Observation of selective plasmon-exciton coupling in nonradiative energy transfer: donor-selective versus acceptor-selective plexcitons.

We report selectively plasmon-mediated nonradiative energy transfer between quantum dot (QD) emitters interacting with each other via Förster-type resonance energy transfer (FRET) under controlled plasmon coupling either to only the donor QDs (i.e., donor-selective) or to only the acceptor QDs (i.e., acceptor-selective). Using layer-by-layer assembled colloidal QD nanocrystal solids with metal nanoparticles integrated at carefully designed spacing, we demonstrate the ability to enable/disable the coupled plasmon-exciton (plexciton) formation distinctly at the donor (exciton departing) site or at the acceptor (exciton feeding) site of our choice, while not hindering the donor exciton-acceptor exciton interaction but refraining from simultaneous coupling to both sites of the donor and the acceptor in the FRET process. In the case of donor-selective plexciton, we observed a substantial shortening in the donor QD lifetime from 1.33 to 0.29 ns as a result of plasmon-coupling to the donors and the FRET-assisted exciton transfer from the donors to the acceptors, both of which shorten the donor lifetime. This consequently enhanced the acceptor emission by a factor of 1.93. On the other hand, in the complementary case of acceptor-selective plexciton we observed a 2.70-fold emission enhancement in the acceptor QDs, larger than the acceptor emission enhancement of the donor-selective plexciton, as a result of the combined effects of the acceptor plasmon coupling and the FRET-assisted exciton feeding. Here we present the comparative results of theoretical modeling of the donor- and acceptor-selective plexcitons of nonradiative energy transfer developed here for the first time, which are in excellent agreement with the systematic experimental characterization. Such an ability to modify and control energy transfer through mastering plexcitons is of fundamental importance, opening up new applications for quantum dot embedded plexciton devices along with the development of new techniques in FRET-based fluorescence microscopy.

Exciton-driven antiferromagnetic metal in a correlated van der Waals insulator.

Collective excitations of bound electron-hole pairs-known as excitons-are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS3 by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and a long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism.

Non-radiative resonance energy transfer in bi-polymer nanoparticles of fluorescent conjugated polymers.

This work demonstrates the comparative studies of non-radiative resonance energy transfer in bi-polymer nanoparticles based on fluorescent conjugated polymers. For this purpose, poly[(9,9-dihexylfluorene) (PF) as a donor (D) and poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene] (MEH-PPV) as an acceptor (A) have been utilized, from which four different bi-polymer nanoparticle systems are designed and synthesized. Both, steady-state fluorescence spectra and time-resolved fluorescence measurements indicate varying energy transfer efficiencies from the host polymer PF to the acceptor polymer MEH-PPV depending on the D-A distances and structural properties of the nanoparticles. The first approach involves the preparation of PF and MEH-PPV nanoparticles separately and mixing them at a certain ratio. In the second approach, first PF and MEH-PPV solutions are mixed prior to nanoparticle formation and then nanoparticles are prepared from the mixture. Third and fourth approaches involve the sequential nanoparticle preparation. In the former, nanoparticles are prepared to have PF as a core and MEH-PPV as a shell. The latter is the reverse of the third in which the core is MEH-PPV and the shell is PF. The highest energy transfer efficiency recorded to be 35% is obtained from the last system, in which a PF layer is sequentially formed on MEH-PPV NPs.