Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Electronic coherent anti-Stokes Raman spectroscopy in CeF sub 3

Journal Article · · Journal of the Optical Society of America, Part B: Optical Physics; (United States)
 [1]
  1. Department of Physics, University of California, Berkeley, Berkeley, California (USA) Materials and Chemical Sciences Division, Lawrence Berkeley Laboratory, Berkeley, California (USA)
The coherent anti-Stokes Raman spectroscopy (CARS) of electronic states of the Ce{sup 3+} ion in a CeF{sub 3} crystal at 3.8 K is reported. CARS resonances involving the ground state of the {sup 2}{ital F}{sub 5/2} manifold and the Stark components of the {sup 2}{ital F}{sub 7/2} manifold at 2161 and 2239 cm{sup {minus}1} have been detected. Measurements were made with both visible ({lambda}{sub 1}{approx}476 nm, {lambda}{sub 2}=532 nm) and near-ultraviolet ({lambda}{sub 1}=355 nm, {lambda}{sub 2}{approx}385 nm) lasers. The enhancement of the third-order susceptibility owing to the electronic transitions, {vert bar}{chi}{sup (3){ital R}}/{chi}{sup (3)NR}{vert bar}{sub max}, is as great as 4.8. This represents an order-of-magnitude increase over that in singly resonant electronic CARS experiments in other rare-earth crystals. The CARS data also yielded accurate measurements of the Ce{sup 3+} electronic Raman cross sections. In the visible region, {sigma}{sub {ital zz}}(2161 cm{sup {minus}1})=(5.0{plus minus}1.1){times}10{sup {minus}30} cm{sup 2} and {sigma}{sub {ital zz}}(2239 cm{sup {minus}1})=(1.9{plus minus}0.7){times}10{sup {minus}30} cm{sup 2}. One could calculate both the absolute magnitude and the dispersion of {vert bar}{chi}{sup (3){ital R}}{vert bar}{sub max} by modeling the virtual intermediate states as a single degenerate 5{ital d} state at 45 000 cm{sup {minus}1}.
DOE Contract Number:
AC03-76SF00098
OSTI ID:
5254108
Journal Information:
Journal of the Optical Society of America, Part B: Optical Physics; (United States), Journal Name: Journal of the Optical Society of America, Part B: Optical Physics; (United States) Vol. 8:9; ISSN JOBPD; ISSN 0740-3224
Country of Publication:
United States
Language:
English