The landscape of second-order nonlinear optical (2nd NLO) responses of a system can be depicted as two-dimensional second-order nonlinear optical spectra in a range of external fields, and this is difficult to be realized in experiment for a wide range of external fields. In the present study, an efficient method for application of sum-over-states model to simulate electronic two-dimensional NLO (2DNLO) spectra has been developed, and techniques to analyze NLO response-structure correlation have been proposed. This 2DNLO method has been applied to simulate the 2DNLO spectra of a series of typical electron push-pull chromophores under external fields of up to 5.00 eV. The correlation between the NLO properties and structure has been disclosed, and a further strategy to enhance the NLO properties of push-pull chromophores has been proposed.
The lowest-lying 10 isomers of C106 satisfying the isolated-pentagon
rule (IPR) were predicted from 1233 IPR isomers with semiempirical
and density functional theory based methods. The structures, stabilities,
IR and UV spectroscopic, and the third-order nonlinear optical (NLO)
properties of those low-lying isomers were explored in detail. C
s
:331, C
2:1194, and C
1:534 are the three
lowest-energy isomers with almost identical energies and could be
observed in experiment. When the entropy effects in the isomeric fullerene
system are taken into account, isomer C
2:1194 prevails up to 3000 °C. In the high temperature region,
the concentrations of those ten low-lying isomers are very similar,
indicating that the isomers at high temperatures will be hard to isolate.
The third-order NLO properties under external fields (0.0–3.0
eV) of the five lowest-lying isomers were analyzed, and the average
NLO properties of those isomers were predicted at room temperature
for experimental exploration.
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