Two-dimensional electronic spectroscopy (2DES) has recently been gaining popularity as an alternative to the more common transient absorption spectroscopy due to the combination of high frequency and time resolution of 2DES. In order to advance the reliable analysis of population dynamics and to optimize the time resolution of the method, one has to understand the numerous field matter interactions that take place at an early and negative time. These interactions have historically been discussed in one-dimensional spectroscopy as coherent artifacts and have been assigned to both resonant and non-resonant system responses during or before the pulse overlap. These coherent artifacts have also been described in 2DES but remain less well-understood due to the complexity of 2DES and the relative novelty of the method. Here, we present 2DES results in two model nanocrystal samples, CdSe and CsPbI3. We demonstrate non-resonant signals due to solvent response during the pulse overlap and resonant signals, which we assign to perturbed free induction decay (PFID), both before and during the pulse overlap. The simulations of the 2DES response functions at early and negative time delays reinforce the assignment of the negative time delay signals to PFID. Modeling reveals that the PFID signals will severely distort the initial picture of the resonant population dynamics. By including these effects in models of 2DES spectra, one is able to push forward the extraction of early time dynamics in 2DES.
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28 February 2023
Research Article|
February 24 2023
Perturbed free induction decay obscures early time dynamics in two-dimensional electronic spectroscopy: The case of semiconductor nanocrystals
Special Collection:
Celebrating 25 Years of Two-dimensional Infrared (2D IR) Spectroscopy
Patrick Brosseau
;
Patrick Brosseau
(Conceptualization, Data curation, Formal analysis, Writing – original draft, Writing – review & editing)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Hélène Seiler
;
Hélène Seiler
(Conceptualization, Data curation)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Samuel Palato
;
Samuel Palato
(Conceptualization, Data curation, Formal analysis)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Colin Sonnichsen
;
Colin Sonnichsen
(Conceptualization, Data curation)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Harry Baker;
Harry Baker
(Data curation)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Etienne Socie
;
Etienne Socie
(Project administration, Resources)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Dallas Strandell
;
Dallas Strandell
(Methodology, Project administration)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
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Patanjali Kambhampati
Patanjali Kambhampati
a)
(Conceptualization, Funding acquisition, Writing – original draft, Writing – review & editing)
Department of Chemistry, McGill University
, Montreal, Quebec H3A 0G4, Canada
a)Author to whom correspondence should be addressed: pat.kambhampati@mcgill.ca
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a)Author to whom correspondence should be addressed: pat.kambhampati@mcgill.ca
Note: This paper is part of the JCP Special Topic on Celebrating 25 Years of Two-dimensional Infrared (2D IR) Spectroscopy.
J. Chem. Phys. 158, 084201 (2023)
Article history
Received:
December 09 2022
Accepted:
February 08 2023
Citation
Patrick Brosseau, Hélène Seiler, Samuel Palato, Colin Sonnichsen, Harry Baker, Etienne Socie, Dallas Strandell, Patanjali Kambhampati; Perturbed free induction decay obscures early time dynamics in two-dimensional electronic spectroscopy: The case of semiconductor nanocrystals. J. Chem. Phys. 28 February 2023; 158 (8): 084201. https://doi.org/10.1063/5.0138252
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