Ultrafast doublon dynamics in photo-excited 1T-TaS${}_2$

Abstract

Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS${}_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $\hslash /J\approx$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.

References in corpus (23)

• Complexity in Strongly Correlated Electronic Systems
• Nonequilibrium dynamical mean-field theory and its applications
• Ultrafast switching to a stable hidden topologically protected quantum state in an electronic crystal
• Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach
• Orbital textures and charge density waves in transition metal dichalcogenides
• Nanoscale manipulation of the Mott insulating state coupled to charge order in 1T-TaS2
• Momentum-dependent snapshots of a melting charge density wave
• Ultrafast melting of a charge-density wave in the Mott insulator 1T-TaS2
• A new high-temperature quantum spin liquid with polaron spins
• Thermalization of a pump-excited Mott insulator
• Photo-induced states in a Mott insulator
• Ultrafast charge recombination in photoexcited Mott-Hubbard insulator
• Relaxation dynamics of the Holstein polaron
• Mechanism of Ultrafast Relaxation of a Photo-Carrier in Antiferromagnetic Spin Background
• Polaronic conductivity in the photoinduced phase of 1T-TaS2
• Phonon anomaly at the charge ordering transition in 1T-TaS2
• Field-induced polaron formation in the Holstein-Hubbard model
• Role of impact ionization in the thermalization of photo-excited Mott insulators
• Dynamics of screening in photo-doped Mott insulators
• Charge Recombination in Undoped Cuprates
• Ultrafast separation of photo-doped carriers in Mott antiferromagnets
• Probing the coupling between a doublon excitation and the charge-density wave in TaS2 by ultrafast optical spectroscopy
• Unusual Two-stage Dynamics of the Spin-Lattice Polaron Formation

Cited by in corpus (75)

• Nonthermal pathways to ultrafast control in quantum materials
• Band insulator to Mott insulator transition in 1T-TaS${}_2$
• Time- and Angle-Resolved Photoemission Studies of Quantum Materials
• Disrupted orbital order and the pseudo-gap in layered 1T-TaS${}_2$
• Collapse of layer dimerization in the photo-induced hidden state of 1T-TaS2
• Direct identification of Mott Hubbard band pattern beyond charge density wave superlattice in monolayer 1T-NbSe2
• Distinguishing a Mott Insulator from a Trivial Insulator with Atomic Adsorbates
• A quantitative comparison of time-of-flight momentum microscopes and hemispherical analyzers for time- and angle-resolved photoemission spectroscopy experiments
• Low rank compression in the numerical solution of the nonequilibrium Dyson equation
• Preferential out-of-plane conduction and quasi-one-dimensional electronic states in layered 1T-TaS2
• Photoexcitation Induced Quantum Dynamics of Charge Density Wave and Emergence of a Collective Mode in 1T-TaS${}_2$
• Charge-density-wave melting in the one-dimensional Holstein model
• Quantum Simulation Meets Nonequilibrium Dynamical Mean Field Theory: Exploring the Periodically Driven, Strongly Correlated Fermi-Hubbard Model
• Mott versus hybridization gap in the low-temperature phase of $1T$-TaS${}_2$
• Finite-temperature density-matrix renormalization group method for electron-phonon systems: Thermodynamics and Holstein-polaron spectral functions
• Mottness collapse without metallisation in the domain walls of triangular-lattice Mott insulator 1T-TaS${}_2$
• A time-domain phase diagram of metastable states in a charge ordered quantum material
• Photo-induced phase transition and associated time scales in the excitonic insulator Ta${}_2$NiSe${}_5$
• Detecting superconductivity out-of-equilibrium
• Effective theory of lattice electrons strongly coupled to quantum electromagnetic fields
• Coherent phonons and the interplay between charge density wave and Mott phases in 1$T$-TaSe${}_2$
• Nonequilibrium steady-state theory of photodoped Mott insulators
• Doublon formation by ions impacting a strongly correlated finite lattice system
• Ultrafast Transient Absorption Spectroscopy of the Charge-Transfer Insulator NiO: Beyond the Dynamical Franz-Keldysh Effect
• Photo-induced nonequilibrium states in Mott insulators
• Exploring the Charge Density Wave phase of 1$T$-TaSe${}_2$: Mott or Charge-transfer Gap?
• Memory truncated Kadanoff-Baym equations
• Hund excitations and the efficiency of Mott solar cells
• Photo-enhanced excitonic correlations in a Mott insulator with nonlocal interactions
• Surface structure and stacking of the commensurate $\left(\sqrt{13}\times \sqrt{13}\right)$R13.9° charge density wave phase of 1T-TaS${}_2$(0001)
• Noise Correlations in time- and angular-resolved photoemission spectroscopy
• Doublon bottleneck in the ultrafast relaxation dynamics of hot electrons in 1T-TaS_2
• Dynamical Mean-Field Theory of Strongly Correlated Electron Systems
• Doublon-like excitations and their phononic coupling in a Mott charge-density-wave system
• Photo-induced charge dynamics in 1$T$-TaS${}_2$
• Charge density wave surface reconstruction in a van der Waals layered material
• Control of Competing Superconductivity and Charge Order by Non-equilibrium Currents
• Light-induced insulator-metal transition in Sr${}_2$IrO${}_4$ reveals the nature of the insulating ground state
• Causal versus local $GW$+EDMFT scheme and application to the triangular-lattice extended Hubbard model
• Dynamical Mean Field Theory extension to the nonequilibrium Two-Particle Self-Consistent approach
• Structural dynamics probed by high-coherence electron pulses
• Mobile Kink Solitons in a Van der Waals Charge-Density-Wave Layer
• Phase-resolved frequency-domain analysis of the photoemission spectra for photoexcited 1T-TaS2 in the Mott insulating charge density wave state
• Twisted chiral superconductivity in photodoped frustrated Mott insulators
• Time-dependent spectral functions of the Anderson impurity model in response to a quench with application to time-resolved photoemission spectroscopy
• Impact ionization and multiple photon absorptions in the two-dimensional photoexcited Hubbard model
• Dynamically induced doublon repulsion in the Fermi-Hubbard model probed by a single-particle density of states
• Real-time evolution of static electron-phonon models in time-dependent electric fields
• Phonon-induced electronic relaxation in a strongly correlated system: the Sn/Si(111) $(\sqrt{3}\times \sqrt{3})$ adlayer revisited
• Laser-induced ultrafast insulator-metal transition in ${\text{BaBiO}}_3$
• Distinguishing and controlling Mottness in 1T-TaS${}_2$ by ultrafast light
• Local interpretation of time-resolved X-ray absorption in Mott insulators: Insights from nonequilibrium dynamical mean-field theory
• Multidimensional coherent spectroscopy of correlated lattice systems
• Photo-induced insulator-metal transition in paramagnetic (V${}_{1-x}$Cr${}_x$)${}_2$O${}_3$
• Formation of Spatial Patterns by Spin-selective Excitations of Interacting Fermions
• Electron-magnon dynamics triggered by an ultrashort laser pulse: A real-time Dual $GW$ study
• Superconducting optical response of photodoped Mott insulators
• Interacting electrons in a flat-band system within the Generalized Kadanoff-Baym Ansatz
• Probing complex stacking in a layered material via electron-nuclear quadrupolar coupling
• First-order kinetics bottleneck during photoinduced ultrafast insulator-metal transition in 3D orbitally-driven Peierls insulator CuIr${}_2$S${}_4$
• Time-resolved photoemission and RIXS study of a site-selective Mott insulator
• Ultrafast X-ray Absorption Spectroscopy of Strongly Correlated Systems: Core Hole Effect
• INQ, a modern GPU-accelerated computational framework for (time-dependent) density functional theory
• Infinite Grassmann time-evolving matrix product operators for quantum impurity problems after a quench
• Anomalous amplitude mode dynamics below the expected charge-density-wave transition in 1$T$-VSe${}_2$
• Momentum-dependent relaxation dynamics of the doped repulsive Hubbard model
• Time-Resolved Photoemission Spectroscopy of Quantum Materials Using High Harmonic Generation: Probing Electron-Phonon Interactions and Non-Equilibrium Dynamics
• Van der Waals devices for surface-sensitive experiments
• Topical review: the nature of the ground state and possibility of a quantum spin liquid in 1T metal dichalcogenides
• Distinct charge and spin recovery dynamics in a photo-excited Mott insulator
• Uncovering the nature of transient and metastable non-equilibrium phases in 1$T$-TaS${}_2$
• Emergent quantum phenomena in two-dimensional 1T-TaS2
• Ultrafast Electronic Structure Engineering in 1$T$-TaS${}_2$: Role of Doping and Amplitude Mode Dynamics
• Electronic Coherence Evolution at the Nearly Commensurate Incommensurate CDW Boundary of 1T-TaS2
• Phase transitions from Heating to non-heating in SU(1, 1) quantum dynamics: applications to Bose-Einstein condensates and periodically driven coupled oscillators