Metal–organic frameworks (MOFs) are emerging as an appealing class of highly tailorable electrically conducting materials with potential applications in optoelectronics. Yet, the realization of their proof‐of‐concept devices remains a daunting challenge, attributed to their poor electrical properties. Following recent work on a semiconducting Fe3(THT)2(NH4)3 (THT: 2,3,6,7,10,11‐triphenylenehexathiol) 2D MOF with record‐high mobility and band‐like charge transport, here, an Fe3(THT)2(NH4)3 MOF‐based photodetector operating in photoconductive mode capable of detecting a broad wavelength range from UV to NIR (400–1575 nm) is demonstrated. The narrow IR bandgap of the active layer (≈0.45 eV) constrains the performance of the photodetector at room temperature by band‐to‐band thermal excitation of charge carriers. At 77 K, the device performance is significantly improved; two orders of magnitude higher voltage responsivity, lower noise equivalent power, and higher specific detectivity of 7 × 108 cm Hz1/2 W−1 are achieved under 785 nm excitation. These figures of merit are retained over the analyzed spectral region (400–1575 nm) and are commensurate to those obtained with the first demonstrations of graphene‐ and black‐phosphorus‐based photodetectors. This work demonstrates the feasibility of integrating conjugated MOFs as an active element into broadband photodetectors, thus bridging the gap between materials' synthesis and technological applications.

Indium selenide (InSe) and gallium selenide (GaSe), members of the III−VI chalcogenide family, are emerging two-dimensional (2D) semiconductors with appealing electronic properties. However, their devices are still lagging behind because of their sensitivity to air and device fabrication processes which induce structural damage and hamper their intrinsic properties. Thus, in order to obtain high-performance and stable devices, effective passivation of these air-sensitive materials is strongly required. Here, we demonstrate a hexagonal boron nitride (hBN)-based encapsulation technique, where 2D layers of InSe and GaSe are covered entirely between two layers of hBN. To fabricate devices out of fully encapsulated 2D layers, we employ the lithography-free via-contacting scheme. We find that hBN acts as an excellent encapsulant and a near-ideal substrate for InSe and GaSe by passivating them from the environment and isolating them from the charge disorder at the SiO 2 surface. As a result, the encapsulated InSe devices are of high quality and ambient-stable for a long time and show an improved two-terminal mobility of 30−120 cm 2 V −1 s −1 as compared to mere ∼1 cm 2 V −1 s −1 for unencapsulated devices. On employing this technique to GaSe, we obtain a strong and reproducible photoresponse. In contrast to previous studies, where either good performance or long-term stability was achieved, we demonstrate a combination of both in our devices. This work thus provides a systematic study of fully encapsulated devices based on InSe and GaSe, which has not been reported until now. We believe that this technique can open ways for fundamental studies as well as toward the integration of these materials in technological applications.

Lattice defects and dielectric environment play a crucial role for 2D materials. Gas molecules can get physisorbed easily on the surface through van der Waals forces and can modify dramatically their electronic and optical properties. In this work, we investigate the impact of the physisorbed gas molecules on the optical properties of MoSe2 monolayers by means of low-temperature photoluminescence (PL). More specifically, we focus on the physics of excitons localized by gas molecules. The associated PL peak is observed to show a systematic and large red-shift with temperature and a blue-shift with laser irradiation. Both energy shifts are explained in terms of thermal instability of the localization in combination with hopping effects. Finally, a model is presented, which can reproduce the experimental data with excellent agreement.