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Register a new userPhoto-induced Dirac cone flattening in BaNiS$_2$
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Using a real-time implementation of the self-consistent $GW$ method, we theoretically investigate the photo-induced changes in the electronic structure of the quasi two-dimensional semi-metal BaNiS$_2$. This material features four Dirac cones in the unit cell and our simulation of the time- and momentum-resolved nonequilibrium spectral function reveals a flattening of the Dirac bands after a photo-doping pulse with a 1.5 eV laser. The simulation results are consistent with the recently reported experimental data on photo-doped BaNiS$_2$ and ZrSiSe, another Dirac semi-metal. A detailed analysis of the numerical data allows us to attribute the nonequilibrium modifications of the Dirac bands to (i) an increased effective temperature after the photo-excitation, which affects the screening properties of the system, and (ii) to nontrivial band shifts in the photo-doped state, which are mainly induced by the Fock term.
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BaNiS$_2$ is a system dominated by a fourfold Dirac-cone network. We measured the optical conductivity and Landau level spectra of the Dirac nodal lines and quantitatively modeled the response through ab initio calculations. The optical conductivity shows a highly unusual temperature-independent isosbestic line. Magneto-optical spectra show a nearly $sqrt{B}$ behavior, the hallmark of a conical dispersion. BaNiS$_2$ is a simple prototype of a Dirac nodal line semimetal: its Dirac nodal lines are only slightly gapped, and they disperse exclusively along the out-of-plane direction. Our first-principles calculations account for the observed isosbestic conductivity, which terminates in a Van Hove singularity. We argue that such an optical response is universal for Dirac cones, which must connect with each other within the Brillouin zone by breaking their conical shape.
By means of pump-probe time- and angle-resolved photoelectron spectroscopy, we provide evidence of a sizeable reduction of the Fermi velocity of out-of-equilibrium Dirac bands in the quasi-two-dimensional semimetal BaNiS$_2$. First-principle calculations indicate that this band renormalization is ascribed to a change in non-local electron correlations driven by a photo-induced enhancement of screening properties. This effect is accompanied by a slowing down of the Dirac fermions and by a non-rigid shift of the bands at the center of the Brillouin zone. This result suggests that other similar electronic structure renormalizations may be photoinduced in other materials in presence of strong non-local correlations.
The emergence of photo-induced topological phases and their phase transitions are theoretically predicted in organic salt $alpha$-(BEDT-TTF)$_2$I$_3$, which possesses inclined Dirac cones in its band structure. By analyzing a photo-driven tight-binding model describing conduction electrons in the BEDT-TTF layer using the Floquet theorem, we demonstrate that irradiation with circularly polarized light opens a gap at the Dirac points, and the system eventually becomes a Chern insulator characterized by a quantized topological invariant. A rich phase diagram is obtained in plane of amplitude and frequency of light, which contains Chern insulator, semimetal, and normal insulator phases. We find that the photo-induced Hall conductivity provides a sensitive means to detect the predicted phase evolutions experimentally. This work contributes towards developing the optical manipulation of electronic states in matter through broadening the range of target materials that manifest photo-induced topological phase transitions.
Optical measurements and band structure calculations are reported on 3D Dirac materials. The electronic properties associated with the Dirac cone are identified in the reflectivity spectra of Cd$_3$As$_2$ and Na$_3$Bi single crystals. In Na$_3$Bi, the plasma edge is found to be strongly temperature dependent due to thermally excited free carriers in the Dirac cone. The thermal behavior provides an estimate of the Fermi level $E_F=25$ meV and the z-axis Fermi velocity $v_z = 0.3 text{ eV} AA$ associated with the heavy bismuth Dirac band. At high energies above the $Gamma$-point Lifshitz gap energy, a frequency and temperature independent $epsilon_2$ indicative of Dirac cone interband transitions translates into an ab-plane Fermi velocity of $3 text{ eV} AA$. The observed number of IR phonons rules out the $text{P}6_3text{/mmc}$ space group symmetry but is consistent with the $text{P}bar{3}text{c}1$ candidate symmetry. A plasmaron excitation is discovered near the plasmon energy that persists over a broad range of temperature. The optical signature of the large joint density of states arising from saddle points at $Gamma$ is strongly suppressed in Na$_3$Bi consistent with band structure calculations that show the dipole transition matrix elements to be weak due to the very small s-orbital character of the Dirac bands. In Cd$_3$As$_2$, a distinctive peak in reflectivity due to the logarithmic divergence in $epsilon_1$ expected at the onset of Dirac cone interband transitions is identified. The center frequency of the peak shifts with temperature quantitatively consistent with a linear dispersion and a carrier density of $n=1.3times10^{17}text{ cm}^{-3}$. The peak width gives a measure of the Fermi velocity anisotropy of $10%$, indicating a nearly spherical Fermi surface. The lineshape gives an upper bound estimate of 7 meV for the potential fluctuation energy scale.
We investigate the non-equilibrium electronic structure and characteristic time scales in a candidate excitonic insulator, Ta$_2$NiSe$_5$, using time- and angle-resolved photoemission spectroscopy with a temporal resolution of 50 fs. Following a strong photoexcitation, the band gap closes transiently within 100 fs, i.e., on a time scale faster than the typical lattice vibrational period. Furthermore, we find that the characteristic time associated with the rise of the photoemission intensity above the Fermi energy decreases with increasing excitation strength, while the relaxation time of the electron population towards equilibrium shows an opposite behaviour. We argue that these experimental observations can be consistently explained by an excitonic origin of the band gap in the material. The excitonic picture is supported by microscopic calculations based on the non-equilibrium Greens function formalism for an interacting two-band system. We interpret the speedup of the rise time with fluence in terms of an enhanced scattering probability between photo-excited electrons and excitons, leading to an initially faster decay of the order parameter. We show that the inclusion of electron-phonon coupling at a semi-classical level changes only the quantitative aspects of the proposed dynamics, while the qualitative features remain the same. The experimental observations and microscopic calculations allow us to develop a simple and intuitive phenomenological model that captures the main dynamics after photoexcitation in Ta$_2$NiSe$_5$.
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