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By comparing optical spectral results of both Sn-rich and Sn-poor Cu2ZnSnS4 (CZTS) with the previously calculated defect levels, we confirm that the band-tail states in CZTS originate from the high concentration of 2CuZn + SnZn defect clusters, whereas the deep-donor states originate from the high concentration of SnZn. In Sn-rich CZTS, the absorption, reflectance, and photocurrent (PC) spectra show band-tail states that shrink the bandgap to only ∼1.34 eV, while photoluminescence (PL) and PC spectra consistently show that abundant CuZn + SnZn donor states produce a PL peak at ∼1.17 eV and abundant SnZn deep-donor states produce a PL peak near 0.85 eV. In contrast, Sn-poor CZTS shows neither bandgap shrinking nor any deep-donor-defect induced PL and PC signals. These results highlight that a Sn-poor composition is critical for the reduction of band-tailing effects and deep-donor defects and thus the overcoming of the severe open-circuit voltage (V oc) deficiency problem in CZTS solar cells.

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2D Bi 2 O 2 Se has shown great potential in photodetector from visible to infrared (IR) owing to its high mobility, ambient stability, and layer-tunable bandgaps. However, for the terahertz (THz) band with longer wavelength and richer spectral information, there are few reports on the research of THz detection based on 2D materials. Herein, an antenna-assisted Bi 2 O 2 Se photodetector is constructed to achieve broadband photodetection from IR to THz ranges driven by multi-mechanism of electromagnetic waves to electrical conversion. The good tradeoff between the bandgap and high mobility results in a broad spectral detection. In the IR region, the nonequilibrium carriers result from photo-induced electron-hole pairs in the Bi 2 O 2 Se body. While in the THz region, the carriers are caused by the injected electrons from the metal electrodes by the electromagnetic-induced well. The Bi 2 O 2 Se photodetector achieves a broadband responsivity of 58 A W-1 at 1550 nm, 2.7 × 10 4 V W-1 at 0.17 THz, and 1.9 × 10 8 V W-1 at 0.029 THz, respectively. Surprisingly, an ultrafast response time of 476 ns and a quite low noise equivalent power of 0.2 pW Hz-1/2 are acquired at room temperature. Our researches exhibit promising prospects of Bi 2 O 2 Se in broadband detection, THz imaging, and ultrafast sensing.

Two-dimensional (2D) van-der-Waals (vdW) layered ferroelectric semiconductors are highly desired for in-memory computing and ferroelectric photovoltaics or detectors. Beneficial from the weak interlayer vdW-force, controlling the structure by interlayer twist/translation or doping is an effective strategy to manipulate the fundamental properties of 2D-vdW semiconductors, which has contributed to the newly-emerging sliding ferroelectricity. Here, we report unconventional room-temperature ferroelectricity, both out-of-plane and in-plane, in vdW-layered γ-InSe semiconductor triggered by yttrium-doping (InSe:Y). We determine an effective piezoelectric constant of ∼7.5 pm/V for InSe:Y flakes with thickness of ∼50 nm, about one order of magnitude larger than earlier reports. We directly visualize the enhanced sliding switchable polarization originating from the fantastic microstructure modifications including the stacking-faults elimination and a subtle rhombohedral distortion due to the intralayer compression and continuous interlayer pre-sliding. Our investigations provide new freedom degrees of structure manipulation for intrinsic properties in 2D-vdW-layered semiconductors to expand ferroelectric candidates for next-generation nanoelectronics.