Identifying atomically thin isolated-band channels for intrinsic steep-slope transistors by high-throughput study.

Developing low-power FETs holds significant importance in advancing logic circuits, especially as the feature size of MOSFETs approaches sub-10 nanometers. However, this has been restricted by the thermionic limitation of SS, which is limited to 60 mV per decade at room temperature. Herein, we proposed a strategy that utilizes 2D semiconductors with an isolated-band feature as channels to realize sub-thermionic SS in MOSFETs. Through high-throughput calculations, we established a guiding principle that combines the atomic structure and orbital interaction to identify their sub-thermionic transport potential. This guides us to screen 192 candidates from the 2D material database comprising 1608 systems. Additionally, the physical relationship between the sub-thermionic transport performances and electronic structures is further revealed, which enables us to predict 15 systems with promising device performances for low-power applications with supply voltage below 0.5 V. This work opens a new way for the low-power electronics based on 2D materials and would inspire extensive interests in the experimental exploration of intrinsic steep-slope MOSFETs.

Probing Electronic Band Structures of Dielectric Polymers via Pre-Breakdown Conduction.

The electronic band structure, especially the defect states at the conduction band tail, dominates electron transport and electrical degradation of a dielectric material under an extremely high electric field. However, the electronic band structure in a dielectric is barely well studied due to experimental challenges in detecting the electrical conduction to an extremely high electric field, i.e., prebreakdown. In this work, the electronic band structure of polymer dielectric films is probed through an in situ prebreakdown conduction measurement method in conjunction with a space-charge-limited-current spectroscopic analysis. An exponential distribution of defect states at the conduction band tail with varying trap levels is observed in accordance with the specific morphological disorder in the polymer dielectric, and the experimental defect states show also a favorable agreement with the calculated density of states from the density functional theory. The methodology demonstrated in this work bridges the molecule-structure-determined electronic band structure and the macro electrical conduction behavior with a highly improved understanding of material properties that control the electrical breakdown, and paves a way for guiding the modification of existing material and the exploration of novel materials for high electric field applications.

Decade Milestone Advancement of Defect-Engineered g-C3N4 for Solar Catalytic Applications.

Over the past decade, graphitic carbon nitride (g-C3N4) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C3N4 is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the "all-in-one" defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultra-active coordinated environment (M-Nx, M-C2N2, M-O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra (fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C3N4 "customization", motivating more profound thinking and flourishing research outputs on g-C3N4-based photocatalysis.

On-Surface-Assembled Single-Layer Metal-Organic Frameworks with Extended Conjugation.

Single-layer metal-organic frameworks with extended conjugation (SL-cMOFs) exhibit electronic bands that lead to high conductivity or non-trivial quantum phases. Experimental realization of SL-cMOFs has been demonstrated using on-surface coordination self-assembly. The tunability and adaptability of coordination assembly offers rich opportunities for designing and fabricating SL-cMOFs with various geometric characteristics. In this Review, we discuss the recent experimental advances in on-surface synthesis of SL-cMOFs and characterization of their band structures. Special attention has been paid to the MOFs featuring Kagome lattices. Starting from the general principles of their structural design, the SL-cMOFs recently achieved via on-surface coordination self-assembly are subsequently divided into three categories, that is, M3 L2 , M2 L3 , and M3 L MOFs (M for metal and L for ligand), and the corresponding works are overviewed. The current challenges and prospective directions are also discussed.

Revealing the Modulation Effects on the Electronic Band Structures and Exciton Properties by Stacking Graphene/h-BN/MoS2 Schottky Heterostructures.

Stacking two dimensional tunneling heterostructures has always been an important strategy to improve the optoelectronic device performance. However, there are still many disputes about the blocking ability of monolayer (1L-) h-BN on the interlayer coupling. Graphene/h-BN/MoS2 optoelectronic devices have been reported for superior device results. In this study, starting with graphene/h-BN/MoS2 heterostructures, we report experimental evidence of 1L-h-BN barrier layer modulation effects about the electronic band structures and exciton properties. We find that 1L-h-BN insertion only partially blocks the interlayer carrier transfer. In the meantime, the 1L-h-BN barrier layer weakens the interlayer coupling effect, by decreasing the efficient dielectric screening and releasing the quantum confinement. Consequently, the optical conductivity and plasmon excitation slightly improve, and the electronic band structures remain unchanged in graphene/h-BN/MoS2, explaining their fascinating optoelectronic responses. Moreover, the excitonic binding energies of graphene/h-BN/MoS2 redshift with respect to the graphene/MoS2 counterparts. Our results, as well as the broadband optical constants, will help better understand the h-BN barrier layers, facilitating the developing progress of h-BN-based tunneling optoelectronic devices.

From ß-Na2 B6 O10 to Na3 AlB8 O15 and Na3 Al2 B7 O15 : Structural Tuning of Anionic-Group Architectures by Substitution of [BO4 ] by [AlO4 ] Covalent Tetrahedra.

Two new sodium aluminum borates, Na3 AlB8 O15 and Na3 Al2 B7 O15 , have been successfully synthesized by the high-temperature solution method. They crystallize in the different space groups, P21 /c and P2/c, respectively. The B-O configurations of ß-Na2 B6 O10 , Na3 AlB8 O15 and Na3 Al2 B7 O15 are compared to feature complicated different dimensional open-framework structures caused by the substitution of [BO4 ] by [AlO4 ] covalent tetrahedra. Moreover, the experimental results indicate that Na3 AlB8 O15 and Na3 Al2 B7 O15 have short ultraviolet (UV) cutoff edges (<187 nm). The first-principles calculations show that Na3 AlB8 O15 and Na3 Al2 B7 O15 have moderate birefringence (0.075 and 0.041@1064 nm, respectively).

Electrodeposition of Silver Vanadate Films: A Tale of Two Polymorphs.

Two polymorphs of AgVO3 , namely the α- and ß- forms, were prepared and their physical, structural, optical, electrochemical, and photoelectrochemical characteristics were compared using a battery of experimental and theoretical tools. A two-step method, previously developed in the our laboratory for the electrodeposition of inorganic semiconductor films, was applied to the electrosynthesis of silver vanadate (AgVO3 ) films on transparent, conducting oxide surfaces. In the first step, silver was cathodically deposited from a non-aqueous bath containing silver nitrate. In the second step, the silver film was anodically stripped in an aqueous medium containing ammonium metavanadate. The anodically generated silver ions at the interface underwent a precipitation reaction with the vanadate species to generate the desired product in situ. Each of these steps were mechanistically corroborated via the use of electrochemical quartz crystal microgravimetry, used in conjunction with voltammetry and coulometry. As-deposited films were crystalline and showed p-type semiconductor behavior. Theoretical insights are provided for the electronic origin of the αâ†’ß phase transformation in AgVO3 and the disparate optical band gaps of the two polymorphs. Finally, implications for the application of this material in solar cells are provided.