Landau Levels of Topologically-Protected Surface States Probed by Dual-Gated Quantum Capacitance.

Spectroscopy of discrete Landau levels (LLs) in bulk-insulating three-dimensional topological insulators (3D TIs) in perpendicular magnetic field characterizes the Dirac nature of their surface states. Despite a number of studies demonstrating the quantum Hall effect (QHE) of topological surface states, quantitative evaluation of the LL energies, which serve as fundamental electronic quantities for study of the quantum states, is still limited. In this work, we explore the density of states of LLs by measuring quantum capacitance (CQ) in a truly bulk insulating 3D TI via a van der Waals heterostructure configuration. By applying dual-gate voltages, we access the individual surface states' LLs and extract their chemical potentials to quantify the LL spacings of each surface. We evaluate the LLs' energies at two distinguished QH states, namely, dissipationless (ν = ±1) and dissipative (ν = 0) states in the 3D TI.

Spin-optoelectronic devices based on hybrid organic-inorganic trihalide perovskites.

Recently the hybrid organic-inorganic trihalide perovskites have shown remarkable performance as active layers in photovoltaic and other optoelectronic devices. However, their spin characteristic properties have not been fully studied, although due to the relatively large spin-orbit coupling these materials may show great promise for spintronic applications. Here we demonstrate spin-polarized carrier injection into methylammonium lead bromide films from metallic ferromagnetic electrodes in two spintronic-based devices: a 'spin light emitting diode' that results in circularly polarized electroluminescence emission; and a 'vertical spin valve' that shows giant magnetoresistance. In addition, we also apply a magnetic field perpendicular to the injected spins orientation for measuring the 'Hanle effect', from which we obtain a relatively long spin lifetime for the electrically injected carriers. Our measurements initiate the field of hybrid perovskites spin-related optoelectronic applications.

Topological Insulator-Based van der Waals Heterostructures for Effective Control of Massless and Massive Dirac Fermions.

Three dimensional (3D) topological insulators (TIs) are an important class of materials with applications in electronics, spintronics and quantum computing. With the recent development of truly bulk insulating 3D TIs, it has become possible to realize surface dominated phenomena in electrical transport measurements e.g. the quantum Hall (QH) effect of massless Dirac fermions in topological surface states (TSS). However, to realize more advanced devices and phenomena, there is a need for a platform to tune the TSS or modify them e.g. gap them by proximity with magnetic insulators, in a clean manner. Here we introduce van der Waals (vdW) heterostructures in the form of topological insulator/insulator/graphite to effectively control chemical potential of the TSS. Two types of gate dielectrics, normal insulator hexagonal boron nitride (hBN) and ferromagnetic insulator Cr2Ge2Te6 (CGT) are utilized to tune charge density of TSS in the quaternary TI BiSbTeSe2. hBN/graphite gating in the QH regime shows improved quantization of TSS by suppression of magnetoconductivity of massless Dirac fermions. CGT/graphite gating of massive Dirac fermions in the QH regime yields half-quantized Hall conductance steps and a measure of the Dirac gap. Our work shows the promise of the vdW platform in creating advanced high-quality TI-based devices.

Hexaaminobenzene as a building block for a Family of 2D Coordination Polymers.

A family of 2D coordination polymers were successfully synthesized through "bottom-up" techniques using Ni2+, Cu2+, Co2+, and hexaaminobenzene. Liquid-liquid and air-liquid interfacial reactions were used to realize thick (∼1-2 µm) and thin (<10 nm) stacked layers of nanosheet, respectively. Atomic-force microscopy and scanning electron microscopy both revealed the smooth and flat nature of the nanosheets. Selected area diffraction was used to elucidate the hexagonal crystal structure of the framework. Electronic devices were fabricated on thin samples of the Ni analogue and they were found to be mildly conducting and also showed back gate dependent conductance.

Raman spectroscopy of folded and scrolled graphene.

Here we examine the effects of folding and scrolling on the Raman spectra of mechanically exfoliated single- and bilayer graphene prepared on SiO(2) substrates. We find that incommensurate folding in bilayer graphene results in a shift of the second-order G' band frequency, similar to that observed in folded single-layer graphene due to fold-induced changes in the phonon/electronic energy dispersion. Importantly, we show that the contrasting Raman shifts reported for the G' band frequency in folded graphene can be rationalized by taking into account the relative strength of fold-induced electron/phonon renormalization. More interestingly, we find that curvature in scrolled graphene lifts the degeneracy of the G band and results in a splitting of the G band and the appearance of low-frequency radial breathing-like (RBLM) modes. This study highlights a variety of Raman signatures for fold-induced and curvature-induced graphene and sets the stage for further theoretical and experimental studies of these novel structures.

Photosensitization of carbon nanotubes using dye aggregates.

Ordered assemblies of dye molecules, dye aggregates, possess significantly larger molar optical absorptivity than dye monomers. Yet, aggregates have not been utilized for photosensitizing nanoscale electronic devices. We find that single-walled carbon nanotubes, which are cleaned down to the atomic scale, template the growth of squaraine dye aggregates and these aggregates effectively photosensitize nanotubes. Templating of aggregates by nanotubes and functionalization of nanotubes with ordered molecular films are reported for the first time. The sensitivity achieved by aggregate-functionalized nanotube network devices is approximately an order of magnitude better than those of similar nanotube devices functionalized with dye monomers and photoactive polymers.

Effects of layer stacking on the combination Raman modes in graphene.

We have observed new combination modes in the range from 1650 to 2300 cm(-1) in single-(SLG), bi-, few-layer and incommensurate bilayer graphene (IBLG) on silicon dioxide substrates. A peak at ∼1860 cm(-1) (iTALO-) is observed due to a combination of the in-plane transverse acoustic (iTA) and the longitudinal optical (LO) phonons. The intensity of this peak decreases with increasing number of layers and this peak is absent for bulk graphite. The overtone of the out-of-plane transverse optical (oTO) phonon at ∼1750 cm(-1), also called the M band, is suppressed for both SLG and IBLG. In addition, two previously unidentified modes at ∼2200 and ∼1880 cm(-1) are observed in SLG. The 2220 cm(-1) (1880 cm(-1)) mode is tentatively assigned to the combination mode of in-plane transverse optical (iTO) and TA phonons (oTO+LO phonons) around the K point in the graphene Brillouin zone. Finally, the peak frequency of the 1880 (2220) cm(-1) mode is observed to increase (decrease) linearly with increasing graphene layers.