Mid-infrared Kerr index evaluation via cross-phase modulation with a near-infrared probe beam

We propose a simple method to measure nonlinear Kerr refractive index in mid-infrared frequency range that avoids using sophisticated infrared detectors. Our approach is based on using a near-infrared probe beam which interacts with a mid-IR beam via wavelength-non-degenerate cross-phase modulation (XPM). By carefully measuring XPM-induced spectral modifications in the probe beam and comparing the experimental data with simulation results we extract the value for the non-degenerate Kerr index. Finally, in order to obtain the value of degenerate mid-IR Kerr index we use the well-established two-band formalism of Sheik-Bahae et al., which is shown to become particularly simple in the limit of low frequencies. The proposed technique is complementary to the conventional techniques such as z-scan and has the advantage of not requiring any mid-infrared detectors

Dispersive effects in ultrafast non-linear phenomena

It is a basic principle that an effect cannot come before the cause. Dispersive relations that follow from this fundamental fact have proven to be an indispensable tool in physics and engineering. They are most powerful in the domain of linear response where they are known as Kramers-Kronig relations. However when it comes to nonlinear phenomena the implications of causality are much less explored, apart from several notable exceptions. Here in this work we demonstrate how to apply the dispersive formalism to analyse the ultrafast nonlinear response in the context of the paradigmatic nonlinear Kerr effect. We find that the requirement of causality introduces a noticeable effect even under assumption that Kerr effect is mediated by quasi-instantaneous off-resonant electronic hyperpolarizability. We confirm this by experimentally measuring the time resolved Kerr dynamics in GaAs by means of a hybrid pump-probe Mach-Zehnder interferometer and demonstrate the presence of an intrinsic lagging between amplitude and phase responses as predicted by dispersive analysis. Our results describe a general property of the time-resolved nonlinear processes thereby highlighting the importance of accounting for dispersive effects in the nonlinear optical processes involving ultrashort pulses

Confinement-Deconfinement Transition as an Indication of Spin-Liquid-Type Behavior in Na2_2IrO3_3

We use ultrafast optical spectroscopy to observe binding of charged single-particle excitations (SE) in the magnetically frustrated Mott insulator Na$_2$IrO$_3$. Above the antiferromagnetic ordering temperature ($T_N$) the system response is due to both Hubbard excitons (HE) and their constituent unpaired SE. The SE response becomes strongly suppressed immediately below $T_N$. We argue that this increase in binding energy is due to a unique interplay between the frustrated Kitaev and the weak Heisenberg-type ordering term in the Hamiltonian, mediating an effective interaction between the spin-singlet SE. This interaction grows with distance causing the SE to become trapped in the HE, similar to quark confinement inside hadrons. This binding of charged particles, induced by magnetic ordering, is a result of a confinement-deconfinement transition of spin excitations. This observation provides evidence for spin liquid type behavior which is expected in Na$_2$IrO$_3$.Comment: 5 pages, 3 figure

The origin of exciton mass in a frustrated Mott insulator Na2_2IrO3_3

We use a three-pulse ultrafast optical spectroscopy to study the relaxation processes in a frustrated Mott insulator Na$_2$IrO$_3$. By being able to independently produce the out-of-equilibrium bound states (excitons) of doublons and holons with the first pulse and suppress the underlying antiferromagnetic order with the second one, we were able to elucidate the relaxation mechanism of quasiparticles in this system. By observing the difference in the exciton dynamics in the magnetically ordered and disordered phases we found that the mass of this quasiparticle is mostly determined by its interaction with the surrounding spins

Confinement-Deconfinement Transition as an Indication of Spin-Liquid-Type Behavior in Na\u3csub\u3e2\u3c/sub\u3eIrO\u3csub\u3e3\u3c/sub\u3e

We use ultrafast optical spectroscopy to observe binding of charged single-particle excitations (SE) in the magnetically frustrated Mott insulator Na2IrO3. Above the antiferromagnetic ordering temperature (TN) the system response is due to both Hubbard excitons (HE) and their constituent unpaired SE. The SE response becomes strongly suppressed immediately below TN. We argue that this increase in binding energy is due to a unique interplay between the frustrated Kitaev and the weak Heisenberg-type ordering term in the Hamiltonian, mediating an effective interaction between the spin-singlet SE. This interaction grows with distance causing the SE to become trapped in the HE, similar to quark confinement inside hadrons. This binding of charged particles, induced by magnetic ordering, is a result of a confinement-deconfinement transition of spin excitations. This observation provides evidence for spin liquid type behavior which is expected in Na2IrO3

STM imaging of a bound state along a step on the surface of the topological insulator Bi2_2Te3_3

Detailed study of the LDOS associated with the surface-state-band near a step-edge of the strong topological-insulator Bi2Te3, reveal a one-dimensional bound state that runs parallel to the stepedge and is bound to it at some characteristic distance. This bound state is clearly observed in the bulk gap region, while it becomes entangled with the oscillations of the warped surface band at high energy, and with the valence band states near the Dirac point. Using the full effective Hamiltonian proposed by Zhang et al., we obtain a closed formula for this bound state that fits the data and provide further insight into the general topological properties of the electronic structure of the surface band near strong structural defects.Comment: 5 pages, 4 figure

Disorder enabled band structure engineering of a topological insulator surface

Three dimensional topological insulators are bulk insulators with $\mathbf{Z}_2$ topological electronic order that gives rise to conducting light-like surface states. These surface electrons are exceptionally resistant to localization by non-magnetic disorder, and have been adopted as the basis for a wide range of proposals to achieve new quasiparticle species and device functionality. Recent studies have yielded a surprise by showing that in spite of resisting localization, topological insulator surface electrons can be reshaped by defects into distinctive resonance states. Here we use numerical simulations and scanning tunneling microscopy data to show that these resonance states have significance well beyond the localized regime usually associated with impurity bands. At native densities in the model Bi$_2$X$_3$ (X=Bi, Te) compounds, defect resonance states are predicted to generate a new quantum basis for an emergent electron gas that supports diffusive electrical transport

STM imaging of impurity resonances on Bi2_2Se3_3

In this paper we present detailed study of the density of states near defects in Bi$_2$Se$_3$. In particular, we present data on the commonly found triangular defects in this system. While we do not find any measurable quasiparticle scattering interference effects, we do find localized resonances, which can be well fitted by theory once the potential is taken to be extended to properly account for the observed defects. The data together with the fits confirm that while the local density of states around the Dirac point of the electronic spectrum at the surface is significantly disrupted near the impurity by the creation of low-energy resonance state, the Dirac point is not locally destroyed. We discuss our results in terms of the expected protected surface state of topological insulators.Comment: 5 pages, 6 figure

Bond polarizability as a probe of local crystal fields in hybrid lead-halide perovskites

A rotating organic cation and a dynamically disordered soft inorganic cage are the hallmark features of hybrid organic-inorganic lead-halide perovskites. Understanding the interplay between these two subsystems is a challenging problem but it is this coupling that is widely conjectured to be responsible for the unique behaviour of photo-carriers in these materials. In this work, we use the fact that the polarizability of the organic cation strongly depends on the ambient electrostatic environment to put the molecule forward as a sensitive probe of local crystal fields inside the lattice cell. We measure the average polarizability of the C/N--H bond stretching mode by means of infrared spectroscopy, which allows us to deduce the character of the motion of the cation molecule, find the magnitude of the local crystal field and place an estimate on the strength of the hydrogen bond between the hydrogen and halide atoms. Our results pave the way for understanding electric fields in lead-halide perovskites using infrared bond spectroscopy

Effective model for studying optical properties of lead-halide perovskites

We use general symmetry-based arguments to construct an effective model suitable for studying optical properties of lead-halide perovskites. To build the model, we identify an atomic-level interaction between electromagnetic fields and the spin degree of freedom that should be added to a minimally-coupled $\mathbf{k\cdot p}$ Hamiltonian. As an application, we study two basic optical characteristics of the material: the Verdet constant and the refractive index