M. Umar Farooq

Anisotropic bias dependent transport property of defective phosphorene layer

Phosphorene is receiving great research interests because of its peculiar physical properties. Nonetheless, no systematic studies on the transport properties modified due to defects have been performed. Here, we present the electronic band structure, defect formation energy and bias dependent transport property of various defective systems. We found that the defect formation energy is much less than that in graphene. The defect configuration strongly affects the electronic structure. The band gap vanishes in single vacancy layers, but the band gap reappears in divacancy layers. Interestingly, a single vacancy defect behaves like a p-type impurity for transport property. Unlike the common belief, we observe that the vacancy defect can contribute to greatly increasing the current. Along the zigzag direction, the current in the most stable single vacancy structure was significantly increased as compared with that found in the pristine layer. In addition, the current along the armchair direction was always greater than along the zigzag direction and we observed a strong anisotropic current ratio of armchair to zigzag direction.

Manipulation of Magnetic State in Armchair Black Phosphorene Nanoribbon by Charge Doping.

Using first-principles studies, we investigated the width-dependent magnetic properties of armchair black phosphorene nanoribbons (APNRs) by controlling the electron charge doping. In the unrelaxed APNRs the antiferromagnetic coupling between two phosphorus atoms in the same edge was found. However, the edge magnetic moment vanished after structure relaxation, and all of the APNRs showed a semiconducting feature. Interestingly, the charge doping substantially altered the band structures of the APNRs because the metallic states reappeared in the charge-doped APNRs. Besides this, the magnetic moment was found in the charge-doped systems. We found that the Stoner condition could nicely explain the magnetic moment at the edge atoms. Moreover, we propose that the edge-to-edge magnetic coupling can be manipulated by charge doping because the transition from the antiferromagnetic to ferromagnetic state was achieved. Our findings may bring interesting issues for spintronics applications.

Ultra-high capacity hydrogen storage in a Li decorated two-dimensional C2N layer

Owing to naturally existing uniform periodic pores in two-dimensional (2D) C2N layers, they can be an ideal candidate for hydrogen storage materials among other 2D materials. Here, we explored the potential application of ultra-high capacity hydrogen storage using the first principles method. Remarkably, Li was strongly bonded with the C2N layer via a Kubas-type interaction with a large binding energy of 3–5 eV. This unique interaction does not exist in graphene or other 2D materials, and it rules out the possibility of Li alkali metal cluster formations. We found that the Li-decorated C2N could show a very high theoretical gravimetric density of 13 weight percentage (wt%). Very interestingly, this gravimetric density is not only 40% and 30% higher than those found in MgH2 and C60 but also significantly higher than the values obtained in alkali metal decorated graphene, MoS2 and phosphorene. Irrespective of the theoretical capacity, the most important physical quantity is the practical capacity (the difference in the number of adsorbed and desorbed hydrogen molecules) under ambient conditions of pressure and temperature. Our thermodynamic analysis showed that 75% of the adsorbed hydrogen molecules could be released under practical conditions of temperature and pressure and the practical capacity is about 10 wt%. Our findings suggest that the Li decorated C2N can be a very promising material for room-temperature hydrogen storage under realistic conditions.

Ferromagnetism controlled by electric field in tilted phosphorene nanoribbon

Study on phosphorene nanoribbon was mostly focused on zigzag and armchair structures and no ferromagnetic ground state was observed in these systems. Here, we investigated the magnetic property of tilted black phosphorene nanoribbons (TPNRs) affected by an external electric field. We also studied the edge passivation effect on the magnetism and thermal stability of the nanoribbons. The pure TPNR displayed an edge magnetic state, but it disappeared in the edge reconstructed TPNR due to the self-passivation. In addition, we found that the bare TPNR was mechanically unstable because an imaginary vibration mode was obtained. However, the imaginary vibration mode disappeared in the edge passivated TPNRs. No edge magnetism was observed in hydrogen and fluorine passivated TPRNs. In contrast, the oxygen passivated TPNR was more stable than the pure TPNR and the edge-to-edge antiferromagntic (AFM) ground state was obtained. We found that the magnetic ground state could be tuned by the electric field from antiferromagnetic (AFM) to ferromagnetic (FM) ground state. Interestingly, the oxygen passivated TPNR displayed a half-metallic state at a proper electric field in both FM and AFM states. This finding may provoke an intriguing issue for potential spintronics application using the phosphorene nanoribbons.

Long-Range Magnetic Ordering and Switching of Magnetic State by Electric Field in Porous Phosphorene.

We explored the possibility of long-range magnetic ordering in two-dimensional porous phosphorene (PP) layer by means of ab-initio calculations. The self-passivated pore geometry showed a nonmagnetic state while the pore geometry with dangling bond at two zigzag edges with a distance of 7.7 Å preferred an antiferromagnetic ordering (AFM). Pore to pore magnetic interaction with a distance of 13.5 Å between two pores was found to be remarkably long ranged, and this emerges from the interactions between the magnetic tails of the edge states in the armchair direction. The AFM state was persisted by the oxidation of the edge. Interestingly, the long-range AFM ordering changed to long-range ferromagnetic (FM) ordering by external electric field. The results are noteworthy in the interplay between electric field and electronic spin degree of freedom in phosphorene studies and may also open a promising way to explore phosphorene-based spintronics devices.

Two-Dimensional Magnetic Semiconductor in Feroxyhyte

A few years ago, it was claimed that the two-dimensional (2D) feroxyhyte (δ-FeOOH) layer could possess a net magnetic moment and it could be applied for potential spintronics applications because it showed a band gap. However, the exact crystal structure is still unknown. Hereby, we investigate the crystal structure, electronic band structure, and magnetic and optical properties of 2D δ-FeOOH using density functional calculations. On the basis of the experimental observation and dynamical stability calculations, we propose that the 2D δ-FeOOH originates from bulk Fe(OH)2 via oxidation. A perfect antiferromagnetic ground state was observed in the monolayer structure with an indirect band gap of 2.4 eV. On the other hand, the bilayer structure displayed a direct band gap of 0.87 eV, and we obtained a ferrimagnetic state. The net magnetic moment in the bilayer was 1.49 μB per cell. The interlayer distance and film thickness in bilayer δ-FeOOH were 1.68 and 7.37 Å, respectively. This interlayer distance was suppressed to 1.47 Å in a trilayer system, and the band gap of 1.6 eV was found. The trilayer δ-FeOOH had a film thickness of 11.57 Å, and this is comparable to the experimental thickness of 12 Å. To compare with the experimental band gap of 2.2 eV obtained from a UV-visible optical spectrum measurement, we also calculated the absorption spectra, and the onset of the absorption peak in the monolayer, bilayer, and trilayer appeared at 3.2, 2.8, and 2.2 eV, respectively. Overall, considering the magnetic state, optical absorption, and film thickness, we propose that the trilayer structure agrees with the experimentally synthesized structure.

Superconductivity in two-dimensional ferromagnetic MnB

Using the universal structure predictor algorithm, we proposed that two-dimensional MnB structures with p4mmm (α-MnB) and pmma (β-MnB) symmetries could be synthesized. This finding was verified by calculating the dynamical stability, molecular dynamics, and mechanical properties. The α-MnB had an in-plane stiffness Yx (=Yy) around 100 N/m while the β-Mn displayed an asymmetric mechanical stiffness of Yx = 186 N/m and Yy = 139 N/m. Both systems displayed a ferromagnetic ground state with metallic band structures. The calculated magnetic moments were 2.14 and 2.34 µB per Mn-B pair in the α-MnB and β-MnB. Furthermore, we investigated the potential superconductivity. In the α-MnB, we found the unique feature of Kohn anomaly at q~2kF in the diagonal direction of the Brillouin zone. The β-MnB phonon spectra showed a valley of degenerated localized softening vibration modes at the edge of the Brillouin zone. The ZA and LA phonon branches in this valley induced the largest contribution to electron-phonon coupling strength. The calculated total electron-phonon coupling parameters were 1.20 and 0.89 in α-MnB and β-MnB systems. Overall, we predict that the α-MnB and β-MnB systems can display 2D ferromagnetic superconducting states with the estimated critical temperatures of Tc ≈ 10−13 K.