arXiv subjects

M. Chergui

Publications and source records attributed to M. Chergui.

10 recordsLinked to original sources

arXiv2024

Light-induced renormalization of the band structure of chiral tellurium

Chirality in tellurium derives from a Peierls distortion driven by strong electron-phonon coupling, making this material a unique candidate for observing a light-induced topological phase transition. By using time- and angle-resolved photoelectron spectroscopy (trARPES), we reveal that upon near-infrared photoexcitation the Peierls gap is modulated by displacively excited coherent phonons with $\mathrm{A_{1g}}$ symmetry as well as chiral-symmetry-breaking $\mathrm{E'_{LO}}$ modes. By comparison with state-of-the-art TDDFT+U calculations, we reveal the microscopic origin of the in-phase oscillations of band edges, due to phonon-induced modulation of the effective Hubbard $U$ term.

cond-mat.mtrl-sci↗

arXiv2023

Ultraviolet superradiance from mega-networks of tryptophan in biological architectures

Networks of tryptophan -- an aromatic amino acid with strong fluorescent response -- are ubiquitous in biological systems, forming diverse architectures in transmembrane proteins, cytoskeletal filaments, sub-neuronal elements, photoreceptor complexes, virion capsids, and other cellular structures. We analyze the cooperative effects induced by ultraviolet (UV) excitation of several biologically relevant tryptophan mega-networks, thus giving insight into novel mechanisms for cellular signalling and control. Our theoretical analysis in the single-excitation manifold predicts the formation of strongly superradiant states due to collective interactions among organized arrangements of up to more than $10^5$ tryptophan UV-excited transition dipoles in microtubule architectures, which leads to an enhancement of the fluorescence quantum yield that is confirmed by our experiments. We demonstrate the observed consequences of this superradiant behavior in the fluorescence quantum yield for hierarchically organized tubulin structures, which increases in different geometric regimes at thermal equilibrium before saturation -- highlighting the effect's persistence in the presence of disorder.

quant-ph↗

arXiv2020

Strain Wave Pathway to Semiconductor-to-Metal Transition revealed by time resolved X-ray powder diffraction

Thanks to the remarkable developments of ultrafast science, one of today's challenges is to modify material state by controlling with a light pulse the coherent motions that connect two different phases. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a macroscopic transformation pathway for the semiconducting-to-metal transition with large volume change in bistable Ti$_3$O$_5$ nanocrystals. Femtosecond powder X-ray diffraction allowed us to quantify the structural deformations associated with the photoinduced phase transition on relevant time scales. We monitored the early intra-cell distortions around absorbing metal dimers, but also long range crystalline deformations dynamically governed by acoustic waves launched at the laser-exposed Ti$_3$O$_5$ surface. We rationalize these observations with a simplified elastic model, demonstrating that a macroscopic transformation occurs concomitantly with the propagating acoustic wavefront on the picosecond timescale, several decades earlier than the subsequent thermal processes governed by heat diffusion.

cond-mat.mtrl-sci↗

arXiv2019

Light-induced renormalization of the Dirac quasiparticles in the nodal-line semimetal ZrSiSe

In nodal-line semimetals linearly dispersing states form Dirac loops in the reciprocal space, with high degree of electron-hole symmetry and almost-vanishing density of states near the Fermi level. The result is reduced electronic screening and enhanced correlations between Dirac quasiparticles. Here we investigate the electronic structure of ZrSiSe, by combining time- and angle-resolved photoelectron spectroscopy with ab initio density functional theory (DFT) complemented by an extended Hubbard model (DFT +U +V). We show that electronic correlations are reduced on an ultrashort timescale by optical excitation of high-energy electrons-hole pairs, which transiently screen the Coulomb interaction. Our findings demonstrate an all-optical method for engineering the band structure of a quantum material.

cond-mat.str-el↗

arXiv2019

Evidence of large polarons in photoemission band mapping of the perovskite semiconductor CsPbBr$_3$

Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic structure of the inorganic LHP CsPbBr$_3$ by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass $0.26\pm0.02\,\,m_e$, 50% heavier than the bare mass $m_0 =0.17 m_e$ predicted by density functional theory. Calculations of electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fr\"ohlich coupling parameter $\alpha=1.82$. A good agreement with our experimental data is obtained within the Feynmann polaron model, validating a viable theorical method to predict the carrier effective mass of LHPs ab-initio.

cond-mat.mtrl-sci↗

arXiv2019

X-ray Absorption Linear Dichroism at the Ti K-edge of TiO2 anatase single crystals

Anatase TiO2 (a-TiO2) exhibits a strong X-ray absorption linear dichroism with the X-ray incidence angle in the pre-edge, the XANES and the EXAFS at the titanium K-edge. In the pre-edge region the behaviour of the A1-A3 and B peaks, originating from the 1s-3d transitions, is due to the strong $p$-orbital polarization and strong $p-d$ orbital mixing. An unambiguous assignment of the pre-edge peak transitions is made in the monoelectronic approximation with the support of ab initio finite difference method calculations and spherical tensor analysis in quantitative agreement with the experiment. It is found that A1 is mostly an on-site 3d-4p hybridized transition, while peaks A3 and B are non-local transitions, with A3 being mostly dipolar and influence by the 3d-4p intersite hybridization, while B is due to interactions at longer range. Finally, peak A2 which was previously assigned to a transition involving pentacoordinated titanium atoms exhibits a quadrupolar angular evolution with incidence angle. These results pave the way to the use of the pre-edge peaks at the K-edge of a-TiO2 to characterize the electronic structure of related materials and in the field of ultrafast XAS where the linear dichroism can be used to compare the photophysics along different axes.

cond-mat.mtrl-sci↗

arXiv2018

Observation of a phonon avalanche in highly photoexcited hybrid perovskite single crystals

In hybrid lead halide perovskites, the coupling between photogenerated charges and the ionic degrees of freedom plays a crucial role in defining the intrinsic limit of carrier mobility and lifetime. However, direct investigation of this fundamental interaction remains challenging because its relevant dynamics occur on ultrashort spatial and ultrafast temporal scales. Here, we unveil the coupled electron-lattice dynamics of a CH3NH3PbI3 single crystal upon intense photoexcitation through a unique combination of ultrafast electron diffraction, time-resolved photoelectron spectroscopy, and time-dependent ab initio calculations. We observe the structural signature of a hot-phonon bottleneck effect that prevents rapid carrier relaxation, and we uncover a phonon avalanche mechanism responsible for breaking the bottleneck. The avalanche involves a collective emission of low-energy phonons - mainly associated with the organic sub-lattice - that proceeds in a regenerative manner and correlates with the accumulation and confinement of photocarriers at the crystal surface. Our results indicate that in hybrid perovskites carrier transport and spatial confinement are key to controlling the electron-phonon interaction and their rational engineering is relevant for future applications in optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2014

Temperature-dependent electron-phonon coupling in La$_{2-x}$Sr$_x$CuO$_4$ probed by femtosecond X-ray diffraction

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their re-equilibration by monitoring the transient lattice temperature through femtosecond X-ray diffraction in La$_{2-x}$Sr$_x$CuO$_4$ single crystals with $x$=0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the \textit{ab-initio} calculated shape of the electronic density-of-states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular in superconductors.

cond-mat.supr-con↗

arXiv2013

Coupling of a high-energy excitation to superconducting quasiparticles in a cuprate from Coherent Charge Fluctuation Spectroscopy

Dynamical information on spin degrees of freedom of proteins or solids can be obtained by Nuclear Magnetic Resonance (NMR) and Electron Spin Resonance (ESR). A technique with similar versatility for charge degrees of freedom and their ultrafast correlations could move forward the understanding of systems like unconventional superconductors. By perturbing the superconducting state in a high-Tc cuprate using a femtosecond laser pulse, we generate coherent oscillations of the Cooper pair condensate which can be described by an NMR/ESR formalism. The oscillations are detected by transient broad-band reflectivity and found to resonate at the typical scale of Mott physics (2.6 eV), suggesting the existence of a non-retarded contribution to the pairing interaction, as in unconventional (non Migdal-Eliashberg) theories.

cond-mat.supr-con↗

arXiv2012

Evidence for a Peierls phase-transition in a three-dimensional multiple charge-density waves solid

The effect of dimensionality on materials properties has become strikingly evident with the recent discovery of graphene. Charge ordering phenomena can be induced in one dimension by periodic distortions of a material's crystal structure, termed Peierls ordering transition. Charge-density waves can also be induced in solids by strong Coulomb repulsion between carriers, and at the extreme limit, Wigner predicted that crystallization itself can be induced in an electrons gas in free space close to the absolute zero of temperature. Similar phenomena are observed also in higher dimensions, but the microscopic description of the corresponding phase transition is often controversial, and remains an open field of research for fundamental physics. Here, we photoinduce the melting of the charge ordering in a complex three-dimensional solid and monitor the consequent charge redistribution by probing the optical response over a broad spectral range with ultrashort laser pulses. Although the photoinduced electronic temperature far exceeds the critical value, the charge-density wave is preserved until the lattice is sufficiently distorted to induce the phase transition. Combining this result with it ab initio} electronic structure calculations, we identified the Peierls origin of multiple charge-density waves in a three-dimensional system for the first time.

cond-mat.str-el↗