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Results for “time & angle resolved photoemission spectroscopy”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

High resolution time- and angle-resolved photoemission spectroscopy with 11 eV laser pulses

Performing time- and angle-resolved photoemission (tr-ARPES) spectroscopy at high momenta necessitates extreme ultraviolet laser pulses, which are typically produced via high harmonic generation (HHG). Despite current advances, HHG-based setups still require large pulse energies (from hundreds of μ J to mJ) and their energy resolution is limited to tens of meV. Here, we present a novel 11 eV tr-ARPES setup that generates a flux of 5 × 10 10 photons/s and achieves an unprecedented energy resolution of 16 meV. It can be operated at high repetition rates (up to 250 kHz) while using input pulse energies down to 3 µ J. We demonstrate these unique capabilities by simultaneously capturing the energy and momentum resolved dynamics in two well-separated momentum space regions of a charge density wave material ErTe 3 . This novel setup provides the opportunity to study the non-equilibrium band structure of solids with exceptional energy and time resolutions at high repetition rates.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Tuning time and energy resolution in time-resolved photoemission spectroscopy with nonlinear crystals

Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. In this work, we demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB 2 O 4 crystals for frequency upconversion, providing a flexible experiment design. We achieve time resolutions of 58–103 fs and corresponding energy resolutions of 55–27 meV. We propose a method to select crystal thickness based on desired experimental resolutions.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Momentum-resolved analysis of condensate dynamic and Higgs oscillations in quenched superconductors with time-resolved ARPES

Higgs oscillations in nonequilibrium superconductors provide a unique tool to obtain information about the underlying order parameter. Several properties like the absolute value, existence of multiple gaps, and the symmetry of the order parameter can be encoded in the Higgs oscillation spectrum. Studying Higgs oscillations with time-resolved angle-resolved photoemission spectroscopy (ARPES) has the advantage over optical measurements that a momentum-resolved analysis of the condensate dynamic is possible. In this paper, we investigate the time-resolved spectral function measured in ARPES for different quench protocols. We find that analyzing amplitude oscillations of the ARPES intensity in the whole Brillouin zone allows to understand how the condensate dynamic contributes to the emerging of collective Higgs oscillations. Furthermore, by evaluating the phase of these oscillations, the symmetry deformation dynamic of the condensate can be revealed, which gives insight about the ground state symmetry of the system. With such an analysis, time-resolved ARPES experiments might be used in the future as a powerful tool in the field of Higgs spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Observing photo-induced chiral edge states of graphene nanoribbons in pump-probe spectroscopies

Photo-induced edge states in low-dimensional materials have attracted considerable attention due to the tunability of topological properties and dispersion. Specifically, graphene nanoribbons have been predicted to host chiral edge modes upon irradiation with circularly polarized light. Here, we present numerical calculations of time-resolved angle resolved photoemission spectroscopy and trRIXS of a graphene nanoribbon. We characterize pump-probe spectroscopic signatures of photo-induced edge states, illustrate the origin of distinct spectral features that arise from Floquet topological edge modes, and investigate the roles of incoming photon energies and finite core–hole lifetime in RIXS. With momentum, energy, and time resolution, pump-probe spectroscopies can play an important role in understanding the behavior of photo-induced topological states of matter.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Giant self-driven exciton-Floquet signatures in time-resolved photoemission spectroscopy of MoS 2 from time-dependent GW approach

Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS 2 . We show that photoexcited excitons may be measured and quantified as satellite bands and lead to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton-Floquet phenomenon induced by an exciton time–dependent bosonic field, which are orders of magnitude stronger than those of laser field–induced Floquet bands in low-dimensional semiconductors. Our findings imply a way to engineer Floquet matter through the coherent oscillation of excitons and open the new door for mechanisms for band structure engineering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Connection between coherent phonons and electron-phonon coupling in Sb (111)

We report time- and angle-resolved photoemission spectroscopy (trARPES) measurements on the Sb(111) surface. We observe band- and momentum-dependent binding-energy oscillations in the bulk and surface bands driven by $A_{1g}$ and $E_{g}$ coherent phonons. While the bulk band shows simultaneous $A_{1g}$ and $E_{g}$ oscillations, the surface bands show either $A_{1g}$ or $E_{g}$ oscillations. The observed behavior is reproduced by frozen-phonon calculations based on density-functional theory. Furthermore, this evidences the connection between electron-phonon coupling and coherent binding energy dynamics tied to lattice vibration and confirms that band-, momentum-, and mode-dependent electron-phonon coupling can indeed be probed by trARPES in the low fluence limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Ubiquitous suppression of the nodal coherent spectral weight in Bi-based cuprates

High-temperature superconducting cuprates exhibit an intriguing phenomenology for the low-energy elementary excitations. In particular, an unconventional temperature dependence of the coherent spectral weight (CSW) has been observed in the superconducting phase by angle-resolved photoemission spectroscopy (ARPES), both at the antinode where the d-wave paring gap is maximum, as well as along the gapless nodal direction. In this work, we combine equilibrium and time-resolved ARPES to track the temperature-dependent meltdown of the nodal CSW in Bi-based cuprates with unprecedented sensitivity. We find the nodal suppression of CSW upon increasing temperature to be ubiquitous across single- and bi-layer Bi cuprates, and uncorrelated to superconducting and pseudogap onset temperatures. We quantitatively model both the lineshape of the nodal spectral features and the anomalous suppression of CSW within the Fermi-liquid framework, establishing the key role played by the normal state electrodynamics in the description of nodal quasiparticles in superconducting cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

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.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Switching of the electron-phonon interaction in 1 T –VSe 2 assisted by hot carriers

We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1T-VSe 2 . Ultrafast snapshots of the light-induced hot carrier dynamics and nonequilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. Furthermore, the hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of (200 ± 40) fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasiequilibrium state that is experimentally observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Origin of light-induced metastability in ZrTe 5

Here we study the nonequilibrium electronic structure of a model Dirac semimetal ZrTe 5 by using time-and-angle resolved photoemission spectroscopy and density functional theory–based electron and phonon calculations. By measuring the electronic dispersion near the Γ point at time delays up to 10 picoseconds, we discovered that the band spectral weight does not recover during the measured temporal window, revealing the existence of a light-induced metastable state in the electronic structure of this material. Our calculations find that the photoexcited A 1⁢g phonon mode leads to a band renormalization that both supports our experimental observations at the zone center and predicts changes to the band structure outside of our experimental window, ultimately showing the evolution from a direct to an indirect gap semimetal; such band renormalization dramatically reduces the electron-hole recombination rate giving rise to the metastability in this system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Development of deflector mode for spin-resolved time-of-flight photoemission spectroscopy

Spin- and angle-resolved photoemission spectroscopy (“spin-ARPES”) is a powerful technique for probing the spin degree-of-freedom in materials with nontrivial topology, magnetism, and strong correlations. Spin-ARPES faces severe experimental challenges compared to conventional ARPES attributed to the dramatically lower efficiency of its detection mechanism, making it crucial for instrumentation developments that improve the overall performance of the technique. Here in this paper, we demonstrate the functionality of our spin-ARPES setup based on time-of-flight spectroscopy and introduce our recent development of an electrostatic deflector mode to map out spin-resolved band structures without sample rotation. We demonstrate the functionality by presenting the spin-resolved spectra of the topological insulator Bi2Te3 and describe in detail the spectrum calibrations based on numerical simulations. By implementing the deflector mode, we minimize the need for sample rotation during measurements, hence improving the overall efficiency of experiments on small or inhomogeneous samples.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Ultrafast optical induction of magnetic order at a quantum critical point

Abstract Time-resolved ultrafast spectroscopy has emerged as a promising tool to dynamically induce and manipulate non-trivial electronic states of matter out-of-equilibrium. Here we theoretically investigate light pulse driven dynamics in a Kondo lattice system close to quantum criticality. Based on a time-dependent auxiliary fermion mean-field calculation we show that light can dehybridize the local Kondo screening and induce oscillating magnetic order out of a previously paramagnetic state. Depending on the laser pulse field amplitude and frequency the Kondo singlet can be completely deconfined, inducing a dynamic Lifshitz transition that changes the Fermi surface topology. These phenomena can be identified in harmonic generation and time-resolved angle-resolved photoemission spectroscopy spectra. Our results shed new light on non-equilibrium states in heavy fermion systems.

Fauseweh, Benedikt (ORCID:0000000248617101)↗
DOE OSTI2020

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 a high degree of electron-hole symmetry and a reduced density of states near the Fermi level. The result is reduced electronic screening and enhanced correlations between Dirac quasiparticles. In this study 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 ) and by time-dependent 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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Nonequilibrium spectral moment sum rules of the Holstein–Hubbard model

Abstract We derive a general procedure for evaluating the n th derivative of a time-dependent operator in the Heisenberg representation and employ this approach to calculate the zeroth to third spectral moment sum rules of the retarded electronic Green’s function and self-energy for a system described by the Holstein–Hubbard model allowing for arbitrary spatial and time variation of all parameters (including spatially homogeneous electric fields and parameter quenches). For a translationally invariant (but time-dependent) Hamiltonian, we also provide sum rules in momentum space. The sum rules can be applied to various different phenomena like time-resolved angle-resolved photoemission spectroscopy and benchmarking the accuracy of numerical many-body calculations. This work also corrects some errors found in earlier work on simpler models.

Physics↗
DOE OSTI2020

Detecting superconductivity out of equilibrium

Recent pump-probe experiments on underdoped cuprates and similar systems suggest the existence of a transient superconducting state above Tc. This poses the question of how to reliably identify the emergence of long-range order, in particular superconductivity, out of equilibrium. We investigate this point by studying a quantum quench in an extended Hubbard model and by computing various observables, which are used to identify (quasi-)long-range order in equilibrium. Our findings imply that, in contrast to current experimental studies, it does not suffice to study the time evolution of the optical conductivity to identify superconductivity. In turn, we suggest to utilize time-resolved angle-resolved photoemission spectroscopy experiments to probe for the formation of a condensate in the two-particle channel.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Exciton thermalization dynamics in monolayer MoS2: A first-principles Boltzmann equation study

Understanding exciton thermalization is critical for optimizing optoelectronic and photocatalytic processes in many materials. However, it is hard to access the dynamics of such processes experimentally, especially on systems such as monolayer transition metal dichalcogenides, where various low-energy excitations pathways can compete for exciton thermalization. Here, we study exciton dynamics due to exciton-phonon scattering in monolayer MoS2 from a first-principles, interacting Green's function approach, to obtain the relaxation and thermalization of low-energy excitons following different initial excitations at different temperatures. We find that the thermalization occurs on a picosecond time scale at 300 K but can increase by an order of magnitude at 100 K. The long total thermalization time, owing to the nature of its excitonic band structure, is dominated by slow spin-flip scattering processes in monolayer MoS2. In contrast, thermalization of excitons in individual spin-aligned and spin-anti-aligned channels can be achieved within a few hundred fs when exciting higher-energy excitons. We further simulate the intensity spectrum of time-resolved angle-resolved photoemission spectroscopy experiments and anticipate that such calculations may serve as a map to correlate spectroscopic signatures with microscopic exciton dynamics.

Chan, Yang-hao↗