Pulse overlap artifacts and double quantum coherence spectroscopy

Hedse, Albin; Kalaee, Alex Arash Sand; Wacker, Andreas; Pullerits, Tõnu (2023-04). Pulse overlap artifacts and double quantum coherence spectroscopy. Journal of Chemical Physics, 158, (14)
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DOI:
| Published | English
Authors:
Hedse, Albin ; Kalaee, Alex Arash Sand ; Wacker, Andreas ; Pullerits, Tõnu
Department:
LU Profile Area: Light and Materials
LTH Profile Area: Nanoscience and Semiconductor Technology
Chemical Physics
NanoLund: Centre for Nanoscience
Mathematical Physics
LTH Profile Area: Photon Science and Technology
eSSENCE: The e-Science Collaboration
Abstract:

The double quantum coherence (DQC) signal in nonlinear spectroscopy gives information about the many-body correlation effects not easily available by other methods. The signal is short-lived, consequently, a significant part of it is generated during the pulse overlap. Since the signal is at two times the laser frequency, one may intuitively expect that the pulse overlap-related artifacts are filtered out by the Fourier transform. Here, we show that this is not the case. We perform explicit calculations of phase-modulated two-pulse experiments of a two-level system where the DQC is impossible. Still, we obtain a significant signal at the modulation frequency, which corresponds to the DQC, while the Fourier transform over the pulse delay shows a double frequency. We repeat the calculations with a three-level system where the true DQC signal occurs. We conclude that with realistic dephasing times, the pulse-overlap artifact can be significantly stronger than the DQC signal. Our results call for great care when analyzing such experiments. As a rule of thumb, we recommend that only delays larger than 1.5 times the pulse length should be used.

Keywords:
Atom and Molecular Physics and Optics ; Signal Processing
ISSN:
0021-9606
LUP-ID:
d5b56044-3f14-4ebd-9cec-fe05c8906983 | Link: https://lup.lub.lu.se/record/d5b56044-3f14-4ebd-9cec-fe05c8906983 | Statistics

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