Title: Hard x-ray – optical four-wave mixing using a split-and-delay line

Abstract

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray,more » x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.« less

Authors:

Peters, William K. ;

• Search DOE PAGES for author "Peters, William K."
• Search DOE PAGES for ORCID "0000-0002-1270-7623"

Feltman, Jacob; Jones, Travis ;

• Search DOE PAGES for author "Jones, Travis"
• Search DOE PAGES for ORCID "0000-0001-9209-9869"

Song, Sanghoon; Chollet, Matthieu; Robinson, Joseph; Padmanabhan, Prashant; Foglia, Laura; Bencivenga, Filippo; Coffee, Ryan; Bowlan, Pamela

• Search DOE PAGES for author "Bowlan, Pamela"
• Search DOE PAGES for ORCID "0000-0002-5325-6451"

Publication Date:

Fri Sep 08 00:00:00 EDT 2023

Research Org.:

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:

USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

2293615

Alternate Identifier(s):

OSTI ID: 1999562

Report Number(s):

LA-UR-22-29673
Journal ID: ISSN 1094-4087; OPEXFF

Grant/Contract Number:  

20180242ER; 20210290ER; AC02-76SF00515; 89233218CNA000001

Resource Type:

Published Article

Journal Name:

Optics Express

Additional Journal Information:

Journal Name: Optics Express Journal Volume: 31 Journal Issue: 19; Journal ID: ISSN 1094-4087

Publisher:

Optical Society of America

Country of Publication:

United States

Language:

English

Subject:

47 OTHER INSTRUMENTATION; Materials Science