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Monolayer semiconductors are emerging platforms for strong nonlinear light-matter interaction, which is enhanced by the giant oscillator strength of tightly bound excitons. Little attention has been paid to the impact of excitonic resonances on the temporal dynamics of nonlinear light-matter interaction, since harmonic generation and optical-wave mixing are generally considered instantaneous processes. We find that a significant time difference, ranging from -40 fs to +120 fs, is necessary between two light pulses for optimal sum-frequency generation (SFG) and four-wave mixing (FWM) to occur from monolayer WSe2 when one of the pulses is in resonance with an excitonic transition. These resonances involve both band-edge A-excitons (AX) as well as high-lying excitons (HX) comprising electrons from conduction bands far above the gap. Numerical simulations of the density-matrix evolution reproduce and explain the distinct dynamics of SFG and FWM. The interpulse delays for maximal SFG and FWM are governed primarily by the lifetime of the one-photon and two-photon resonant states, respectively. The method therefore offers an unconventional probe of excitonic dynamics that are either one-photon or two-photon allowed. Remarkably, the longest delay times occur at the lowest excitation powers, indicating a strong nonlinearity that offers exploration potential for excitonic quantum nonlinear optics.

Strong dipole–dipole coupling within and between π‐conjugated segments shifts electronic transitions, and modifies vibronic coupling and excited‐state lifetimes. Since J‐type coupling between monomers along the conjugated‐polymer (CP) chain and H‐type coupling of chromophores between chains of a CP compete, a superposition of the spectral modifications arising from each type of coupling emerges, making the two couplings hard to discern in the ensemble. We introduce a single‐molecule H‐type aggregate of fixed spacing and variable length of up to 10 nm. HJ‐type aggregate formation is visualized intuitively in the scatter of single‐molecule spectra., Coupling therapy: In organic electronics, J‐type coupling between monomers along the chain and H‐type coupling of chromophores between chains compete, which makes the two types of coupling hard to discern in the ensemble. A single‐molecule H‐type aggregate of fixed spacing and variable length of up to 10 nm is introduced, and HJ‐type aggregate formation is visualized intuitively in the scatter of single‐molecule spectra.

We demonstrate that a simple phenazine derivative can serve as a dual emitter for organic light-emitting diodes, showing simultaneous luminescence from the singlet and triplet excited states at room temperature without the need of heavy-atom substituents. Although devices made with this emitter achieve only low quantum efficiencies of < 0.2%, changes in fluorescence and phosphorescence intensity on the subpercent scale caused by an external magnetic field of up to 30 mT are clearly resolved with an ultra-low-noise optical imaging technique. The results demonstrate the concept of using simple reporter molecules, available commercially, to optically detect the spin of excited states formed in an organic light-emitting diode and thereby probe the underlying spin statistics of recombining electron-hole pairs. A clear anticorrelation of the magnetic-field dependence of singlet and triplet emission shows that it is the spin interconversion between singlet and triplet which dominates the magnetoluminescence response: the phosphorescence intensity decreases by the same amount as the fluorescence intensity increases. The concurrent detection of singlet and triplet emission as well as device resistance at cryogenic and room temperature constitute a useful tool to disentangle the effects of spin-dependent recombination from spin- dependent transport mechanisms.

Nonlinear continuum generation from diffraction-limited hot spots in rough silver films exhibits striking narrow-band intensity resonances in excitation wavelength. Time-domain Fourier spectroscopy uncovers how these resonances arise due to the formation of a "plasmon staircase", a discreteness in the fundamental oscillation of the plasmon excitations responsible for generating the white-light continuum. Whereas multiple scattering from discrete antennas can be invoked to explain hot spot formation in random assemblies of isolated particles, hot spots in films of fused nanoparticles are excited by interfering propagating surface plasmons, launched by scattering from individual nanoparticle antennas. For closed films, discrete propagating plasmons interact coherently over distances of tens of microns to pump the hot spot.