Pulse overlap artifacts and double quantum coherence spectroscopy
Hedse, Albin LU ; Kalaee, Alex Arash Sand LU ; Wacker, Andreas LU
and Pullerits, Tõnu
LU
(2023)
In Journal of Chemical Physics
158(14).
- 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... (More)
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.
(Less)
- author
- Hedse, Albin
LU
; Kalaee, Alex Arash Sand
LU
; Wacker, Andreas
LU
and Pullerits, Tõnu
LU
- organization
- publishing date
- 2023-04
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Chemical Physics
- volume
- 158
- issue
- 14
- article number
- 141104
- publisher
- American Institute of Physics (AIP)
- external identifiers
-
- pmid:37061484
- scopus:85152525886
- ISSN
- 0021-9606
- DOI
- 10.1063/5.0146148
- language
- English
- LU publication?
- yes
- id
- d5b56044-3f14-4ebd-9cec-fe05c8906983
- date added to LUP
- 2023-07-13 11:01:23
- date last changed
- 2024-11-16 21:24:16
@article{d5b56044-3f14-4ebd-9cec-fe05c8906983,
abstract = {{<p>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.</p>}},
author = {{Hedse, Albin and Kalaee, Alex Arash Sand and Wacker, Andreas and Pullerits, Tõnu}},
issn = {{0021-9606}},
language = {{eng}},
number = {{14}},
publisher = {{American Institute of Physics (AIP)}},
series = {{Journal of Chemical Physics}},
title = {{Pulse overlap artifacts and double quantum coherence spectroscopy}},
url = {{http://dx.doi.org/10.1063/5.0146148}},
doi = {{10.1063/5.0146148}},
volume = {{158}},
year = {{2023}},
}