Nonlinear optical properties of one-dimensional organic molecular aggregates in nanometer films

Abstract

Nonlinear optical properties of one-dimensional organic molecular aggregates in nanometer films Markov, R.V.; Plekhanov, A.I.; Shelkovnikov, V.V.; Knoester, J. Take-down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim.Downloaded from the University of Groningen/UMCG research database (Pure): http://www.rug.nl/research/portal. For technical reasons the number of authors shown on this cover page is limited to 10 maximum. AbstractNanometer films of molecular J-aggregates of pseudoisocyanine (PIC) with various degrees of both static and dynamic disorder were prepared. The amount of static disorder was varied by modifying the local environment of the J-aggregates in the films, while the dynamic disorder was varied by changing the film temperature. Through these variations, the delocalization length N of the excitons was controlled, as could be monitored from the width of the exciton absorption del (3) line. This has allowed us to establish the scaling of the nonlinear optical susceptibility per aggregate molecule, x /N, with

Resonant enhancement of third‐order nonlinear optical property in J‐like aggregates of a cyanine dye

“…A supralinear scaling of the cubic optical nonlinearity χ (3) with the exciton delocalization size (so-called size-enhancement) has been theoretically predicted for ordered aggregates [7] as well as for aggregates with static diagonal disorder [8]. Markov et al [15] studied the nanometer films of J-aggregates of pseudoisocyanine (PIC) with various degrees of both static and dynamic disorder, and established the scaling of the nonlinear optical susceptibility per aggregate molecule, χ (3) /N, with the delocalization length as χ (3) /N µN γ del , with γ = 2.3 ± 0.2. This power scaling agrees very well with the theoretical prediction of γ = 2.36 for the size-enhancement in one-dimensional aggregates with static diagonal disorder [8].…”

Ternary AOT/water/hexane systems as “micellar sieves” for cyanine dye J-aggregates

“…Strong dipole-dipole interactions between transient dipole moments of dye monomers favor the propagation of electronic excitation in the aggregate over several hundred molecules in the form of Frenkel exciton [2]. Collective excitation gives rise to unique linear and nonlinear properties of J-aggregates, such as resonance fluorescence [2], exciton superradiance (i.e., enhanced radiative decay rate which scales linearly with the aggregate size) [3], and giant nonlinear optical susceptibilities [4].…”

Large resonant third-order optical nonlinearity of thin film containing J-like aggregates of a bis[4-(N-dibutylamino)phenyl]squarylium dye

“…A supralinear scaling of the cubic optical nonlinearity, χ (3) , with the exciton delocalization size (so-called size-enhancement) has been theoretically predicted for ordered aggregates as well as for aggregates with static diagonal disorder (Knoester 2003). Markov et al (2003) studied the nanometer films of J-aggregates of pseudoisocyanine (PIC) with various degrees of both static and dynamic disorder, and established the scaling of the nonlinear optical susceptibility per aggregate molecule, χ (3) /N , with the delocalization length as χ (3) N ∝ N γ Del , with γ = 2•3 ± 0•2. This power scaling agrees very well with the theoretical prediction of γ = 2 • 36 for the size-enhancement in one-dimensional aggregates with static diagonal disorder (Knoester 2003).…”