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Reid, Alexander H.

Publications and source records attributed to Reid, Alexander H..

18 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light–matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Response of fs-Laser-Irradiated Diamond by Ultrafast Electron Diffraction

Structural details of the proposed solid–liquid phase transition of carbon have remained elusive, despite years of study. While it is theorized that novel carbon materials form from a liquid precursor, experimental studies have lacked the temporal and spatial resolution necessary to fully characterize the purported liquid state. Here, in this work, we utilize megaelectronvolt-ultrafast electron diffraction (MeV-UED) to study laser irradiated submicron diamond thin films in a pump–probe scheme with picosecond time resolution to visualize potential structural changes of excited diamond. We probe the structure of diamond using a combination of fluences (13, 40 J/cm 2 ) and time delays (10, 25, 100 ps), but observe negligible changes in the static diffraction pattern of diamond and an overall decrease in diffraction intensity up to 100 ps after the excitation pulse. We thus conclude that no appreciable amount of liquid or graphitized carbon is present and highlight the structural resilience of bulk diamond to intense 800 nm ultrafast laser pulses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

UV-Induced Reaction Pathways in Bromoform Probed with Ultrafast Electron Diffraction

For many chemical reactions, it remains notoriously difficult to predict and experimentally determine the rates and branching ratios between different reaction channels. This is particularly the case for reactions involving short-lived intermediates, whose observation requires ultrafast methods. The UV photochemistry of bromoform (CHBr 3 ) is among the most intensely studied photoreactions. Yet, a detailed understanding of the chemical pathways leading to the production of atomic Br and molecular Br 2 fragments has proven challenging. In particular, the role of isomerization and/or roaming and their competition with direct C–Br bond scission has been a matter of continued debate. Here, in this work, gas-phase ultrafast megaelectronvolt electron diffraction (MeV-UED) is used to directly study structural dynamics in bromoform after single 267 nm photon excitation with femtosecond temporal resolution. The results show unambiguously that isomerization contributes significantly to the early stages of the UV photochemistry of bromoform. In addition to direct C–Br bond breaking within <200 fs, formation of iso-CHBr 3 (Br-CH-Br-Br) is observed on the same time scale and with an isomer lifetime of >1.1 ps. The branching ratio between direct dissociation and isomerization is determined to be 0.4 ± 0.2:0.6 ± 0.2, i.e., approximately 60% of molecules undergo isomerization within the first few hundred femtoseconds after UV excitation. The structure and time of formation of iso-CHBr 3 compare favorably with the results of an ab initio molecular dynamics simulation. The lifetime and interatomic distances of the isomer are consistent with the involvement of a roaming reaction mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La 1.65 Eu 0.2 Sr 0.15 CuO 4

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump–probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu L 3 and O K resonances, we investigate nonequilibrium dynamics of Q a = Q b = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La 1.65 Eu 0.2 Sr 0.15 CuO 4 . The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2 p and Cu 3 d states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Direct observation of strong momentum-dependent electron-phonon coupling in a metal

Phonon scattering in metals is one of the most fundamental processes in materials science. However, understanding such processes has remained challenging and requires detailed information on interactions between phonons and electrons. We use an ultrafast electron diffuse scattering technique to resolve the nonequilibrium phonon dynamics in femtosecond–laser-excited tungsten in both time and momentum. We determine transient populations of phonon modes which show strong momentum dependence initiated by electron-phonon coupling. For phonons near Brillouin zone border, we observe a transient rise in their population on a timescale of approximately 1 picosecond driven by the strong electron-phonon coupling, followed by a slow decay on a timescale of approximately 8 picosecond governed by the weaker phonon-phonon relaxation process. We find that the exceptional harmonicity of tungsten is needed for isolating the two processes, resulting in long-lived nonequilibrium phonons in a pure metal. Our finding highlights that electron-phonon scattering can be the determinant factor in the phonon thermal transport of metals.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Spin-mediated shear oscillators in a van der Waals antiferromagnet

Understanding how microscopic spin configuration gives rise to exotic properties at the macroscopic length scale has long been pursued in magnetic materials. One seminal example is the Einstein-de Haas effect in ferromagnets, in which angular momentum of spins can be converted into mechanical rotation of an entire object. However, for antiferromagnets without net magnetic moment, how spin ordering couples to macroscopic movement remains elusive. Here we observed a seesaw-like rotation of reciprocal lattice peaks of an antiferromagnetic nanolayer film, whose gigahertz structural resonance exhibits more than an order-of-magnitude amplification after cooling below the Neel temperature. Using a suite of ultrafast diffraction and microscopy techniques, we directly visualize this spin-driven rotation in reciprocal space at the nanoscale. This motion corresponds to interlayer shear in real space, in which individual micro-patches of the film behave as coherent oscillators that are phase-locked and shear along the same in-plane axis. Using time-resolved optical polarimetry, we further show that the enhanced mechanical response strongly correlates with ultrafast demagnetization, which releases elastic energy stored in local strain gradients to drive the oscillators. Finally, our work not only offers the first microscopic view of spin-mediated mechanical motion of an antiferromagnet but it also identifies a new route towards realizing high-frequency resonators up to the millimetre band, so the capability of controlling magnetic states on the ultrafast timescale can be readily transferred to engineering the mechanical properties of nanodevices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Understanding and Controlling Photothermal Responses in MXenes

MXenes have the potential for efficient light-to-heat conversion in photothermal applications. To effectively utilize MXenes in such applications, it is important to understand the underlying nonequilibrium processes, including electron–phonon and phonon–phonon couplings. Here, we use transient electron and X-ray diffraction to investigate the heating and cooling of photoexcited MXenes at femtosecond to nanosecond time scales. Our results show extremely strong electron–phonon coupling in Ti 3 C 2 -based MXenes, resulting in lattice heating within a few hundred femtoseconds. We also systematically study heat dissipation in MXenes with varying film thicknesses, chemical surface terminations, flake sizes, and annealing conditions. We find that the thermal boundary conductance (TBC) governs the thermal relaxation in films thinner than the optical penetration depth. In conclusion, we achieve a 2-fold enhancement of the TBC, reaching 20 MW m –2 K –1 , by controlling the flake size or chemical surface termination, which is promising for engineering heat dissipation in photothermal and thermoelectric applications of the MXenes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Ultrafast Optomechanical Strain in Layered GeS

Strong coupling between light and mechanical strain forms the foundation for next-generation optical micro- and nano-electromechanical systems. Such optomechanical responses in two-dimensional materials present novel types of functionalities arising from the weak van der Waals bond between atomic layers. In this paper, by using structure-sensitive megaelectronvolt ultrafast electron diffraction, we report the experimental observation of optically driven ultrafast in-plane strain in the layered group IV monochalcogenide germanium sulfide (GeS). Surprisingly, the photoinduced structural deformation exhibits strain amplitudes of order 0.1% with a 10 ps fast response time and a significant in-plane anisotropy between zigzag and armchair crystallographic directions. Rather than arising due to heating, experimental and theoretical investigations suggest deformation potentials caused by electronic density redistribution and converse piezoelectric effects generated by photoinduced electric fields are the dominant contributors to the observed dynamic anisotropic strains. Our observations define new avenues for ultrafast optomechanical control and strain engineering within functional devices.

2D materials↗
DOE OSTI2022

Symmetry-dependent ultrafast manipulation of nanoscale magnetic domains

Symmetry is a powerful concept in physics, but its applicability to far-from-equilibrium states is still being understood. Recent attention has focused on how far-from-equilibrium states lead to spontaneous symmetry breaking. Conversely, ultrafast optical pumping can be used to drastically change the energy landscape and quench the magnetic order parameter in magnetic systems. Here, we find a distinct symmetry-dependent ultrafast behaviour by use of ultrafast x-ray scattering from magnetic patterns with varying degrees of isotropic and anisotropic symmetry. After pumping with an optical laser, the scattered intensity reveals a radial shift exclusive to the isotropic component and exhibits a faster recovery time from quenching for the anisotropic component. These features arise even when both symmetry components are concurrently measured, suggesting a correspondence between the excitation and the magnetic order symmetry. Our results underline the importance of symmetry as a critical variable to manipulate the magnetic order in the ultrafast regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Light-Driven Ultrafast Polarization Manipulation in a Relaxor Ferroelectric

Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg 1/3 Nb 2/3 O 3 -0.32PbTiO 3 (PMN-0.32PT) by probing its atomic-scale response via femtosecond-resolution, electron-scattering approaches. By combining these structural measurements with dynamic phase-field simulations, we show that femtosecond light pulses drive a change in both the magnitude and direction of the polarization vector within polar nanodomains on few-picosecond time scales. This study defines new opportunities for dynamic reconfigurable control of the polarization in nanoscale relaxor ferroelectrics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer

Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to fifth order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. Here, the broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain-wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer

Ultrafast optical pumping of systems with spatially nonuniform magnetic textures is known to cause far-from-equilibrium spin transport effects, such as the broadening of domain-walls. Here, we study the dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers subject to a femtosecond optical pump and find an ultrafast domain dilation by 6% within 1.6 ps. This surprising result is based on the unambiguous determination of a harmonically-related shift of ultrafast magnetic X-ray diffraction for the first- and third-order rings. Domain dilation is plausible from conservation of momentum arguments, whereby inelastic scattering from a hot, quasi-ballistic, radial current transfers momentum to the magnetic domains. Our results suggest a potentially rich variety of unexpected physical phenomena associated with far-from-equilibrium inelastic electron-magnon scattering processes in the presence of spin textures.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi 2 Te 4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi 2 Te 4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. Here, by quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nonequilibrium sub-10 nm spin-wave soliton formation in FePt nanoparticles

Magnetic nanoparticles such as FePt in the L1 0 phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magnetocrystalline anisotropy. This, in turn, reduces the magnetic exchange length to just a few nanometers, enabling magnetic structures to be induced within the nanoparticles. Here, we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved x-ray diffraction and micromagnetic modeling that spin-wave solitons of sub–10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin precession frequency of 0.1 THz positions this system as a platform to develop novel miniature devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers

We use transient absorption spectroscopy with circularly polarized x rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level, an instantaneous and significantly stronger demagnetization is observed, above the Fermi level, the demagnetization is delayed by 35 ± 10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
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↗