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Register a new userNanoscopy Reveals Metallic Black Phosphorus
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Layered and two-dimensional (2D) materials such as graphene, boron nitride, transition metal dichalcogenides(TMDCs), and black phosphorus (BP) have intriguing fundamental physical properties and bear promise of numerous important applications in electronics and optics. Of them, BP is a novel 2D material that has been theoretically predicted to acquire plasmonic behavior for frequencies below ~0.4 eV when highly doped. The electronic properties of BP are unique due to an anisotropic structure, which could strongly influence collective electronic excitations. Advantages of BP as a material for nanoelectronics and nanooptics are due to the fact that, in contrast to metals, the free carrier density in it can be dynamically controlled by electrostatic gating, which has been demonstrated by its use in field-effect transistors. Despite all the interest that BP attracts, near-field and plasmonic properties of BP have not yet been investigated experimentally. Here we report the first observation of nanoscopic near-field properties of BP. We have discovered near field patterns of outside bright fringes and high surface polarizability of nanofilm BP consistent with its surface-metallic, plasmonic behavior at mid-infrared (mid-IR) frequencies. This behavior is highly frequency-dispersive, disappearing above frequency, {omega} =1070 cm-1, which allowed us to estimate the plasma frequency and carrier density. We have also observed similar behavior in other 2D semiconductors such as TMDCs but not in 2D insulators such as boron nitride. This new phenomenon is attributed to surface charging of the semiconductor nanofilms. This discovery opens up a new field of research and potential applications in nanoplasmonics and optoelectronics.
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Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. Finally, the blue shift of the emission with increasing temperature is well described using a two oscillator model for the temperature dependence of the band gap.
We report about the energy and momentum resolved optical response of black phosphorus (BP) in its bulk form. Along the armchair direction of the puckered layers we find a highly dispersive mode that is trongly suppressed in the perpendicular (zig-zag) direction. This mode emerges out of the single-particle continuum for finite values of momentum and is therefore interpreted as an exciton. We argue that this exciton, which has already been predicted theoretically for phosphorene -- the monolayer form of BP -- can be detected by conventional optical spectroscopy in the two-dimensional case and might pave the way for optoelectronic applications of this emerging material.
Black phosphorus (BP), a layered van der Waals material, reportedly has a band gap sensitive to external perturbations and manifests a Dirac-semimetal phase when its band gap is closed. Previous studies were focused on effects of each perturbation, lacking a unified picture for the band-gap closing and the Dirac-semimetal phase. Here, using pseudospins from the glide-reflection symmetry, we study the electronic structures of mono- and bilayer BP and construct the phase diagram of the Dirac-semimetal phase in the parameter space related to pressure, strain, and electric field. We find that the Dirac-semimetal phase in BP layers is singly connected in the phase diagram, indicating the phase is topologically identical regardless of the gap-closing mechanism. Our findings can be generalized to the Dirac semimetal phase in anisotropic layered materials and can play a guiding role in search for a new class of topological materials and devices.
Resistivity measurements of a few-layer black phosphorus (bP) crystal in parallel magnetic fields up to 45 T are reported as a function of the angle between the in-plane field and the source-drain (S-D) axis of the device. The crystallographic directions of the bP crystal were determined by Raman spectroscopy, with the zigzag axis found within 5{deg} of the S-D axis, and the armchair axis in the orthogonal planar direction. A transverse magneto-resistance (TMR) as well as a classically-forbidden longitudinal magneto-resistance (LMR) are observed. Both are found to be strongly anisotropic and non-monotonic with increasing in-plane field. Surprisingly, the relative magnitude (in %) of the positive LMR is larger than the TMR above $sim$32 T. Considering the known anisotropy of bP whose zigzag and armchair effective masses differ by a factor of approximately seven, our experiment strongly suggests this LMR to be a consequence of the anisotropic Fermi surface of bP.
Black phosphorus (bP) is the second known elemental allotrope with a layered crystal structure that can be mechanically exfoliated down to atomic layer thickness. We have fabricated bP naked quantum wells in a back-gated field effect transistor geometry with bP thicknesses ranging from $6pm1$ nm to $47pm1$ nm. Using an encapsulating polymer superstrate, we have suppressed bP oxidation and have observed field effect mobilities up to 600 cm$^2$/Vs and on/off current ratios exceeding $10^5$. Importantly, Shubnikov-de Haas (SdH) oscillations observed in magnetotransport measurements up to 35 T reveal the presence of a 2-D hole gas with Schrodinger fermion character in an accumulation layer at the bP/oxide interface. Our work demonstrates that 2-D electronic structure and 2-D atomic structure are independent. 2-D carrier confinement can be achieved in layered semiconducting materials without necessarily approaching atomic layer thickness, advantageous for materials that become increasingly reactive in the few-layer limit such as bP.
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