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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: 289; Prenosov: 4
.pdf Celotno besedilo (2,30 MB)
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Tanusree 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: 1122; Prenosov: 24
.pdf Celotno besedilo (13,34 MB)

Dissecting Mott and charge-density wave dynamics in the photoinduced phase of 1T-TaS[sub]2
Alberto 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: 2249; Prenosov: 0
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Chemical and structural investigation of the cobalt phthalocyanine
Matija Stupar, 2015, magistrsko delo

Opis: In the last two decades, studies on organic molecules mimicking substances of fundamental importance in nature, like chlorophyll or hemoglobin, have attracted researchers’ attention. These molecules are building blocks for a family of materials also referred to as “organic semiconductors”. Such compounds can be implemented in numerous applications, ranging from data-storage to light harvesting. Some of their fundamental advantages include low cost, light weight, relatively easy engineering and mechanical flexibility, compatible with bending plastic substrates. In this thesis work we investigated the chemical, structural and electronic properties of cobalt phthalocyanines (CoPc). These molecules have promising applications in the field of magnetic data storage and spintronics in general, due to the ferromagnetic properties of the cobalt atom. Several techniques like photoemission core-level spectroscopy and valence band spectroscopy, together with X-ray absorption, have been used in order to determine the CoPc properties in gaseous phase, i.e. in the absence of interaction with the surrounding environment. Another set of experiments was devoted to the commissioning of the CITIUS time-resolved photoemission setup, that will be used in future studies of CoPc molecules on surfaces.
Ključne besede: Cobalt phthalocyanine (CoPc), photoemission spectroscopy (PES), X-ray absorption spectroscopy (XAS), synchrotron radiation, laser, high order harmonic generation (HHG), time resolved spectroscopy
Objavljeno v RUNG: 29.09.2015; Ogledov: 8606; Prenosov: 279
.pdf Celotno besedilo (2,96 MB)

The CITIUS light source
Sandra Gardonio, Giovanni De Ninno, Barbara Ressel, 2013, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: femtosecond laser source, time resolved photoemission spectroscopy, correlated electron materials
Objavljeno v RUNG: 06.05.2014; Ogledov: 6831; Prenosov: 37
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