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Register a new userTime-resolved observation of band-gap shrinking and electron-lattice thermalization within X-ray excited gallium arsenide
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Femtosecond X-ray irradiation of solids excites energetic photoelectrons that thermalize on a timescale of a few hundred femtoseconds. The thermalized electrons exchange energy with the lattice and heat it up. Experiments with X-ray free-electron lasers have unveiled so far the details of the electronic thermalization. In this work we show that the data on transient optical reflectivity measured in GaAs irradiated with femtosecond X-ray pulses can be used to follow electron-lattice relaxation up to a few tens of picoseconds. With a dedicated theoretical framework, we explain the so far unexplained reflectivity overshooting as a result of band-gap shrinking. We also obtain predictions for a timescale of electron-lattice thermalization, initiated by conduction band electrons in the temperature regime of a few eVs. The conduction and valence band carriers were then strongly non-isothermal. The presented scheme is of general applicability and can stimulate further studies of relaxation within X-ray excited narrow band-gap semiconductors.
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We develop a theory of energy relaxation in semiconductors and insulators highly excited by the long-acting external irradiation. We derive the equation for the non-equilibrium distribution function of excited electrons. The solution for this function breaks up into the sum of two contributions. The low-energy contribution is concentrated in a narrow range near the bottom of the conduction band. It has the typical form of a Fermi distribution with an effective temperature and chemical potential. The effective temperature and chemical potential in this low-energy term are determined by the intensity of carriers generation, the speed of electron-phonon relaxation, rates of inter-band recombination and electron capture on the defects. In addition, there is a substantial high-energy correction. This high-energy tail covers largely the conduction band. The shape of the high-energy tail strongly depends on the rate of electron-phonon relaxation but does not depend on the rates of recombination and trapping. We apply the theory to the calculation of a non-equilibrium distribution of electrons in irradiated GaN. Probabilities of optical excitations from the valence to conduction band and electron-phonon coupling probabilities in GaN were calculated by the density functional perturbation theory. Our calculation of both parts of distribution function in gallium nitride shows that when the speed of electron-phonon scattering is comparable with the rate of recombination and trapping then the contribution of the non-Fermi tail is comparable with that of the low-energy Fermi-like component. So the high-energy contribution can affect essentially the charge transport in the irradiated and highly doped semiconductors.
The monolayer Gallium sulfide (GaS) was demonstrated as a promising two-dimensional semiconductor material with considerable band gaps. The present work investigates the band gap modulation of GaS monolayer under biaxial or uniaxial strain by using Density functional theory calculation. We found that GaS monolayer shows an indirect band gap that limits its optical applications. The results show that GaS monolayer has a sizable band gap. The uniaxial strain shifts band gap from indirect to direct in Gallium monochalcogenides (GaS). This behavior, allowing applications such as electroluminescent devices and laser. The detailed reasons for the band gap modulation are also discussed by analyzing the projected density of states (PDOS). It indicates that due to the role of p$_y$ orbital through uniaxial strain become more significant than others near the Fermi level. The indirect to direct band gap transition happen at $varepsilon$=-10y$%$. Moreover, by investigating the strain energy and transverse response of structures under uniaxial strain, we show that the GaS monolayer has the Poissons ratio of 0.23 and 0.24 in the zigzag (x) and armchair (y) directions, respectively. Thus, we conclude that the isotropic nature of mechanical properties under strain.
Structural and electronic properties of hypothetical zinc blende Tl(x)Ga(1-x)N alloys have been investigated from first principles. The structural relaxation, preformed within the LDA approach, leads to a linear dependence of the lattice parameter a on the Tl content x. In turn, band structures obtained by MBJLDA calculations are significantly different from the corresponding LDA results. The decrease of the band-gap in Tl-doped GaN materials (for x<0.25) is predicted to be a linear function of x, i.e. 0.08 eV per atomic % of thallium. The semimetallic character is expected for materials with x>0.5. The obtained spin-orbit coupling driven splitting between the heavy-hole and split-off band at the Gamma point of the Brillouin zone in Tl(x)Ga(1-x)N systems is significantly weaker when compared to that of Tl-doped InN materials.
The dilute magnetic semiconductors have promise in spin-based electronics applications due to their potential for ferromagnetic order at room temperature, and various unique switching and spin-dependent conductivity properties. However, the precise mechanism by which the transition-metal doping produces ferromagnetism has been controversial. Here we have studied a dilute magnetic semiconductor (5% manganese-doped gallium arsenide) with Bragg-reflection standing-wave hard X-ray angle-resolved photoemission spectroscopy, and resolved its electronic structure into element- and momentum- resolved components. The measured valence band intensities have been projected into element-resolved components using analogous energy scans of Ga 3d, Mn 2p, and As 3d core levels, with results in excellent agreement with element-projected Bloch spectral functions and clarification of the electronic structure of this prototypical material. This technique should be broadly applicable to other multi-element materials.
Eutectic related reaction is a special chemical/physical reaction involving multiple phases, solid and liquid. Visualization of phase reaction of composite nanomaterials with high spatial and temporal resolution provides a key understanding of alloy growth with important industrial applications. However, it has been a rather challenging task. Here we report the direct imaging and control of the phase reaction dynamics of a single, as-grown free-standing gallium arsenide nanowire encapped with a gold nanoparticle, free from environmental confinement or disturbance, using four-dimensional electron microscopy. The non-destructive preparation of as-grown free-standing nanowires without supporting films allows us to study their anisotropic properties in their native environment with better statistical character. A laser heating pulse initiates the eutectic related reaction at a temperature much lower than the melting points of the composite materials, followed by a precisely time-delayed electron pulse to visualize the irreversible transient states of nucleation, growth and solidification of the complex. Combined with theoretical modeling, useful thermodynamic parameters of the newly formed alloy phases and their crystal structures could be determined. This technique of dynamical control and 4D imaging of phase reaction processes on the nanometer-ultrafast time scale open new venues for engineering various reactions in a wide variety of other systems.
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