Single photon multiclock lock-in detection by picosecond timestamping

Extracting signals at low single-photon count rates from large backgrounds is a challenge in many optical experiments and technologies. Here, we demonstrate a single-photon lock-in detection scheme based on continuous photon timestamping to improve the SNR by more than two orders of magnitude. Through time-resolving the signal modulation induced by periodic perturbations, 98% of dark counts are filtered out and the &lt; 1 c o u n t / s contributions from several different nonlinear processes identified. As a proof-of-concept, coherent anti-Stokes Raman measurements are used to determine the vibrational lifetime of few molecules in a plasmonic nanocavity. This detection scheme can be applied to all single-photon counting experiments with any number of simultaneous modulation frequencies, greatly increasing SNR and resolving physical processes with picosecond time resolution while keeping the photon dosage small. The open instrumentation package provided here enables low-cost implementation.</jats:p

Localized Nanoresonator Mode in Plasmonic Microcavities.

Submicron-thick hexagonal boron nitride crystals embedded in noble metals form planar Fabry-Perot half-microcavities. Depositing Au nanoparticles on top of these microcavities forms previously unidentified angle- and polarization-sensitive nanoresonator modes that are tightly laterally confined by the nanoparticle. Comparing dark-field scattering with reflection spectroscopies shows plasmonic and Fabry-Perot-like enhancements magnify subtle interference contributions, which lead to unexpected redshifts in the dark-field spectra, explained by the presence of these new modes

Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses

Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. Here, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light–matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light–matter) potentials in the strong light–matter coupling regime and bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a route towards ultrafast molecular spectroscopy with plasmonic nanocavitiesThis work has been funded by the European Research Council grant ERC-2016-STG-714870 and the Spanish Ministry for Science, Innovation, and Universities—AEI grants RTI2018-099737-B-I00, PCI2018-093145 (through the QuantERA program of the European Commission), and CEX2018-000805-M (through the María de Maeztu program for Units of Excellence in R&D

Plasmon-Induced Trap State Emission from Single Quantum Dots

Charge carriers trapped at localized surface defects play a crucial role in quantum dot (QD) photophysics. Surface traps offer longer lifetimes than band-edge emission, expanding the potential of QDs as nanoscale light-emitting excitons and qubits. Here, we demonstrate that a nonradiative plasmon mode drives the transfer from two-photon-excited excitons to trap states. In plasmonic cavities, trap emission dominates while the band-edge recombination is completely suppressed. The induced pathways for excitonic recombination not only shed light on the fundamental interactions of excitonic spins, but also open new avenues in manipulating QD emission, for optoelectronics and nanophotonics applications

Ultrafast long-range energy transport via light-matter coupling in organic semiconductor films

The formation of exciton-polaritons allows the transport of energy over hundreds of nanometres at velocities up to 10^6 m s^-1 in organic semiconductors films in the absence of external cavity structures

Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106 m s−1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polariton