Manipulating a quantum state via electrostatic gating has been of great importance for many model systems in nanoelectronics. Until now, however, controlling the electron spins or, more specifically, the magnetism of a system by electric-field tuning has proven challenging. Recently, atomically thin magnetic semiconductors have attracted significant attention due to their emerging new physical phenomena. However, many issues are yet to be resolved to convincingly demonstrate gate-controllable magnetism in these two-dimensional materials. Here, we show that, via electrostatic gating, a strong field effect can be observed in devices based on few-layered ferromagnetic semiconducting CrGeTe. At different gate doping, micro-area Kerr measurements in the studied devices demonstrate bipolar tunable magnetization loops below the Curie temperature, which is tentatively attributed to the moment rebalance in the spin-polarized band structure. Our findings of electric-field-controlled magnetism in van der Waals magnets show possibilities for potential applications in new-generation magnetic memory storage, sensors and spintronics.

Thermoelectric power generation technology has emerged as a clean "heat engine" that can convert heat to electricity. Recently, the discovery of an ultrahigh thermoelectric figure of merit in SnSe crystals has drawn a great deal of attention. In view of their facile processing and scale-up applications, polycrystalline SnSe materials with ZT values comparable to those of the SnSe crystals are greatly desired. Here we achieve a record high ZT value ∼2.1 at 873 K in polycrystalline SnSe with Sn vacancies. We demonstrate that the carrier concentration increases by artificially introducing Sn vacancies, contributing significantly to the enhancements of electrical conductivity and thermoelectric power factor. The detailed analysis of the data in the light of first-principles calculations results indicates that the increased carrier concentration can be attributed to the Sn-vacancy-induced Fermi level downshift and the interplay between the vacancy states and valence bands. Furthermore, vacancies break translation symmetry and thus enhance phonon scattering, leading to extralow thermal conductivity. Such high ZT value ∼2.1 is achieved by synergistically optimizing both electrical- and thermal-transport properties of polycrystalline SnSe. The vast increase in ZT for polycrystalline SnSe may accelerate practical applications of this material in highly effective solid-state thermoelectric devices.

Layered gallium telluride (GaTe) has attracted much attention recently, due to its extremely high photoresponsivity, short response time, and promising thermoelectric performance. Different from most commonly studied two-dimensional (2D) materials, GaTe has in-plane anisotropy and a low symmetry with the C2h(3) space group. Investigating the in-plane optical anisotropy, including the electron-photon and electron-phonon interactions of GaTe is essential in realizing its applications in optoelectronics and thermoelectrics. In this work, the anisotropic light-matter interactions in the low-symmetry material GaTe are studied using anisotropic optical extinction and Raman spectroscopies as probes. Our polarized optical extinction spectroscopy reveals the weak anisotropy in optical extinction spectra for visible light of multilayer GaTe. Polarized Raman spectroscopy proves to be sensitive to the crystalline orientation of GaTe, and shows the intricate dependences of Raman anisotropy on flake thickness, photon and phonon energies. Such intricate dependences can be explained by theoretical analyses employing first-principles calculations and group theory. These studies are a crucial step toward the applications of GaTe especially in optoelectronics and thermoelectrics, and provide a general methodology for the study of the anisotropy of light-matter interactions in 2D layered materials with in-plane anisotropy.

Phosphorene is emerging as an important two-dimensional semiconductor, but controlling the surface chemistry of phosphorene remains a significant challenge. Here, we show that controlled oxidation of phosphorene determines the composition and spatial distribution of the resulting oxide. We used X-ray photoemission spectroscopy to measure the binding energy shifts that accompany oxidation. We interpreted these spectra by calculating the binding energy shift for 24 likely bonding configurations, including phosphorus oxides and hydroxides located on the basal surface or edges of flakes. After brief exposure to high-purity oxygen or high-purity water vapor at room temperature, we observed phosphorus in the +1 and +2 oxidation states; longer exposures led to a large population of phosphorus in the +3 oxidation state. To provide insight into the spatial distribution of the oxide, transmission electron microscopy was performed at several stages during the oxidation. We found crucial differences between oxygen and water oxidants: while pure oxygen produced an oxide layer on the van der Waals surface, water oxidized the material at pre-existing defects such as edges or steps. We propose a mechanism based on the thermodynamics of electron transfer to interpret these observations. This work opens a route to functionalize the basal surface or edges of two-dimensional (2D) black phosphorus through site-selective chemical reactions and presents the opportunity to explore the synthesis of 2D phosphorene oxide by oxidation.

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We study the second-order Raman process of mono-and few-layer MoTe2, by combining ab initio density functional perturbation calculations with experimental Raman spectroscopy using 532, 633 and 785 nm excitation lasers. The calculated electronic band structure and the density of states show that the resonance Raman process occurs at the M point in the Brillouin zone, where a strong optical absorption occurs due to a logarithmic Van-Hove singularity of electronic density of states. Double resonance Raman process with inter-valley electron-phonon coupling connects two of the three inequivalent M points in the Brillouin zone, giving rise to second-order Raman peaks due to the M point phonons. The calculated vibrational frequencies of the second-order Raman spectra agree with the observed laser-energy dependent Raman shifts in the experiment.

We use ultrafast electron crystallography to study structural changes induced in graphite by a femtosecond laser pulse. At moderate fluences of ≤21 mJ/cm 2 , lattice vibrations are observed to thermalize on a time scale of ≈8 ps. At higher fluences approaching the damage threshold, lattice vibration amplitudes saturate. Following a marked initial contraction, graphite is driven nonthermally into a transient state with sp 3 -like character, forming interlayer bonds. Using ab initio density functional calculations, we trace the governing mechanism back to electronic structure changes following the photo-excitation.

We combine scanning tunneling microscopy (STM) measurements with ab initio calculations to study the self-assembly of long chain alkanes and related alcohol and carboxylic acid molecules on graphite. For each system, we identify the optimum adsorption geometry and explain the energetic origin of the domain formation observed in the STM images. Our results for the hierarchy of adsorbate-adsorbate and adsorbate-substrate interactions provide a quantitative basis to understand the ordering of long chain alkanes in self-assembled monolayers and ways to modify it using alcohol and acid functional groups.