
M3 - Journal article
C2 - 38009949
VL - 62
SP - 20142
EP - 20152
JO - Inorganic Chemistry
JF - Inorganic Chemistry
SN - 0020-1669
IS - 49
ER -