Nonlinear Optical Response in two-dimensional Mott Insulators

We study the third-order nonlinear optical susceptibility $\chi^{(3)}$ and photoexcited states of two-dimensional (2D) Mott insulators by using an effective model in the strong-coupling limit of a half-filled Hubbard model. In the numerically exact diagonalization calculations on finite-size clusters, we find that the coupling of charge and spin degrees of freedom plays a crucial role in the distribution of the dipole-allowed states with odd parity and the dipole-forbidden states with even parity in the photoexcited states. This is in contrast with the photoexcited states in one dimension, where the charge and spin degrees of freedom are decoupled. In the third-harmonic generation (THG) spectrum, main contribution is found to come from the process of three-photon resonance associated with the odd-parity states. As a result, the two-photon resonance process is less pronounced in the THG spectrum. The calculated THG spectrum is compared with recent experimental data. We also find that $\chi^{(3)}$ with cross-polarized configuration of pump and probe photons shows spectral distributions similar to $\chi^{(3)}$ with co-polarized configuration, although the weight is small. These findings will help the analyses of the experimental data of $\chi^{(3)}$ in the 2D Mott insulators.Comment: 9 pages,5 figures,RevTeX

Temperature dependent dynamics of photoexcited carriers of Si2Te3 nanowires

We report an optical study of the dynamics of photoexcited carriers in Si2Te3 nanowires at various temperatures and excitation powers. Si2Te3 nanowires were synthesized, by using gold as a catalyst, on a silicon substrate by the chemical vapor deposition method. The photoluminescence spectrum of Si2Te3 nanowires was primary dominated by defect and surface states related emission at both low and room temperatures. We observed that the decay time of photoexcited carries was very long (> 10 ns) at low temperatures and became shorter (< 2 ns) at room temperature. Further, the carrier decay time became faster at high excitation rates. The acceleration of the photoexcited carrier decay rates indicate the thermal quenching along with the non-radiative recombination at high temperature and excitation power. Our results have quantitatively elucidated decay mechanisms that are important towards understanding and controlling of the electronic states in Si2Te3 nanostructures for optoelectronic applications.Comment: 12 pages, 4 figures, submitte

Photoexcitation of electron wave packets in quantum spin Hall edge states: effects of chiral anomaly from a localised electric pulse

We show that, when a spatially localised electric pulse is applied at the edge of a quantum spin Hall system, electron wavepackets of the helical states can be photoexcited by purely intra-branch electrical transitions, without invoking the bulk states or the magnetic Zeeman coupling. In particular, as long as the electric pulse remains applied, the photoexcited densities lose their character of right- and left-movers, whereas after the ending of the pulse they propagate in opposite directions without dispersion, i.e. maintaining their space profile unaltered. Notably we find that, while the momentum distribution of the photoexcited wave packets depends on the temperature $T$ and the chemical potential $\mu$ of the initial equilibrium state and displays a non-linear behavior on the amplitude of the applied pulse, in the mesoscopic regime the space profile of the wave packets is independent of $T$ and $\mu$. Instead, it depends purely on the applied electric pulse, in a linear manner, as a signature of the chiral anomaly characterising massless Dirac electrons. We also discuss how the photoexcited wave packets can be tailored with the electric pulse parameters, for both low and finite frequencies.Comment: 15 pages, 5 figure

Dynamics of photoexcited states in one-dimensional dimerized Mott insulators

Dynamical properties of photoexcited states are theoretically studied in a one-dimensional Mott insulator dimerized by the spin-Peierls instability. Numerical calculations combined with a perturbative analysis have revealed that the lowest photoexcited state without nearest-neighbor interaction corresponds to an interdimer charge transfer excitation that belongs to dispersive excitations. This excited state destabilizes the dimerized phase, leading to a photoinduced inverse spin-Peierls transition. We discuss the purely electronic origin of midgap states that are observed in a latest photoexcitation experiment of an organic spin-Peierls compound, K-TCNQ (potassium-tetracyanoquinodimethane).Comment: 13 pages, 13 figures, accepted for publication in PR

Photoinduced metallic properties of one-dimensional strongly correlated electron systems

We study photoinduced optical responses of one-dimensional strongly correlated electron systems. The optical conductivity spectra are calculated for the ground state and a photoexcited state in the one-dimensional Hubbard model at half filling by using the exact diagonalization method. It is found that, in the Mott insulator phase, the photoexcited state has large spectral weights including the Drude weight below the optical gap. As a consequence, the spectral weight above the optical gap is largely reduced. These results imply that a metallic state is induced by photoexcitation. Comparison between the photoexcited and hole-doped states shows that the photoexcitation is similar to chemical doping.Comment: 4 pages, 4 figures, submitted to J. Phys. Soc. Jp

Observation of Competing Order in a High-TcT_{c} Superconductor with Femtosecond Optical Pulses

We present studies of the photoexcited quasiparticle dynamics in Tl$_{2}$Ba$_{2}$Ca$_{2}$Cu$_{3}$O$_{y}$ (Tl-2223) using femtosecond optical techniques. Deep into the superconducting state (below 40 K), a dramatic change occurs in the temporal dynamics associated with photoexcited quasiparticles rejoining the condensate. This is suggestive of entry into a coexistence phase which, as our analysis reveals, opens a gap in the density of states (in addition to the superconducting gap), and furthermore, competes with superconductivity resulting in a depression of the superconducting gap.Comment: 5 pages, 3 figure

Effect of Mn doping on ultrafast carrier dynamics in thin films of the topological insulator Bi2Se3

Transient reflectivity (TR) measured at laser photon energy 1.51 eV from the indirectly intersurface coupled topological insulator Bi2-xMnxSe3 films (12 nm thick) revealed a strong dependence of the rise-time and initial decay-time constants on photoexcited carrier density and Mn content. In undoped samples (x = 0), these time constants are exclusively governed by electron-electron and electron-phonon scattering, respectively, whereas in films with x = 0.013 - 0.27 ultrafast carrier dynamics are completely controlled by photoexcited electron trapping by ionized Mn2+ acceptors and their dimers. The shortest decay-time (~0.75 ps) measured for the film with x = 0.27 suggests a great potential of Mn-doped Bi2Se3 films for applications in high-speed optoelectronic devices. Using Raman spectroscopy exploiting similar laser photon energy (1.58 eV), we demonstrate that due to indirect intersurface coupling in the films, the photoexcited electron trapping in the bulk enhances the electron-phonon interaction strength in Dirac surface states