Time-Frequency Signatures of Electronic Coherence of Colloidal CdSe Quantum Dot Dimer Assemblies Probed at Room Temperature by Two-Dimensional Electronic Spectroscopy

James R Hamilton; Edoardo Amarotti; Carlo N Dibenedetto; Marinella Striccoli; Raphael D Levine; Elisabetta Collini; Francoise Remacle

doi:10.3390/nano13142096

Time-Frequency Signatures of Electronic Coherence of Colloidal CdSe Quantum Dot Dimer Assemblies Probed at Room Temperature by Two-Dimensional Electronic Spectroscopy

Nanomaterials (Basel). 2023 Jul 18;13(14):2096. doi: 10.3390/nano13142096.

Authors

James R Hamilton¹, Edoardo Amarotti², Carlo N Dibenedetto^{3

4}, Marinella Striccoli³, Raphael D Levine⁵, Elisabetta Collini², Francoise Remacle¹

Affiliations

¹ Department of Theoretical Physical Chemistry, University of Liège, B4000 Liège, Belgium.
² Department of Chemical Sciences, University of Padova, 35131 Padova, Italy.
³ CNR-IPCF SS Bari, c/o Chemistry Department, University of Bari Aldo Moro, 70126 Bari, Italy.
⁴ Chemistry Department, University of Bari Aldo Moro, 70126 Bari, Italy.
⁵ The Fritz Haber Research Center for Molecular Dynamics, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.

Abstract

Electronic coherence signatures can be directly identified in the time-frequency maps measured in two-dimensional electronic spectroscopy (2DES). Here, we demonstrate the theory and discuss the advantages of this approach via the detailed application to the fast-femtosecond beatings of a wide variety of electronic coherences in ensemble dimers of quantum dots (QDs), assembled from QDs of 3 nm in diameter, with 8% size dispersion in diameter. The observed and computed results can be consistently characterized directly in the time-frequency domain by probing the polarization in the 2DES setup. The experimental and computed time-frequency maps are found in very good agreement, and several electronic coherences are characterized at room temperature in solution, before the extensive dephasing due to the size dispersion begins. As compared to the frequency-frequency maps that are commonly used in 2DES, the time-frequency maps allow exploiting electronic coherences without additional post-processing and with fewer 2DES measurements. Towards quantum technology applications, we also report on the modeling of the time-frequency photocurrent response of these electronic coherences, which paves the way to integrating QD devices with classical architectures, thereby enhancing the quantum advantage of such technologies for parallel information processing at room temperature.

Keywords: 2D femtosecond electronic spectroscopy; CdSe quantum dot dimers; electronic coherences in quantum dot dimers; photocurrent action spectroscopy; quantum technologies.

Grants and funding

The work of J.R.H. and F.R. is supported by the Fonds National de la Recherche, F.R.S.—FNRS (Belgium), #T.0205.20. Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.—FNRS under Grant #2.5020.11. E.C. acknowledges partial support by “CQ-TECH” Supporting Talent in Research at the University of Padova (STARS), Grant 2019 (2019-UNPD0Z9-0166571). E.C. and M.S. acknowledge the Project NEST—NETWORK 4 ENERGY SUSTAINABLE TRANSITION SPOKE 9: ENERGY-SUSTAINABLE ADVANCED MATERIALS, code PE0000021, Concession Decree No. 1561 of 11 October 2022 by Ministero dell’Università e della Ricerca (MUR) (CUP C93C22005230007—University of Padua, CUP B53C22004060006—CNR).