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At least 595 records · Page 33

Cavity-assisted magnetization switching in a quantum spin-phonon chain

Néel order switching in antiferromagnets has typically required intense optical driving, leading to substantial heating and limited efficiency. By placing antiferromagnets inside a terahertz-driven optical cavity, we propose a multi-particle mechanism for Néel order switching that benefits from reduced heating. Our analysis reveals that phonons are indispensable to this mechanism. A driven cavity mode couples to a spin-phonon chain, with all excitations dissipating energy through external baths. Mean-field analysis shows that cavity photons induce sublattice spin-density imbalance—an intrinsic symmetry-breaking effect absent without the cavity. Contrary to known (1–10 V/nm) laser fields required to switch the Néel order, our mechanism enables switching at remarkably low laser fields (1–5 V/μm), selectively targeting low-energy and perpendicular magnon modes. By virtue of the suppressed heating, the switching remains highly tunable through laser fluence, damping, and photon loss, establishing a low-dissipation route toward cavity-assisted opto-spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Extended x-ray emission times of clusters in intense x-ray pulses

Novel experimental spectroscopic and imaging techniques have been developed to exploit x-ray free-electron laser (XFEL) for studying structure and dynamic of non-periodic entities at atomic spatial resolution and femtosecond timescales.Recently, intensity correlation of x-ray fluorescence, based on the principle introduced by Hanbury Brown and Twiss [R. Hanbury Brown and R. Q. Twiss, Nature (London) 177, 27 (1956)], has been proposed for high-resolution imaging of a three-dimensional arrangement of atoms. To explore the applicability of this fluorescence approach, we theoretically investigate fluorescence dynamics of nonperiodic systems subject to x-ray free electron laser (XFEL) pulses over a range of fluences from the linear to nonlinear x-ray absorption regimes as a function of system size, from a single atom to a cluster of 149 171 atoms. Fluorescence dynamics in the nonlinear x-ray regime differs from that in the weak x-ray field in that intense x-ray pulses interrupt the fluorescence dynamics by multiphoton absorption creating a dense electron environment within the sample on a femtosecond timescale. In large systems, the presence of both recombination and photoionization pathways gives rise to an enhanced Kα and Kα h emission yield and an extended emission time beyond the lifetime of the core-excited states. Our analysis suggests that, in an intense x-ray pulse, the Kα h emission line can be a good candidate for fluorescence imaging as it has a higher yield and an emission time that is short relative to the x-ray-induced lattice distortion time.

74 ATOMIC AND MOLECULAR PHYSICS↗

Subthreshold Erosion of an Organic Polymer Induced by Multiple Shots of an X-Ray Free-Electron Laser

We report solids irradiated by energetic photons can be eroded in two modes, depending on the radiation intensity. High average, low-peak power sources, e.g., synchrotron radiation and high-order harmonics, induce desorption of the material at a low etch rate. In contrast, high-peak-power radiation from extreme ultraviolet and x-ray lasers usually causes a massive removal of the material even by a single shot. In this contribution, an effective material erosion is reported in PMMA exposed to multiple accumulated pulses generated by the free-electron x-ray-laser Linac Coherent Light Source (LCLS, tuned at a photon energy of 830 eV in this study, operated in Menlo Park at Stanford, CA, USA) at a fluence below the single-pulse ablation threshold. The effect is caused by polymer-chain scissions initiated by single photons carrying enough energy to break the C—C bounds. High efficiency of the erosion is supposed to occur due to a correlation of the single-photon effects. The subthreshold damage exhibits a nonlinear dose dependence resulting from a competition between chain scissions and cross-linking processes. The cross-linking is proven by Raman spectroscopy of the irradiated polymer. Two theoretical models of the x-ray free-electron-laser-induced erosion are suggested, which provide an excellent agreement with the experimental results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Photochemically induced acousto-optics in gases

Acousto-optics consists of launching acoustic waves in a medium (usually a crystal) in order to modulate its refractive index and create a tunable optical grating. Here, in this article, we present the theoretical basis of an alternative scheme to generate acousto-optics in a gas, where the acoustic waves are initiated by the localized absorption (and thus gas heating) of spatially modulated UV light, as was demonstrated by Michine and Yoneda [Commun. Phys. 3, 24 (2020)]. We identify the chemical reactions initiated by the absorption of UV light via the photodissociation of ozone molecules present in the gas, and calculate the resulting temperature increase in the gas as a function of space and time. Solving the Euler fluid equations shows that the modulated, isochoric heating initiates a mixed acoustic-entropy wave in the gas, whose high-amplitude density (and thus refractive index) modulation can be used to manipulate a high-power laser. We calculate that diffraction efficiencies near 100% can be obtained using only a few millimeters of gas containing a few percent ozone fraction at room temperature, with UV fluences of less than 100 mJ/cm 2 —consistent with the experimental measurements. Our analysis suggests possible ways to optimize the diffraction efficiency by changing the buffer gas composition. Gases have optics damage thresholds 2–3 orders of magnitude beyond those of solids; these optical elements should therefore be able to manipulate kilojoule-class lasers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strain modulation using defects in two-dimensional MoS 2

We investigate the nature of strain in MoS 2 and correlate it to defect types and densities, while systematically assessing the tolerance of this low dimensional material to He and Au ion irradiations. Through a series of theoretical predictions and experimental observations, we establish the onset of the crystalline-to-amorphous transition in MoS 2 and identify sulfur vacancies as the most favorable defects introduced during irradiation. We note the presence of both tensile and compressive strains, which depend on the types of defects introduced into the lattice and vary with increasing fluence. In conclusion, the results show that defects can be used to tune strain in two-dimensional materials and provide an exciting pathway for using external stimuli to control properties of low dimensional materials.

2-dimensional systems↗

Ultrafast dynamics in the high-symmetry and in the charge density wave phase of 2 H –NbSe 2

Here we investigate carrier and collective mode dynamics in 2H-NbSe 2 using time-resolved optical pump-probe spectroscopy and compare the results with first-principles calculations. Broadband ultrafast reflectivity studies of 2H-NbSe 2 in a wide temperature interval covering the normal, charge density wave (CDW) and superconducting phase were performed. Spectral features observed in the transient reflectivity experiment were associated with specific optical transitions obtained from band structure calculations. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations of the soft phonon mode across the whole spectral range. Temperature evolution of this coherent phonon mode in the low-excitation linear regime shows softening of the mode down to the CDW transition temperature T CDW with subsequent hardening below T CDW . The global fit of the broadband probe data reveals four different relaxation times associated with characteristic electron-electron, electron-phonon, and phonon-phonon relaxation processes. From first-principles calculations of electron-phonon coupling we associate the few picosecond electron-phonon relaxation time $\tau_2$ with a specific group of phonons with frequencies around 20 meV. On the other hand, the anomalously long relaxation time of $\tau_3 \sim$ to 100 ps is associated with anharmonicity-driven phonon-phonon scattering. All relaxation processes result from anomalies near the second order CDW phase transition that are reflected in the temperature dependencies of the characteristic relaxation times and amplitudes of coherent oscillations. At the highest fluences we observe electronic melting of the CDW and disappearance of the mode hardening below T CDW .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Behavior of thermally quenched topological defects in quasicrystal artificial spin ices

We report that understanding the formation of topological defects in connected magnetic nanowires such as in artificial spin ices (ASIs) is critical to controlling their behavior. Moreover, emergent frustration behavior of these defects can be expected due to complex underlying lattice geometry of the ASIs. We have explored in situ thermalization and quenching of quasicrystalline ASIs, which exhibit additional frustration due to aperiodicity from near the Curie temperature, and we observe the formation of two sets of topological vortex defects: within the magnetic bars and within the vertices at which the bars meet. By varying the laser fluence, we show that the number of defects in the vertices varies as the quenching rate changes following a power law relation, which we interpret as being related to the ferromagnetic-to-paramagnetic phase transition. Conversely, the defects formed within the bars are metastable states related to the spontaneous magnetization reversal of the magnetic bars and are therefore strongly dependent on underlying lattice geometry. These results provide insight into the emergence and control of topological defects in confined frustrated magnetic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Disentangling electronic, lattice, and spin dynamics in the chiral helimagnet Cr 1/3 NbS 2

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet Cr 1/3 NbS 2 above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic $ab$-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, NbS 2 , and Cr-intercalated compounds. Time-resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, subpicosecond relaxation and subsequent buildup (τ > 50ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half-metallicity in Cr 1/3 NbS 2 , such a long demagnetization dynamic likely results from spin-lattice relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in Cr 1/3 NbS 2 with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Scanning ultrafast electron microscopy reveals photovoltage dynamics at a deeply buried $p^- \mathrm{Si/SiO_2}$ interface

The understanding and control of charge carrier interactions with defects at buried insulator/semiconductor interfaces is essential for achieving optimum performance in modern electronics. In this work, we report on the use of scanning ultrafast electron microscopy (SUEM) to remotely probe the dynamics of excited carriers at a Si surface buried below a thick thermal oxide. Our measurements illustrate a previously unidentified SUEM contrast mechanism, whereby optical modulation of the space-charge field in the semiconductor modulates the electric field in the thick oxide, thus affecting its secondary electron yield. By analyzing the SUEM contrast as a function of time and laser fluence we demonstrate the diffusion mediated capture of excited carriers by interfacial traps.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Atomlike interaction and optically tunable giant band-gap renormalization in large-area atomically thin MoS2

Coulomb interactions in atomically thin transition metal dichalcogenides can be dynamically engineered by exploiting the dielectric environment to control the optical and electronic properties. Here we demonstrate an optically tunable giant band-gap renormalization (BGR) ~1200 and 850 meV from the edge of the conduction band and complete suppression of the exciton absorption in large-area single-layer (1L) and three-layer (3L) MoS2, respectively. The observed giant BGR is two orders of magnitude larger than that in the conventional semiconductors, and it persists for tens of ps. Strikingly, our results demonstrate photoinduced transparency at the electronic band gap using an intense optical field at room temperature. Exciton bleach recovery in 1L and 3L show a contrasting fluence-dependent response, demonstrating the layer-dependent optical tuning of exciton lifetime in a way that would be both reversible and real time. We find that the optical band gap (exciton resonance peak) shows a transient redshift followed by an anomalous blueshift from the lowest energy point as a function of the photo-generated carrier density. The observed exciton energy shift is analogous to atom-atom interactions, and it varies as a Lennard-Jones like potential as a function of the interexciton separation.

2D semiconductors↗

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↗

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↗

Unveiling the underlying interactions in Ta 2 NiSe 5 from photoinduced lifetime change

We present a generic procedure for quantifying the interplay of electronic and lattice degrees of freedom in photodoped insulators through a comparative analysis of theoretical many-body simulations and time- and angle-resolved photoemission spectroscopy (TR-ARPES) of the transient response of the candidate excitonic insulator Ta 2 NiSe 5 . Our analysis demonstrates that the electron-electron interactions dominate the electron-phonon ones. In particular, a detailed analysis of the TR-ARPES spectrum enables a clear separation of the dominant broadening (electronic lifetime) effects from the much smaller band-gap renormalization. Theoretical calculations show that the observed strong spectral broadening arises from the electronic scattering of the photoexcited particle-hole pairs and cannot be accounted for in a model in which electron-phonon interactions are dominant. The competing interactions were quantified using the scaling analysis in the weak fluence regime. We demonstrate that the magnitude of the weaker subdominant band-gap renormalization sensitively depends on the distance from the semiconductor/semimetal transition in the high-temperature state, which could explain the apparent contradictions between various TR-ARPES experiments. The analysis presented here indicates that electron-electron interactions play a vital role (albeit not the sole one) in stabilizing the insulating state, and establishes the comparison between lifetime and gap evolution as an important probe of correlated insulators.

36 MATERIALS SCIENCE↗

Transient energy dissipation at the Fermi velocity in a magnetocaloric metal

Realizing fast energy dissipation in crystalline materials over macroscopic length scales is critical for energy-efficient devices and applications toward a carbon-neutral society but is usually dominated by electron-lattice interactions that cap the energy dissipation at the phonon velocity. Going beyond this velocity has been the focus of many studies, and the physical limit is the Fermi velocity where the energy is predominantly carried away by electrons throughout the materials. However, whether and how the Fermi velocity can be reached over macroscopic distances experimentally remain largely elusive. Here we show ultrafast energy dissipation at the Fermi velocity in the magnetocaloric metal LaFe 10.6 Co 1.0 Si 1.4 . Using time-resolved powder x-ray diffraction, we observe negative thermal expansion of the lattice throughout the micron-sized crystals in less than 600 fs with an incident optical fluence higher than 8 J cm -2 . The ultrafast timescale is in sharp contrast to the normal energy dissipation and shows the existence of a macroscopic momentum-relaxing electron mean free path immediately after the optical excitation. In conclusion, our findings open a different regime in energy dissipation and demonstrate the possibility of manipulating macroscopic material properties by strong optical pulses.

Chen, Yanna↗

Characteristic exciton energy scales in antiferromagnetic NiPS 3

Two-dimensional antiferromagnets are promising materials for spintronics. The van der Waals antiferromagnet NiPS 3 has attracted extensive interest due to its ultranarrow exciton feature which is closely linked with the magnetic ordering. Here, we use time-resolved terahertz spectroscopy to investigate photoexcited carriers in NiPS 3 . We identify the onset of interband transitions and estimate the exciton dissociation energy from the excitation wavelength and fluence dependence of the transient spectral weight. Furthermore, our results provide key insights to quantify the exciton characteristics and validate the band structure for NiPS 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Determining the 9 $\mathrm{Be}$($n, γ$) 10 $\mathrm{Be}$ integral cross section at fission neutron energies

The 9 B neutron capture cross section has significant implications for Be materials in the nuclear industry as well as the α process in stellar nucleosynthesis. While the cross section is well constrained at thermal neutron energies, there is a lack of experimental data at higher neutron energies, and the evaluated nuclear data libraries can differ by up to two orders of magnitude. We calculate the 9 Be(n, γ) 10 Be integral cross section at fission neutron energies in an effort to resolve disagreements amongst the nuclear data libraries. Foil irradiation experiments were performed using the Flattop critical assembly at the National Criticality Experiments Research Center with either the highly enriched U or Pu cores, with target foil stacks placed at multiple locations to exploit different neutron energy profiles. Accelerator mass spectrometry was used to measure the 10 Be/ 9 Be ratio in irradiated Be foils, while all other activation products were quantified through gamma spectrometry. The experiments were simulated using the Monte Carlo N-Particle radiation transport code and combined with experimental results to determine the total neutron fluence, while the staysl-pnnl suite and fispact-ii code were used to validate the model and assess the systematic uncertainty. The new 9 Be(n, γ) 10 Be integral cross sections calculated in this work are 26.5 ± 2.2µb at 0.59 ± 0.07 MeV, 24 ± 3 µb at 0.98 ± 0.14 MeV, 21.7 ± 1.3 µb at 1.26 ± 0.11 MeV, 21.8 ± 1.4 µb at 1.32 ± 0.11 MeV, and 18.6 ± 1.1 µb at 1.46 ± 0.13 MeV. These results do not agree with integral cross sections from any of the nuclear data library evaluations. Discrepancies between the new integral cross sections reported here and the nuclear data libraries suggest a more complex cross-section structure in the MeV range which allows for more resonance contributions, and more work is needed to further constrain the evaluated cross sections.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Fast radio burst dispersion measure distribution as a probe of helium reionization

Fast radio burst (FRB) discoveries are occurring rapidly, with thousands expected from upcoming surveys. The dispersion measures (DM) observed for FRB include important information on cosmological distances and the ionization state of the universe from the redshift of emission until today. Rather than considering the DM–redshift relation, we investigate the statistical ensemble of the distribution of dispersion measures. Here, we explore the use of this abundance information, with and without redshift information, to probe helium reionization through simulated data to redshift z = 6. Carrying out Monte Carlo simulations of FRB survey samples, we examine the effect of different source redshift distributions, host galaxy models, sudden vs gradual reionization, and covariance with cosmological parameters on determination of helium reionization properties. We find that a fluence limited survey with 10 4 FRBs can discriminate different helium reionization histories at ~6σ using the DM-distribution of bursts, without redshift information (and ~10σ with redshifts).

79 ASTRONOMY AND ASTROPHYSICS↗

Analysis of a tau neutrino origin for the near-horizon air shower events observed by the fourth flight of the Antarctic Impulsive Transient Antenna

In this work, we study in detail the sensitivity of the Antarctic Impulsive Transient Antenna (ANITA) to possible ν τ point source fluxes detected via τ-lepton-induced air showers. This investigation is framed around the observation of four upward-going extensive air shower events very close to the horizon seen in ANITA-IV. We find that these four upgoing events are not observationally inconsistent with τ-induced EASs from Earth-skimming ν τ both in their spectral properties as well as in their observed locations on the sky. These four events as well as the overall diffuse and point source exposure to Earth-skimming ν τ are also compared against published ultrahigh-energy neutrino limits from the Pierre Auger Observatory. While none of these four events occurred at sky locations simultaneously visible by Auger, the implied fluence necessary for ANITA to observe these events is in strong tension with limits set by Auger across a wide range of energies and is additionally in tension with ANITA’s Askaryan in-ice neutrino channel above 10 19 eV. We conclude by discussing some of the technical challenges with simulating and analyzing these near horizon events and the potential for future observatories to observe similar events.

79 ASTRONOMY AND ASTROPHYSICS↗