Showing papers by "Joshua E. Goldberger published in 2018"

Raman Spectroscopy, Photocatalytic Degradation, and Stabilization of Atomically Thin Chromium Tri-iodide.

Abstract: As a 2D ferromagnetic semiconductor with magnetic ordering, atomically thin chromium tri-iodide is the latest addition to the family of two-dimensional (2D) materials. However, realistic exploration of CrI3-based devices and heterostructures is challenging due to its extreme instability under ambient conditions. Here, we present Raman characterization of CrI3 and demonstrate that the main degradation pathway of CrI3 is the photocatalytic substitution of iodine by water. While simple encapsulation by Al2O3, PMMA, and hexagonal BN (hBN) only leads to modest reduction in degradation rate, minimizing light exposure markedly improves stability, and CrI3 sheets sandwiched between hBN layers are air-stable for >10 days. By monitoring the transfer characteristics of the CrI3/graphene heterostructure over the course of degradation, we show that the aquachromium solution hole-dopes graphene.

Synthesis of 1T, 2H, and 6R Germanane Polytypes

Abstract: Polytypism, or the ability for materials to crystallize with different stacking sequences, often leads to fundamentally different properties in families of two-dimensional materials Here, we show that is possible to control the polytype of GeH, a representative two-dimensional material that is synthesized topotactically by first controlling the polytype sequence of the precursor Zintl phase 1T, 2H, and 6R GeH can be prepared by the topotactic deintercalation of 1T EuGe2, 2H α-CaGe2, and 6R β-CaGe2, respectively The 6R and 1T GeH polytypes exhibit remarkably similar properties and feature band gaps of 163 and 159 eV, respectively However, the 2H CaGe2 precursor forms due to the incorporation of small amounts of In flux in the germanium lattice, which is retained when converted to GeH Consequently, 2H GeH has a reduced band gap of 145 eV Finally, temperature dependent diffraction of 6R GeH shows a negative coefficient of thermal expansion along the a-axis and a positive coefficient of thermal expan

Covalent functionalization of two-dimensional group 14 graphane analogues

Abstract: The sp3-hybridized group 14 graphane analogues are a unique family of 2D materials in which every atom requires a terminal ligand for stability. Consequently, the optical, electronic, and thermal properties of these materials can be manipulated via covalent chemistry. Herein, we review the methodologies for preparing these materials, and compare their functionalization densities to Si/Ge(111) surfaces and other covalently terminated 2D materials. We discuss how the electronic structure, optical properties, and thermal stability of the 2D framework can be broadly tuned with the ligand identity and framework element. We highlight their recent application in electronics, optoelectronics, photocatalysis, and batteries. Overall, these materials are an intriguing regime in materials design in which both surface functionalization and solid-state chemistry can be uniquely exploited to systematically design properties and phenomena.

Revealing the Spectrum of Unknown Layered Materials with Superhuman Predictive Abilities.

Abstract: We discover the chemical composition of over 1000 materials that are likely to exhibit layered and 2D phases but have yet to be synthesized. This includes two materials our calculations indicate can exist in distinct structures with different band gaps, expanding the short list of 2D phase-change materials. Whereas databases of over 1000 layered materials have been reported, we provide the first full database of materials that are likely layered but are yet to be synthesized, providing a roadmap for the synthesis community. We accomplish this by combining physics with machine learning on experimentally obtained data and verify a subset of candidates using density functional theory. We find that our model performs five times better than practitioners in the field at identifying layered materials and is comparable to or better than professional solid-state chemists. Finally, we find that semisupervised learning can offer benefits for materials design where labels for some of the materials are unknown.

Identification of Ge vacancies as electronic defects in methyl- and hydrogen-terminated germanane

Abstract: We use a combination of optical and electrostatic surface science techniques to measure electronically active native defects in multilayer GeCH3 and GeH, two-dimensional (2D) functionalized materials. Chemical processing techniques coupled with density functional theory enable us to identify the specific physical nature of both native point defects and synthesis-related impurities which can limit the optical and charge transport properties of these materials. Direct comparison of optical measurements with calculated electronic levels provides identification of these localized, deep level gap states and confirms partial H-passivation of dangling bonds, revealing synthesis and processing methods needed to control specific defects and optimize these 2D materials for emergent solid state-electronics.We use a combination of optical and electrostatic surface science techniques to measure electronically active native defects in multilayer GeCH3 and GeH, two-dimensional (2D) functionalized materials. Chemical processing techniques coupled with density functional theory enable us to identify the specific physical nature of both native point defects and synthesis-related impurities which can limit the optical and charge transport properties of these materials. Direct comparison of optical measurements with calculated electronic levels provides identification of these localized, deep level gap states and confirms partial H-passivation of dangling bonds, revealing synthesis and processing methods needed to control specific defects and optimize these 2D materials for emergent solid state-electronics.