NONLINEAR OPTICAL SUSCEPTIBILITIES OF DISORDERED AGGREGATES - A COMPARISON OF SCHEMES TO ACCOUNT FOR INTERMOLECULAR INTERACTIONS

被引:75
作者
KNOESTER, J
机构
[1] Chemical Physics, University of Groningen, 9747 AG Groningen
来源
PHYSICAL REVIEW A | 1993年 / 47卷 / 03期
关键词
D O I
10.1103/PhysRevA.47.2083
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
The performance of approximate theories for the collective nonlinear optical response of assemblies of interacting molecules is investigated by comparing their predictions to exact calculations. To this end, the nonlinear absorption coefficient of linear molecular aggregates with energetic disorder is studied with the aid of Monte Carlo simulations. It is shown that the well-known local-field approximation (LFA) cannot describe the near-resonance nonlinear absorption spectrum for disorder values up to the nearest-neighbor intermolecular interactions; surprisingly, it is found that the validity of the LFA does not at all improve with growing disorder. By contrast, the ''excitonic two-level system'' approximation, in which each collective one-photon transition (Frenkel exciton) of the assembly is treated as an independent two-level system, turns out to describe the collective nonlinear response of the aggregates in a much better way and, moreover, rapidly improves for growing disorder values. It is shown that both models correctly describe the linear optical response and that, within the framework of the LFA, a close connection exists between the rotating-wave approximation and the Heitler-London approximation.
引用
收藏
页码:2083 / 2098
页数:16
相关论文
共 27 条
[21]   Theoretical study on near-resonant third-order nonlinear optical properties (γ) of dendritic molecular aggregates:: Intermolecular-interaction and relaxation effects on γ [J].
Fujita, H ;
Nakano, M ;
Takahata, M ;
Kiribayashi, S ;
Yamaguchi, K .
MOLECULAR CRYSTALS AND LIQUID CRYSTALS, 2001, 371 :261-264
[22]   Theoretical Study on Third-Order Nonlinear Optical Property of One-Dimensional Cyclic Thiazyl Radical Aggregates: Intermolecular Distance, Open-Shell Nature, and Spin State Dependences [J].
Matsui, Hiroshi ;
Yamane, Masaki ;
Tonami, Takayoshi ;
Nakano, Masayoshi ;
de Wergifosse, Marc ;
Seidler, Tomasz ;
Champagne, Benoit .
JOURNAL OF PHYSICAL CHEMISTRY C, 2018, 122 (12) :6779-6785
[23]   Anisotropic atom-atom potentials from X-ray charge densities: application to intermolecular interactions and lattice energies in some biological and nonlinear optical materials [J].
Abramov, YA ;
Volkov, A ;
Coppens, P .
JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM, 2000, 529 :27-35
[24]   Impact of intermolecular charge transfer interactions on structural, spectral and third-order nonlinear optical properties of a semiorganic crystal: Poly (bis 4-methoxybenzylammonium) tetra-μ-chlorido-cadmate (II) [J].
Umarani, P. ;
Aarthi, R. ;
Kayalvizhi, M. ;
Vasuki, G. ;
Raja, C. Ramachandra .
OPTIK, 2018, 171 :337-346
[25]   Stimulated Raman scattering spectroscopy of Y0.4Gd0.6VO4 crystals with partly disordered zircon-type structure-observation of new χ(3)-nonlinear optical interactions [J].
Kaminskii, A. A. ;
Zhang, J. ;
Lux, O. ;
Rhee, H. ;
Eichler, H. J. ;
Tang, D. V. ;
Yu, H. H. ;
Zhang, H. J. ;
Wang, J. ;
Yoneda, H. ;
Shirakawa, A. .
LASER PHYSICS LETTERS, 2014, 11 (12)
[26]   Synthesis, DFT calculations, intermolecular interactions and third order nonlinear optical properties of new organoammonium tetrabromocadmate (II): (C5H6N2Cl)2 [CdBr4]•H2O [J].
Msalmi, Rawia ;
Elleuch, Slim ;
Hamdi, Besma ;
Zouari, Ridha ;
Naili, Houcine .
JOURNAL OF MOLECULAR STRUCTURE, 2020, 1222
[27]   Intriguing Influence of -COOH-Driven Intermolecular Aggregation and Acid-Base Interactions with N,N-Dimethylformamide on the Second-Order Nonlinear-Optical Response of 5,15 Push-Pull Diarylzinc(II) Porphyrinates [J].
Biroli, Alessi Orbelli ;
Tessore, Francesca ;
Righetto, Stefania ;
Forni, Alessandra ;
Macchioni, Alceo ;
Rocchigiani, Luca ;
Pizzotti, Maddalena ;
Di Carlo, Gabriele .
INORGANIC CHEMISTRY, 2017, 56 (11) :6438-6450