Two photon absorption

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skma
Posts: 2
Joined: 07 Oct 2014, 09:19
First name(s): Mahasin
Middle name(s): Alam
Last name(s): SK
Affiliation: NTU
Country: Singapore

Two photon absorption

Post by skma » 07 Oct 2014, 09:40

Dear All,

I am a new user of Dalton. I am using Dalton2013 for two-photon absorption. I used benzene as starting material.
Below is my input.dal file and summary of output file.
My questions are
1) how to get the TPA wavelength? Is it the half of excitation enegry (in eV) e.g., S0-->S1 converted to nm?
2) How to get the TPA cross-section? Is it the "sigma" value mentioned in the summary Table?
3) If the "sigma" values in the table are TPA cross-scetions, then which value is to consider because there is two "sigma" value, one for linear and other for circular polarization?

I will be greatfull if any one please answer my above questions. Thank you very much for your help in advace.

Warm regards

Mahasin

input.dal
**GENERAL
.RUN RESPONSE
#.DIRECT
.PARALLEL
**WAVE FUNCTION
.DFT
B3LYP ! Comment out for running CAM-B3LYP
#CAMB3LYP ! Uncomment for running CAM-B3LYP
**RESPONS
*QUADRATIC
.TWO-PHOTON
.ROOTS
15
**END

+-----------------------------------+
| Two-photon absorption summary |
+-----------------------------------+
---------------------------------------------------------------------------------
Sym No Energy Polarization Df Dg D sigma R
---------------------------------------------------------------------------------
1 1 5.54 Linear 0.667E-14 0.642E-14 0.390E-13 0.879E-15 0.65
1 1 5.54 Circular 0.667E-14 0.642E-14 0.252E-13 0.568E-15 0.65
1 2 6.31 Linear 0.179E-16 0.348E-15 0.143E-14 0.417E-16 1.44
1 2 6.31 Circular 0.179E-16 0.348E-15 0.205E-14 0.599E-16 1.44
1 3 7.38 Linear 0.338E-17 0.404E-17 0.229E-16 0.914E-18 0.76
1 3 7.38 Circular 0.338E-17 0.404E-17 0.175E-16 0.697E-18 0.76
1 4 7.38 Linear 0.235E-17 0.770E-17 0.355E-16 0.142E-17 1.17
1 4 7.38 Circular 0.235E-17 0.770E-17 0.415E-16 0.165E-17 1.17
1 5 7.87 Linear 0.587E-21 0.235E-20 0.106E-19 0.481E-21 1.22
1 5 7.87 Circular 0.587E-21 0.235E-20 0.129E-19 0.588E-21 1.22
1 6 7.98 Linear 0.208E-20 0.569E-17 0.228E-16 0.106E-17 1.50
1 6 7.98 Circular 0.208E-20 0.569E-17 0.342E-16 0.159E-17 1.50
1 7 7.98 Linear 0.286E-20 0.120E-19 0.537E-19 0.251E-20 1.23
1 7 7.98 Circular 0.286E-20 0.120E-19 0.663E-19 0.309E-20 1.23
1 8 7.99 Linear 0.491E-20 0.136E-17 0.545E-17 0.255E-18 1.50
1 8 7.99 Circular 0.491E-20 0.136E-17 0.815E-17 0.381E-18 1.50
1 9 8.06 Linear 0.176E-16 0.953E-02 0.381E-01 0.181E-02 1.50
1 9 8.06 Circular 0.176E-16 0.953E-02 0.572E-01 0.272E-02 1.50
1 10 8.06 Linear 0.173E-16 0.952E-02 0.381E-01 0.181E-02 1.50
1 10 8.06 Circular 0.173E-16 0.952E-02 0.571E-01 0.272E-02 1.50
1 11 9.11 Linear 0.121E-06 0.117E+02 0.469E+02 0.286E+01 1.50
1 11 9.11 Circular 0.121E-06 0.117E+02 0.704E+02 0.428E+01 1.50
1 12 9.11 Linear 0.393E-09 0.117E+02 0.469E+02 0.285E+01 1.50
1 12 9.11 Circular 0.393E-09 0.117E+02 0.704E+02 0.428E+01 1.50
1 13 9.43 Linear 0.377E-17 0.555E-17 0.297E-16 0.194E-17 0.87
1 13 9.43 Circular 0.377E-17 0.555E-17 0.258E-16 0.168E-17 0.87
1 14 9.52 Linear 0.287E-17 0.636E-17 0.312E-16 0.207E-17 1.04
1 14 9.52 Circular 0.287E-17 0.636E-17 0.324E-16 0.215E-17 1.04
1 15 9.52 Linear 0.399E-17 0.580E-17 0.312E-16 0.207E-17 0.86
1 15 9.52 Circular 0.399E-17 0.580E-17 0.268E-16 0.178E-17 0.86
---------------------------------------------------------------------------------

lyzhao
Posts: 74
Joined: 11 Nov 2013, 00:36
First name(s): Youzhao
Last name(s): Lan
Affiliation: Institute of Physical Chemistry
Country: China

Re: Two photon absorption

Post by lyzhao » 07 Oct 2014, 15:29

Dear Mahasin,
1) how to get the TPA wavelength? Is it the half of excitation enegry (in eV) e.g., S0-->S1 converted to nm?
Yes, if you use the keyword of .TWO-PHOTON. please read the Dalton manual.
2) How to get the TPA cross-section? Is it the "sigma" value mentioned in the summary Table?
Yes. The sigma is TPA cross-section.
3) If the "sigma" values in the table are TPA cross-scetions, then which value is to consider because there is two "sigma" value, one for linear and other for circular polarization?
Physical text will tell you what the linear and circular polarization are. Or use Google.
The ratio of linear to circular may be mentioned in Refs. J. Chem. Phys. 55(1971)2789 and 57(1972)2264.

Bests,
Lan

skma
Posts: 2
Joined: 07 Oct 2014, 09:19
First name(s): Mahasin
Middle name(s): Alam
Last name(s): SK
Affiliation: NTU
Country: Singapore

Re: Two photon absorption

Post by skma » 16 Oct 2014, 03:06

Dear Lan,

Thank you for your reply.

Can you please tell me how to run Two-photon calculation in dimethylformamide (DMF) solvent. Thank you again.

Warm regards

Mahasin

lyzhao
Posts: 74
Joined: 11 Nov 2013, 00:36
First name(s): Youzhao
Last name(s): Lan
Affiliation: Institute of Physical Chemistry
Country: China

Re: Two photon absorption

Post by lyzhao » 16 Oct 2014, 05:22

The following example is for benzene solvent, please read the manual to see how to define the solvent by yourself.
Hint in manual, "it is also possible to define a solvent by the keywords .EPS, .EPSINF and .RSOLV."

**DALTON INPUT
.RUN RESPONS
.PARALLEL
*PCM <----define the solvent here
.SOLVNT
BENZENE
.NEQRSP
*PCMCAV
**INTEGRAL
.DIPLEN
**WAVE FUNCTIONS
.DFT
LDA
*DFT INPUT
.FINE
**RESPONS
.MAXRM <---- for large system, please increase MAXRM
2000
*QUADRATIC
.SINGLE
.TWO-PHOTON
.ROOTS
10 10 <-----based on the symmetry of your system
**END OF DALTON INPUT

Best regards.
Lan

saisudhakar
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First name(s): Saisudhakar
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Affiliation: Birla Institute of Technology and Science
Country: India

Re: Two photon absorption

Post by saisudhakar » 28 Nov 2015, 07:53

Hi, What are the units of Two-Photon Absorption cross section (sigma) which has given in the output file?

Regards
Saisudhakar

lyzhao
Posts: 74
Joined: 11 Nov 2013, 00:36
First name(s): Youzhao
Last name(s): Lan
Affiliation: Institute of Physical Chemistry
Country: China

Re: Two photon absorption

Post by lyzhao » 28 Nov 2015, 08:42

Have you seen the following output before Sigma?
The two-photon absorption strength for an average molecular
orientation is computed according to formulas given by
P.R. Monson and W.M. McClain in J. Chem. Phys. 53:29, 1970
and W.M. McClain in J. Chem. Phys. 55:2789, 1971.
The absorption depends on the light polarization.
A monochromatic light source is assumed.

All results are presented in atomic units, except the
excitation energy which is given in eV and two-photon cross
section which is given in GM. A FWHM of 0.1 eV is assumed.

Conversion factors:
1 a.u. = 1.896788 10^{-50} cm^4 s/photon
1 GM = 10^{-50} cm^4 s/photon

saisudhakar
Posts: 12
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First name(s): Saisudhakar
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Affiliation: Birla Institute of Technology and Science
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Re: Two photon absorption

Post by saisudhakar » 30 Nov 2015, 10:06

| Two-photon transition tensor S |
+--------------------------------+
---------------------------------------------------------------
Sym No Energy Sxx Syy Szz Sxy Sxz Syz
---------------------------------------------------------------
1 1 4.25 0.0 0.0 -0.0 0.0 0.5 0.4
1 2 8.40 7.4 3.4 0.3 -5.8 -0.0 0.0
1 3 8.76 -0.0 -0.0 0.0 0.0 0.7 -1.8
1 4 10.36 0.0 0.0 -0.0 0.0 1.0 1.1
---------------------------------------------------------------


Transition probabilities (a.u.)
-----------------------------------------
D = 2*Df + 4*Dg, Linear polarization
D = -2*Df + 6*Dg, Circular polarization
Df = sum(i,j){ S_ii * S_jj }/30
Dg = sum(i,j){ S_ij * S_ij }/30

Two-photon cross sections
---------------------------------------------------
sigma = 8*pi^3*alpha^2*hbar/e^4 * E^2*D (a.u.)

Polarization ratio
-------------------------------
R = (-Df+3*Dg)/(Df+2*Dg)


This is I have in my output file. I have the sigma (TPA cross section) value in terms of some variables. How do I convert it into numbers?

sonco
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Re: Two photon absorption

Post by sonco » 30 Nov 2015, 10:24

You need to look a few lines below what you wrote us in your output: there should be a table like this
(the actual digits in the table are from another system than yours, so do not bother. You need to look into your output file)

| Two-photon absorption summary |
+-----------------------------------+
---------------------------------------------------------------------------------
Sym No Energy Polarization Df Dg D sigma R
---------------------------------------------------------------------------------
1 1 4.24 Linear 0.719E-01 0.385E-01 0.298E+00 0.392E-02 0.29
1 1 4.24 Circular 0.719E-01 0.385E-01 0.873E-01 0.115E-02 0.29


The Df, Dg, D, sigma and R values tabulated are computed according to the formulas written before the table.

I hope this clarifies your doubts
Sonia

saisudhakar
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Re: Two photon absorption

Post by saisudhakar » 30 Nov 2015, 10:39

Thank you Sonco. I have TPA summary in my output file. One thing I do not understand is the calculation of TPA cross section. How to calculate cross section from output file?

sonco
Posts: 87
Joined: 06 Sep 2013, 13:49
First name(s): Sonia
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Affiliation: DTU Chemistry
Country: Denmark

Re: Two photon absorption

Post by sonco » 30 Nov 2015, 11:02

Hi,
I admit you lost me... in the table I mention there should be tabulated the values of the cross section (sigma) for different values of energy
and for two different polarization (linear and circular) - 8th column in the "Two-photon absorption summary ".
Isn't that what you need?
Sonia

saisudhakar
Posts: 12
Joined: 13 Nov 2015, 05:49
First name(s): Saisudhakar
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Affiliation: Birla Institute of Technology and Science
Country: India

Re: Two photon absorption

Post by saisudhakar » 01 Dec 2015, 04:21

Thank you Sonco its clear now. But is it possible to draw the TPA spectra?

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