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Creation, stabilization, characterization, and control of single transition metal (TM) atoms may lead to significant advancement of the next-generation catalyst. Metal organic network (MON) in which single TM atoms are coordinated and separated by organic ligands is a promising class of material that may serve as a single atom catalyst. Our density functional theory-based calculations of MONs in which dipyridyl tetrazine (DPTZ) ligands coordinate with a TM atom to form linear chains leads to two types of geometries of the chains. Those with V, Cr, Mo, Fe, Co, Pt, or Pd atoms at the coordination center are planar while those with Au, Ag, Cu, or Ni are non-planar. The formation energies of the chains are high (∼2.0–7.9 eV), suggesting that these MON can be stabilized. Moreover, the calculated adsorption energies of CO and O₂on the metal atom at center of the chains with the planar configuration lie in the range 1.0–3.0 eV for V, Cr, Mo, Fe, and Co at the coordination center, paving the way for future studies of CO oxidation on TM-DPTZ chains with the above five atoms at the coordination center.

 

A chiral 3D coordination compound, [Gd 2 (L) 2 (ox) 2 (H 2 O) 2 ], arranged around a dinuclear Gd unit has been characterized by X-ray photoemission and X-ray absorption measurements in the context of density functional theory studies. Core level photoemission of the Gd 5p multiplet splittings indicates that spin orbit coupling dominates over j–J coupling evident in the 5p core level spectra of Gd metal. Indications of spin–orbit coupling are consistent with the absence of inversion symmetry due to the ligand field. Density functional theory predicts antiferromagnet alignment of the Gd 2 dimers and a band gap of the compound consistent with optical absorption. 

Abstract In this brief perspective we analyze the present status of the field of defect engineering of oxide surfaces. In particular we discuss the tools and techniques available to generate, identify, quantify, and characterize point defects at oxide surfaces and the main areas where these centers play a role in practical applications. 

Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO₂supported Pt single atom catalysts with precisely controlled coordination environments are successfully fabricated. The joint experimental and theoretical analysis reveals that the Pt single atoms on Pt₁/CeO₂prepared at 550 °C (Pt/CeO₂-550) are mainly located at the edge sites of CeO₂with a Pt–O coordination number ofca. 5, while those prepared at 800 °C (Pt/CeO₂-800) are predominantly located at distorted Ce substitution sites on CeO₂terrace with a Pt–O coordination number ofca. 4. Pt/CeO₂-550 and Pt/CeO₂-800 with different Pt₁-CeO₂coordination environments exhibit a reversal of activity trend in CO oxidation and NH₃oxidation due to their different privileges in reactants activation and H₂O desorption, suggesting that the catalytic performance of Pt single atom catalysts in different target reactions can be maximized by optimizing their local coordination structures.

 

Abstract Applications of quantum information science (QIS) generally rely on the generation and manipulation of qubits. Still, there are ways to envision a device with a continuous readout, but without the entangled states. This concise perspective includes a discussion on an alternative to the qubit, namely the solid-state version of the Mach–Zehnder interferometer, in which the local moments and spin polarization replace light polarization. In this context, we provide some insights into the mathematics that dictates the fundamental working principles of quantum information processes that involve molecular systems with large magnetic anisotropy. Transistors based on such systems lead to the possibility of fabricating logic gates that do not require entangled states. Furthermore, some novel approaches, worthy of some consideration, exist to address the issues pertaining to the scalability of quantum devices, but face the challenge of finding the suitable materials for desired functionality that resemble what is sought from QIS devices. 

Future molecular microelectronics require the electronic conductivity of the device to be tunable without impairing the voltage control of the molecular electronic properties. This work reports the influence of an interface between a semiconducting polyaniline polymer or a polar poly-D-lysine molecular film and one of two valence tautomeric complexes, i.e. , [Co III (SQ)(Cat)(4-CN-py) 2 ] ↔ [Co II (SQ) 2 (4-CN-py) 2 ] and [Co III (SQ)(Cat)(3-tpp) 2 ] ↔ [Co II (SQ) 2 (3-tpp) 2 ]. The electronic transitions and orbitals are identified using X-ray photoemission, X-ray absorption, inverse photoemission, and optical absorption spectroscopy measurements that are guided by density functional theory. Except for slightly modified binding energies and shifted orbital levels, the choice of the underlying substrate layer has little effect on the electronic structure. A prominent unoccupied ligand-to-metal charge transfer state exists in [Co III (SQ)(Cat)(3-tpp) 2 ] ↔ [Co II (SQ) 2 (3-tpp) 2 ] that is virtually insensitive to the interface between the polymer and tautomeric complexes in the Co II high-spin state.