Ultrafast Dynamics in Condensed Matter Studied with Attosecond Extreme Ultraviolet Transient Reflectivity

Ultrafast Dynamics in Condensed Matter Studied with Attosecond Extreme Ultraviolet Transient Reflectivity

Ultrafast Dynamics in Condensed Matter Studied with Attosecond Extreme Ultraviolet Transient Reflectivity By Christopher J Kaplan A dissertation submitted in partial satisfaction of the requirements for the degree of Doctor of Philosophy in Chemistry in the Graduate Division of the University of California, Berkeley Committee in charge: Professor Stephen R. Leone, co-Chair Professor Daniel M. Neumark, Co-Chair Professor William H. Miller Professor David Attwood Spring 2019 Ultrafast Dynamics in Condensed Matter Studied with Attosecond Extreme Ultraviolet Transient Reflectivity Copyright 2019 by Christopher J Kaplan Abstract Ultrafast Dynamics in Condensed Matter Studied with Attosecond Extreme Ultraviolet Transient Reflectivity by Christopher J Kaplan Doctor of Philosophy in Chemistry University of California, Berkeley Professor Stephen R. Leone, Co-Chair Professor Daniel M. Neumark, Co-Chair The advent of attosecond pulse duration light sources has enabled the study of fundamental light-matter interactions. Condensed matter systems are of particular interest, as they are often significantly impacted by many body interactions, and thus provide a natural environment for the observation and study of such interactions in the time domain. In this dissertation, an apparatus for extreme ultraviolet (XUV) transient reflectivity is described, and several studies on ultrafast dynamics in solids are performed. In the first chapter, background on ultrafast spectroscopy, light matter interaction, and reflection from surfaces is provided, giving the necessary underpinnings for the subsequent discussion. In the second chapter, the development and capabilities of the constructed XUV transient reflection apparatus are reviewed. Additionally, the static refractive index of germanium (a commonly employed semiconductor), is recovered from multi angle reflection measurements. In the third chapter, femtosecond dynamics in germanium are studied by XUV transient reflection. The results are analyzed and interpreted in the context of the existing optical literature. In the fourth chapter, preliminary attosecond resolved measurements in germanium are presented, and the results are tentatively interpreted in the context of light dressed states. In the fifth chapter, attosecond dynamics of core excitons in magnesium oxide (MgO) are studied. The results are analyzed and interpreted as a light induced modification of excitonic coherence. This body of work is intended to establish XUV transient reflectivity as a technique for study of solid-state systems and to provide example studies in two representative systems, a semiconductor and an insulator. “For me, it is far better to grasp the Universe as it really is than to persist in delusion, however satisfying and reassuring.” – Carl Sagan ++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++ 0+0#!"#" #!" (++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++0 0+0+0 $ , !" #!" (++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++1 0+0+1#!"# !"""""+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++2 0+0+2!!#+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++3 0+1!,%" #!" (+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++4 0+1+0#!"#!$#$!""++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++4 0+1+1"! #++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++6 0+1+2#!$#"!%"++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++6 0+1+3%#"!#+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++8 0+1+4 !#),!$+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++0/ 0+1+5"! #!#*#$#% !"++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++00 0+1+6$%""$!""#%#(!#%#(++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++01 ++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++! 1+0' !#%!%&+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++03 1+0+0!#" #!#!++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++07 1+0+1 ##!# #++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++1/ 1+0+2!!!##"# !"##(++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++11 1+1 %!("##!!#%'!$++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++12 1+1+0 #!"#"++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++14 1+2 "$#""$""++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++15 1+2+0 %!(!!#%'+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++15 1+2+1("" %!(+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++17 1+2+2("" !#% '++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++2/ 1+3$"+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++22 +++++++++++++++++++++++++++++++++++++++++++++++++++++ ! 2+0 #!$#+++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++24 2+1 #"++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++25 2+1+0!"# #%#(++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++++25 2*1*1 # ******************************************************************************************************************28 2*2 "$#""$""***************************************************************************************************************30 2*2*0!"# #%#(************************************************************************************************************30 2*2*1"##!"#!#%#(#!!!"!("#***********************************31 2*2*2""###!"%#!$#*************************************************************34 2*2*3""#%#(#****************************************************************************************************36 2*2*4!!!#!)##"**************************************************************************38 2*3$"*********************************************************************************************************************************42 ***************************************************************** 3*0#!$#*******************************************************************************************************************************44 3*1 #"************************************************************************************************************************************46 3*1*0!"# #%#(************************************************************************************************************46 3*1*1,#!$#$!$#"**************************************************************************************************47 3*1*2""##+"#!$*************************************************************************************5/ 3*1*3#(""##"#!"#!#%#(""******************************************************50 3*2 "$#""$""***************************************************************************************************************51 3*2*0!"##$!"****************************************************************************************************************51 3*2*1!!!(""#!#%'#****************************************************************************54 3*2*2!""##$#"***************************************************************************************************56 3*2*2 $# $#"**************************************************************************************************6/ 3*3$"*********************************************************************************************************************************61 ***************************************************************************** 4*0#!$#*******************************************************************************************************************************62 4*0*0'#"""******************************************************************************************************************63 4*0*1#!##$#!'#" ********************************************************************65 4*1'!#******************************************************************************************************************************67 4*2 "$#"***************************************************************************************************************************************68 4*2*0##!#"#!$****************************************************************************************************68 4*2*1 %!(#'%$!!#%'******************************************************************70 4*2*2!"#!# ***********************************************************************************************72 4*2*3 &!**************************************************************************************************************76

View Full Text

Details

  • File Type
    pdf
  • Upload Time
    -
  • Content Languages
    English
  • Upload User
    Anonymous/Not logged-in
  • File Pages
    120 Page
  • File Size
    -

Download

Channel Download Status
Express Download Enable

Copyright

We respect the copyrights and intellectual property rights of all users. All uploaded documents are either original works of the uploader or authorized works of the rightful owners.

  • Not to be reproduced or distributed without explicit permission.
  • Not used for commercial purposes outside of approved use cases.
  • Not used to infringe on the rights of the original creators.
  • If you believe any content infringes your copyright, please contact us immediately.

Support

For help with questions, suggestions, or problems, please contact us