Ruddlesden–Popper 2D perovskites of type (C(6)H(9)C(2)H(4)NH(3))(2)(CH(3)NH(3))(n−1)Pb(n)I(3n+1) (n = 1–4) for optoelectronic applications

Ruddlesden–Popper (RP) phase metal halide organo perovskites are being extensively studied due to their quasi-two dimensional (2D) nature which makes them an excellent material for several optoelectronic device applications such as solar cells, photo-detectors, light emitting diodes (LEDs), lasers etc. While most of reports show use of linear carbon chain based organic moiety, such as n-Butylamine, as organic spacer in RP perovskite crystal structure, here we report a new series of quasi 2D perovskites with a ring type cyclic carbon group as organic spacer forming RP perovskite of type (CH)(2)(MA)(n−1)Pb(n)I(3n+1); CH = 2-(1-Cyclohexenyl)ethylamine; MA = Methylamine). This work highlights the synthesis, structural, thermal, optical and optoelectronic characterizations for the new RP perovskite series n = 1–4. The demonstrated RP perovskite of type for n = 1–4 have shown formation of highly crystalline thin films with alternate stacking of organic and inorganic layers, where the order of PbI(6) octahedron layering are controlled by n-value, and shown uniform direct bandgap tunable from 2.51 eV (n = 1) to 1.92 eV (n = 4). The PL lifetime measurements supported the fact that lifetime of charge carriers increase with n-value of RP perovskites [154 ps (n = 1) to 336 ps (n = 4)]. Thermogravimetric analysis (TGA) showed highly stable nature of reported RP perovskites with linear increase in phase transition temperatures from 257 °C (n = 1) to 270 °C (n = 4). Scanning electron microscopy (SEM) and energy dispersive X-ray analysis (EDAX) are used to investigate the surface morphology and elemental compositions of thin films. In addition, the photodetectors fabricated for the series using (CH)(2)(MA)(n−1)Pb(n)I(3n+1) RP perovskite as active absorbing layer and without any charge transport layers, shown sharp photocurrent response from 17 nA/cm(2) for n = 1 to 70 nA/cm(2) for n = 4, under zero bias and low power illumination conditions (470 nm LED, 1.5 mW/cm(2)). Furthermore, for lowest bandgap RP perovskite n = 4, (CH)(2)MA(3)Pb(4)I(13) the photodetector showed maximum photocurrent density of ~ 508 nA/cm(2) at 3 V under similar illumination condition, thus giving fairly large responsivity (46.65 mA/W). Our investigations show that 2-(1-Cyclohexenyl)ethylamine based RP perovskites can be potential solution processed semiconducting materials for optoelectronic applications such as photo-detectors, solar cells, LEDs, photobatteries etc.