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Dynamical Evolution of Anisotropic Response in Black Phosphorus under Ultrafast Photoexcitation

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 Added by Dong Sun
 Publication date 2015
  fields Physics
and research's language is English




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Black phosphorus has recently emerged as a promising material for high performance electronic and optoelectronic device for its high mobility, tunable mid-infrared bandgap and anisotropic electronic properties. Dynamical evolution of photo excited carriers and its induced change of transient electronic properties are critical for materials high field performance, but remains to be explored for black phosphorus. In this work, we perform angle resolved transient reflection spectroscopy to study the dynamical evolution of anisotropic properties of black phosphorus under photo excitation. We find that the anisotropy of reflectivity is enhanced in the pump induced quasi-equilibrium state, suggesting an extraordinary enhancement of the anisotropy in dynamical conductivity in hot carrier dominated regime. These results raise enormous possibilities of creating high field, angle sensitive electronic, optoelectronic and remote sensing devices exploiting the dynamical electronic anisotropic with black phosphorus.



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Black phosphorus (BP) has emerged as a direct-bandgap semiconducting material with great application potentials in electronics, photonics, and energy conversion. Experimental characterization of the anisotropic thermal properties of BP, however, is extremely challenging due to the lack of reliable and accurate measurement techniques to characterize anisotropic samples that are micrometers in size. Here, we report measurement results of the anisotropic thermal conductivity of bulk BP along three primary crystalline orientations, using the novel time-resolved magneto-optical Kerr effect (TR-MOKE) with enhanced measurement sensitivities. Two-dimensional beam-offset TR-MOKE signals from BP flakes yield the thermal conductivity along the zigzag crystalline direction to be 84 ~ 101 W/(m*K), nearly three times as large as that along the armchair direction (26 ~ 36 W/(m*K)). The through-plane thermal conductivity of BP ranges from 4.3 to 5.5 W/(m*K). The first-principles calculation was performed for the first time to predict the phonon transport in BP both along the in-plane zigzag and armchair directions and along the through-plane direction. This work successfully unveiled the fundamental mechanisms of anisotropic thermal transport along the three crystalline directions in bulk BP, as demonstrated by the excellent agreement between our first-principles-based theoretical predictions and experimental characterizations on the anisotropic thermal conductivities of bulk BP.
Black phosphorus presents a very anisotropic crystal structure, making it a potential candidate for hyperbolic plasmonics, characterized by a permittivity tensor where one of the principal components is metallic and the other dielectric. Here we demonstrate that atomically thin black phosphorus can be engineered to be a hyperbolic material operating in a broad range of the electromagnetic spectrum from the entire visible spectrum to ultraviolet. With the introduction of an optical gain, a new hyperbolic region emerges in the infrared. The character of this hyperbolic plasmon depends on the interplay between gain and loss along the two crystalline directions.
The travel of heat in insulators is commonly pictured as a flow of phonons scattered along their individual trajectory. In rare circumstances, momentum-conserving collision events dominate, and thermal transport becomes hydrodynamic. One of these cases, dubbed the Poiseuille flow of phonons, can occur in a temperature window just below the peak temperature of thermal conductivity. We report on a study of heat flow in bulk black phosphorus between 0.1 and 80 K. We find a thermal conductivity showing a faster than cubic temperature dependence between 5 and 12 K. Consequently, the effective phonon mean free path shows a nonmonotonic temperature dependence at the onset of the ballistic regime, with a size-dependent Knudsen minimum. These are hallmarks of Poiseuille flow previously observed in a handful of solids. Comparing the phonon dispersion in black phosphorus and silicon, we showthat the phase space for normal scattering events in black phosphorus is much larger. Our results imply that the most important requirement for the emergence of Poiseuille flowis the facility ofmomentum exchange between acoustic phonon branches. Proximity to a structural transition can be beneficial for the emergence of this behavior in clean systems, even when they do not exceed silicon in purity.
Black phosphorus has recently attracted significant attention for its highly anisotropic properties. A variety of ultrafast optical spectroscopies has been applied to probe the carrier response to photoexcitation, but the complementary lattice response has remained unaddressed. Here we employ femtosecond electron diffraction to explore how the structural anisotropy impacts the lattice dynamics after photoexcitation. We observe two timescales in the lattice response, which we attribute to electron-phonon and phonon-phonon thermalization. Pronounced differences between armchair and zigzag directions are observed, indicating a nonthermal state of the lattice lasting up to ~60 ps. This nonthermal state is characterized by a modified anisotropy of the atomic vibrations compared to equilibrium. Our findings provide insights in both electron-phonon as well as phonon-phonon coupling and bear direct relevance for any application of black phosphorus in nonequilibrium conditions.
Black phosphorus has attracted interest as a material for use in optoelectronic devices due to many favorable properties such as a high carrier mobility, field-effect, and a direct bandgap that can range from 0.3 eV in its bulk crystalline form to 2 eV for a single atomic layer. The low bandgap energy for bulk black phosphorus allows for direct transition photoabsorption that enables detection of light out to mid-infrared frequencies. In this work we characterize the room temperature optical response of a black phosphorus photoconductive detector at wavelengths ranging from 1.56 $mu$m to 3.75 $mu$m. Pulsed autocorrelation measurements in the near-infrared regime reveal a strong, sub-linear photocurrent nonlinearity with a response time of 1 ns, indicating that gigahertz electrical bandwidth is feasible. Time resolved photoconduction measurements covering near- and mid-infrared frequencies show a fast 65 ps rise time, followed by a carrier relaxation with a time scale that matches the intrinsic limit determined by autocorrelation. The sublinear photoresponse is shown to be caused by a reduction in the carrier relaxation time as more energy is absorbed in the black phosphorus flake and is well described by a carrier recombination model that is nonlinear with excess carrier density. The device exhibits a measured noise-equivalent power of 530 pW/$sqrt{text{Hz}}$ which is the expected value for Johnson noise limited performance. The fast and sensitive room temperature photoresponse demonstrates that black phosphorus is a promising new material for mid-infrared optoelectronics.
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