skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses

Authors:
; ; ORCiD logo; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1257498
Grant/Contract Number:
FG02-04ER15571
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physica Scripta
Additional Journal Information:
Journal Volume: T169; Related Information: CHORUS Timestamp: 2016-06-17 03:27:02; Journal ID: ISSN 0031-8949
Publisher:
IOP Publishing
Country of Publication:
Sweden
Language:
English

Citation Formats

Bennett, Kochise, Zhang, Yu, Kowalewski, Markus, Hua, Weijie, and Mukamel, Shaul. Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses. Sweden: N. p., 2016. Web. doi:10.1088/0031-8949/T169/1/014002.
Bennett, Kochise, Zhang, Yu, Kowalewski, Markus, Hua, Weijie, & Mukamel, Shaul. Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses. Sweden. doi:10.1088/0031-8949/T169/1/014002.
Bennett, Kochise, Zhang, Yu, Kowalewski, Markus, Hua, Weijie, and Mukamel, Shaul. Thu . "Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses". Sweden. doi:10.1088/0031-8949/T169/1/014002.
@article{osti_1257498,
title = {Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses},
author = {Bennett, Kochise and Zhang, Yu and Kowalewski, Markus and Hua, Weijie and Mukamel, Shaul},
abstractNote = {},
doi = {10.1088/0031-8949/T169/1/014002},
journal = {Physica Scripta},
number = ,
volume = T169,
place = {Sweden},
year = {Thu Jun 16 00:00:00 EDT 2016},
month = {Thu Jun 16 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1088/0031-8949/T169/1/014002

Citation Metrics:
Cited by: 3works
Citation information provided by
Web of Science

Save / Share:
  • Expressions for the two-dimensional stimulated x-ray Raman spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth (181 as, 14.2 eV FWHM) pulses tuned to the oxygen and nitrogen K-edges. Crosspeaks in 2D signals reveal electronic Franck-Condon overlaps between valence orbitals and relaxed orbitals in the presence of the core-hole.
  • We propose two-dimensional x-ray coherent correlation spectroscopy for the study of interactions between core-electron and valence transitions. This technique may find experimental applications in the future when very high intensity x-ray sources become available. Spectra obtained by varying two delay periods between pulses show off-diagonal crosspeaks induced by coupling of core transitions of two different types. Calculations of the N1s and O1s signals of aminophenol isomers illustrate how novel information about many-body effects in electronic structure and excitations of molecules can be extracted from these spectra.
  • Spontaneous and stimulated resonant inelastic x-ray Raman-scattering signals are calculated using the Keldysh-Schwinger closed-time path loop and expressed as overlaps of doorway and window electron-hole wave packets. These are recast in terms of the one-particle Green's functions and expansion coefficients of configuration-interaction singles for valence excitations, which can be obtained from standard electronic structure codes. Calculation for many-body states of ground and core-excited systems is avoided.
  • Cited by 8
  • A method is presented to simplify Bragg coherent X-ray diffraction imaging studies of complex heterogeneous crystalline materials with a two-stage screening/imaging process that utilizes polychromatic and monochromatic coherent X-rays and is compatible with in situ sample environments. Coherent white-beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three-dimensional reciprocal-space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifyingin situchamber design. This approach was demonstrated with Au nanoparticles and will enable,more » for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.« less