Interband Excitation Research Articles

Temperature evolution of the photoexcited charge carriers dynamics in Ge/Si quantum dots

The kinetics of the photoinduced mid-infrared intraband hole absorption after the short interband excitation pulse has been studied in an dense array of surfactant-mediated Ge/Si(001) quantum dots. Absorption decay curves reveal two processes characterized by fast and slow decay times at low temperatures. A specific temperature evolution of the absorption transients was observed with the increase in temperature. A model of charge carrier kinetics has been developed based on the rate equation analysis. Measured transient characteristics of charge carriers are well described within this model. The energetic gap between two conduction band electron states within the quantum dots and the valence band energetic barrier at the quantum dot interface have been evaluated.

Fractionalized excitations in the partially magnetized spin liquid candidate YbMgGaO4

Quantum spin liquids (QSLs) are exotic states of matter characterized by emergent gauge structures and fractionalized elementary excitations. The recently discovered triangular lattice antiferromagnet YbMgGaO4 is a promising QSL candidate, and the nature of its ground state is still under debate. Here we use neutron scattering to study the spin excitations in YbMgGaO4 under various magnetic fields. Our data reveal a dispersive spin excitation continuum with clear upper and lower excitation edges under a weak magnetic field (H = 2.5 T). Moreover, a spectral crossing emerges at the Γ point at the Zeeman-split energy. The corresponding redistribution of the spectral weight and its field-dependent evolution are consistent with the theoretical prediction based on the inter-band and intra-band spinon particle-hole excitations associated with the Zeeman-split spinon bands, implying the presence of fractionalized excitations and spinon Fermi surfaces in the partially magnetized QSL state in YbMgGaO4.

In-situ Cl− ions formation during photocatalytic reaction of platinized nanocomposite for hydrogen generation

Platinised Titania is emerging as a promising catalyst for its chemical stability, large surface area, and good electronic charge transfer. It is one of the most efficient materials and has been studied over past few decades for photocatalytic hydrogen generation. Photodeposition of Pt nanoparticles on TiO2 surface enhances trapping of photoexcited electrons and restricts recombination process. In this article we explored the influence of chloride ion formed during in-situ photocatalytic process, on photocatalytic hydrogen generation by scavenging holes. Illumination under UV–Visible light (400 nm < λ < 700 nm) improves interband excitation and transfer of photogenerated electron to the conduction band of TiO2. Transmission electron microscopy (TEM) results reveal average particle size of Pt nanoparticle in the range of 10 nm with uniform distribution on TiO2 surface. In-situ photodeposition of Pt nanoparticle on TiO2 resulted in incredibly active photocatalyst for hydrogen generation due to in-situ generated Cl− ions. Also, to one of the highest reported (6.72%). The hydrogen evolution rate of 17 mmol h−1 with apparent quantum yield (AQE). The AQE significantly higher than that for catalyst under solar AM (1.5 G) illumination (0.04%).

Intrinsic lithium indium diselenide: Scintillation properties and defect states

A scintillating lithium indium diselenide (LISe) single crystal has recently been found to exhibit an eight-fold increase in its apparent light yield within 80 µm across the surface when excited by cold neutrons. The cause of this observation is currently unknown. In this paper, we report on our investigations to explain the previous observations of nonuniformity in scintillating LISe. Using a two-photon interband excitation instrument, we found that the lower and higher light yield regions “scintillate” at peak emission energies of 1.98 eV and 2.4 eV, respectively, and no region investigated exhibited both. Volumetric evaluation found a relatively uniform scintillation response in each region, verifying that the relatively flat spatial resolution of LISe substrates of varying thickness applied to neutron imaging is not from only near-surface scintillation mechanisms. Raman investigations indicate that the vibrational modes of the scintillating LISe substrate is somewhat different than that reported in literature, but no apparent difference between the two regions was observed. Using ToF-SIMS in each region, we found that the 1.98 eV emission region contains additional lithium, which is consistent with neutron absorption results. We suspect that the sharp transition in peak scintillation emission is due to a change in the charge state of Li-In antisites, but that the observed scintillation light yield and emission energy change is not directly correlated to crystal color. Qualitative comparison between the observed noise in the two-photon “scintillation” spectra indicates that the light yield between each region is not due to the quantum efficiency of the CCD used during cold neutron interrogation experiments, but an actual change in the light yield.

Time-dependent Hartree-Fock study of electron-hole interaction effects on high-order harmonic generation from periodic crystals

We investigate the multielectron effects on high-harmonic generation from solid-state materials using the time-dependent Hartree-Fock theory. We find qualitative change in harmonic spectra, in particular, multiple-plateau formation at significantly lower laser intensities than within the independent-electron approximation. We reveal its origin in terms of interband polarization, i.e, electron-hole polarization, enabling interband excitation at remote crystal momenta via Coulomb potential.

Transient localized surface plasmon induced by femtosecond interband excitation in gold nanoparticles

Localized surface plasmon resonance (LSPR) is essentially a collective oscillation of free electrons in nanostructured metals. Interband excitation may also produce conduction-band electrons above the Fermi level. However, a question here is whether these excited electrons can take part in plasmonic oscillation. To answer this question, femtosecond pump-probe measurements on gold nanoparticles were performed using interband excitation, where the pump pulse produced a large amount of electrons in the sp-conduction band and left holes in the d-band. Probing by transient absorption spectroscopy, we resolved an induced LSPR feature located at a red-shifted spectrum. This feature cannot be observed for a pumping photon energy lower than the threshold for interband transition. The commonly observed red-shift or broadening of LSPR spectrum due to electron-electron and electron-phonon scattering under strong optical excitation can be ruled out for understanding this feature by a comparison between the plasmonic dynamics at a pump above and below the interband-transition threshold. In particular, a “holding” time of about 1 ps was resolved for the interband-excitation-induced electrons to relax to the LSPR oscillation.

Features of the Current Flow in Injection Structures Based on PbSnTe:In Films

This paper reports a study of the current–voltage (I–V) features of the p-i-p structures based on Pb1–xSnxTe:In films with the tin content х ≈ 0.31 in which the metal–insulator transition occurs. It is shown that the photocurrent is the hole current under light interband excitation, and electron trapping is dominant. The experimental and theoretical data are compared.

Ultrafast Dynamics of Photoexcited Hot Carrier Generation and Injection in AgNWs@TiO2@GNS Nanostructures

The generation and injection of hot electrons in plasmonic nanostructures have received a wide-range potential application in the next generation of ultrafast nanophotonics as well as energy harvesting, storage and conversion. In many cases, the energetic carriers with high energy beyond Fermi level are desirable for photochemical reactions due to the tremendous efficient hot electron injection. However, directly electron–electron scattering lifetime observations have few reported and hot electrons generally suffer from a low generation efficiency in conventional plasmonic nanostructures. This paper reports on the fabrication of hybrid AgNWs@TiO2@Au core–shell nanostructures and the investigation of the ultrafast dynamics of their energetic carriers based on interband and intraband excitations through transient absorption spectroscopy measurements. Finally, the different electronic transition processes are discussed in terms of ultrafast decay response, which is necessary to design proper nanostructures a...

Band-to-Band Tunneling-Dominated Thermo-Enhanced Field Electron Emission from p-Si/ZnO Nanoemitters.

Thermo-enhancement is an effective way to achieve high performance field electron emitters, and enables the individually tuning on the emission current by temperature and the electron energy by voltage. The field emission current from metal or n-doped semiconductor emitter at a relatively lower temperature (i.e., < 1000 K) is less temperature sensitive due to the weak dependence of free electron density on temperature, while that from p-doped semiconductor emitter is restricted by its limited free electron density. Here, we developed full array of uniform individual p-Si/ZnO nanoemitters and demonstrated the strong thermo-enhanced field emission. The mechanism of forming uniform nanoemitters with well Si/ZnO mechanical joint in the nanotemplates was elucidated. No current saturation was observed in the thermo-enhanced field emission measurements. The emission current density showed about ten-time enhancement (from 1.31 to 12.11 mA/cm2 at 60.6 MV/m) by increasing the temperature from 323 to 623 K. The distinctive performance did not agree with the interband excitation mechanism but well-fit to the band-to-band tunneling model. The strong thermo-enhancement was proposed to be benefit from the increase of band-to-band tunneling probability at the surface portion of the p-Si/ZnO nanojunction. This work provides promising cathode for portable X-ray tubes/panel, ionization vacuum gauges and low energy electron beam lithography, in where electron-dose control at a fixed energy is needed.

Phase transition kinetics for a Bose Einstein condensate in a periodically driven band system

The dynamical transition of an atomic Bose–Einstein condensate from a spatially periodic state to a staggered state with alternating sign in its wavefunction is experimentally studied using a one-dimensional phase modulated optical lattice. We observe the crossover from quantum to thermal fluctuations as the triggering mechanism for the nucleation of staggered states. In good quantitative agreement with numerical simulations based on the truncated Wigner method, we experimentally investigate how the nucleation time varies with the renormalized tunneling rate, the atomic density, and the driving frequency. The effective inverted energy band in the driven lattice is identified as the key ingredient which explains the emergence of gap solitons as observed in numerics and the possibility to nucleate staggered states from interband excitations as reported experimentally.

Picosecond absorption spectroscopy of self-trapped excitons and transient Ce states in LaBr3 and LaBr3 :Ce

Picosecond time-resolved optical absorption spectra induced by two-photon interband excitation of ${\mathrm{LaBr}}_{3}$ are reported. The spectra are similar in general characteristics to self-trapped exciton (STE) absorption previously measured in alkali halides and alkaline-earth halides. A broad ultraviolet absorption band results from excitation of the self-trapped hole within the STE. A series of infrared and red-visible bands results from excitation of the bound outer electron within the STE similar to bands found in alkali halides corresponding to different degrees of ``off-center'' relaxation. Induced absorption in cerium-doped ${\mathrm{LaBr}}_{3}$ after band-gap excitation of the host exhibits similar STE spectra, except it decays faster on the tens-of-picoseconds scale in proportion to the Ce concentration. This is attributed to dipole-dipole energy transfer from STE to ${\mathrm{Ce}}^{3+}$ dopant ions. The absorption spectra were also measured after direct excitation of the ${\mathrm{Ce}}^{3+}$ ions with sufficient intensity to drive two- and three-photon resonantly enhanced excitation. In this case, the spectrum attributed to STEs created adjacent to ${\mathrm{Ce}}^{3+}$ ions decays in 1 ps suggesting dipole-dipole transfer from the nearest-neighbor separation. A transient absorption band at 2.1 eV growing with Ce concentration is found and attributed to a charge-transfer excitation of the ${\mathrm{Ce}}^{3+*}$ excited state responsible for scintillation in ${\mathrm{LaBr}}_{3}$:Ce crystals. This study concludes that the energy transport from host to activator responsible for the scintillation of ${\mathrm{LaBr}}_{3}$:Ce proceeds by STE creation and dipole-dipole transfer more than by sequential trapping of holes and electrons on ${\mathrm{Ce}}^{3+}$ ions.

Photocurrent characteristics of metal–AlGaN/GaN Schottky-on-heterojunction diodes induced by GaN interband excitation

The photocurrent characteristics of metal–AlGaN/GaN Schottky-on-heterojunction diodes were investigated. When the photon energy of incident light was larger than the bandgap of GaN but smaller than that of AlGaN, the alternating-current (ac) photocurrent measured using lock-in techniques increased with the chopper frequency. Analyzing the generation and flow processes of photocarriers revealed that the photocurrent induced by GaN interband excitation featured a transient behavior, and its direction reversed when the light excitation was removed. The abnormal dependence of the measured ac photocurrent magnitude on the chopper frequency was explained considering the detection principles of a lock-in amplifier.

Interband excitations in the 1D limit of two-band fractional Chern insulators

We investigate the stability of the one-dimensional limit of ν=1/3 Laughlin-like fractional Chern insulator with respect to the interband interaction. We propose a construction for the excitations in the infinite-interaction case and show that the energy gap remains finite in the thermodynamic limit. Next, by means of exact diagonalization and Density Matrix Renormalization Group approaches, we consider deviations from ideal dimerization and show that they reduce the stability of the FCI-like states. Finally, to show that our approach is not restricted to one model, we identify the dimer structure behind the thin-torus limit of other system – the checkerboard lattice.

Optical Conductivity in a Two-Dimensional Extended Hubbard Model for an Organic Dirac Electron System α-(BEDT-TTF)2I3

The optical conductivity in the charge order phase is calculated in the two-dimensional extended Hubbard model describing an organic Dirac electron system α -(BEDT-TTF) 2 I 3 using the mean field theory and the Nakano-Kubo formula. Because the interband excitation is characteristic in a two-dimensional Dirac electron system, a peak structure is found above the charge order gap. It is shown that the peak structure originates from the Van Hove singularities of the conduction and valence bands, where those singularities are located at a saddle point between two Dirac cones in momentum space. The frequency of the peak structure exhibits drastic change in the vicinity of the charge order transition.

Strong Quantum Confinement Effects and Chiral Excitons in Bio-Inspired ZnO–Amino Acid Cocrystals

Elucidating the underlying principles behind band gap engineering is paramount for the successful implementation of semiconductors in photonic and optoelectronic devices. Recently it has been shown that the band gap of a wide and direct band gap semiconductor, such as ZnO, can be modified upon co-crystallization with amino acids, with the role of the biomolecules remaining unclear. Here, by probing and modeling the light emitting properties of ZnO-amino acid co-crystals, we identify the amino acids role on this band gap modulation and demonstrate their effective chirality transfer to the inter-band excitations in ZnO. Our 3D quantum model suggests that the strong band edge emission blue shift in the co-crystals can be explained by a quasi-periodic distribution of amino acid potential barriers within the ZnO crystal lattice. Overall, our findings indicate that biomolecule co-crystallization can be used as a truly bio-inspired means to induce chiral quantum confinement effects in quasi-bulk semiconductors.

Electrically Active States of Charge Capture and Transfer Causing Slow Recombination in Thallium-Bromide Crystals at Low Temperatures

TlBr single crystals grown by the Bridgman–Stockbarger method are studied. It is established that frozen-conductivity effects manifest themselves under interband excitation by light at temperatures below 200 K. Herewith, clearly pronounced superlinear dependences of the induced photoconductivity on the strength of the applied electric field manifest themselves. The results of studying thermally stimulated conductivity evidence that these phenomena can be associated with the filling of trap states with thermal activation energies of 0.08–0.12 eV. This state can be removed due to thermal quenching at temperatures of ≳180 K because of the emptying of energy states with an activation energy of 0.63–0.65 eV filled after optical generation.

Optically adjustable valley Hall current in single-layer transition metal dichalcogenides

The illumination of a single-layer transition metal dichalcogenide with an elliptically polarized light beam is shown to give rise to a differential rate of inter-band carrier excitation between the valence and conduction states around the valley edges, K and K′. This rate with a linear dependence on the beam ellipticity and inverse of the optical gap manifests as an asymmetric Fermi distribution between the valleys or a non-equilibrium population which under an external field and a Berry curvature induced anomalous velocity, results in an externally tunable finite valley Hall current. Surface imperfections that influence the excitation rates are included through the self-consistent Born approximation. Further, we describe applications centered around circular dichroism, quantum computing, and spin torque via optically excited spin currents within the framework of the suggested formalism. A closing summary points to the possibility of extending the calculations to composite charged particles like trions. The role of the substrate in renormalizing the fundamental band gap and moderating the valley Hall current is also discussed.

Электрически активные состояния захвата и переноса заряда, обусловливающие медленную рекомбинацию в кристаллах бромида таллия при низких температурах

AbstractTlBr single crystals grown by the Bridgman–Stockbarger method are studied. It is established that frozen-conductivity effects manifest themselves under interband excitation by light at temperatures below 200 K. Herewith, clearly pronounced superlinear dependences of the induced photoconductivity on the strength of the applied electric field manifest themselves. The results of studying thermally stimulated conductivity evidence that these phenomena can be associated with the filling of trap states with thermal activation energies of 0.08–0.12 eV. This state can be removed due to thermal quenching at temperatures of ≳180 K because of the emptying of energy states with an activation energy of 0.63–0.65 eV filled after optical generation.

Effect of thermal treatment on ZnO:Tb3+ nano-crystalline thin films and application for spectral conversion in inverted organic solar cells.

Down conversion has been applied to minimize thermalization losses in photovoltaic devices. In this study, terbium-doped ZnO (ZnO:Tb3+) thin films were deposited on ITO-coated glass, quartz and silicon substrates using the RF magnetron sputtering technique fitted with a high-purity (99.99%) Tb3+-doped ZnO target (97% ZnO, 3% Tb) for use in organic solar cells as a bi-functional layer. A systematic study of the film crystallization dynamics was carried out through elevated temperature annealing in Ar ambient. The films were characterized using grazing incidence (XRD), Rutherford backscattering spectrometry (RBS), atomic force microscopy, and UV-visible transmittance and photoluminescence measurements at an excitation wavelength of 244 nm. The tunability of size and bandgap of ZnO:Tb3+ nanocrystals with annealing exhibited quantum confinement effects, which enabled the control of emission characteristics in ZnO:Tb3+. Energy transfer of ZnO → Tb3+ (5D3–7F5) was also observed from the photoluminescence (PL) spectra. At an inter-band resonance excitation of around 300–400 nm, a typical emission band from Tb3+ was obtained. The ZnO:Tb3+ materials grown on ITO-coated glass were then used as bi-functional layers in an organic solar cell based on P3HT:PCBM blend, serving as active layers in an inverted device structure. Energy transfer through down conversion between ZnO and Tb3+ led to enhanced absorption in P3HT:PCBM in the 300–400 nm range and subsequently augmented Jsc of a Tb3+-based device by 17%.

Population decay time and distribution of exciton states analyzed by rate equations based on theoretical phononic and electron-collisional rate coefficients

Population distributions and transition fluxes of the $A$ exciton in bulk GaN are theoretically analyzed using rate equations of states of the principal quantum number $n$ up to 5 and the continuum. These rate equations consist of the terms of radiative, electron-collisional, and phononic processes. The dependence of the rate coefficients on temperature is revealed on the basis of the collisional-radiative model of hydrogen plasma for the electron-collisional processes and theoretical formulation using Fermi's ``golden rule'' for the phononic processes. The respective effects of the variations in electron, exciton, and lattice temperatures are exhibited. This analysis is a base of the discussion on nonthermal equilibrium states of carrier-exciton-phonon dynamics. It is found that the exciton dissociation is enhanced even below 150 K mainly by the increase in the lattice temperature. When the thermal-equilibrium temperature increases, the population fluxes between the states of $ng1$ and the continuum become more dominant. Below 20 K, the severe deviation from the Saha-Boltzmann distribution occurs owing to the interband excitation flux being higher than the excitation flux from the $1S$ state. The population decay time of the $1S$ state at 300 K is more than ten times longer than the recombination lifetime of excitons with kinetic energy but without the upper levels $(ng1$ and the continuum). This phenomenon is caused by a shift of population distribution to the upper levels. This phonon-exciton-radiation model gives insights into the limitations of conventional analyses such as the ABC model, the Arrhenius plot, the two-level model $(n=1$ and the continuum), and the neglect of the upper levels.