We demonstrate a new 3D fabrication method to achieve the same results as those obtained by the two-photon excitation technique, by using a simple one-photon elaboration method in a very low absorption regime. Desirable 2D and 3D submicrometric structures, such as spiral, chiral, and woodpile architectures, with feature size as small as 190 nm have been fabricated, by using just a few milliwatts of a continuous-wave laser at 532 nm and a commercial SU8 photoresist. Different aspects of the direct laser writing based on ultralow one-photon absorption (LOPA) technique are investigated and compared with the TPA technique, showing several advantages, such as simplicity and low cost.

Improving the performances of photovoltaic (PV) devices by suppressing nonradiative energy losses through surface defect passivation and enhancing the stability to the level of standard PV represents one critical challenge for perovskite solar cells. Here, reported are the advantages of introducing a tetrapropylammonium (TPA + ) cation that combines two key functionalities, namely surface passivation of CH 3 NH 3 PbI 3 nanocrystals through strong ionic interaction with the surface and bulk passivation via formation of a type I heterostructure that acts as a recombination barrier. As a result, nonencapsulated perovskite devices with only 2 mol% of TPA + achieve power conversion efficiencies over 18.5% with higher V OC under air mass 1.5G conditions. The devices fabricated retain more than 85% of their initial performances for over 1500 h under ambient conditions (55% RH ± 5%). Furthermore, devices with TPA + also exhibit excellent operational stability by retaining over 85% of the initial performance after 250 h at maximum power point under 1 sun illumination. The effect of incorporation of TPA + on the structural and optoelectronic properties is studied by X-ray diffraction, ultraviolet-visible absorption spectroscopy, ultraviolet photon-electron spectroscopy, time-resolved photoluminescence, and scanning electron microscopy imaging. Atomic-level passivation upon addition of TPA + is elucidated employing 2D solid-state NMR spectroscopy.

With respect to experimental condition, we have investigated the point spread function of a high numerical aperture objective lens, taking into account the absorption effect of the studied material. By using a material possessing an ultralow one-photon absorption (LOPA) coefficient at the excitation wavelength, the light beam can penetrate deeply inside the material and be tightly focused into a subwavelength spot, almost the same as in the absence of material. Combining tight focusing and ultralow absorption conditions, we show that LOPA-based microscopy is thus capable of three-dimensional imaging and fabrication with long penetration depth up to 300 μm. As compared to the commonly used two-photon absorption microscope, the LOPA method allows simplification of the experimental setup and also minimization of the photodamaging or bleaching effect of materials.