Non-resonant Coherent Amplitude Transfer in Attosecond Four-Wave Mixing Spectroscopy

Abstract

Attosecond four-wave mixing spectroscopy using an XUV pulse and two noncollinear near-infrared pulses is employed to measure Rydberg wavepacket dynamics resulting from extreme ultraviolet excitation of a 3s electron in atomic argon into a series of autoionizing 3s-1np Rydberg states around 29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the four wave mixing emission signals of each individually detected state. A wavepacket decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s-1(n+1)p states to the observed 3s-1np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. The theory highlights that coherent amplitude transfer is driven non-resonantly to the 3s-1np states by the near-infrared light through 3s-1(n+1)s and 3s-1(n-1)d dark states during the four-wave mixing process.

References in corpus (3)

• Solid-state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy
• A Coherent Light Shift on Alkaline-Earth Rydberg Atoms from Isolated Core Excitation without Auto-Ionization
• Raman interferometry between autoionizing states to probe ultrafast wavepacket dynamics with high spectral resolution

Cited by in corpus (2)

• Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four wave mixing spectroscopy
• Probing coherent electronic superpositions of singly- and doubly-excited states of krypton with attosecond four-wave mixing spectroscopy