Raman Interferometry between Autoionizing States to Probe Ultrafast Wave-Packet Dynamics with High Spectral Resolution

Journal Article · 22 February 2022 · Physical Review Letters

DOI: https://doi.org/10.1103/physrevlett.128.083001 · OSTI ID:1980263

Plunkett, A.  ^[1]; Alarcón, M.  A.  ^[2]; Wood, J.  K.  ^[3]; Greene, C.  H.  ^[2]; Sandhu, A.  ^[3]

---

1. Univ. of Arizona, Tucson, AZ (United States); OSTI
2. Purdue Univ., West Lafayette, IN (United States)
3. Univ. of Arizona, Tucson, AZ (United States)

Photoelectron interferometry with femtosecond and attosecond light pulses is a powerful probe of the fast electron wave-packet dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain both high temporal and spectral resolution by stimulating Raman interferences with one light pulse and monitoring the modification of the electron yield in a separate step. Applying this spectroscopic approach to the autoionizing states of argon, we experimentally resolved its electronic composition and time evolution in exquisite detail. Theoretical calculations show remarkable agreement with the observations and shed light on the light-matter interaction parameters. Using appropriate Raman probing and delayed detection steps, this technique enables highly sensitive probing and control of electron dynamics in complex systems.

• Research Organization: Purdue Univ., West Lafayette, IN (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
• Grant/Contract Number: SC0010545
• OSTI ID: 1980263
• Journal Information: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 8 Vol. 128; ISSN 0031-9007
• Publisher: American Physical Society (APS)Copyright Statement
• Country of Publication: United States
• Language: English