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Title

Ultrafast optical multidimensional spectroscopy without interferometry

Author(s)

Davis, J. A.;  Calhoun, T. R.;  Nugent, K. A.;  Quiney, H. M.

Abstract

We present here the details of a phase retrieval technique that provides access to multidimensional modalities that are not currently available using existing interferometric techniques. The development of multidimensional optical spectroscopy has facilitated significant insights into electronic processes in physics, chemistry, and biology. The versatility and number of available techniques are, however, significantly limited by the requirement that the detection be interferometric. Many of these techniques are closely related to the vast range of multidimensional NMR spectroscopies, which revolutionized analytical chemistry more than 30 years ago. We focus here on the specific case of two-color multidimensional spectroscopy (analogous to heteronuclear NMR) and discuss the details of an iterative algorithm that recovers the relative phase relationships required to perform the Fourier transformation and find the unique solution for the 2D spectrum. A detailed guide is provided that describes the practical implementation of such algorithms. The effectiveness and accuracy of the phase retrieval process are assessed for simulated one- and two-color experiments. It is also compared with one-color experimental data for which the target phase information has been obtained independently by interferometry. In all the cases, the present algorithm yields results that compare well with the solutions obtained by other means. There are, however, some limitations and potential pitfalls that are identified and discussed. We conclude with a discussion of the potential applications and further advances that may be possible by adopting iterative phase retrieval algorithms of the type discussed here.

Publication type

Journal article

Research centre

Swinburne University of Technology. Faculty of Engineering and Industrial Sciences. Centre for Atom Optics and Ultrafast Spectroscopy

Source

Journal of Chemical Physics, Vol. 134, no. 2 (Jan 2011), paper no. 024504

Publication year

2011

FOR Code(s)

0202 Atomic, Molecular, Nuclear, Particle and Plasma Physics;  0306 Physical Chemistry (Incl. Structural);  0904 Chemical Engineering

Keyword(s)

Interferometric techniques;  Multidimensional spectroscopy;  Optical spectroscopy

Publisher

American Institute of Physics

ISSN

0021-9606

Publisher URL

http://dx.doi.org/10.1063/1.3528985

Copyright

Copyright © 2011 American Institute of Physics. The published version is reproduced with the kind permission of the publisher.

Additional information

The authors acknowledge support from the Discovery Project grant from the Australian Research Council and the ARC Centre of Excellence for Coherent X-ray Science.

Full text

Peer reviewed