Abstract
Two-dimensional electronic spectroscopy based on passive phase stabilization methods is now well known and widely employed worldwide. In the most recent fully non-collinear implementations, a great phase stability is often achieved at the expense of the independent control over the pulse timings, limiting the full potential of the technique. Here we propose several modifications in the experiment geometry, calibration procedures, and data acquisition and processing routines. The setup is easily tunable to record different phase-matching directions, such as rephasing, non-rephasing and double quantum signals, still maintaining high levels of phase control and phase stability. The performances of the proposed setup are exemplified by measures on the standard dye zinc phtalocyanine and porphyrin J-aggregates.
Highlights
Two-dimensional electronic spectroscopy (2DES) is a thirdorder non-linear technique which is successfully spreading in the latest years thanks to its capability of unraveling fine details of the ultrafast dynamics of the systems under investigation [1,2,3]. 2DES is based on the interaction of three ultrafast laser pulses with an optical sample
It follows that the higherfrequency components are subjected to a longer delay than the lower-frequency components, resulting in a frequency shift after Fourier transforming from the time to the frequency domain
The Fourier transform of the SI is the simplest method to correlate the position of the stages with the time delay between the local oscillator (LO) and the selected pulse: when a spectral interference between two pulses is Fourier transformed, a peak in the time domain is obtained, which is centered at the delay time between the interfering pulses
Summary
Two-dimensional electronic spectroscopy (2DES) is a thirdorder non-linear technique which is successfully spreading in the latest years thanks to its capability of unraveling fine details of the ultrafast dynamics of the systems under investigation [1,2,3]. 2DES is based on the interaction of three ultrafast laser pulses with an optical sample. Many different approaches have been used to increase the phase stability in fully non-collinear 2DES experiments, including active [14] and passive phase stabilization methods, through diffractive optics (DO) [15,16], pulse shaping [17] and, more in general, particular geometries that allow the phase-locking of specific pulse pairs [18,19]. These last methods, in particular, achieve a great phase stability working in a full optical rotating frame, but they require coupling the motion of pairs of pulses, partially losing the independent control of timings. The full potential of the described approach is exemplified through the characterization of the full 2D response of solutions of J-aggregates of the diacid form of the water-soluble tetra-(p sulphonato)-phenylporphyrin (H2TPPS)
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