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Nonlinear reversal of photoexcitation on the attosecond time scale improves ultrafast X-ray diffraction images
The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.
Attosecond Coherence Time Characterization in Hard X-Ray Free-Electron Laser
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Generation of Terawatt Attosecond Pulses from Relativistic Transition Radiation
When a femtosecond duration and hundreds of kiloampere peak current electron beam traverses the vacuum and high-density plasma interface, a new process, that we call here relativistic transition radiation (RTR), generates an intense ~ 100 as pulse containing ~ 1 terawatt power of coherent vacuum ultraviolet (VUV) radiation accompanied by several smaller femtosecond duration satellite pulses. This pulse inherits the radial polarization of the incident beam field and has a ring intensity distribution. This RTR is emitted when the beam density is comparable to the plasma density and the spot size much larger than the plasma skin depth. Physically, it arises from the return current or backward relativistic motion of electrons starting just inside the plasma that Doppler up shifts the emitted photons. The number of RTR pulses is determined by the number of groups of plasma electrons that originate at different depths within the first plasma wake period and emit coherently before phase mixing.
Attosecond Intramolecular Scattering and Vibronic Delays
We study the temporal and vibrational signature of the universal nuclear recoil associated with the electron emission and intramolecular scattering that accompanies the photoelectric effect. We illustrate these phenomena in the photoionization of the CO molecule from the C-1s orbital using an analytical model that reproduces the entangled character of the nuclear and electronic motion in this process. We show that the photoelectron emission delay can be decomposed into its localization and resonant-confinement components. Photoionization by a broadband x-ray pulse results in a coherent vibrational ionic state delayed compared to the classical sudden-photoemission limit.
Techniques to generate intense isolated attosecond pulses from relativistic plasma mirrors
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Attosecond electronic dynamics of core-excited states of N 2 O in the soft x-ray region
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Charge migration and attosecond solitons in conjugated organic molecules
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Asymmetric Attosecond Photoionization in Molecular Shape Resonance
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Spooktroscopy: a new approach to attosecond spectroscopy
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Probing Attosecond Electron Dynamics With an X-Ray Free-Electron Laser
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