Coherent multidimensional spectroscopy in the gas phase

Recent work applying multidimentional coherent electronic spectroscopy at dilute samples in the gas phase is reviewed. The development of refined phase-cycling approaches with improved sensitivity has opened-up new opportunities to probe even dilute gas-phase samples. In this context, first results of 2-dimensional spectroscopy performed at doped helium droplets reveal the femtosecond dynamics upon electronic excitation of cold, weakly-bound molecules, and even the induced dynamics from the interaction with the helium environment. Such experiments, offering well-defined conditions at low temperatures, are potentially enabling the isolation of fundamental processes in the excitation and charge transfer dynamics of molecular structures which so far have been masked in complex bulk environments.Comment: Invited Review Articl

Efficient Downlink Channel Reconstruction for FDD Multi-Antenna Systems

In this paper, we propose an efficient downlink channel reconstruction scheme for a frequency-division-duplex multi-antenna system by utilizing uplink channel state information combined with limited feedback. Based on the spatial reciprocity in a wireless channel, the downlink channel is reconstructed by using frequency-independent parameters. We first estimate the gains, delays, and angles during uplink sounding. The gains are then refined through downlink training and sent back to the base station (BS). With limited overhead, the refinement can substantially improve the accuracy of the downlink channel reconstruction. The BS can then reconstruct the downlink channel with the uplink-estimated delays and angles and the downlink-refined gains. We also introduce and extend the Newtonized orthogonal matching pursuit (NOMP) algorithm to detect the delays and gains in a multi-antenna multi-subcarrier condition. The results of our analysis show that the extended NOMP algorithm achieves high estimation accuracy. Simulations and over-the-air tests are performed to assess the performance of the efficient downlink channel reconstruction scheme. The results show that the reconstructed channel is close to the practical channel and that the accuracy is enhanced when the number of BS antennas increases, thereby highlighting that the promising application of the proposed scheme in large-scale antenna array systems

Modeling Earthen Dike Stability: Sensitivity Analysis and Automatic Calibration of Diffusivities Based on Live Sensor Data

The paper describes concept and implementation details of integrating a finite element module for dike stability analysis Virtual Dike into an early warning system for flood protection. The module operates in real-time mode and includes fluid and structural sub-models for simulation of porous flow through the dike and for dike stability analysis. Real-time measurements obtained from pore pressure sensors are fed into the simulation module, to be compared with simulated pore pressure dynamics. Implementation of the module has been performed for a real-world test case - an earthen levee protecting a sea-port in Groningen, the Netherlands. Sensitivity analysis and calibration of diffusivities have been performed for tidal fluctuations. An algorithm for automatic diffusivities calibration for a heterogeneous dike is proposed and studied. Analytical solutions describing tidal propagation in one-dimensional saturated aquifer are employed in the algorithm to generate initial estimates of diffusivities

Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale

We report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.Comment: 12 pages, 4 figures. Changes from previous version: added panel labels to figures 3-

All-optical retrieval of the global phase for two-dimensional Fourier-transform spectroscopy

A combination of spatial interference patterns and spectral interferometry are used to find the global phase for non-collinear two-dimensional Fourier-transform (2DFT) spectra. Results are compared with those using the spectrally resolved transient absorption (STRA) method to find the global phase when excitation is with co-linear polarization. Additionally cross-linear polarized 2DFT spectra are correctly phased using the all-optical technique, where the SRTA is not applicable.Comment: 6 pages, 7 figures, journal publicatio

Sum-over-states vs quasiparticle pictures of coherent correlation spectroscopy of excitons in semiconductors; femtosecond analogues of multidimensional NMR

Two-dimensional correlation spectroscopy (2DCS) based on the nonlinear optical response of excitons to sequences of ultrafast pulses, has the potential to provide some unique insights into carrier dynamics in semiconductors. The most prominent feature of 2DCS, cross peaks, can best be understood using a sum-over-states picture involving the many-body eigenstates. However, the optical response of semiconductors is usually calculated by solving truncated equations of motion for dynamical variables, which result in a quasiparticle picture. In this work we derive Green's function expressions for the four wave mixing signals generated in various phase-matching directions and use them to establish the connection between the two pictures. The formal connection with Frenkel excitons (hard-core bosons) and vibrational excitons (soft-core bosons) is pointed out.Comment: Accepted to Phys. Rev.