We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an incoherent nonlinear response due to pairs of photoexcitations produced via linear excitation pathways contributes to the measured signal as an unexpected background [Grégoire et al., J. Chem. Phys. 147, 114201 (2017)]. Here, we simulate the effect of such incoherent population mixing in the photocurrent signal collected from a GaAs solar cell by acting externally on the transimpedance amplifier circuit used for phase-sensitive detection, and we identify an effective strategy to recognize the presence of incoherent population mixing in 2D data. While we find that incoherent mixing is reflected by the crosstalk between the linear amplitudes at the two time-delay variables in the four-pulse excitation sequence, we do not observe any strict phase correlations between the coherent and incoherent contributions, as expected from modeling of a simple system.
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28 November 2022
Research Article|
November 22 2022
Identifying incoherent mixing effects in the coherent two-dimensional photocurrent excitation spectra of semiconductors
Ilaria Bargigia
;
Ilaria Bargigia
a)
(Formal analysis, Investigation, Supervision, Writing – original draft, Writing – review & editing)
1
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
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Elizabeth Gutiérrez-Meza
;
Elizabeth Gutiérrez-Meza
(Formal analysis, Investigation, Writing – review & editing)
1
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
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David A. Valverde-Chávez
;
David A. Valverde-Chávez
(Investigation, Methodology, Writing – review & editing)
1
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
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Sarah R. Marques;
Sarah R. Marques
(Formal analysis, Investigation)
1
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
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Ajay Ram Srimath Kandada
;
Ajay Ram Srimath Kandada
(Supervision, Writing – original draft, Writing – review & editing)
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
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Carlos Silva
Carlos Silva
b)
(Conceptualization, Funding acquisition, Project administration, Supervision, Visualization, Writing – original draft, Writing – review & editing)
1
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
3
School of Physics, Georgia Institute of Technology
, 837 State Street, Atlanta, Georgia 30332, USA
4
School of Materials Science and Engineering, Georgia Institute of Technology
, 771 Ferst Drive NW, Atlanta, Georgia 30332, USA
b)Author to whom correspondence should be addressed: [email protected]
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a)
Current address: Center for Nano Science and Technology@PoliMi, Istituto Italiano di Tecnologia, via Pascoli 70/3, 20133 Milano, Italy.
b)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 157, 204202 (2022)
Article history
Received:
August 18 2022
Accepted:
November 07 2022
Citation
Ilaria Bargigia, Elizabeth Gutiérrez-Meza, David A. Valverde-Chávez, Sarah R. Marques, Ajay Ram Srimath Kandada, Carlos Silva; Identifying incoherent mixing effects in the coherent two-dimensional photocurrent excitation spectra of semiconductors. J. Chem. Phys. 28 November 2022; 157 (20): 204202. https://doi.org/10.1063/5.0121635
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