Photocurrent detected 2D spectroscopy via a pulse shaper : insights and strategies for optimally untangling the nonlinear response
Amarotti, Edoardo LU ; Bolzonello, Luca ; Lee, Sun Ho ; Zigmantas, Donatas LU
; Park, Nam Gyu
; Hulst, Niek Van
and Pullerits, Tönu
LU
(2026)
In Optics Express
34(2).
p.2409-2423
- Abstract
Action-detected two-dimensional electronic spectroscopy (A-2DES) provides valuable insights into ultrafast dynamics within functional materials and devices by measuring incoherent signals like photocurrent. This work details the implementation and optimization of a pulse-shaper-based A-2DES setup, focusing on methodological strategies crucial for acquiring high-fidelity data. We present a comprehensive analysis of phase modulation routines, elucidating the critical interplay between pattern parameters (N, ni), pattern repetitions (Nrep), laser repetition rate, and acousto-optic pulse shaper constraints (e.g., streaming rate, radio frequency generator nonlinearities). Utilizing a perovskite solar cell as a model... (More)
Action-detected two-dimensional electronic spectroscopy (A-2DES) provides valuable insights into ultrafast dynamics within functional materials and devices by measuring incoherent signals like photocurrent. This work details the implementation and optimization of a pulse-shaper-based A-2DES setup, focusing on methodological strategies crucial for acquiring high-fidelity data. We present a comprehensive analysis of phase modulation routines, elucidating the critical interplay between pattern parameters (N, ni), pattern repetitions (Nrep), laser repetition rate, and acousto-optic pulse shaper constraints (e.g., streaming rate, radio frequency generator nonlinearities). Utilizing a perovskite solar cell as a model system, we systematically identify and characterize significant inaccuracies inherent to A-2DES measurements. These include distortions originating from Fourier transform processing of improperly trimmed time-domain data (phase leakage), signal accumulation effects due to insufficient sample response discharge between pulse sequences at high repetition rates, and shortcomings induced by pulse shaper operation at elevated streaming powers. Crucially, we demonstrate robust data post-processing strategies, including precise data point selection for Fourier analysis and a phase correction routine, to mitigate these imperfections and retrieve accurate 2D spectra effectively. This rigorous methodological investigation and anomalous features characterization provide essential guidelines for optimizing pulse-shaper-based A-2DES experiments, ensuring data integrity and enabling reliable extraction of complex photophysical information in complex systems.
(Less)
- author
- Amarotti, Edoardo
LU
; Bolzonello, Luca
; Lee, Sun Ho
; Zigmantas, Donatas
LU
; Park, Nam Gyu
; Hulst, Niek Van
and Pullerits, Tönu
LU
- organization
- publishing date
- 2026-01
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Optics Express
- volume
- 34
- issue
- 2
- pages
- 15 pages
- publisher
- Optical Society of America
- external identifiers
-
- scopus:105028621218
- ISSN
- 1094-4087
- DOI
- 10.1364/OE.566553
- language
- English
- LU publication?
- yes
- id
- 251acb57-f38c-4b0c-ab7c-773578c56e16
- date added to LUP
- 2026-02-19 14:10:10
- date last changed
- 2026-02-19 14:11:26
@article{251acb57-f38c-4b0c-ab7c-773578c56e16,
abstract = {{<p>Action-detected two-dimensional electronic spectroscopy (A-2DES) provides valuable insights into ultrafast dynamics within functional materials and devices by measuring incoherent signals like photocurrent. This work details the implementation and optimization of a pulse-shaper-based A-2DES setup, focusing on methodological strategies crucial for acquiring high-fidelity data. We present a comprehensive analysis of phase modulation routines, elucidating the critical interplay between pattern parameters (N, n<sub>i</sub>), pattern repetitions (N<sub>rep</sub>), laser repetition rate, and acousto-optic pulse shaper constraints (e.g., streaming rate, radio frequency generator nonlinearities). Utilizing a perovskite solar cell as a model system, we systematically identify and characterize significant inaccuracies inherent to A-2DES measurements. These include distortions originating from Fourier transform processing of improperly trimmed time-domain data (phase leakage), signal accumulation effects due to insufficient sample response discharge between pulse sequences at high repetition rates, and shortcomings induced by pulse shaper operation at elevated streaming powers. Crucially, we demonstrate robust data post-processing strategies, including precise data point selection for Fourier analysis and a phase correction routine, to mitigate these imperfections and retrieve accurate 2D spectra effectively. This rigorous methodological investigation and anomalous features characterization provide essential guidelines for optimizing pulse-shaper-based A-2DES experiments, ensuring data integrity and enabling reliable extraction of complex photophysical information in complex systems.</p>}},
author = {{Amarotti, Edoardo and Bolzonello, Luca and Lee, Sun Ho and Zigmantas, Donatas and Park, Nam Gyu and Hulst, Niek Van and Pullerits, Tönu}},
issn = {{1094-4087}},
language = {{eng}},
number = {{2}},
pages = {{2409--2423}},
publisher = {{Optical Society of America}},
series = {{Optics Express}},
title = {{Photocurrent detected 2D spectroscopy via a pulse shaper : insights and strategies for optimally untangling the nonlinear response}},
url = {{http://dx.doi.org/10.1364/OE.566553}},
doi = {{10.1364/OE.566553}},
volume = {{34}},
year = {{2026}},
}