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, izvirni znanstveni članek Opis: 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).
Ključne besede: angle resolved photoemission, time resolved photoemission, 2D materials, charge density wave, Mott insulator
Objavljeno v RUNG: 15.01.2024; Ogledov: 1352; Prenosov: 5
 Celotno besedilo (2,30 MB)
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2. ULTRAFAST ELECTRON DYNAMICS IN CORRELATED SYSTEMS PROBED BY TIME-RESOLVED PHOTOEMISSION SPECTROSCOPYTanusree Saha, 2023, doktorska disertacija Opis: 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.
Ključne besede: complex systems, charge density wave, excitonic insulator, metastable phase, Mott insulator, non-equilibrium, spin density wave, timescales, time- and angle-resolved photoemission, ultrafast dynamics
Objavljeno v RUNG: 01.06.2023; Ogledov: 2175; Prenosov: 36
Celotno besedilo (13,34 MB) |
3. Orbital selective dynamics in Fe-pnictides triggered by polarized pump pulse excitationsGanesh Adhikary, Tanusree Saha, Primož Rebernik Ribič, Matija Stupar, Barbara Ressel, Jurij Urbančič, Giovanni De Ninno, A. Thamizhavel, Kalobaran Maiti, 2021, izvirni znanstveni članek Opis: Quantum materials display exotic behaviours related to the interplay between temperature-driven phase transitions. Here, we study the electron dynamics in one such material, CaFe$_2$As$_2$, a parent Fe-based superconductor, employing time and angle-resolved photoemission spectroscopy. CaFe$_2$As$_2$ exhibits concomitant transition to spin density wave state and tetragonal to orthorhombic structure below 170 K. The Fermi surface of this material consists of three hole pockets ($\alpha$, $\beta$ and $\gamma$) around $\Gamma$-point and two electron pockets around $X$-point. The hole pockets have $d_{xy}$, $d_{yz}$ and $d_{zx}$ orbital symmetries. The $\beta$ band constituted by $d_{xz}$/$d_{yz}$ orbitals exhibit a gap across the magnetic phase transition. We discover that polarized pump pulses can induce excitations of electrons of a selected symmetry. More specifically, while $s$-polarized light (polarization vector perpendicular to the $xz$-plane) excites electrons corresponding to all the three hole bands, $p$-polarized light excites electrons essentially from ($\alpha$,$\beta$) bands which are responsible for magnetic order. Interestingly, within the magnetically ordered phase, the excitation due to the $p$-polarized pump pulses occur at a time scale of 50 fs, which is significantly faster than the excitation induced by $s$-polarized light ($\sim$ 200 fs). These results suggest that the relaxation of different ordered phases occurs at different time scales and this method can be used to achieve selective excitations to disentangle complexity in the study of quantum materials.
Ključne besede: Electronic structure, Pnictides and chalcogenides, Time-resolved spectroscopy
Objavljeno v RUNG: 13.10.2021; Ogledov: 2408; Prenosov: 8
Celotno besedilo (9,56 MB) |
4. 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, izvirni znanstveni članek Opis: 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.
Ključne besede: ultrafast phenomena, time resolved photoemission, strongly correlated systems, transition metal dichalcogenide
Objavljeno v RUNG: 13.04.2021; Ogledov: 3111; Prenosov: 0
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