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

  title={Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses},
  author={R. E. F. Silva and Javier del Pino and Francisco J. Garc'ia-Vidal and Johannes Feist},
  journal={Nature Communications},
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… 
Theoretical Challenges in Polaritonic Chemistry
Polaritonic chemistry exploits strong light–matter coupling between molecules and confined electromagnetic field modes to enable new chemical reactivities. In systems displaying this functionality,
Revealing Coupling Strength in Biological Plasmon-Exciton Systems through Far-Field Microscopy
Optical coupling plays a pivotal role in nanophotonic systems, which can be divided into weak, intermediate, and strong coupling regimes. Determining coupling strength is, therefore, the key to
Impact of Vibrational Modes in the Plasmonic Purcell Effect of Organic Molecules
It is demonstrated that including the whole set of vibrational modes is necessary to capture most of the dynamics and the corresponding spectrum of the large Purcell effect and shed light into the quenching phenomenology taking place in the system.
Molecular photodissociation enabled by ultrafast plasmon decay.
The concept of enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon is demonstrated using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle and the photodism efficiency as a function of various system parameters is explored.
Probing Light-Induced Conical Intersections by Monitoring Multidimensional Polaritonic Surfaces.
The interaction of a molecule with the quantized electromagnetic field of a nanocavity gives rise to light-induced conical intersections between polaritonic potential energy surfaces. We demonstrate
A Theoretical Perspective on Molecular Polaritonics
In the past decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction
Photoprotecting Uracil by Coupling with Lossy Nanocavities
This work identifies the operative conditions in which strong coupling with the cavity mode can open an efficient photoprotective channel, resulting in a relaxation dynamics twice as fast as the natural one, and finds that the photorelaxation efficiency is maximized when an optimal trade-off between light–matter coupling strength and photon decay rate is satisfied.
Controlling plexcitonic strong coupling via multidimensional hotspot nanoengineering
Plexcitonic strong coupling has ushered in an era of room-temperature quantum electrodynamics that is achievable at the nanoscale, with potential applications rang-ing from high-precision
Plasmonic Purcell Effect in Organic Molecules
By means of quantum tensor network calculations, we investigate the large Purcell effect experienced by an organic molecule placed in the vicinity of a plasmonic nanostructure. In particular, we
Permutational symmetry for identical multilevel systems: A second-quantized approach
We develop a framework that provides a straightforward approach to fully exploit the permutational symmetry of identical multi-level systems. By taking into account the permutational symmetry, we


Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity
The coupling between a single dye molecule and plasmonic nanocavity at room temperature is reported and insight into the statistical properties of the emission is provided and non-classical emission is observed, with photon bunching and anti-bunching regimes dependent on the excitation wavelength.
Attosecond Physics
  • F. Krausz
  • Physics
    2007 Conference on Lasers and Electro-Optics - Pacific Rim
  • 2007
Summary form only given. Fundamental processes in atoms, molecules, as well as condensed matter are triggered or mediated by the motion of electrons inside or between atoms. Electronic dynamics on
Single-molecule strong coupling at room temperature in plasmonic nanocavities
Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.
Plasmon exciton-polariton lasing
Strong light-matter interaction leads to the appearance of new states, i.e. exciton-polaritons, with photophysical properties rather distinct from their constituents. Recent developments in
Nanoscale Mapping and Control of Antenna-Coupling Strength for Bright Single Photon Sources.
With nanometer resolution, this work map and tune the coupling strength between a dipole nanoantenna-cavity and a single molecule, obtaining a coupling rate of gmax ∼ 200 GHz, which provides ideal conditions for fast and pure nonclassical single photon emission with brightness exceeding 109 photons/sec.
Strong exciton–photon coupling in an organic semiconductor microcavity
The modification and control of exciton–photon interactions in semiconductors is of both fundamental and practical interest, being of direct relevance to the design of improved light-emitting diodes,
Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings.
Numerical results show how the branching ratio between the covalent and ionic dissociation channels can be strongly manipulated by the optical cavity, avoiding the limitations set by the rotating wave approximation when the field is expanded in Fock space.
Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating
We summarize the problem of measuring an ultrashort laser pulse and describe in detail a technique that completely characterizes a pulse in time: frequency-resolved optical gating. Emphasis is placed
Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity.
This work uses strong coupling in an optical microcavity to mix the electronic transitions of two J-aggregated molecular dyes and uses both non-resonant photoluminescence emission and photolumsinescence excitation spectroscopy to show that hybrid-polariton states act as an efficient and ultrafast energy-transfer pathway between the two exciton states.