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Register a new userTuning energy barriers by doping 2D group-IV monochalcogenides
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Added by
Salvador Barraza-Lopez
Publication date
2020
fields
Physics
and research's language is
English
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Structural degeneracies underpin the ferroic behavior of next-generation two-dimensional materials, and lead to peculiar two-dimensional structural transformations under external fields, charge doping and/or temperature. The most direct indicator of the ease of these transformations is an {em elastic energy barrier}, defined as the energy difference between the (degenerate) structural ground state unit cell, and a unit cell with an increased structural symmetry. Proximity of a two-dimensional material to a bulk substrate can affect the magnitude of the critical fields and/or temperature at which these transformations occur, with the first effect being a relative charge transfer, which could trigger a structural quantum phase transition. With this physical picture in mind, we report the effect of modest charge doping (within $-0.2$ and $+0.2$ electrons per unit cell) on the elastic energy barrier of ferroelastic black phosphorene and nine ferroelectric monochalcogenide monolayers. The elastic energy barrier $J_s$ is the energy needed to create a $Pnm2_1to P4/nmm$ two-dimensional structural transformation. Similar to the effect on the elastic energy barrier of ferroelastic SnO monolayers, group-IV monochalcogenide monolayers show a tunable elastic energy barrier for similar amounts of doping: a decrease (increase) of $J_s$ can be engineered under a modest hole (electron) doping of no more than one tenth of an electron or a hole per atom.
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The family of group IV-VI monochalcogenides has an atomically puckered layered structure, and their atomic bond configuration suggests the possibility for the realization of various polymorphs. Here, we report the synthesis of the first hexagonal polymorph from the family of group IV-VI monochalcogenides, which is conventionally orthorhombic. Recently predicted four-atomic-thick hexagonal GeSe, so-called {gamma}-GeSe, is synthesized and clearly identified by complementary structural characterizations, including elemental analysis, electron diffraction, high-resolution transmission electron microscopy imaging, and polarized Raman spectroscopy. The electrical and optical measurements indicate that synthesized {gamma}-GeSe exhibits high electrical conductivity of 3x10^5 S/m, which is comparable to those of other two-dimensional layered semimetallic crystals. Moreover, {gamma}-GeSe can be directly grown on h-BN substrates, demonstrating a bottom-up approach for constructing vertical van der Waals heterostructures incorporating {gamma}-GeSe. The newly identified crystal symmetry of {gamma}-GeSe warrants further studies on various physical properties of {gamma}-GeSe.
The two-dimensional ferroelectrics GeS, GeSe, SnS and SnSe are expected to have large spontaneous in-plane electric polarization and enhanced shift-current response. Using density functional methods, we show that these materials also exhibit the largest effective second harmonic generation reported so far. It can reach magnitudes up to $10$ nm/V which is about an order of magnitude larger than that of prototypical GaAs. To rationalize this result we model the optical response with a simple one-dimensional two-band model along the spontaneous polarization direction. Within this model the second-harmonic generation tensor is proportional to the shift-current response tensor. The large shift current and second harmonic responses of GeS, GeSe, SnS and SnSe make them promising non-linear materials for optoelectronic applications.
Using electrically detected magnetic resonance spectroscopy, we demonstrate that doping the conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) with ethylene glycol allows for the control of effective local charge carrier hyperfine fields through motional narrowing. These results suggest that doping of organic semiconductors could enable the tuning of macroscopic material properties dependent on hyperfine fields such as magnetoresistance, the magneto-optical responses and spin-diffusion.
We study the injection current response tensor (also known as circular photogalvanic effect or ballistic current) in ferrolectric monolayer GeS, GeSe, SnS, and SnSe. We find that the injection current is perpendicular to the spontaneous in-plane polarization and could reach peak (bulk) values of the order of $10^{10}$A/V$^{2}$s in the visible spectrum. The magnitude of the injection current is the largest reported in the literature to date for a two dimensional material. To rationalize the large injection current, we correlate the injection current spectrum with the joint density of states, electric polarization, strain, etc. We find that various factors such as anisotropy, in-plane polarization and wave function delocalization are important in determining the injection current tensor in these materials. We also find that compression along the polar axis can increase the injection current (or change its sign), and hence strain can be an effective control knob for their nonlinear optical response. Conversely, the injection current can be a sensitive probe of the crystal structure.
We survey the state-of-the-art knowledge of ferroelectric and ferroelastic group-IV monochalcogenide monolayers. These semiconductors feature remarkable structural and mechanical properties, such as a switchable in-plane spontaneous polarization, soft elastic constants, structural degeneracies, and thermally-driven two-dimensional structural transformations. Additionally, these 2D materials also display selective valley excitations, valley Hall effects, and persistent spin helix behavior. After a description of their Raman spectra, a discussion of optical properties arising from their lack of centrosymmetry---such as an unusually strong second-harmonic intensity, large bulk photovoltaic effects, photostriction, and tunable exciton binding energies---is provided as well. The physical properties observed in these materials originate from (correlate with) their intrinsic and switchable electric polarization, and the physical behavior hereby reviewed could be of use in non-volatile memory, valleytronic, spintronic, and optoelectronic devices: these 2D multiferroics enrich and diversify the 2D materials toolbox.
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