1. Uncovering the nature of transient and metastable nonequilibrium phases in 1T − ▫$TaS_2$ ▫Tanusree Saha, Arindam Pramanik, Barbara Ressel, Alessandra Ciavardini, Fabio Frassetto, Federico Galdenzi, Luca Poletto, Arun Ravindran, Primož Rebernik Ribič, Giovanni De Ninno, 2023, original scientific article Abstract: Complex systems are characterized by strong coupling between different microscopic degrees of freedom. Photoexcitation of such materials can drive them into new transient and metastable hidden phases that may not have any counterparts in equilibrium. By exploiting femtosecond time- and angle-resolved photoemission spectroscopy, we probe the photoinduced transient phase and the recovery dynamics of the ground state in a complex material: the charge density wave (CDW)–Mott insulator 1T-TaS2. We reveal striking similarities between the band structures of the transient phase and the (equilibrium) structurally undistorted metallic phase, with evidence for the coexistence of the low-temperature Mott insulating phase and high-temperature metallic phase. Following the transient phase, we find that the restorations of the Mott and CDW orders begin around the same time. This highlights that the Mott transition is tied to the CDW structural distortion, although earlier studies have shown that the collapses of Mott and CDW phases are decoupled from each other. Interestingly, as the suppressed order starts to recover, a metastable phase emerges before the material recovers to the ground state. Our results demonstrate that it is the CDW lattice order that drives the material into this metastable phase, which is indeed a commensurate CDW–Mott insulating phase but with a smaller CDW amplitude. Moreover, we find that the metastable phase emerges only under strong photoexcitation (∼3.6 mJ/cm2) and has no evidence when the photoexcitation strength is weak (∼1.2 mJ/cm2). Keywords: angle resolved photoemission, time resolved photoemission, 2D materials, charge density wave, Mott insulator Published in RUNG: 15.01.2024; Views: 1845; Downloads: 6 Full text (2,30 MB) This document has many files! More... |
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3. ULTRAFAST ELECTRON DYNAMICS IN CORRELATED SYSTEMS PROBED BY TIME-RESOLVED PHOTOEMISSION SPECTROSCOPYTanusree Saha, 2023, doctoral dissertation Abstract: Complex systems in condensed matter are characterized by strong coupling
between different degrees of freedom constituting a solid. In materials
described by many-body physics, these interactions may lead to
the formation of new ground states such as excitonic insulators, Mott
insulators, and charge and spin density waves. However, the inherent
complexity in such materials poses a challenge to identifying the
dominant interactions governing these phases using equilibrium studies.
Owing to the distinct timescales associated with the elementary interactions,
such complexities can be readily addressed in the non-equilibrium
regime. Additionally, these materials might also show the emergence
of new, metastable “hidden“ phases under non-equilibrium. The thesis
investigates the ultrafast timescales of fundamental interactions in candidate
systems by employing time-and angle-resolved photoemission spectroscopy
in the femtosecond time domain. In the (supposed) excitonic
insulator model system Ta2NiSe5, the timescale of band gap closure
and the dependence of rise time (of the photoemission signal) on the
photoexcitation strength point to a predominantly electronic origin of
the band gap at the Fermi level. The charge density wave (CDW) -
Mott insulator 1T-TaS2 undergoes photoinduced phase transition to two
different phases. The initial one is a transient phase which resembles
the systems’s high temperature equilibrium phase, followed by a long-lived
“hidden“ phase with a different CDW amplitude and is primarily
driven by the CDW lattice order. For the spin density wave system
CaFe2As2 where multiple bands contribute in the formation of Fermi surfaces,
selective photoexcitation was used to disentangle the role played
by different electron orbitals. By varying the polarization of photoexcitation
pulses, it is observed that dxz/dyz orbitals primarily contribute to
the magnetic ordering while the dxy orbitals have dominant role in the
structural order. The findings of the present study provide deeper perspectives
on the underlying interactions in complex ground phases of
matter, therefore, initiating further experimental and theoretical studies
on such materials. Keywords: complex systems, charge density wave, excitonic insulator, metastable phase, Mott insulator, non-equilibrium, spin density wave, timescales, time- and angle-resolved photoemission, ultrafast dynamics Published in RUNG: 01.06.2023; Views: 2582; Downloads: 39 Full text (13,34 MB) |
4. Experimental and Theoretical Photoemission Study of Indole and Its Derivatives in the Gas PhaseO. Plekan, H. Sa'adeh, A. Ciavardini, C. Callegari, G. Cautero, C. Dri, M. Di Fraia, K.C. Prince, R. Richter, R. Sergo, L. Stebel, M. Devetta, D. Faccialà, C. Vozzi, L. Avaldi, P. Bolognesi, M.C Castrovilli, D. Catone, M. Coreno, F. Zuccaro, E. Bernes, G. Fronzoni, D. Toffoli, 2020, original scientific article Keywords: Binding energy, Calculations, Core levels, Electronic structure, Ionization of gases, Ionization potential, Molecular orbitals, Photoelectron spectroscopy, Photoelectrons, Photoemission, Photoionization, Photons, Polycyclic aromatic hydrocarbons, X rays Published in RUNG: 21.01.2022; Views: 2748; Downloads: 0 This document has many files! More... |
5. Ultrafast relaxation of photoexcited superfluid He nanodropletsM. Mudrich, A.C. LaForge, A. Ciavardini, P. O'Keeffe, C. Callegari, M. Coreno, A. Demidovich, M. Devetta, M. Di Fraia, M. Drabbels, P. Finetti, O. Gessner, C. Grazioli, A. Hernando, D.M. Neumark, Y. Ovcharenko, P. Piseri, O. Plekan, K.C. Prince, R. Richter, M.P. Ziemkiewicz, T. Moller, J. Eloranta, M. Pi, M. Barranco, F. Stienkemeier, 2020, original scientific article Keywords: helium, helium nanodroplet, nanomaterial, density functional theory, dipole, excitation, ionization, photoelectron spectroscopy, photoexcitation, photon, simulation, ultraviolet radiation, ultrafast photoemission, free electron laser, ultrafast spectrscopy Published in RUNG: 20.01.2022; Views: 2561; Downloads: 0 This document has many files! More... |
6. Topological properties and self-energy effects in elemental YbPolina M. Sheverdyaeva, F. Offi, Sandra Gardonio, Luka Novinec, M. I. Trioni, D. Ceresoli, S. Iacobucci, A. Ruocco, Giovanni Stefani, L. Petaccia, 2021, original scientific article Keywords: electronic structure, topological materials, lanthanides, angle-resolved photoemission spectroscopy Published in RUNG: 03.12.2021; Views: 2509; Downloads: 39 Link to full text This document has many files! More... |
7. Dissecting Mott and charge-density wave dynamics in the photoinduced phase of 1T-TaS[sub]2Alberto Simoncig, Matija Stupar, Barbara Ressel, Tanusree Saha, Primož Rebernik Ribič, Giovanni De Ninno, 2021, original scientific article Abstract: The two-dimensional transition-metal dichalcogenide 1T−TaS2 is a complex material standing out for its puzzling low temperature phase marked by signatures amenable to both Mott-insulating and charge-density wave states. Electronic Mott states, coupled to a lattice, respond to coherent optical excitations via a modulation of the lower (valence) Hubbard band. Such dynamics is driven by strong electron-phonon coupling and typically lasts for tens of picoseconds, mimicking coherent structural distortions. Instead, the response occurring at the much faster timescale, mainly dominated by electronic many-body effects, is still a matter of intense research. By performing time- and angle-resolved photoemission spectroscopy, we investigated the photoinduced phase of 1T−TaS2 and found out that its lower Hubbard band promptly reacts to coherent optical excitations by shifting its binding energy towards a slightly larger value. This process lasts for a time comparable to the optical pump pulse length, mirroring a transient change of the onsite Coulomb repulsion energy (U). Such an observation suggests that the correction to the bare value of U, ascribed to the phonon-mediated screening which slightly opposes the Hubbard repulsion, is lost within an interval of a few tens of femtoseconds and can be understood as a fingerprint of electronic states largely decoupled from the lattice. Additionally, these results enforce the hypothesis, envisaged in the current literature, that the transient photoinduced states belong to a sort of crossover phase instead of an equilibrium metallic one. Keywords: ultrafast phenomena, time resolved photoemission, strongly correlated systems, transition metal dichalcogenide Published in RUNG: 13.04.2021; Views: 3447; Downloads: 0 This document has many files! More... |
8. Advantages and disadvantages of experiments with ultrashort two-color pulsesMatija Stupar, 2020, doctoral dissertation Abstract: Advances in the development of lasers have led to a new class of radiation sources generating coherent, tunable, ultrashort light pulses in the spectral region ranging from infrared to soft X-rays. This includes high-order harmonics generation in gas (HHG), on which relies the CITIUS facility at University of Nova Gorica (Slovenia), and free-electron lasers (FELs), such as the facility FERMI at Elettra-Sincrotrone Trieste (Italy). The distinctive structure of HHG and FEL radiation paved the way to time-resolved experiments, which are performed to investigate events occurring on a short, or very short, temporal scale, from picoseconds to femtoseconds.
This work focuses on the advantages and disadvantages of some experimental techniques based on using these novel light sources to investigate the microscopic and/or ultrafast dynamics of matter samples, which have been previously driven out of equilibrium.
Advantages rely on the implementation of various applications based on two-color schemes and, more specifically, include the possibility of acquiring two-dimensional frequency maps, measuring electrons’ effective masses, or investigating electronic properties decoupled from the influence of the lattice. Particular focus will be put on experimental methods relying on photoelectric effect and photoelectron spectroscopy. In all experiments, we took advantage of one or more specific properties of HHG and FEL sources, such as controllable chirp, to study laser dressed states in helium, variable polarization, to study electronic properties of iron-based pnictides and ultrashort pulses (< 10 fs) to study the purely electronic dynamics in transition metal dichalcogenides.
On the other hand, the study of the interface between a molecule and a topological insulator revealed some intrinsic limitations and physical drawbacks of the technique, such as spurious effects originating from the high power pulses, like multiphoton absorption and the space charge effect, or the reduction of experimental resolution when pushing for shorter and shorter pulse durations. Some disadvantages are also connected to the current state-of-the-art in the field of ultrashort laser systems, where a trade-off needs to be found between repetition rate and laser power.
Finally, state-of-the-art experiments based on the ability to generate ultrashort pulses carrying orbital angular momentum in visible, near-infrared as well as extreme UV range will be presented. The use of these pulses opens the door to the investigation of new physical phenomena, such as probing magnetic vortices using extreme ultraviolet light from a free-electron laser or imprinting the spatial distribution of an ultrashort infrared pulse carrying orbital angular momentum onto a photoelectron wave packet. Keywords: ultrafast lasers, two-color experiments, photoemission, high-order harmonic generation, free-electron lasers, hot-electrons dynamics, surface science, pump-probe photoemission, ultraviolet photoemission, orbital angular momentum Published in RUNG: 02.12.2020; Views: 5179; Downloads: 143 Full text (19,78 MB) |
9. Ultra-Fast-VUV Photoemission Study of UV Excited 2-NitrophenolA. Ciavardini, Marcello Coreno, Carlo Callegari, C. Spezzani, Giovanni De Ninno, Barbara Ressel, Cesare Grazioli, Monica de Simone, Antti Kivimak̈i, Paolo Miotti, Fabio Frassetto, Luca Poletto, Petra Rudolf, Simona Fornarini, Marco Pezzella, Enrico Bodo, Susanna Piccirillo, 2019, original scientific article Abstract: The initial deactivation pathways of gaseous 2-nitrophenol excited at 268 nm were investigated by time-resolved photoelectron spectroscopy (TRPES) with femtosecond-VUV light, produced by a monochromatized high harmonic generation source. TRPES allowed us to obtain new, valuable experimental information about the ultrafast excited-state dynamics of 2-nitrophenol in the gas phase. In accord with recent ab initio on-the-fly nonadiabatic molecular dynamic simulations, our results validate the occurrence of an ultrafast intersystem crossing leading to an intermediate state that decays on a subpicosecond time scale with a branched mechanisms. Two decay pathways are experimentally observed. One probably involves proton transfer, leading to the most stable triplet aci-form of 2-nitrophenol; the second pathway may involve OH rotation. We propose that following intersystem crossing, an ultrafast fragmentation channel leading to OH or HONO loss could also be operative. Keywords: Ultrafast photoemission, nitrophenol Published in RUNG: 12.02.2019; Views: 4448; Downloads: 0 This document has many files! More... |
10. Scanning Photoelectron Spectro‐Microscopy: A Modern Tool for the Study of Materials at the NanoscalePatrick Zeller, Matteo Amati, Hikmet Sezen, Mattia Scardamaglia, Claudia Struzzi, Carla Bittencourt, Gabriel Lantz, Mahdi Hajlaoui, Evangelos Papalazarou, Marino Marsi, Mattia Fanetti, Stefano Ambrosini, Silvia Rubini, Luca Gregoratti, 2018, review article Keywords: Scanning photoemission microscopy, graphene, GaAs, nanowires, Fermi Level, Mott-Hubbard transition Published in RUNG: 07.12.2018; Views: 4535; Downloads: 0 This document has many files! More... |