Hubbard exciton revealed by time-domain optical spectroscopy

We use broadband ultra-fast pump-probe spectroscopy in the visible range to study the lowest excitations across the Mott-Hubbard gap in the orbitally ordered insulator YVO3. Separating thermal and non-thermal contributions to the optical transients, we show that the total spectral weight of the two lowest peaks is conserved, demonstrating that both excitations correspond to the same multiplet. The pump-induced transfer of spectral weight between the two peaks reveals that the low-energy one is a Hubbard exciton, i.e. a resonance or bound state between a doublon and a holon. Finally, we speculate that the pump-driven spin-disorder can be used to quantify the kinetic energy gain of the excitons in the ferromagnetic phase.Comment: 5 pages and 6 figures, 9 pages and 12 figures with additional material

Pulsed homodyne Gaussian quantum tomography with low detection efficiency

Pulsed homodyne quantum tomography usually requires a high detection efficiency limiting its applicability in quantum optics. Here, it is shown that the presence of low detection efficiency ($<50\%$) does not prevent the tomographic reconstruction of quantum states of light, specifically, of Gaussian type. This result is obtained by applying the so-called "minimax" adaptive reconstruction of the Wigner function to pulsed homodyne detection. In particular, we prove, by both numerical and real experiments, that an effective discrimination of different Gaussian quantum states can be achieved. Our finding paves the way to a more extensive use of quantum tomographic methods, even in physical situations in which high detection efficiency is unattainable

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.Comment: 9 pages, 4 figure

Ultrafast Dynamics of Massive Dirac Fermions in Bilayer Graphene

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tuneable band gap. However, no consistent picture of the gap's effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second sub-state of the conduction band, in which the excited electrons decay through fast, phonon-assisted inter-band transitions.Comment: 5 pages, 4 figure

Ultrafast light-driven optical rotation and hidden orders in bulk WSe2_2

Single-layer semiconducting transition-metal dichalcogenides, lacking point inversion symmetry, provide an efficient platform for valleytronics, where the electronic, magnetic, valley and lattice degrees of freedom can be selectively manipulated by using polarized light. This task is however thought to be limited in parent bulk compounds where the point inversion symmetry is restored. Exploiting the underlying quantum physics in bulk materials is thus one of the biggest paradigmatic challenges. Here we show that a sizable optical Kerr rotation can be efficiently generated in a wide energy range on ultrafast timescales in bulk WSe$_2$, by means of circularly-polarized light. We rationalize these findings as a result of the hidden spin/layer/valley quantum entanglement. The spectral analysis reveals clear features at the three characteristic frequencies corresponding to the A-, B- and C-exciton edges. The origin and the relative sign of all these features is shown to stem from the selective Pauli blocking of intralayer and interlayer optical transitions. The long lifetime of the broadband Kerr response ($\tau \sim 500$ fs) provides a strong indication that coupled photo-induced electron and hole densities survive in bulk compounds longer than previously expected. The present report demonstrates that a hidden quantum entanglement is operative also in bulk centrosymmetric layered materials, opening the way for an effective exploitation of bulk WSe$_2$ in optoelectronic applications

Ultrafast light-driven optical rotation and hidden orders in bulk WSe2_2

Single-layer semiconducting transition-metal dichalcogenides, lacking point inversion symmetry, provide an efficient platform for valleytronics, where the electronic, magnetic, valley and lattice degrees of freedom can be selectively manipulated by using polarized light. This task is however thought to be limited in parent bulk compounds where the point inversion symmetry is restored. Exploiting the underlying quantum physics in bulk materials is thus one of the biggest paradigmatic challenges. Here we show that a sizable optical Kerr rotation can be efficiently generated in a wide energy range on ultrafast timescales in bulk WSe$_2$, by means of circularly-polarized light. We rationalize these findings as a result of the hidden spin/layer/valley quantum entanglement. The spectral analysis reveals clear features at the three characteristic frequencies corresponding to the A-, B- and C-exciton edges. The origin and the relative sign of all these features is shown to stem from the selective Pauli blocking of intralayer and interlayer optical transitions. The long lifetime of the broadband Kerr response ($\tau \sim 500$ fs) provides a strong indication that coupled photo-induced electron and hole densities survive in bulk compounds longer than previously expected. The present report demonstrates that a hidden quantum entanglement is operative also in bulk centrosymmetric layered materials, opening the way for an effective exploitation of bulk WSe$_2$ in optoelectronic applications

Sub-nanosecond free carrier recombination in an indirectly excited quantum-well heterostructure

Nanometer-thick quantum-well structures are quantum model systems offering a few discrete unoccupied energy states that can be impulsively filled and that relax back to equilibrium predominantly via spontaneous emission of light. Here we report on the response of an indirectly excited quantum-well heterostructure, probed by means of time and frequency resolved photoluminescence spectroscopy. This experiment provides access to the sub-nanosecond evolution of the free electron density, indirectly injected in the quantum-wells. In particular, the modelling of the time-dependent photoluminescence spectra unveils the time evolution of the temperature and of the chemical potentials for electrons and holes, from which the sub-nanosecond time-dependent electron density is determined. This information allows to prove that the recombination of excited carriers is mainly radiative and bimolecular at early delays after excitation, while, as the carrier density decreases, a monomolecular and non-radiative recombination channel becomes relevant. Access to the sub-nanosecond chronology of the mechanisms responsible for the relaxation of charge carriers provides a wealth of information for designing novel luminescent devices with engineered spectral and temporal behavior

Ultrafast Band Structure Dynamics in Bulk 1TT-VSe2_2

Complex materials encompassing different phases of matter can display new photoinduced metastable states differing from those attainable under equilibrium conditions. These states can be realized when energy is injected in the material following a non-equilibrium pathway, unbalancing the unperturbed energy landscape of the material. Guided by the fact that photoemission experiments allow for detailed insights in the electronic band structure of ordered systems, here we study bulk 1T-VSe$_2$ in its metallic and charge-density-wave phase by time- and angle-resolved photoelectron spectroscopy. After near-infrared optical excitation, the system shows a net increase of the density of states in the energy range of the valence bands, in the vicinity of the Fermi level, lasting for several picoseconds. We discuss possible origins as band shifts or correlation effects on the basis of a band structure analysis. Our results uncover the possibility of altering the electronic band structure of bulk 1T-VSe$_2$ for low excitation fluences, contributing to the understanding of light-induced electronic states

Strain-induced enhancement of the charge-density-wave in the kagome metal ScV6_6Sn6_6

The kagome geometry is an example of frustrated configuration in which rich physics takes place, including the emergence of superconductivity and charge density wave (CDW). Among the kagome metals, ScV$_6$Sn$_6$ hosts an unconventional CDW, with its electronic order showing a different periodicity than that of the phonon which generates it. In this material, a CDW-softened flat phonon band has a second-order collapse at the same time that the first order transition occurs. This phonon band originates from the out-of-plane vibrations of the Sc and Sn atoms, and it is at the base of the electron-phonon-coupling driven CDW phase of ScV$_6$Sn$_6$. Here, we use uniaxial strain to tune the frequency of the flat phonon band, tracking the strain evolution via time-resolved optical spectroscopy and first-principles calculations. Our findings emphasize the capability to induce an enhancement of the unconventional CDW properties in ScV$_6$Sn$_6$ kagome metal through control of strain.Comment: Main text + S

Quasi-particles dynamics in underdoped Bi2212 under strong optical perturbation.

In this work an optical pump-probe set-up is used to study the photo-induced non-equilibrium dynamics of a superconducting underdoped Bi2212 single crystal in a strong excitation regime (10<<600 \ub5J/cm2). The use of a tunable repetition rate 120 fs pulsed laser source allows us to avoid significant average heating of the sample and to optimize the signal-to-noise ratio in the detection of the transient reflectivity variation. A discontinuity of the transient reflectivity is observed at high excitation intensities (~70 \ub5J/cm2). Numerical simulations of the heat diffusion problem indicate that, in this regime, the local temperature of the sample is lower than TC, confirming the impulsive nature of this phenomenon. The quasi-particles (QP) dynamics in the strongly perturbed superconducting state (10<<70 \ub5J/cm2) is analysed within the framework of the Rotwarf-Taylor model. The picture emerging from the data is consistent with a dynamics governed by high-frequency phonon (HFP) population, which causes a bottleneck effect in the QP recombinatio