Entangled two-photon absorption (ETPA) has recently become a topic of lively debate, mainly due to the apparent inconsistencies in the experimentally reported ETPA cross sections of organic molecules obtained by a number of groups. In this work, we provide a thorough experimental study of ETPA in the organic molecules Rhodamine B (RhB) and zinc tetraphenylporphirin (ZnTPP). Our contribution is 3-fold: first, we reproduce previous results from other groups; second, we on the one hand determine the effects of different temporal correlationsintroduced as a controllable temporal delay between the signal and idler photons to be absorbedon the strength of the ETPA signal, and on the other hand, we introduce two concurrent and equivalent detection systems with and without the sample in place as a useful experimental check; third, we introduce, and apply to our data, a novel method to quantify the ETPA rate based on taking into account the full photon-pair behavior rather than focusing on singles or coincidence counts independently. Through this experimental setup we find that, surprisingly, the purported ETPA signal is not suppressed for a temporal delay much greater than the characteristic photon-pair temporal correlation time. While our results reproduce the previous findings from other authors, our full analysis indicates that the signal observed is not actually due to ETPA but simply to linear losses. Interestingly, for higher RhB concentrations, we find a two-photon signal that, contrary to expectations, likewise does not correspond to ETPA.
We performed a combined experimental and theoretical study of the conjugates obtained from single-walled carbon nanotubes and anticancer antibiotic doxorubicin (DOX). Atomic force microscopy (AFM) imaging at lower magnification revealed, extended regions of single-walled carbon nanotubes (SWNTS) fully covered with DOX adsorbed molecules, along with some bare parts without the adsorbed drug, thus suggesting that the DOX adsorption is a cooperative process. Ambient atmosphere scanning tunneling microscopy (STM) at higher resolutions found that individual SWNTs-DOX conjugates exhibit a periodic texture, whose most important morphological feature is alternating depressions and protrusions along the nanotube. Based on the images and profiles measured, we suggest that doxorubicin molecules self-assemble on SWNTs sidewall according to a helical pattern, in which their tetracyclic fragments are turned with respect to the nanotube axis by about 50[Formula: see text]. To provide an additional insight into the structure of noncovalent SWNTs-DOX conjugates, we employed density functional theory (DFT) calculations with three long-range corrected functionals: M05-2X, wB97X-D and LCBLYP, of which M05-2X yielded the most realistic results in terms of geometries and energies.
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