Nonlinear Optics - Time Dependent Hartree-Fock
- In MOPAC2009, it is possible to perform calculations of the first and second static hyperpolarizabilities, as well as of other nonlinear optical properties of a lanthanide complex, by using the
POLAR keyword.
- As an example, let us consider the complex LOWBEE: [(1,10-(1,1'-Dimethylene-3,3'-biisoquinoline-2,2'-dioxide)-4,7,13,16-tetraoxa-1,10-diazaoctadecaphane)-(trifluoromethanesulfonato-O,O')-europium(iii)], below:
- First you must draw the structure of your complex and prepare a MOPAC2009 input data file. For that purpose, please follow the Drawing Complexes tutorial.
- In the Drawing Complexes tutorial, instead of step 5 of the Optimize the geometry of the lanthanide complex with MOPAC2009 do the following: in the field “Additional keywords”, replace
GNORM=0.01 by GNORM=0.25, add SPARKLE, and add POLAR(E=(0.0)), as such: GNORM=0.25 SPARKLE POLAR(E=(0.0)).
- Finish the Drawing Complexes tutorial. As an example, we provide the MOPAC2009 input file lowbee.mop.
- The nonlinear optics results are presented in the end of the MOPAC2009 .out file, as shown below:
<![CDATA[
******************** TDHF POLARIZABILITIES ********************
ENERGY OF "REORIENTED" SYSTEM WITHOUT FIELD: 103.7009259626
NFREQ= 1 IWFLB= 0 IBET= 1 IGAM= 1
ATOL= 0.10000D-02 BTOL= 0.10000D-02 MAXITU= 500 MAXITA= 150
*****************************************************************
CALCULATION OF STATIC FIELD QUANTITIES
*****************************************************************
+++++ ALPHA AT 0.00000 EV.
COMPONENTS OF ALPHA
*X *Y *Z
*=X: 490.7466 70.1518 -64.4160
*=Y: 70.1518 457.4762 94.8438
*=Z: -64.4138 94.8407 543.4913
ISOTROPIC AVERAGE ALPHA = 497.23805 A.U. = 73.68308 ANG.**3
+++++ BETA (SECOND HARMONIC GENERATION) AT 0.00000 EV.
COMPONENTS OF BETA
*XX *XY *YY *XZ *YZ *ZZ
*=X -418.45256 57.73681 -3.66392 -129.64914 56.17695 226.10560
*=Y 57.76086 -3.70124 66.35581 56.09767 122.54567 121.59046
*=Z -129.63230 56.12991 122.53061 226.08379 121.57058 5.49809
AVERAGE BETAX(SHG) VALUE AT 0.00000 EV = -117.6302 a.u. = -0.101626E-29 ESU
AVERAGE BETAY(SHG) VALUE AT 0.00000 EV = 147.4067 a.u. = 0.127351E-29 ESU
AVERAGE BETAZ(SHG) VALUE AT 0.00000 EV = -0.9629 a.u. = -0.831866E-32 ESU
AVERAGE BETA (SHG) VALUE AT 0.00000 EV = 188.5909 a.u. = 0.162932E-29 ESU
(1 a.u. = 8.639418X10-33 esu)
+++++ ALPHA AT 0.00000 EV.
COMPONENTS OF ALPHA
*X *Y *Z
*=X: 490.7466 70.1518 -64.4160
*=Y: 70.1518 457.4762 94.8438
*=Z: -64.4138 94.8407 543.4913
ISOTROPIC AVERAGE ALPHA = 497.23805 A.U. = 73.68308 ANG.**3
GAMMA (THIRD HARMONIC GENERATION) AT 0.00000 EV.
GAMMA(X,X,X,X) = 65367.73738
GAMMA(Y,Y,Y,Y) = 39838.07460
GAMMA(Z,Z,Z,Z) = 269371.79491
GAMMA(X,X,Y,Y) = 18570.97627
GAMMA(X,X,Z,Z) = 40182.46797
GAMMA(Y,Y,X,X) = 18570.97651
GAMMA(Y,Y,Z,Z) = 54604.78176
GAMMA(Z,Z,X,X) = 40182.47118
GAMMA(Z,Z,Y,Y) = 54604.78627
AVERAGE GAMMA VALUE AT 0.00000 = 120258.81337 a.u. = 60570.78755 ESU (X10-39)
TOTAL CPU TIME: 507.08 SECONDS
== MOPAC DONE ==
]]>
- For convenience, we provide the MOPAC2009 output file lowbee.out.
- You can specify the energies of the radiation to be used in eV with the E=(n) option. For example, if instead of the static values for these properties, E=(0.0), you want to compute them for a 0.25eV laser source, simply specify:
POLAR(E=(0.25)).
- Further nonlinear optical properties of lanthanide complexes can also be computed by selecting additional keywords. Example, for a 1.0eV laser source, use the following keywords to compute:
- Second Harmonic Generation:
POLAR(E=(1.0), IWFLB=1)
- Noniterative calculation of Second Harmonic Generation:
POLAR(E=(1.0), BETA=-1)
- Electrooptical Pockels Effect:
POLAR(E=(1.0), IWFLB=2)
- Noniterative calculation of Electrooptical Pockels Effect:
POLAR(E=(1.0),BETA=-2)
- Optical Rectification:
POLAR(E=(1.0), IWFLB=3)
- Noniterative calculation of Optical Rectification:
POLAR(E=(1.0), BETA=-3)
- Third Harmonic Generation:
POLAR(E=(1.0), GAMMA=1)
- DC-EFISH:
POLAR(E=(1.0), GAMMA=2)
- Intensity Dependent Index of Refraction:
POLAR(E=(1.0), GAMMA=3)
- Optical Kerr Effect:
POLAR(E=(1.0), GAMMA=4)
- For more information on these keywords, refer to "Time-Dependent Hartree-Fock" on the MOPAC2009 manual.
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