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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 1,153 records · Page 64
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Direct momentum imaging of charge transfer following site-selective ionization

We study ultrafast charge rearrangement in dissociating 2-iodopropane (2-C 3 H 7 I) using site-selective core-ionization at the iodine atom. Clear signatures of electron transfer between the neutral propyl fragment and multiply charged iodine ions are observed in the recorded delay-dependent ion momentum distributions. The detected charge transfer pathway is only favorable within a small (few angstrom), charge-state-dependent spatial window located at C-I distances longer than that of the neutral ground-state molecule. Lastly, these results offer new insights into the physics underpinning charge transfer in isolated molecules and pave the way for a new class of time-resolved studies.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Quenching of the relaxation pathway in the Weyl semimetal TaAs

Since tantalum arsenide (TaAs) has been experimentally verified as a Weyl semimetal, intensive research has been devoted to study of the unique properties of the material. Despite this, the ultrafast dynamics of TaAs is still not very well understood. In this work, we study the relaxation dynamics in TaAs using transient reflection spectroscopy. From the transient reflection measurement, we observe either a single (fast) or a dual (fast and slow) relaxation, depending on the probing wavelength. The additional relaxation channel is attributed to an asymmetric population of photoexcited electrons and holes.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Quantum interference between the optical Stark effect and resonant harmonic generation in WS 2

An applied field can modulate optical signals by resonance shifting via the Stark effect. The optical Stark effect uses ultrafast light in the transparency region of a material to shift resonances with speeds limited by the pulse duration or system coherence. In this Rapid Communication, we investigate the optical Stark effect in resonant optical harmonic generation using the A exciton transition of WS 2 . Multidimensional pump-harmonic-probe measurements, in which the probe is second- or third-harmonic emission, reveal not only large Stark shifts that are commensurate with the large optical susceptibilities common to WS 2 excitons, but also behaviors more complex than simple optical Stark effect treatments predict. We show how another manifestation of the Stark effect, brought forth by coherent photon exchange between the pump and harmonic generation fundamental fields, can strongly enhance or suppress harmonic generation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Optical subpicosecond nonvolatile switching and electron-phonon coupling in ferroelectric materials

Direct optical ferroelectric switching (FE switch) has the advantage of being ultrafast over the traditional FE switch, which relies on domain nucleation and growth. However, how to realize nonvolatility in such an optical FE switch poses a serious challenge. Time-dependent density-functional theory molecular dynamics study reveals that subpicosecond nonvolatile FE switches can be realized in GeTe and PbTiO 3 . Here, while optical tuning of the transition barrier and initiation of a directional atomic motion are crucial, the dephasing of the excited state holds the key for the realization of nonvolatility.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Transition metal dichalcogenide monolayers in an ultrashort optical pulse: Femtosecond currents and anisotropic electron dynamics

We theoretically study the interaction of an ultrafast intense linearly polarized optical pulse with monolayers of transition metal dichalcogenides (TMDCs). Such a strong pulse redistributes electrons between the bands and generates femtosecond currents during the pulse. Due to the large bandwidth of the incident pulse, this process is completely an off-resonant. While in TMDCs, the time-reversal symmetry is conserved, the inversion symmetry is broken, and these monolayers have axial symmetry along the armchair direction but not along with the zigzag one. The pulse, polarized along with asymmetric directions of TMDC monolayer, generates both longitudinal, i.e., along the direction of polarization, and transverse, i.e., in the perpendicular direction, currents. Such currents result in charge transfer through the system. Finally, we study different TMDC materials and show how the femtosecond transport in TMDC monolayers depend on their parameters, such as lattice constant and bandgap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Effect of lattice excitations on transient near-edge x-ray absorption spectroscopy

Here, time-dependent and constituent-specific spectral changes in soft near-edge x-ray absorption spectroscopy (XAS) of an [Fe/MgO] 8 metal/insulator heterostructure after laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining XAS with ultrafast electron diffraction measurements and ab initio calculations demonstrates that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near-edge XAS to phonons is demonstrated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Optically and thermally driven huge lattice orbital and spin angular momenta from spinning fullerenes

Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes, or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a route to phonon angular momentum in a molecular crystal C 60 . We find that a single laser pulse is able to inject a significant amount of angular momentum to C 60 , and the momentum transfer is helicity dependent. Changing from right-circularly polarized light to left-circularly polarized light switches the direction of phonon angular momentum. On the ultrafast timescale, the orbital angular momentum change closely resembles the displacive excitation of coherent phonons, with a cosine-function dependence on time, different from the spin counterpart. Atomic displacements, even under strong laser excitation, remain far below the Lindemann criterion. Under thermal excitation, spinning C 60 even at room temperature generates a huge angular momentum close to several hundred h¯. Our finding opens the door to a large group of fullerenes, from C 60 , C 70 to their endohedral derivatives, where angular momentum can be generated through light or temperature. Furthermore, this paves the way to the phononic control electronic spin and harvesting thermal energy through phonon angular momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Nonthermal breaking of magnetic order via photogenerated spin defects in the spin-orbit coupled insulator Sr 3 Ir 2 O 7

In many strongly correlated insulators, antiferromagnetic order competes with exotic and technologically relevant phases, like superconductivity. While control of spin order is critical to stabilize different functional states, elucidating the mechanism of laser-induced demagnetization in complex oxides remains a challenge. It is unknown if the optical pulse can quench magnetization nonthermally or if it instead only acts as a heat source. In this study, we used ultrafast, broadband, optical spectroscopy to track the responses of the electronic, lattice, and spin degrees of freedom and their relation to antiferromagnetism in the strongly spin-orbit coupled insulator Sr 3 Ir 2 O 7 . We find that magnetization can be rapidly and strongly suppressed on a sub-150 fs timescale. At low excitation fluences, the magnetic recovery is fast; however, the recovery time increases dramatically with the magnitude of demagnetization. At the same time, we show that the lattice, evidenced through the A g phonon frequencies, appears to remain below T N , suggesting that the system remains nonthermal during the optical modulation of spin order. We suggest that photogenerated spin defects are responsible for the long-lived demagnetized state and discuss its implications for optical control of solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Dynamic short-range correlation in photoinduced disorder phase transitions

Ultrafast photoexcitation can induce a nonequilibrium dynamic with electron-lattice interaction, offering an effective way to study photoinduced phase transitions (PIPTs) in solids. The issue that atomic displacements after photoexcitation belong to a coherent change or disordered process has become controversial in the PIPT community. Using real-time, time-dependent density functional theory (rt-TDDFT) simulations, we were able to obtained both the coherent and the disordered PIPTs (dimer dissociation) in IrTe 2 with different electronic occupations. More importantly, we found that in the disordered phase transition there exists a local correlation between different dimers regarding their dissociation status. We define these Ir-Ir dimers directly connected by Te atoms, including intralayer and vertically across the layers, as a group (group I). Other Ir-Ir dimers separated by five Ir atoms from Ir-Ir dimers in group I are divided into another group (group II). The dimers in the same group will dissociate in a correlated fashion; they either all dissociate or all do not dissociate. On the other hand, the dimers in neighboring groups will have an anticorrelation: If the dimers in one group dissociate, the dimers in the neighboring group tend not to be dissociated, and vice versa.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Influence of local symmetry on lattice dynamics coupled to topological surface states

Herein we investigate coupled electron-lattice dynamics in the topological insulator Bi 2 Te 3 with time-resolved photoemission and time-resolved x-ray diffraction. It is well established that coherent phonons can be launched by optical excitation, but selection rules generally restrict these modes to zone-center wave vectors and Raman-active branches. We find that the topological surface state couples to additional modes, including a continuum of surface-projected bulk modes from both Raman and infrared branches, with possible contributions from surface-localized modes when they exist. Our calculations show that this surface vibrational spectrum occurs naturally as a consequence of the translational and inversion symmetries broken at the surface, without requiring the splitting-off of surface-localized phonon modes. The generality of this result suggests that coherent phonon spectra are useful by providing unique fingerprints for identifying surface states in more controversial materials. These effects may also expand the phase space for tailoring surface state wave functions via ultrafast optical excitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Electronic nematic order in the normal state of strontium ruthenate

Despite significant achievements in characterizing the properties of Sr 2 ⁢RuO 4 over the last three decades, the precise nature of its electronic ground state is still unresolved. In this work, we provide a missing piece of the puzzle by uncovering evidence of electronic nematic order in the normal state of Sr 2 ⁢RuO 4 , revealed by ultrafast time-resolved optical dichroism measurements of uniaxially strained thin films. This nematic order, whose domains are aligned by the strain, spontaneously breaks the fourfold rotational symmetry of the crystal. The temperature dependence of the dichroism resembles an Ising-like order parameter, and optical pumping induces a coherent oscillation of its amplitude mode. The existence of electronic nematic order in the normal state of Sr2⁢RuO4 may have consequences for the form and mechanism of superconductivity in this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Pseudospectral Landau-Lifshitz description of magnetization dynamics

Magnetic materials host a wealth of nonlinear dynamics, textures, and topological defects. This is possible due to the competition between strong nonlinearity and dispersion, which act at the atomic scale, as well as long-range interactions. However, these features are difficult to study analytically and numerically because of the vastly different temporal and spatial scales involved. Here, in this work, we present a pseudospectral approach for the Landau-Lifshitz equation that invokes energy and momentum conservation embodied in the magnon dispersion relation to accurately describe both atomic and continuum limits. Furthermore, this approach enables analytical study at every scale. We show the applicability of this model in both the continuum and atomic limit by investigating modulational instability and ultrafast evolution of magnetization due to transient grating, respectively, in a one-dimensional ferromagnetic chain with perpendicular magnetic anisotropy. This model provides the possibility of grid-independent multiscale numerical approaches that will enable the description of singularities within a single framework.

1-dimensional spin chains↗
DOE OSTI2024

Insights into the laser-assisted photoelectric effect from solid-state surfaces

Photoemission from a solid surface provides a wealth of information about its electronic structure and dynamic evolution. Ultrafast pump-probe experiments offer real-time access to photon-surface interactions and the resulting electron dynamics. Here, we present a femtosecond time-resolved photoelectron spectroscopy study of laser-assisted photoemission (LAPE) from two different metal surfaces, tungsten and platinum. Utilizing synchronized IR laser and x-ray pulses, photoelectron sideband generation up to the sixth order is observed. A significant material-dependent variation of the LAPE response has not been predicted by previous theoretical models, to the best of our knowledge. The observed phenomena are semiquantitatively reproduced by considering distinct dynamic dielectric responses of the two materials. In conclusion, these findings provide a deeper understanding of the LAPE process and insights into the dynamic interplay between optical laser fields and metal surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Second-Order Josephson Effect in Excitonic Insulators

We show that in electron-hole bilayers with excitonic orders arising from conduction and valence bands formed by atomic orbitals that have different parities, nonzero interlayer tunneling leads to a second-order Josephson effect. This means the interlayer electrical current is related to the phase of the excitonic order parameter as J = J c sin 2θ instead of J = J c sin θ and that the system has two degenerate ground states at θ = 0, π that can be switched by an interlayer voltage pulse. When generalized to a three dimensional stack of alternating electron-hole planes or a two dimensional stack of chains, the ac Josephson effect implies that electric field pulses perpendicular to the layers and chains can steer the order parameter phase between the two degenerate ground states, making these devices ultrafast memories. Here, the order parameter steering also applies to the excitonic insulator candidate Ta 2 NiSe 5 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Role of Equilibrium Fluctuations in Light-Induced Order

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are “hidden” under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. Overall, these findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host hidden orders after laser excitation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Signatures of Multiband Effects in High-Harmonic Generation in Monolayer MoS 2

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS 2 , as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. Further, this observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multiband recombination dipoles.

2-dimensional systems↗
DOE OSTI2023

Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy

Strong-field ionization of molecules releases electrons which can be accelerated and driven back to recombine with their parent ion, emitting high-order harmonics. This ionization also initiates attosecond electronic and vibrational dynamics in the ion, evolving during the electron travel in the continuum. Revealing this subcycle dynamics from the emitted radiation usually requires advanced theoretical modeling. Here we show that this can be avoided by resolving the emission from two families of electronic quantum paths in the generation process. The corresponding electrons have the same kinetic energy, and thus the same structural sensitivity, but differ by the travel time between ionization and recombination-the pump-probe delay in this attosecond self-probing scheme. We measure the harmonic amplitude and phase in aligned CO 2 and N 2 molecules and observe a strong influence of laser-induced dynamics on two characteristic spectroscopic features: a shape resonance and multichannel interference. This quantum-path-resolved spectroscopy thus opens wide prospects for the investigation of ultrafast ionic dynamics, such as charge migration.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Differentiating Three-Dimensional Molecular Structures Using Laser-Induced Coulomb Explosion Imaging

Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion images complex single molecules, Nat. Phys. 18, 423 (2022).]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Here, our results reveal that each molecule exhibits a well-localized and distinctive pattern in three-dimensional fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗