arXiv subjects

Shangpu Liu

Publications and source records attributed to Shangpu Liu.

3 recordsLinked to original sources

arXiv2026

Composition Anisotropy Drives Large Bulk Photovoltaic Fields Along the Non-polar Vertical Direction in 2D Hybrid Perovskite Ferroelectrics

The photovoltaic electric field of the bulk photovoltaic effect (BPE) reflects the intrinsic ability of ferroelectrics to separate photoexcited excitons into electrons and holes, and are essential parameters for applications such as voltage-readout photodetectors. Because polarization defines the cation-anion displacement and noncentrosymmetric axis, the polar direction is generally one of the orientations exhibiting strong bulk photovoltaic field (EBPE). Here, we report emergent BPE behavior in 2D hybrid perovskite ferroelectrics (HPFs), where EBPE can be two orders of magnitude higher along the vertical nonpolar direction than along the polar in-plane direction. Its magnitude is up to orders of magnitude higher than that of benchmark photoferroelectrics across different material systems and is the highest among 2D HPFs reported so far. This strong BPE response with emergent directional anisotropy originates from the unique coupling among the shift-current BPE mechanism, an efficient photocarrier-generating inorganic part, and an insulator-like organic part, a combination that is conflicting or inaccessible in traditional photoferroelectrics. This composition and anisotropy also produce basic BPE behavior distinct from that of typical photoferroelectrics, including a laser intensity dependent photovoltage and a nonlinear scaling of photovoltage with material dimension. We analyze and develop a series of formulas to describe the emergent photovoltage phenomena, which should be applicable to this novel 2D ferroelectrics family and to polar systems with similar anisotropy and robust photoelectric response.

cond-mat.mtrl-sci↗

arXiv2024

Light-induced optical orientation of magnetic moments in transition-metal doped hybrid metal halide perovskites

Using optical orientation to manipulate magnetic moments in matter with light is a key objective in opto-spintronics, however, realizations of such control on ultrafast timescales are limited. Here, we report ultrafast optical control of magnetic moment orientation in magnetically doped metal halide perovskites. Employing intense pulses of circularly polarized light, we inject populations of spin-polarized charge carriers in pristine and manganese-doped MAPbBr3 thin films. Using transient Faraday rotation spectroscopy, we probe the ultrafast magnetic moment dynamics following photoexcitation and find that light-induced magnetization in doped samples is increased by a factor of 10. We attribute this to photoexcited carriers acting on the magnetic moments of manganese dopant-ions via the sp-d exchange interaction, which forces them to align on picosecond timescales. Our findings open new avenues for device structures that use hybrid metal halide perovskites for ultrafast optical manipulation and read-out of magnetic order with the potential for high switching rates.

physics.app-ph↗

arXiv2023

Solution-processed NiPS3 thin films from Liquid Exfoliated Inks with Long-Lived Spin-Entangled Excitons

Antiferromagnets are promising materials for future opto-spintronic applications since they show spin dynamics in the THz range and no net magnetization. Recently, layered van der Waals (vdW) antiferromagnets have been reported, which combine low-dimensional excitonic properties with complex spin-structure. While various methods for the fabrication of vdW 2D crystals exist, formation of large area and continuous thin films is challenging because of either limited scalability, synthetic complexity, or low opto-spintronic quality of the final material. Here, we fabricate centimeter-scale thin films of the van der Waals 2D antiferromagnetic material NiPS3, which we prepare using a crystal ink made from liquid phase exfoliation (LPE). We perform statistical atomic force microscopy (AFM) and scanning electron microscopy (SEM) to characterize and control the lateral size and number of layers through this ink-based fabrication. Using ultrafast optical spectroscopy at cryogenic temperatures, we resolve the dynamics of photoexcited excitons. We find antiferromagnetic spin arrangement and spin-entangled Zhang-Rice multiplet excitons with lifetimes in the nanosecond range, as well as ultranarrow emission linewidths, despite the disordered nature of our films. Thus, our findings demonstrate scalable thin-film fabrication of high-quality NiPS3, which is crucial for translating this 2D antiferromagnetic material into spintronic and nanoscale memory devices and further exploring its complex spin-light coupled states.

physics.chem-ph↗