From owner-chemistry@ccl.net Mon Jun 15 13:03:00 2020
From: "prabhleen kaur prabhleen.kr[a]gmail.com" <owner-chemistry/a\server.ccl.net>
To: CCL
Subject: CCL: Use of CASSCF with dynamical correlations to calculate singlet-triplet gap
Message-Id: <-54102-200615022158-4744-CJsGUgVCvL4fiuFFg+7lIg/a\server.ccl.net>
X-Original-From: prabhleen kaur <prabhleen.kr]=[gmail.com>
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Date: Mon, 15 Jun 2020 11:51:40 +0530
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Sent to CCL by: prabhleen kaur [prabhleen.kr : gmail.com]
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Hello everyone,

I am trying to use a multi-reference based CASSCF method to calculate the
singlet-triplet gap in organic-diradicals.
For a given system, I am increasing the active space step wise, like
starting from (2,2) then (4,4) and so on.
CASSCF calculations with only static correlations give the correct ground
state (which in my case is triplet) but upon adding dynamical correlations
(NEVPT2), the ground state of the system is changed to singlet in some
cases.
Is it possible ? What does this signify ? And how can we interpret it ?
when does this kind of issue arise ?
It is happening only in (4,4)  space which is far from the complete state
desired for the system.
Could it be because of the small active space ?

I am using ORCA for all my calculations.

Thank You

Best Regards
Prabhleen Kaur
PhD Scholar
Institute of Nano Science and Technology
Mohali, India

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<div dir=3D"ltr">Hello everyone,<div><br></div><div>I am trying to use a mu=
lti-reference based CASSCF method to calculate the singlet-triplet gap in o=
rganic-diradicals.</div><div>For a given system, I am increasing the active=
 space step wise, like starting from (2,2) then (4,4) and so on.</div><div>=
CASSCF calculations with only static correlations give the correct ground s=
tate (which in my case is triplet) but upon adding dynamical correlations (=
NEVPT2), the ground state of the system is changed to singlet in some cases=
.</div><div>Is it possible ? What does this signify ? And how can we interp=
ret it ? when does this kind of issue arise=C2=A0?</div><div>It is happenin=
g=C2=A0only in (4,4)=C2=A0 space which is far from the complete state desir=
ed for the system.</div><div>Could it be because of the small active space =
?</div><div><br></div><div>I am using ORCA for all my calculations.</div><d=
iv><br></div><div>Thank You</div><div><br></div><div>Best Regards</div><div=
>Prabhleen Kaur</div><div>PhD Scholar</div><div>Institute of Nano Science a=
nd Technology</div><div>Mohali, India</div><div><br></div></div>

--00000000000059224705a8197143--


From owner-chemistry@ccl.net Mon Jun 15 13:38:00 2020
From: "Akshaya N akshayanarayanasamy|*|gmail.com" <owner-chemistry]~[server.ccl.net>
To: CCL
Subject: CCL:G: Reorganization energy in Marcus-Hush formalism
Message-Id: <-54103-200615095816-10326-U3plCQ6WozGKgc2ShTbHJA]~[server.ccl.net>
X-Original-From: "Akshaya  N" <akshayanarayanasamy**gmail.com>
Date: Mon, 15 Jun 2020 09:58:15 -0400


Sent to CCL by: "Akshaya  N" [akshayanarayanasamy!^!gmail.com]
Hello everyone,
            In order to calculate reorganization energy, I ran three geometry 
optimizations: neutral, anion, cation in gaussian 16. Then I  ran anion and 
cation in neutral geometry, the neutral molecule in anion and cation 
geometries. The calculations were carried out with B3LYP functional, DFT 
level of theory and 6-311G basis set.
> From the total energies of these calculations, I tried to determine the 
reorganization energies U according to Eq
lambda_hole = U(neutral, cation geometry) - U(neutral, neutral geometry) +
 U(cation, neutral geometry) - U (cation, cation geometry)
I found lambda_hole to be negative. The U(neutral, cation geometry) was 
lesser than the U(neutral, neutral geometry) which made the whole lambda_hole 
to be negative.
What could be the possible reason to get negative reorganization energy?
Is it valid to take the modulus of  U(neutral, cation geometry) - U(neutral, 
neutral geometry) in order to get positive reorganization energy?


Thanks
Akshaya N
akshaya1717[A]iisertvm.ac.in


From owner-chemistry@ccl.net Mon Jun 15 15:15:01 2020
From: "Geoffrey Hutchison geoff.hutchison(0)gmail.com" <owner-chemistry:_:server.ccl.net>
To: CCL
Subject: CCL: Reorganization energy in Marcus-Hush formalism
Message-Id: <-54104-200615151353-1713-FvTpkj8c0uOd6NHU40tEGA:_:server.ccl.net>
X-Original-From: Geoffrey Hutchison <geoff.hutchison,+,gmail.com>
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Sent to CCL by: Geoffrey Hutchison [geoff.hutchison]~[gmail.com]
> What could be the possible reason to get negative reorganization energy?

Consider a case where the molecule starts in a local minimum - you optimize the cation and bringing back to the neutral, you're in a different part of the potential energy curve. Perhaps some dihedral became more planar increasing conjugation, etc. In that case your single point could be lower in energy than the original.

If you take the cation geometry and the single point of the neutral species is lower in energy than your original "optimized neutral" case, you need to re-optimize from the cation geometry. At the worst, you'd end up optimizing to the same geometry = zero reorganization energy. That would be an interesting compound = no difference in geometry between cation and neutral species!

More likely, if you optimize the neutral species from the cation geometry, you'll go downhill and find a new optimum for the neutral.

In general, before calculating reorganization energies, I'd highly suggest exploring multiple conformers to have confidence you're in a global minima.

-Geoff

---
Prof. Geoffrey Hutchison
Department of Chemistry
University of Pittsburgh
tel: (412) 648-0492
email: geoffh**pitt.edu
twitter: **ghutchis
web: https://hutchison.chem.pitt.edu/


From owner-chemistry@ccl.net Mon Jun 15 22:58:00 2020
From: "Nuno A. G. Bandeira nuno.bandeira++tecnico.ulisboa.pt" <owner-chemistry],[server.ccl.net>
To: CCL
Subject: CCL: Use of CASSCF with dynamical correlations to calculate singlet-triplet gap
Message-Id: <-54105-200615165549-10534-/n+rnl42+cAlhRljHL8bEg],[server.ccl.net>
X-Original-From: "Nuno A. G. Bandeira" <nuno.bandeira\a/tecnico.ulisboa.pt>
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Date: Mon, 15 Jun 2020 21:55:41 +0100
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Sent to CCL by: "Nuno A. G. Bandeira" [nuno.bandeira[]tecnico.ulisboa.pt]
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Dear Prabhleen,

Are the singlet and triplet states nearly degenerate? If so what you descri=
be is perfectly natural.

Are you sure the correct ground state (experimentally) is the triplet?=20

How many roots did you ask for in the minimal CAS ? Depending on your syste=
m you might try to get an idea of the energy spectrum by requesting the 3 s=
inglets in CAS(2,2) and averaging them with the triplet.

If you ran a state specific calculation for just the (one) singlet ground s=
tate this will make sense if there=E2=80=99s a sizable gap with the other r=
oots but not if they=E2=80=99re near degenerate in which case your roots ma=
y flip or even converge to the wrong state.

Also if you have a manifold of near-degenerate states you should request th=
e multi-state formalism QD-NEVPT2 just in case.

The size and nature of the active space may influence the outcome but in si=
nglet/triplet problems the essential static correlation is already sufficie=
ntly described by a CAS(2,2). Again it depends on your system and the type =
of problem you want to tackle.=20

Regards,
Nuno


-----------
Nuno A. G. Bandeira, AMRSC
Email: nuno.bandeira . ciencias.ulisboa.pt=20


BioISI - Biosystems & Integrative Sciences Institute;
8.5.57 - C8, Faculty of Sciences, University of Lisbon
Campo Grande- 1749-016 Lisboa Portugal
=C2=A0
Phone: +351 21 750 01 09
--------
=C2=A0
https://www.researchgate.net/profile/Nuno_Bandeira
http://www.researcherid.com/rid/B-6399-2012=20
http://orcid.org/0000-0002-5754-7328=20
http://www.cienciavitae.pt/pt/4A19-ACC3-E225
http://pt.linkedin.com/pub/nuno-a-g-bandeira/47/55a/2aa
=C2=A0

> From: prabhleen kaur prabhleen.kr[a]gmail.com
Sent: 15 June 2020 20:09
To: Bandeira, Nuno A. G. 
Subject: CCL: Use of CASSCF with dynamical correlations to calculate single=
t-triplet gap

Hello everyone,

I am trying to use a multi-reference based CASSCF method to calculate the s=
inglet-triplet gap in organic-diradicals.
For a given system, I am increasing the active space step wise, like starti=
ng from (2,2) then (4,4) and so on.
CASSCF calculations with only static correlations give the correct ground s=
tate (which in my case is triplet) but upon adding dynamical correlations (=
NEVPT2), the ground state of the system is changed to singlet in some cases=
.
Is it possible ? What does this signify ? And how can we interpret it ? whe=
n does this kind of issue arise=C2=A0?
It is happening=C2=A0only in (4,4)=C2=A0 space which is far from the comple=
te state desired for the system.
Could it be because of the small active space ?

I am using ORCA for all my calculations.

Thank You

Best Regards
Prabhleen Kaur
PhD Scholar
Institute of Nano Science and Technology
Mohali, India



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--></style></head><body lang=3DEN-GB link=3Dblue vlink=3D"#954F72"><div cla=
ss=3DWordSection1><p class=3DMsoNormal><span class=3DDefaultFontHxMailStyle=
><span style=3D'font-size:12.0pt'>Dear Prabhleen,<o:p></o:p></span></span><=
/p><p class=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span style=3D=
'font-size:12.0pt'><o:p>&nbsp;</o:p></span></span></p><p class=3DMsoNormal>=
<span class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'>Are t=
he singlet and triplet states nearly degenerate? If so what you describe is=
 perfectly natural.<o:p></o:p></span></span></p><p class=3DMsoNormal><span =
class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'><o:p>&nbsp;=
</o:p></span></span></p><p class=3DMsoNormal><span class=3DDefaultFontHxMai=
lStyle><span style=3D'font-size:12.0pt'>Are you sure the correct ground sta=
te (experimentally) is the triplet? <o:p></o:p></span></span></p><p class=
=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span style=3D'font-size:=
12.0pt'><o:p>&nbsp;</o:p></span></span></p><p class=3DMsoNormal><span class=
=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'>How many roots d=
id you ask for in the minimal CAS ? Depending on your system you might try =
to get an idea of the energy spectrum by requesting the 3 singlets in CAS(2=
,2) and averaging them with the triplet.<o:p></o:p></span></span></p><p cla=
ss=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span style=3D'font-siz=
e:12.0pt'><o:p>&nbsp;</o:p></span></span></p><p class=3DMsoNormal><span cla=
ss=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'>If you ran a s=
tate specific calculation for just the (one) singlet ground state this will=
 make sense if there=E2=80=99s a sizable gap with the other roots but not i=
f they=E2=80=99re near degenerate in which case your roots may flip or even=
 converge to the wrong state.<o:p></o:p></span></span></p><p class=3DMsoNor=
mal><span class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'><=
o:p>&nbsp;</o:p></span></span></p><p class=3DMsoNormal><span class=3DDefaul=
tFontHxMailStyle><span style=3D'font-size:12.0pt'>Also if you have a manifo=
ld of near-degenerate states you should request the multi-state formalism Q=
D-NEVPT2 just in case.<o:p></o:p></span></span></p><p class=3DMsoNormal><sp=
an class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'><o:p>&nb=
sp;</o:p></span></span></p><p class=3DMsoNormal><span class=3DDefaultFontHx=
MailStyle><span style=3D'font-size:12.0pt'>The size and nature of the activ=
e space may influence the outcome but in singlet/triplet problems the essen=
tial static correlation is already sufficiently described by a CAS(2,2). Ag=
ain it depends on your system and the type of problem you want to tackle. <=
o:p></o:p></span></span></p><p class=3DMsoNormal><span class=3DDefaultFontH=
xMailStyle><span style=3D'font-size:12.0pt'><o:p>&nbsp;</o:p></span></span>=
</p><p class=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span style=
=3D'font-size:12.0pt'>Regards,<o:p></o:p></span></span></p><p class=3DMsoNo=
rmal><span class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'>=
Nuno<o:p></o:p></span></span></p><p class=3DMsoNormal><span class=3DDefault=
FontHxMailStyle><span style=3D'font-size:12.0pt'><o:p>&nbsp;</o:p></span></=
span></p><p class=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span st=
yle=3D'font-size:12.0pt'><o:p>&nbsp;</o:p></span></span></p><p class=3DMsoN=
ormal><span style=3D'font-size:12.0pt;color:black'>-----------<o:p></o:p></=
span></p><p class=3DMsoNormal><span style=3D'font-size:12.0pt;color:black'>=
Nuno A. G. Bandeira, AMRSC<o:p></o:p></span></p><p class=3DMsoNormal><span =
style=3D'font-size:12.0pt;color:black'>Email: <a href=3D"mailto:nuno.bandei=
ra . ciencias.ulisboa.pt"><span style=3D'color:black'>nuno.bandeira . ciencias.=
ulisboa.pt</span></a> <o:p></o:p></span></p><p class=3DMsoNormal><span styl=
e=3D'font-size:12.0pt;color:black'><o:p>&nbsp;</o:p></span></p><p class=3DM=
soNormal><span lang=3DPT style=3D'font-size:12.0pt;color:black'><img border=
=3D0 width=3D124 height=3D84 style=3D'width:1.287in;height:.8796in' id=3D"P=
icture_x0020_3" src=3D"cid:image002.jpg . 01D6435F.B59519D0"></span><span sty=
le=3D'font-size:12.0pt;color:black'><o:p></o:p></span></p><p class=3DMsoNor=
mal><span style=3D'font-size:12.0pt;color:black'>BioISI - Biosystems &amp; =
Integrative Sciences Institute;<o:p></o:p></span></p><p class=3DMsoNormal><=
span style=3D'font-size:12.0pt;color:black'>8.5.57 - C8, Faculty of Science=
s, University of Lisbon<o:p></o:p></span></p><p class=3DMsoNormal><span sty=
le=3D'font-size:12.0pt;color:black'>Campo Grande- 1749-016 Lisboa Portugal<=
o:p></o:p></span></p><p class=3DMsoNormal><span style=3D'font-size:12.0pt;c=
olor:black'>&nbsp;<o:p></o:p></span></p><p class=3DMsoNormal><span style=3D=
'font-size:12.0pt;color:black'>Phone: +351 21 750 01 09<o:p></o:p></span></=
p><p class=3DMsoNormal><span style=3D'font-size:12.0pt;color:black'>-------=
-<o:p></o:p></span></p><p class=3DMsoNormal><span style=3D'font-size:12.0pt=
;color:black'>&nbsp;<o:p></o:p></span></p><p class=3DMsoNormal><span style=
=3D'font-size:12.0pt;color:black'>https://www.researchgate.net/profile/Nuno=
_Bandeira<o:p></o:p></span></p><p class=3DMsoNormal><span style=3D'font-siz=
e:12.0pt;color:black'>http://www.researcherid.com/rid/B-6399-2012 <o:p></o:=
p></span></p><p class=3DMsoNormal><span style=3D'font-size:12.0pt;color:bla=
ck'>http://orcid.org/0000-0002-5754-7328 <o:p></o:p></span></p><p class=3DM=
soNormal><span style=3D'font-size:12.0pt;color:black'>http://www.cienciavit=
ae.pt/pt/4A19-ACC3-E225<o:p></o:p></span></p><p class=3DMsoNormal><span sty=
le=3D'font-size:12.0pt;color:black'>http://pt.linkedin.com/pub/nuno-a-g-ban=
deira/47/55a/2aa<o:p></o:p></span></p><p class=3DMsoNormal><span style=3D'f=
ont-size:12.0pt;color:black'>&nbsp;<o:p></o:p></span></p><p class=3DMsoNorm=
al><span class=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'><o=
:p>&nbsp;</o:p></span></span></p><div style=3D'mso-element:para-border-div;=
border:none;border-top:solid #E1E1E1 1.0pt;padding:3.0pt 0cm 0cm 0cm'><p cl=
ass=3DMsoNormal style=3D'border:none;padding:0cm'><b>From: </b><a href=3D"m=
ailto:owner-chemistry . ccl.net">prabhleen kaur prabhleen.kr[a]gmail.com</a><=
br><b>Sent: </b>15 June 2020 20:09<br><b>To: </b><a href=3D"mailto:nuno.ban=
deira . ist.utl.pt">Bandeira, Nuno A. G. </a><br><b>Subject: </b>CCL:=
 Use of CASSCF with dynamical correlations to calculate singlet-triplet gap=
</p></div><p class=3DMsoNormal><span class=3DDefaultFontHxMailStyle><span s=
tyle=3D'font-size:12.0pt'><o:p>&nbsp;</o:p></span></span></p><div><p class=
=3DMsoNormal>Hello everyone,</p><div><p class=3DMsoNormal><o:p>&nbsp;</o:p>=
</p></div><div><p class=3DMsoNormal>I am trying to use a multi-reference ba=
sed CASSCF method to calculate the singlet-triplet gap in organic-diradical=
s.</p></div><div><p class=3DMsoNormal>For a given system, I am increasing t=
he active space step wise, like starting from (2,2) then (4,4) and so on.</=
p></div><div><p class=3DMsoNormal>CASSCF calculations with only static corr=
elations give the correct ground state (which in my case is triplet) but up=
on adding dynamical correlations (NEVPT2), the ground state of the system i=
s changed to singlet in some cases.</p></div><div><p class=3DMsoNormal>Is i=
t possible ? What does this signify ? And how can we interpret it ? when do=
es this kind of issue arise&nbsp;?</p></div><div><p class=3DMsoNormal>It is=
 happening&nbsp;only in (4,4)&nbsp; space which is far from the complete st=
ate desired for the system.</p></div><div><p class=3DMsoNormal>Could it be =
because of the small active space ?</p></div><div><p class=3DMsoNormal><o:p=
>&nbsp;</o:p></p></div><div><p class=3DMsoNormal>I am using ORCA for all my=
 calculations.</p></div><div><p class=3DMsoNormal><o:p>&nbsp;</o:p></p></di=
v><div><p class=3DMsoNormal>Thank You</p></div><div><p class=3DMsoNormal><o=
:p>&nbsp;</o:p></p></div><div><p class=3DMsoNormal>Best Regards</p></div><d=
iv><p class=3DMsoNormal>Prabhleen Kaur</p></div><div><p class=3DMsoNormal>P=
hD Scholar</p></div><div><p class=3DMsoNormal>Institute of Nano Science and=
 Technology</p></div><div><p class=3DMsoNormal>Mohali, India</p></div></div=
><p class=3DMsoNormal><o:p>&nbsp;</o:p></p><p class=3DMsoNormal><span class=
=3DDefaultFontHxMailStyle><span style=3D'font-size:12.0pt'><o:p>&nbsp;</o:p=
></span></span></p></div></body></html>=

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