A molecular theory for two-photon and three-photon fluorescence polarization

Abstract

In the analysis of molecular structure and local order in heterogeneous samples, multiphoton excitation of fluorescence affords chemically specific information and high-resolution imaging. This report presents the results of an investigation that secures a detailed theoretical representation of the fluorescence polarization produced by one-, two-, and three-photon excitations, with orientational averaging procedures being deployed to deliver the fully disordered limits. The equations determining multiphoton fluorescence response prove to be expressible in a relatively simple, generic form, and graphs exhibit the functional form of the multiphoton fluorescence polarization. Amongst other features, the results lead to the identification of a condition under which the fluorescence produced through the concerted absorption of any number of photons becomes completely unpolarized. It is also shown that the angular variation of fluorescence intensities is reliable indicator of orientational disorder.

On the effects of permanent molecular dipoles in the simultaneous absorption of two photons: Full generalized rotating wave approximation versus analytical results

“…8,9,[34][35][36][37][38][39][40], and citations therein). For many of the reasons they are of importance in fluorescence microscopy, two-photon excitation is also of interest (Refs.…”

Polarization-induced fluorescence modulation in a self-assembled coordination cage-shaped complex

“…Over the past decade, studies on polarizationinduced fluorescence modulation have been mainly confined to organic polymers and crystals [9,10]. New materials that exhibit strong fluorescence are desired for accelerating the development of this field.…”

Three-photon-absorption-induced optical stabilization effects in a bifluorenylidene derivative

“…Novel organic compounds featuring large three-photon absorption (3PA) cross section have been of particular interest since many attractive applications are based on its high-order nonlinearity of media's response to the exciting light. Molecules with large 3PA cross section can be widely used in the fields of ultrahigh-resolution biological imaging (three-photon confocal microscopy) [1][2][3], high-efficiency up-converted stimulated emission [4][5][6][7], optical limiting [8,9], biomedical [10], light-activated therapy field [11][12][13], three-dimensional optical data storage [14], microfabrication [15].…”