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At least 271 records · Page 15

Pulse-by-pulse transient thermal deformation in crystal optics under high-repetition-rate FEL

Time-domain modeling of the thermal deformation of crystal optics can help define acceptable operational ranges across the pulse-energy repetition-rate phase space. In this paper, we have studied the transient thermal deformation of a water-cooled diamond crystal for a cavity-based X-ray free-electron laser (CBXFEL), either an X-ray free-electron laser oscillator (XFELO) or a regenerative amplifier X-ray free-electron laser (RAFEL), by numerical simulations including finite-element analysis and advanced data processing. Pulse-by-pulse transient thermal deformation of a 50 µm-thick diamond crystal has been performed with X-ray pulse repetition rates between 50 kHz and 1 MHz. Results for temperature and thermal deformation have been compared with the results of transient analysis using a continuous wave (CW) power loading. Temperature and thermal deformation results from pulse-by-pulse transient analysis vary with time about the results for the CW case for the same average power. The variation amplitude increases with pulse energy and decreases with repetition rate. When the repetition rate increases to infinity, both temperature and thermal deformation converge to the results for the CW case. Two critical time scales for the operation of crystal optics in a CBXFEL are (1) first-turn time, i.e. the time for the XFEL pulse to complete the first turn around the cavity so that the crystal sees the recirculated XFEL pulse, and (2) period-end time, i.e. the time that the next electron bunch arrives for the amplification, so that the crystal outcouples the amplified FEL power. For the same average power, simulation results show that the crystal thermal deformation seen by the XFEL beam decreases with repetition rate at the first-turn time of a 300 m-long cavity and increases with repetition rate at the period-end time. For the wavefront preservation requirement of the crystal optics, a pulse-energy versus repetition-rate phase space has been established. The upper bounds of the pulse energy at both first-turn and period-end times decreases with repetition rate, especially at the period-end time. The upper bound of the thermal deformation of the crystal at the period-end time for any repetition frequency can be estimated from the CW case. For a water-cooled diamond crystal of dimension 5 mm × 5 mm × 0.05 mm, the time to reach a quasi steady-state is about 50 ms for temperature and 50 µs for thermal deformation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Probing Attosecond Bound Electron Dynamics Driven by Strong-Field Light Transients

The project aimed to drive strong-field excitation of bound electronic coherences in gas-phase atoms and molecules using a novel source of near-single-cycle optical field transients, based on industrial-grade Yb:solid-state laser technology. Key objectives included generating near-single cycle field transients and isolated attosecond pulses, reconstructing time-dependent wave packets in atoms and molecules, probing their decoherence using attosecond interferometry, and controlling the dynamic evolution of systems on attosecond to few-femtosecond timescales. A secondary goal of the project was to develop field-resolved measurement platforms as a novel approach for studying electron dynamics in atomic and molecular systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

Transient periodicities in X-ray-active red dwarfs - First results from Mount Cuba and interpretation with an oscillating loop model

Results from a program at the Mount Cuba Astronomical Observatory to optically monitor transient periodicities in flare stars are reported. The data are analyzed for periodicities by means of a modified autocorrelation approach. A randomization technique is used to assess the statistical significance of periods. In AD Leonis, variability with amplitude 0.4 percent and a period of 4.1 min was detected during one run on March 6, 1991: the probability that this periodicity is due to chance is 10 exp -5. Further observations obtained on AD Leo within 1-2 hr on the same night showed no significant variability (0.01). It is shown that optical periodicities of the sort detected may be interpreted as arising from oscillations in coronal loops.

Mullan, D. J.↗

High-resolution spectroscopy of the optical candidate for the X-ray transient X0331 + 53

High-resolution spectral observations of the optical candidate for the X-ray transient X0331 + 53 are presented. The data show broad hydrogen and helium emission and strong interstellar absorption corresponding to a visual extinction of about 7 mag. No photospheric absorption in the emission lines, and no radial-velocity variations greater than 0.5 km/s were found over a three-day period. It is concluded that the optical continuum does not arise at or near the primary star. As an example of the spectrographic data, a resolution profile of H-alpha emission in X0331 + 53 is provided.

Stocke, J.↗

Proton radiation effects on electronic defect states in MOCVD-grown (010) β -Ga 2 O 3

The impact of 1.8 MeV proton irradiation on metalorganic chemical vapor deposition grown (010) β-Ga 2 O 3 Schottky diodes is presented. It is found that after a 10.8 × 10 13 cm –2 proton fluence the Schottky barrier height of (1.40 ± 0.05 eV) and the ideality factor of (1.05 ± 0.05 ) are unaffected. Capacitance–voltage extracted net ionized doping curves indicate a carrier removal rate of 268 ± 10 cm –1 . The defect states responsible for the observed carrier removal are studied through a combination of deep level transient and optical spectroscopies (DLTS/DLOS) as well as lighted capacitance–voltage (LCV) measurements. The dominating effect on the defect spectrum is due to the E c -2.0 eV defect state observed in DLOS and LCV. This state accounts for ~75 % of the total trap introduction rate and is the primary source of carrier removal from proton irradiation. Of the DLTS detected states, the E c -0.72 eV state dominated but had a comparably smaller contribution to the trap introduction. These two traps have previously been correlated with acceptor-like gallium vacancy-related defects. Several other trap states at E C -0.36, E C -0.63, and E C -1.09 eV were newly detected after proton irradiation, and two pre-existing states at E C -1.2 and E C -4.4 eV showed a slight increase in concentration after irradiation, together accounting for the remainder of trap introduction. However, a pre-existing trap at E c -0.40 eV was found to be insensitive to proton irradiation and, therefore, is likely of extrinsic origin. Furthermore, the comprehensive defect characterization of 1.8 MeV proton irradiation damage can aid the modeling and design for a range of radiation tolerant devices.

42 ENGINEERING↗

Connecting Femtosecond Transient Absorption Microscopy with Spatially Coregistered Time Averaged Optical Imaging Modalities

Multimodal all-optical imaging involving coregistered femtosecond transient absorption microscopy (TAM), time-integrated photoluminescence (PL), and steady-state modalities such as confocal reflectance and transmission offers an appealing approach to gain a comprehensive understanding of complex electronic excited-state phenomena in spatially heterogeneous systems. A unique combination of these modalities allows us to unravel not only the competing electronic excited-state dynamical processes but also the underlying morphological information with simultaneous high temporal and spatial resolution. However, correlating the various images obtained from time-resolved and time-independent modalities is generally nontrivial and particularly challenging when the electronic dynamics under study evolve in both time and space. Here, we demonstrate a new approach for rationally correlating time-resolved microscopy with coregistered time-integrated or steady-state modalities. Specifically, our approach involves an extended global lifetime analysis of the time-resolved microscopic data set to separate distinct dynamical processes taking place on commensurate time scales, and the resulting decay-associated amplitude maps (DAAMs) were applied to explore correlations with the images acquired using time-independent modalities. The feasibility of our approach was validated through analyzing a multimodal data set acquired from a thin film of chloride-containing mixed lead halide perovskites (CH 3 NH 3 PbI 3–x Cl x ) using femtosecond transient absorption, time-integrated PL, and confocal reflectance microscopies. Analysis of the results obtained enable us to gain new insight into the complex ultrafast relaxation dynamics in this highly heterogeneous system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radiolytic degradation of n -dodecane: Insights from time resolved pulsed electron radiolysis using aromatic scavengers

This study uses time-resolved picosecond pulsed electron radiolysis and transient absorbance spectroscopy to investigate early radiolytic processes in n-dodecane, a prototypical organic solvent for reprocessing used nuclear fuel (UNF). The primary radical cation, solvated electron, and excited states in neat n-dodecane are formed and consumed on timescales that are difficult to observe directly. Aromatic solutes, biphenyl and benzophenone, were utilized as scavengers to convert these short-lived species into longer-lived, optically detectable transient products to serve as indirect probes of the fraction of the initial n-dodecane radiolytic products that can be intercepted before undergoing ultrafast decay or competing reactions. The transient absorbance spectra of these scavengers and their radiolytic products were analyzed. Results indicate that while biphenyl and benzophenone effectively capture several radiolytic species, they do not fully scavenge all n-dodecane excited states, suggesting potential inefficiencies or additional side reactions. This study provides insight into the formation and accessibility of radiation-induced excited states and charge carriers in n-dodecane, which play a key role in the degradation of solvent extraction systems used in UNF reprocessing.

58 GEOSCIENCES↗

Detailed measurements of the H beta line shape in a transient plasma using a fiber optics slit system

Through the use of fiber optics, a series of very narrow slits have been constructed and placed at the exit plane of a spectrograph. Plasma radiation which is dispersed by the spectrograph is incident on the slits and is transmitted to separate phototubes via the quartz fibers. With this technique, time resolved measurements of the spectral shape of the hydrogen H beta line have been made and used to determine the electron density of a transient plasma. Data obtained in a shock tube indicated that the thermodynamic conditions behind the reflected shock in a mixture of 20 percent H 80 percent He correspond to theoretically predicted conditions.

Stickford, G. H., Jr.↗

Detailed measurements of the H beta line shape in a transient plasma using a fiber optics slit system.

Through the use of fiber optics, a series of very narrow slits have been constructed and placed at the exit plane of a spectrograph. Plasma radiation which is dispersed by the spectrograph is incident on the slits and is transmitted to separate phototubes via the quartz fibers. With this technique, time resolved measurements of the spectral shape of the hydrogen H beta line have been made and used to determine the electron density of a transient plasma. Data obtained in a shock tube indicated that the thermodynamic conditions behind the reflected shock in a mixture of 20% H2-80% He, at incident shock speeds of 12 to 14 km/sec and pressures of 66.6 to 133.3 N/sq m (0.5 to 1.0 mm Hg), correspond to theoretically predicted conditions. Immediately behind the incident shock at speeds of 17 to 24 km/sec the data indicate that the plasma reached equilibrium then demonstrated a drop in intensity which has been attributed to radiative cooling.

Stickford, G. H., Jr.↗

Autoionizing Polaritons in Attosecond Atomic Ionization

Light-induced states and Autler-Townes splitting of laser-coupled states are common features in the photoionization spectra of laser-dressed atoms. The entangled light-matter character of metastable Autler-Townes multiplets, which makes them autoionizing polaritons, however, is still largely unexplored. We employ attosecond transient-absorption spectroscopy in argon to study the formation of polariton multiplets between the 3s –1 4p and several light-induced states. We measure a controllable stabilization of the polaritons against ionization, in excellent agreement with ab initio theory. Using an extension of the Jaynes-Cummings model to autoionizing states, we show that this stabilization is due to the destructive interference between the Auger decay and the radiative ionization of the polaritonic components. Furthermore, these results give new insights into the optical control of electronic structure in the continuum and unlock the door to applications of radiative stabilization in metastable polyelectronic systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

Transient fading X-ray emission detected during the optical rise of a tidal disruption event

ABSTRACT We report on the SRG/eROSITA detection of ultra-soft ($kT=47^{+5}_{-5}$ eV) X-ray emission (LX =$2.5^{+0.6}_{-0.5} \times 10^{43}$ erg s−1) from the tidal disruption event (TDE) candidate AT 2022dsb ∼14 d before peak optical brightness. As the optical luminosity increases after the eROSITA detection, then the 0.2–2 keV observed flux decays, decreasing by a factor of ∼39 over the 19 d after the initial X-ray detection. Multi-epoch optical spectroscopic follow-up observations reveal transient broad Balmer emission lines and a broad He ii 4686 Å emission complex with respect to the pre-outburst spectrum. Despite the early drop in the observed X-ray flux, the He ii 4686 Å complex is still detected for ∼40 d after the optical peak, suggesting the persistence of an obscured hard ionizing source in the system. Three outflow signatures are also detected at early times: (i) blueshifted H α emission lines in a pre-peak optical spectrum, (ii) transient radio emission, and (iii) blueshifted Ly α absorption lines. The joint evolution of this early-time X-ray emission, the He ii 4686 Å complex, and these outflow signatures suggests that the X-ray emitting disc (formed promptly in this TDE) is still present after optical peak, but may have been enshrouded by optically thick debris, leading to the X-ray faintness in the months after the disruption. If the observed early-time properties in this TDE are not unique to this system, then other TDEs may also be X-ray bright at early times and become X-ray faint upon being veiled by debris launched shortly after the onset of circularization.

Malyali, A. (ORCID:0000000288514019)↗

Searching for Soft Relativistic Jets in Core-Collapse Supernovae with the IceCube Optical Follow-up Program

Context. Transient neutrino sources such as Gamma-Ray Bursts (GRBs) and Supernovae (SNe) are hypothesized to emit bursts of high-energy neutrinos on a time-scale of < or approx.100 s. While GRB neutrinos would be produced in high relativistic jets, core-collapse SNe might host soft-relativistic jets, which become stalled in the outer layers of the progenitor star leading to an efficient production of high-energy neutrinos. Aims. To increase the sensitivity to these neutrinos and identify their sources, a low-threshold optical follow-up program for neutrino multiplets detected with the IceCube observatory has been implemented. Methods. If a neutrino multiplet, i.e. two or more neutrinos from the same direction within 100 s, is found by IceCube a trigger is sent to the Robotic Optical Transient Search Experiment, ROTSE. The 4 ROTSE telescopes immediately start an observation program of the corresponding region of the sky in order to detect an optical counterpart to the neutrino events. Results. No statistically significant excess in the rate of neutrino multiplets has been observed and furthermore no coincidence with an optical counterpart was found. Conclusions. The search allows, for the first time, to set stringent limits on current models predicting a high-energy neutrino flux from soft relativistic hadronic jets in core-collapse SNe. We conclude that a sub-population of SNe with typical Lorentz boost factor and jet energy of 10 and 3 x 10(exp 51) erg, respectively, does not exceed 4:2% at 90% confidence.

Abbasi, R.↗

Multipolariton control in attosecond transient absorption of autoionizing states

Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s –1 4p and dark 3s –1 4f autoionizing states of argon that lead to Autler-Townes-like interactions, forming entangled light-matter states or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dressing-laser frequency. Our experimental measurements and theoretical essential-state simulations show good agreement and reveal how the delay, frequency, and intensity of the dressing pulse govern the properties of autoionizing polariton multiplets. Furthermore, these results demonstrate new pathways for quantum control of autoionizing states with optical fields.

74 ATOMIC AND MOLECULAR PHYSICS↗

Reliable Determination of Pulses and Pulse-Shape Instability in Ultrashort Laser Pulse Trains Using Polarization-Gating and Transient-Grating Frequency-Resolved Optical Gating Using the RANA Approach

Devices that measure the presence of instability in the pulse shapes in trains of ultrashort laser pulses do not exist, so this task necessarily falls to pulse-measurement devices, like Frequency-Resolved Optical Gating (FROG) and its variations, which have proven to be a highly reliable class of techniques for measuring stable trains of ultrashort laser pulses. Fortunately, multi-shot versions of FROG have also been shown to sensitively distinguish trains of stable from those of unstable pulse shapes by displaying readily visible systematic discrepancies between the measured and retrieved traces in the presence of unstable pulse trains. However, the effects of pulse-shape instability and algorithm stagnation can be indistinguishable, so a never-stagnating algorithm—even when instability is present—is required and is generally important. In previous work, we demonstrated that our recently introduced Retrieved-Amplitude N-grid Algorithmic (RANA) approach produces highly reliable (100%) pulse-retrieval in the second-harmonic-generation (SHG) version of FROG for thousands of sample trains of pulses with stable pulse shapes. Further, it does so even for trains of unstable pulse shapes and thus both reliably distinguishes between the two cases and provides a rough measure of the degree of instability as well as a reasonable estimate of most typical pulse parameters. Here, we perform the analogous study for the polarization-gating (PG) and transient-grating (TG) versions of FROG, which are often used for higher-energy pulse trains. We conclude that PG and TG FROG, coupled with the RANA approach, also provide reliable indicators of pulse-shape instability. In addition, for PG and TG FROG, the RANA approach provides an even better estimate of a typical pulse in an unstable pulse train than SHG FROG does, even in cases of significant pulse-shape instability.

47 OTHER INSTRUMENTATION↗

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Reconciling the Different Apparent Decay Pathways for Iron(III) Tetraphenylporphyrin Chloride: Evidence for Excited State Branching

Detailed understanding of the photophysical properties of metalloporphyrins is key to rationally exploiting them in a variety of applications ranging from photocatalysis to opto-magnetics. Previous studies of the ferric-tetraphenylporphyrin chloride have provided contradictory descriptions of the excited state evolution. Optical transient-absorption suggested initial formation of a ππ* excited state, followed by ligand-to-metal charge-transfer (LMCT) from the porphyrin ring and then decay on the ∼2 ps time scale to a metal-centered excited state that had a lifetime of ∼15 ps. In contrast, femtosecond extreme ultraviolet transient-absorption at the Fe M 2,3 -edge, while agreeing on the initial formation of an LMCT state, found evidence that this decayed in ∼2 ps to the ground state. Here, we have used K-edge transient X-ray absorption and X-ray emission, together with time-resolved X-ray solution scattering to explore this system. Based on these data, we propose a new model, consistent with both the earlier and the current data, in which photoexcited FeTPPCl evolves through three different states on the LMCT manifold, with the ∼2 ps decay now seen to involve a branching between return to the ground state (∼70%) and formation of a long-lived LMCT state (∼30%).

Excited states↗