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Molecular constructs define the elementary units in porous materials for efficient CO2 capture. The design of appropriate interpore and intermolecular space is crucial to stabilize CO2 molecules and maximize the capacity. While the molecular construct usually has a fixed dimension, whether its intermolecular space could be self-adjustable during CO2 capture and release, behaving as a balloon, has captured imagination. Here we report a flexible intermolecular space of the double chain structure of self-assembled 1,4-phenylene diisocyanide (PDI) molecules on Ag(110) surface, which dynamically broadens and recovers during the CO2 capture and release. The incipient PDI double chains organize along the [001] direction of Ag(110), in which individual PDI molecules stand up in a zigzag order with the interchain width defined by twice the Ag lattice distance along [11¯0] direction (2α[11¯0]). When CO2 molecules are introduced, they assemble to occupy the interchain spaces, expanding the interchain width to 3α[11¯0], 4α[11¯0] and 5α[11¯0]. Warming up the sample leads to the thermally-driven CO2 desorption that recovers the original interchain space. High-resolution scanning tunneling microscopy (STM) jointly with density functional theory (DFT) calculations determine the structural and electronic interactions of CO2 molecules with the dynamical PDI structures, providing a molecular-level perspective for the design of a self-adjustable metal-organic construct for reversible gas capture and release. 

Abstract It is well-documented that type-III effectors are required by Gram-negative pathogens to directly target different host cellular pathways to promote bacterial infection. However, in the context of legume-rhizobium symbiosis, the role of rhizobial effectors in regulating plant symbiotic pathways remains largely unexplored. Here, we show that NopT, a YopT-type cysteine protease of Sinorhizobium fredii NGR234 directly targets the plant’s symbiotic signaling pathway by associating with two Nod factor receptors (NFR1 and NFR5 of Lotus japonicus). NopT inhibits cell death triggered by co-expression of NFR1/NFR5 in Nicotiana benthamiana. Full-length NopT physically interacts with NFR1 and NFR5. NopT proteolytically cleaves NFR5 both in vitro and in vivo, but can be inactivated by NFR1 as a result of phosphorylation. NopT plays an essential role in mediating rhizobial infection in L. japonicus. Autocleaved NopT retains the ability to cleave NFR5 but no longer interacts with NFR1. Interestingly, genomes of certain Sinorhizobium species only harbor nopT genes encoding truncated proteins without the autocleavage site. These results reveal an intricate interplay between rhizobia and legumes, in which a rhizobial effector protease targets NFR5 to suppress symbiotic signaling. NFR1 appears to counteract this process by phosphorylating the effector. This discovery highlights the role of a bacterial effector in regulating a signaling pathway in plants and opens up the perspective of developing kinase-interacting proteases to fine-tune cellular signaling processes in general. 

By frequency-time spectroscopy, microscopy, and electronic structure theory, we investigate the low coverage adsorption and electronic structure of Ca on an Ag(111) surface. The chemisorption of alkaline-earth Ca atoms starting from their closed 4s2 shell electronic configuration differs from that of the open ns1 shell alkali-metal atoms because they retain some 4s electron charge and can involve hybridization with low-lying unoccupied 3d orbitals. Spectroscopic investigation of the unoccupied electronic structure of Ca on Ag(111) by three-photon photoemission (3PP) reveals the electronic states with dominant 3d-orbital character, as confirmed by electronic structure theory. Coverage-specific spectral features enable attribution to two distinct chemisorption phases at submonolayer coverages, which are confirmed at the atomic scale by scanning tunneling microscopy and spectroscopy measurements. Furthermore, time-resolved 3PP spectroscopy reveals a resonant two-photon transition between occupied (∼−0.3 eV) and unoccupied (∼2.7 eV) states with dominant s- and d-orbital character. Interferometric time-resolved measurements probing this resonance reveal a dephasing time of ∼21 fs and population lifetime of ∼52 fs for the transiently populated d-like state at ∼2.7 eV above EF . Contrary to alkali-metal atom chemisorption, the characteristic development of the chemisorption and electronic structure of Ca reveals the importance of Ca adsorbate and Ag substrate interactions that cause a low-coverage atomic condensation into compact islands. Discovery of the long-lived d-character state informs on the catalytic and optoelectronic applications of the alkaline-earth element Ca. 

Phononic waveguides (PnWGs) are devices with rationally designed periodic structures to manipulate mechanical oscillations and to engineer and control the propagation of acoustic waves, thus allowing for frequency and band selection of wave transmission and routing, promising for both classical and quantum transduction on chip-scale platforms with various constituent materials of interest. They can be incorporated into both electromechanical and optomechanical signal transduction schemes. Here, we present an overview of emerging micro/nanoscale PnWGs and offer perspectives for future. We evaluate the typical structural designs, frequency scaling, and phononic band structures of the PnWGs. Material choices, fabrication techniques, and characterization schemes are discussed based on different PnWG designs. For classical transduction schemes, an all-phononic integrated circuit perspective is proposed. Toward emerging quantum applications, the potential of utilizing PnWGs as universal interfaces and transduction channels has been examined. We envision PnWGs with extraordinary propagation properties, such as nonreciprocity and active tunability, can be realized with unconventional design strategies (e.g., inverse design) and advanced materials (e.g., van der Waals layered crystals), opening opportunities in both classical and quantum signal transduction schemes. 

Visual question answering (VQA) requires systems to perform concept-level reasoning by unifying unstructured (e.g., the context in question and answer; “QA context”) and structured (e.g., knowledge graph for the QA context and scene; “concept graph”) multimodal knowledge. Existing works typically combine a scene graph and a concept graph of the scene by connecting corresponding visual nodes and concept nodes, then incorporate the QA context representation to perform question answering. However, these methods only perform a unidirectional fusion from unstructured knowledge to structured knowledge, limiting their potential to capture joint reasoning over the heterogeneous modalities of knowledge. To perform more expressive reasoning, we propose VQA-GNN, a new VQA model that performs bidirectional fusion between unstructured and structured multimodal knowledge to obtain unified knowledge representations. Specifically, we inter-connect the scene graph and the concept graph through a super node that represents the QA context, and introduce a new multimodal GNN technique to perform inter-modal message passing for reasoning that mitigates representational gaps between modalities. On two challenging VQA tasks (VCR and GQA), our method outperforms strong baseline VQA methods by 3.2% on VCR (Q-AR) and 4.6% on GQA, suggesting its strength in performing concept-level reasoning. Ablation studies further demonstrate the efficacy of the bidirectional fusion and multimodal GNN method in unifying unstructured and structured multimodal knowledge. 

Abstract Natural polymers, particularly plant‐derived nanocelluloses, self‐organize into hierarchical structures, enabling mechanical robustness, bright iridescence, emission, and polarized light reflection. These biophotonic properties are facilitated by the assembly of individual components during evaporation, such as cellulose nanocrystals (CNCs), which exhibit a left‐handed helical pitch in a chiral nematic state. This work demonstrates how optically active films with pre‐programmed opposite handedness (left or right) can be constructed via shear‐induced twisted printing with clockwise and counter‐clockwise shearing vectors. The resulting large‐area thin films are transparent yet exhibit pre‐determined mirror‐symmetrical optical activity, enabling the distinction of absorbed and emitted circularly polarized light. This processing method allows for sequential printing of thin and ultrathin films with twisted layered organization and on‐demand helicity. The complex light polarization behavior is due to step‐like changes in linear birefringence within each deposited layer and circular birefringence, different from that of conventional CNC films as revealed with Muller matrix analysis. Furthermore, intercalating an achiral organic dye into printed structures induces circularly polarized luminescence while preserving high transmittance and controlled handedness. These results suggest that twisted sequential printing can facilitate the construction of chiroptical metamaterials with tunable circular polarization, absorption, and emission for optical filters, encryption, photonic coatings, and chiral sensors.