Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy

Coupling matter excitations to electromagnetic modes inside nano-scale optical resonators leads to the formation of hybrid light-matter states, so-called polaritons, allowing the controlled manipulation of material properties. Here, we investigate the photo-induced dynamics of a prototypical strongly-coupled molecular exciton-microcavity system using broadband two-dimensional Fourier transform spectroscopy and unravel the mechanistic details of its ultrafast photo-induced dynamics. We find evidence for a direct energy relaxation pathway from the upper to the lower polariton state that initially bypasses the excitonic manifold of states, which is often assumed to act as an intermediate energy reservoir, under certain experimental conditions. This observation provides new insight into polariton photophysics and could potentially aid the development of applications that rely on controlling the energy relaxation mechanism, such as in solar energy harvesting, manipulating chemical reactivity, the creation of Bose–Einstein condensates and quantum computing

An Investigation of Heat Transfer in a Mechanically Agitated Vessel

The objective of this study is to optimize experimental conditions of agitating a non-Newtonian liquid using experimental design methodology. The measurements of the temperatures have been carried out in a jacketed vessel equipped with Turbine impellers. The rheological properties of aqueous solutions of carboxymethylcellulose sodium salt had been studied using shear stress/shear rate data. The results of the experimental studies, concerning the effect of the diameter of the impeller, the impeller speed and baffled or unbaffled vessel on the overall heat transfer coefficient have been approximated in the form of equations. Based on the optimization criterion, an agitated vessel equipped with Flat Blade Disc Turbine (FBDT) of diameter ratio d/D = 0.6 and baffles is proposed as the most advantageous for heat transfer processes

Fluorescence kinetics of flavin adenine dinucleotide in different microenvironments

Fluorescence kinetics of flavin adenine dinucleotide was measured in a wide time and spectral range in different media, affecting its intra- end extramolecular interactions, and analyzed by a new method based on compressed sensing

The transition to aeration in two-phase mixing in stirred vessels

We consider the mixing of a viscous fluid by the rotation of a pitched blade turbine inside an open, cylindrical tank, with air as the lighter fluid above. To examine the flow and interfacial dynamics, we utilise a highly-parallelised implementation of a hybrid front-tracking/level-set method that employs a domain-decomposition parallelisation strategy. Our numerical technique is designed to capture faithfully complex interfacial deformation, and changes of topology, including interface rupture and dispersed phase coalescence. As shown via transient, three-dimensional direct numerical simulations, the impeller induces the formation of primary vortices that arise in many idealised rotating flows as well as several secondary vortical structures resembling Kelvin-Helmholtz, vortex breakdown, blade tip vortices, and end-wall corner vortices. As the rotation rate increases, a transition to `aeration' is observed when the interface reaches the rotating blades leading to the entrainment of air bubbles into the viscous fluid and the creation of a bubbly, rotating, free surface flow. The mechanisms underlying the aeration transition are probed as are the routes leading to it, which are shown to exhibit a strong dependence on flow history.Comment: 14 pages, 9 figure

Ultrafast electronic and lattice dynamics in laser-excited crystalline bismuth

Femtosecond spectroscopy is applied to study transient electronic and lattice processes in bismuth. Components with relaxation times of 1 ps, 7 ps and ~ 1 ns are detected in the photoinduced reflectivity response of the crystal. To facilitate the assignment of the observed relaxation to the decay of particular excited electronic states we use pump pulses with central wavelengths ranging from 400 nm to 2.3 mum. Additionally, we examine the variation of parameters of coherent A1g phonons upon the change of excitation and probing conditions. Data analysis reveals a significant wavevector dependence of electron-hole and electron- phonon coupling strength along \Gamma--T direction of the Brillouin zone.Comment: 19 pages, 9 figure

Self-phase modulation of a single-cycle THz pulse

We demonstrate self-phase modulation (SPM) of a single-cycle THz pulse in a semiconductor, using bulk n-GaAs as a model system. The SPM arises from the heating of free electrons in the electric field of the THz pulse. Electron heating leads to an ultrafast reduction of the plasma frequency, which results in a strong modification of the THz-range dielectric function of the material. THz SPM is observed directly in the time domain as a characteristic reshaping of single-cycle THz pulse. In the frequency domain, it corresponds to a strong frequency-dependent refractive index nonlinearity of n-GaAs, which is found to be both positive and negative within the broad spectrum of the THz pulse. The spectral position of zero nonlinearity is defined by the electron momentum relaxation rate. Nonlinear spectral broadening and compression of the single-cycle THz pulse was also observed

Quantum-dynamical Modeling of the Rydberg to Valence Excited-State Internal Conversion in Cyclobutanone and Cyclopentanone

In this paper we present 4-state, 5-dimensional Vibronic Coupling Hamiltonians for cyclobutanone and cyclopentanone. Wave packet calculations using these Hamiltonians reveal that for cyclobutanone the (n,3s) to (n,π*) internal conversion involves direct motion in nuclear modes coupling the two states leading to fast population transfer. For cyclopentanone, internal vibrational energy redistribution is a bottleneck for activating reactive nuclear modes leading to slower population transfer