Analytical chemistry, multidimensional spectral signatures, and the future of coherent multidimensional spectroscopy

Optical multidimensional coherent SPECTROSCOPY

Coherent multidimensional optical spectroscopy.

Multidimensional optical techniques, the focus of this special issue, are analogues of their NMR counterparts; that is, rather than using spin transitions as little spies within a molecule, we use vibrational or optical transitions. Similar to NMR, the spectroscopic states often respond in a very sensitive way to their chemical environment. By modeling the coupling of one of these states to eit...

Frequency combs enable rapid and high-resolution multidimensional coherent spectroscopy.

Dual laser frequency combs can rapidly measure high-resolution linear absorption spectra. However, one-dimensional linear techniques cannot distinguish the sources of resonances in a mixture of different analytes, nor can they separate inhomogeneous and homogeneous broadening. Here, we overcame these limitations by acquiring high-resolution multidimensional nonlinear coherent spectra with frequ...

Chirality-induced signals in coherent multidimensional spectroscopy of excitons.

The nonlocal second- and third-order susceptibilities of an isotropic ensemble of aggregates are calculated by solving the nonlinear exciton equations which map the system into coupled anharmonic oscillators. Both electric and magnetic contributions are included using the minimal-coupling Hamiltonian. The various tensor components are evaluated to first order in the optical wave vector k. Addit...

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

Multidimensional Coherent optical Spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interaction...