Laser pulses for coherent xuv Raman excitation

Abstract

We combine multi-channel electronic structure theory with quantum optimal control to derive Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and phase control facilitated by the pump pulse carrier envelope phase. Our results open a route to creating core-hole excitations in molecules and aggregates that locally address specific atoms and represent the first step towards realization of multidimensional spectroscopy in the xuv and x-ray regimes.

References in corpus (6)

• Decoherence in Attosecond Photoionization
• Theory of Attosecond Transient Absorption Spectroscopy of Krypton for Overlapping Pump and Probe Pulses
• Protecting coherence in Optimal Control Theory: State dependent constraint approach
• The Impact of Multichannel and Multipole Effects on the Cooper Minimum in the High-Harmonics Spectrum of Argon
• Enhanced nonlinear response of Ne${}^{8+}$ to intense ultrafast x rays
• Many-body interaction in semiconductors probed with 2D Fourier spectroscopy

Cited by in corpus (6)

• Training Schrödinger's cat: quantum optimal control
• Strong-field quantum control in the extreme ultraviolet using pulse shaping
• Quantum optimal control of photoelectron spectra and angular distributions
• Maximizing Hole Coherence in Ultrafast Photoionization of Argon with SPA-Optimization
• Dissipative Quantum Dynamics and Optimal Control using Iterative Time Ordering: An Application to Superconducting Qubits
• Optimized pulses for Raman excitation through the continuum: verification using multi-configurational time-dependent Hartree-Fock