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At least 325 records · Page 18

Ballistic Δ S = 2 intersystem crossing in a cobalt cubane following ligand-field excitation probed by extreme ultraviolet spectroscopy

We report femtosecond M 2,3 -edge X-ray absorption near-edge structure (XANES) spectroscopy is used to probe the excited-state dynamics of the cobalt cubane [Co III 4 O 4 ](OAc) 4 (py) 4 (OAc = acetate, py = pyridine), a model for water oxidation catalysts. After ligand-field excitation, intersystem crossing (ISC) to a metal-centered quintet occurs in 38 fs. 30% of the hot quintet undergoes ballistic back-ISC directly to the singlet ground state, with the remainder relaxing to a long-lived triplet.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Extreme ultraviolet time- and angle-resolved photoemission setup with 21.5 meV resolution using high-order harmonic generation from a turn-key Yb:KGW amplifier

Characterizing and controlling electronic properties of quantum materials require direct measurements of nonequilibrium electronic band structures over large regions of momentum space. Here, we demonstrate an experimental apparatus for time- and angle-resolved photoemission spectroscopy using high-order harmonic probe pulses generated by a robust, moderately high power (20 W) Yb:KGW amplifier with a tunable repetition rate between 50 and 150 kHz. By driving high-order harmonic generation (HHG) with the second harmonic of the fundamental 1025 nm laser pulses, we show that single-harmonic probe pulses at 21.8 eV photon energy can be effectively isolated without the use of a monochromator. The on-target photon flux can reach 5 × 1010 photons/s at 50 kHz, and the time resolution is measured to be 320 fs. The relatively long pulse duration of the Yb-driven HHG source allows us to reach an excellent energy resolution of 21.5 meV, which is achieved by suppressing the space-charge broadening using a low photon flux of 1.5 × 108 photons/s at a higher repetition rate of 150 kHz. The capabilities of the setup are demonstrated through measurements in the topological semimetal ZrSiS and the topological insulator Sb2−xGdxTe3.

Liu, Yangyang↗

Probing coherent electronic superpositions of singly and doubly excited states of krypton with extreme-ultraviolet four-wave-mixing spectroscopy

Radiative nonlinear four-wave mixing can monitor the evolution of electronic wave packets, providing access to lifetimes and quantifying the light-induced couplings between excited states. In this article, we report the observation of quantum beats in an autoionizing electronic wave packet in krypton, probed using this technique. Analysis of the signal reveals that these beats originate from the contribution of previously unassigned, doubly excited states interacting with singly excited ones. We introduce a minimal theoretical model, based on multichannel quantum-defect theory, which quantitatively reproduces both the wave-packet dynamics and the static spectrum. This work combines a versatile, noncommensurate XUV-IR-based experimental scheme with a tractable model, establishing a powerful approach for the metrology and control of complex, correlated electronic states.

74 ATOMIC AND MOLECULAR PHYSICS↗

Resonant propagation of extreme-ultraviolet pulses through strongly driven high-density media

We show that by combining strong-field dressing and resonant propagation of XUV pulses, the transition of absorption lines from their natural Lorentzian profiles through Fano and complex multipeak shapes all the way back to broadened near-Lorentzian profiles can be achieved, in the limit of optically thick samples. The final stage of this spectral modification can be understood in terms of a significant temporal stretching and delay of the resonant XUV pulse as it propagates through the dense gas, which alters the ultrafast absorption that is modified by the time-synchronized few-femtosecond laser pulse. We first demonstrate this concept in numerical calculations, both using a model system and through a fully coupled solution of the time-dependent Schrödinger equation and the Maxwell wave equation. The applicability and generality of the underlying mechanism is then illustrated in proof-of-principle attosecond transient absorption measurements in a helium gas with a widely varying atomic density. These results provide insights into the interaction of ultrashort laser pulses with dense media and its coherent control. Published by the American Physical Society 2025

He, Yu (ORCID:0000000152120176)↗

Atomic layer deposition and its derivatives for extreme ultraviolet (EUV) photoresist applications

Solution-processed photoresists have been forerunners in semiconductor patterning for decades. Even with the drastic reduction in photolithography wavelength, traditional spin-on resists still support the fabrication of the most advanced, sub-5 nm node logic and memory devices using EUV lithography (EUVL) (λ = 13.5 nm). However, trade-off between resolution, sensitivity, and roughness in the conventional resists pose a critical challenge in the race towards device downscaling to 1 nm node. While great efforts are being made to improve spin-on EUV photoresist performance, there has been emergence of new approaches focused on developing novel resists via vapor-phase processing routes, such as atomic layer deposition (ALD) and its analogs. This review summarizes recent advances in EUVL photoresist development based on ALD and its derivative techniques, which include ALD-based inorganic–organic dry resists and hybrid resists synthesized by infiltrating conventional spin-on resists. Despite being in the early stage, initial studies have shown the great potential of ALD applications in EUVL photoresist development.

36 MATERIALS SCIENCE↗

Polarizers for the extreme ultraviolet.

Polarization characteristics of materials in XUV AND development of transmitting and reflecting polarizers, using multilayer metal films

ULTRAVIOLET SPECTRUM↗