arXiv subjects

M. Puppin

Publications and source records attributed to M. Puppin.

13 recordsLinked to original sources

arXiv2025

Floquet topological state induced by light-driven band inversion in SnTe

High intensity coherent light can dress matter, realizing new hybrid phases that are not accessible in equilibrium. This effect results from the coherent interaction between Bloch states inside the solid and the periodic field of impinging photons which produces hybrid light-matter states called Floquet-Bloch states that can alter properties of the solid. Optically inducing a topological state in a semiconductor using so-called Floquet engineering is an exciting prospect. However, it has not been realized, despite its theoretical prediction more than 10 years ago. Here we show that an ultrashort-lived topological state that is absent at equilibrium in the ground state of SnTe can be created with femtosecond light pulses. This occurs when the photoexcitation is similar in energy with the band gap of this polar semiconductor. We observe a concomitant renormalization of the band dispersions that reveals the generation of Floquet states connecting to the topological state. We therefore provide the first direct experimental observation of a Floquet topological state and propose that it is driven by a light-induced band inversion in SnTe. Our discovery opens the way for controlling optically on-demand the topological properties of semiconductors.

cond-mat.str-el↗

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↗

arXiv2024

Magneto-optical response of magnetic semiconductors EuCd2X2 (X= P, As, Sb)

In this study, we identify EuCd2X2 (for X = P, As, Sb) as a series of magnetic semiconductors. We examine how the band gap of the series responds to X changing from phosphorus (P), to arsenic (As), and finally antimony (Sb). We characterize the samples using electronic transport and magnetization measurements. Based on infrared spectroscopy, we find that the band gap reduces progressively from 1.23 eV in EuCd2P2, to 0.77 eV in EuCd2As2, and finally 0.52 eV in EuCd2Sb2. In a magnetic field, all three systems show a strong response and their band gaps decrease at 4 K. This decrease is non-monotonic as we change X. It is strongest in the phosphorous compound and weakest in the antimony compound. For all the three compositions, EuCd2X2 remains a semiconductor up to the highest magnetic field applied (16 T).

cond-mat.mtrl-sci↗

arXiv2023

EuCd$_2$As$_2$: a magnetic semiconductor

EuCd$_2$As$_2$ is now widely accepted as a topological semimetal in which a Weyl phase is induced by an external magnetic field. We challenge this view through firm experimental evidence using a combination of electronic transport, optical spectroscopy and excited-state photoemission spectroscopy. We show that the EuCd$_2$As$_2$ is in fact a semiconductor with a gap of 0.77 eV. We show that the externally applied magnetic field has a profound impact on the electronic band structure of this system. This is manifested by a huge decrease of the observed band gap, as large as 125~meV at 2~T, and consequently, by a giant redshift of the interband absorption edge. However, the semiconductor nature of the material remains preserved. EuCd$_2$As$_2$ is therefore a magnetic semiconductor rather than a Dirac or Weyl semimetal, as suggested by {\em ab initio} computations carried out within the local spin-density approximation.

cond-mat.mtrl-sci↗

arXiv2022

Coherent Modulation of Quasiparticle Scattering Rates in a Photoexcited Charge-Density-Wave System

We present a complementary experimental and theoretical investigation of relaxation dynamics in the charge-density-wave (CDW) system TbTe$_3$ after ultrafast optical excitation. Using time- and angle-resolved photoemission spectroscopy, we observe an unusual transient modulation of the relaxation rates of excited photocarriers. A detailed analysis of the electron self-energy based on a nonequilibrium Green's function formalism reveals that the phase space of electron-electron scattering is critically modulated by the photoinduced collective CDW excitation, providing an intuitive microscopic understanding of the observed dynamics and revealing the impact of the electronic band structure on the self-energy.

cond-mat.mtrl-sci↗

arXiv2021

Excited-state band structure mapping

Angle-resolved photoelectron spectroscopy is an extremely powerful probe of materials to access the occupied electronic structure with energy and momentum resolution. However, it remains blind to those dynamic states above the Fermi level that determine technologically relevant transport properties. In this work, we extend band structure mapping into the unoccupied states and across the entire Brillouin zone by using a state-of-the-art high repetition rate, extreme ultraviolet fem- tosecond light source to probe optically excited samples. The wide-ranging applicability and power of this approach are demonstrated by measurements on the 2D semiconductor WSe2, where the energy-momentum dispersion of valence and conduction bands are observed in a single experiment. This provides a direct momentum-resolved view not only on the complete out-of-equilibrium band gap but also on its renormalization induced by electron-hole interaction and screening. Our work establishes a new benchmark for measuring the band structure of materials, with direct access to the energy-momentum dispersion of the excited-state spectral function.

cond-mat.mtrl-sci↗

arXiv2021

Nonequilibrium Charge-Density-Wave Order Beyond the Thermal Limit

The interaction of many-body systems with intense light pulses may lead to novel emergent phenomena far from equilibrium. Recent discoveries, such as the optical enhancement of the critical temperature in certain superconductors and the photo-stabilization of hidden phases, have turned this field into an important research frontier. Here, we demonstrate nonthermal charge-density-wave (CDW) order at electronic temperatures far greater than the thermodynamic transition temperature. Using time- and angle-resolved photoemission spectroscopy and time-resolved X-ray diffraction, we investigate the electronic and structural order parameters of an ultrafast photoinduced CDW-to-metal transition. Tracking the dynamical CDW recovery as a function of electronic temperature reveals a behaviour markedly different from equilibrium, which we attribute to the suppression of lattice fluctuations in the transient nonthermal phonon distribution. A complete description of the system's coherent and incoherent order-parameter dynamics is given by a time-dependent Ginzburg-Landau framework, providing access to the transient potential energy surfaces.

cond-mat.mtrl-sci↗

arXiv2020

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↗

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 Fröhlich coupling parameter $α=1.82$. 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

Excited state band mapping and momentum-resolved ultrafast population dynamics in In/Si(111) nanowires investigated with XUV based time- and angle-resolved photoemission spectroscopy

We investigate the excited state electronic structure of the model phase transition system In/Si(111) using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) with an XUV laser source at 500 kHz . Excited state band mapping is used to characterize the normally unoccupied electronic structure above the Fermi level in both structural phases of indium nanowires on Si(111): the metallic (4x1) and the gapped (8x2) phases. The extracted band positions are compared with the band structure calculated using density functional theory (DFT) within both the LDA and GW approximations. While good overall agreement is found between the GW calculated band structure and experiment, deviations in specific momentum regions may indicate the importance of excitonic effects not accounted for at this level of approximation. To probe the dynamics of these excited states, their momentum-resolved transient population dynamics are extracted. The transient intensities are then simulated by a spectral function determined by a state population employing a transient elevated electronic temperature as determined experimentally. This allows the momentum-resolved population dynamics to be quantitatively reproduced, revealing important insights into the transfer of energy from the electronic system to the lattice. In particular, a comparison between the magnitude and relaxation time of the transient electronic temperature observed by trARPES with those of the lattice as probed in previous ultrafast electron diffraction studies imply a highly non-thermal phonon distribution at the surface following photo-excitation. This suggests the energy from the excited electronic system is initially transferred to high energy optical phonon modes followed by cooling and thermalization of the photo-excited system by much slower phonon-phonon coupling.

cond-mat.str-el↗

arXiv2019

Time- and angle-resolved photoemission spectroscopy of solids in the extreme ultraviolet at 500 kHz repetition rate

Time- and angle-resolved photoelectron spectroscopy (trARPES) employing a 500 kHz extreme-ultravioled (XUV) light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification (OPCPA), and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than $10^{11}$ photons/second on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynamics in occupied and normally unoccupied (excited) states in the entire Brillouin zone and with a temporal system response function below 40 fs.

physics.ins-det↗

arXiv2016

Revealing the role of electrons and phonons in the ultrafast recovery of charge density wave correlations in 1$T$-TiSe$_2$

Using time- and angle-resolved photoemission spectroscopy with selective near- and mid-infrared photon excitations, we investigate the femtosecond dynamics of the charge density wave (CDW) phase in 1$T$-TiSe$_2$, as well as the dynamics of CDW fluctuations at 240 K. In the CDW phase, we observe the coherent oscillation of the CDW amplitude mode. At 240 K, we single out an ultrafast component in the recovery of the CDW correlations, which we explain as the manifestation of electron-hole correlations. Our momentum-resolved study of femtosecond electron dynamics supports a mechanism for the CDW phase resulting from the cooperation between the interband Coulomb interaction, the mechanism of excitonic insulator phase formation, and electron-phonon coupling.

cond-mat.str-el↗