Xiaolong Chen

High-quality sandwiched black phosphorus heterostructure and its quantum oscillations

Two-dimensional materials such as graphene and transition metal dichalcogenides have attracted great attention because of their rich physics and potential applications in next-generation nanoelectronic devices. The family of two-dimensional materials was recently joined by atomically thin black phosphorus which possesses high theoretical mobility and tunable bandgap structure. However, degradation of properties under atmospheric conditions and high-density charge traps in black phosphorus have largely limited its actual mobility thus hindering its future applications. Here, we report the fabrication of stable sandwiched heterostructures by encapsulating atomically thin black phosphorus between hexagonal boron nitride layers to realize ultra-clean interfaces that allow a high field-effect mobility of ∼1,350u2009cm2V−1u2009s−1 at room temperature and on–off ratios exceeding 105. At low temperatures, the mobility even reaches ∼2,700u2009cm2V−1u2009s−1 and quantum oscillations in black phosphorus two-dimensional hole gas are observed at low magnetic fields. Importantly, the sandwiched heterostructures ensure that the quality of black phosphorus remains high under ambient conditions.

Probing the electron states and metal-insulator transition mechanisms in molybdenum disulphide vertical heterostructures

The metal-insulator transition is one of the remarkable electrical properties of atomically thin molybdenum disulphide. Although the theory of electron-electron interactions has been used in modelling the metal-insulator transition in molybdenum disulphide, the underlying mechanism and detailed transition process still remain largely unexplored. Here we demonstrate that the vertical metal-insulator-semiconductor heterostructures built from atomically thin molybdenum disulphide are ideal capacitor structures for probing the electron states. The vertical configuration offers the added advantage of eliminating the influence of large impedance at the band tails and allows the observation of fully excited electron states near the surface of molybdenum disulphide over a wide excitation frequency and temperature range. By combining capacitance and transport measurements, we have observed a percolation-type metal-insulator transition, driven by density inhomogeneities of electron states, in monolayer and multilayer molybdenum disulphide. In addition, the valence band of thin molybdenum disulphide layers and their intrinsic properties are accessed.

Universal low-temperature Ohmic contacts for quantum transport in transition metal dichalcogenides

Low carrier mobility and high electrical contact resistance are two major obstacles prohibiting explorations of quantum transport in TMDCs. Here, we demonstrate an effective method to establish low-temperature Ohmic contacts in boron nitride encapsulated TMDC devices based on selective etching and conventional electron-beam evaporation of metal electrodes. This method works for most extensively studied TMDCs in recent years, including MoS2, MoSe2, WSe2, WS2, and 2H-MoTe2. Low electrical contact resistance is achieved at 2 K. All of the few-layer TMDC devices studied show excellent performance with remarkably improved field-effect mobilities ranging from 2300 cm2/V s to 16000 cm2/V s, as verified by the high carrier mobilities extracted from Hall effect measurements. Moreover, both high-mobility n-type and p-type TMDC channels can be realized by simply using appropriate contact metals. Prominent Shubnikov-de Haas oscillations have been observed and investigated in these high-quality TMDC devices.

Modifying electronic transport properties of graphene by electron beam irradiation

We demonstrate that electron beam irradiation with precise dosage control under clean vacuum conditions can induce bond disorder and inter-valley scattering but not necessarily lattice damage in high quality single-layer graphene, as evidenced by the changes of temperature-dependent transport properties, quantum Hall effects, and large negative magnetoresistance effects observed at cryogenic temperatures. The bond disorder significantly modified the Raman scattering and electronic transport properties of graphene, which is consistent with that observed in hydrogenated graphene. In situ transport measurements at different sample treatment stages revealed an interesting activation process of graphene through electron beam irradiation. The activated graphene samples are very sensitive to oxygen and water vapors.

van der Waals Epitaxial Growth of Atomically Thin Bi2Se3 and Thickness-Dependent Topological Phase Transition

Two-dimensional (2D) atomic-layered heterostructures stacked by van der Waals interactions recently introduced new research fields, which revealed novel phenomena and provided promising applications for electronic, optical, and optoelectronic devices. In this study, we report the van der Waals epitaxial growth of high-quality atomically thin Bi2Se3 on single crystalline hexagonal boron nitride (h-BN) by chemical vapor deposition. Although the in-plane lattice mismatch between Bi2Se3 and h-BN is approximately 65%, our transmission electron microscopy analysis revealed that Bi2Se3 single crystals epitaxially grew on h-BN with two commensurate states; that is, the (1̅21̅0) plane of Bi2Se3 was preferably parallel to the (1̅100) or (1̅21̅0) plane of h-BN. In the case of the Bi2Se3 (2̅110) ∥ h-BN (11̅00) state, the Moiré pattern wavelength in the Bi2Se3/h-BN superlattice can reach 5.47 nm. These naturally formed thin crystals facilitated the direct assembly of h-BN/Bi2Se3/h-BN sandwiched heterostructures without introducing any impurity at the interfaces for electronic property characterization. Our quantum capacitance (QC) measurements showed a compelling phenomenon of thickness-dependent topological phase transition, which was attributed to the coupling effects of two surface states from Dirac Fermions at/or above six quintuple layers (QLs) to gapped Dirac Fermions below six QLs. Moreover, in ultrathin Bi2Se3 (e.g., 3 QLs), we observed the midgap states induced by intrinsic defects at cryogenic temperatures. Our results demonstrated that QC measurements based on h-BN/Bi2Se3/h-BN sandwiched structures provided rich information regarding the density of states of Bi2Se3, such as quantum well states and Landau quantization. Our approach in fabricating h-BN/Bi2Se3/h-BN sandwiched device structures through the combination of bottom-up growth and top-down dry transferring techniques can be extended to other two-dimensional layered heterostructures.

Density of States and Its Local Fluctuations Determined by Capacitance of Strongly Disordered Graphene

We demonstrate that fluctuations of the local density of states (LDOS) in strongly disordered graphene play an important role in determining the quantum capacitance of the top-gate graphene devices. Depending on the strength of the disorder induced by metal-cluster decoration, the measured quantum capacitance of disordered graphene can dramatically decrease in comparison with pristine graphene. This is opposite to the common belief that quantum capacitance should increase with disorder. To explain this counterintuitive behavior, we present a two-parameter model which incorporates both the non-universal power law behavior for the ADOS and a lognormal distribution of LDOS. We find excellent quantitative agreements between the model and measured quantum capacitance for three disordered samples in a wide range of Fermi energies. Thus, by measuring the quantum capacitance, we can simultaneously determine the ADOS and its fluctuations. It is the LDOS fluctuations that cause the dramatic reduction of the quantum capacitance.

Detection of interlayer interaction in few-layer graphene

Research Grants Council of Hong Kong [604112, N_HKUST613/12, 16302215, HKUST9/CRF/08, CRF_HKU9/CRF/13G]; Raith-HKUST Nanotechnology Laboratory electron-beam lithography facility [SEG HKUST08]

Negative Quantum Capacitance Induced by Midgap States in Single-layer Graphene

We demonstrate that single-layer graphene (SLG) decorated with a high density of Ag adatoms displays the unconventional phenomenon of negative quantum capacitance. The Ag adatoms act as resonant impurities and form nearly dispersionless resonant impurity bands near the charge neutrality point (CNP). Resonant impurities quench the kinetic energy and drive the electrons to the Coulomb energy dominated regime with negative compressibility. In the absence of a magnetic field, negative quantum capacitance is observed near the CNP. In the quantum Hall regime, negative quantum capacitance behavior at several Landau level positions is displayed, which is associated with the quenching of kinetic energy by the formation of Landau levels. The negative quantum capacitance effect near the CNP is further enhanced in the presence of Landau levels due to the magnetic-field-enhanced Coulomb interactions.

Probing the electronic states and impurity effects in black phosphorus vertical heterostructures

Atomically thin black phosphorus (BP) is a promising two-dimensional material for fabricating electronic and optoelectronic nano-devices with high mobility and tunable bandgap structures. However, the charge-carrier mobility in few-layer phosphorene (monolayer BP) is mainly limited by the presence of impurity and disorders. In this study, we demonstrate that vertical BP heterostructure devices offer great advantages in probing the electron states of monolayer and few-layer phosphorene at temperatures down to 2 K through capacitance spectroscopy. Electronic states in the conduction and valence bands of phosphorene are accessible over a wide range of temperature and frequency. Exponential band tails have been determined to be related to disorders. Unusual phenomena such as the large temperature-dependence of the electron state population in few-layer phosphorene have been observed and systematically studied. By combining the first-principles calculation, we identified that the thermal excitation of charge trap states and oxidation-induced defect states were the main reasons for this large temperature dependence of the electron state population and degradation of the on-off ratio in phosphorene field-effect transistors.

Electron-electron interactions in monolayer graphene quantum capacitors

AbstractWe demonstrate the effects of electron-electron (e-e) interactions in monolayer graphene quantum capacitors. Ultrathin yttrium oxide showed excellent performance as the dielectric layer in top-gate device geometry. The structure and dielectric constant of the yttrium oxide layers have been carefully studied. The inverse compressibility retrieved from the quantum capacitance agreed fairly well with the theoretical predictions for the e-e interactions in monolayer graphene at different temperatures. We found that electron-hole puddles played a significant role in the low-density carrier region in graphene. By considering the temperature-dependent charge fluctuation, we established a model to explain the round-off effect originating from the e-e interactions in monolayer graphene near the Dirac point.n