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Collective Excitonic Structure Governs Anomalously Weak Thermal Optical Dephasing in Conjugated Polymers
Henry J. Kantrow, Elizabeth Gutiérrez-Meza, Eric R. Bittner +2
Conjugated polymer aggregates exhibit optical decoherence in the presence of strong vibronic coupling and substantial diversity in chemical structure, solid-state organization, and…
Biexcitons in Ruddlesden-Popper Metal Halides Probed by Nonlinear Coherent Spectroscopy
Katherine A. Koch, Carlos Silva-Acuña, Ajay Ram Srimath Kandada
Excitons and their correlated complexes underpin the rich photophysics of quantum-confined semiconductors. Among these, biexcitons -- bound states of two electrons and two holes --…
Spectroscopic signatures of biexcitons: A case study in Ruddlesden-Popper lead-halides
Katherine A. Koch, Esteban Rojas-Gatjens, Martin Gomez-Dominguez +3
Exciton-exciton interactions are fundamental to the light-emitting properties of semiconductors, influencing applications from lasers to quantum light sources. In this study, we in…
Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime
Victoria Quirós-Cordero, Esteban Rojas-Gatjens, Martín Gómez-Dominguez +7
Multi-particle correlations of exciton-polaritons and reservoir-excitons in the strong light-matter coupling regime dictate the quantum dynamics of optical microcavities. In this l…
Unveiling multi-quantum excitonic correlations in push-pull polymer semiconductors
Yulong Zheng, Esteban Rojas-Gatjens, Myeongyeon Lee +2
Bound and unbound Frenkel-exciton pairs are essential transient precursors for a variety of photophysical and biochemical processes. In this work, we identify bound and unbound {Fr…
Exciton-photocarrier interference in mixed lead-halide-perovskite nanocrystals
Esteban Rojas-Gatjens, Quinten A. Akkerman, Liberato Manna +2
The use of semiconductor nanocrystals in scalable quantum technologies requires characterization of the exciton coherence dynamics in an \emph{ensemble} of electronically isolated…
Exciton Bimolecular Annihilation Dynamics in Push-Pull Semiconductor Polymers
Yulong Zheng, Rahul Venkatesh, Esteban Rojas-Gatjens +2
Exciton-exciton annihilation is a ubiquitous nonlinear dynamical phenomenon in materials hosting Frenkel excitons, that has been employed to probe exciton diffusion processes in co…
Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide
Esteban Rojas Gatjens, Hao Li, Alejandro Vega Flick +5
We present a study on the many-body exciton interactions in a prototype Ruddlesden-Popper metal halide (RPMH), namely \ce{(PEA)2SnI4} (PEA = phenylethylammine), using coherent two-…
Resolving nonlinear recombination dynamics in semiconductors via ultrafast excitation correlation spectroscopy: Photoluminescence versus photocurrent detection
Esteban Rojas-Gatjens, Kaila Yallum, Yangwei Shi +7
We explore the application of excitation correlation spectroscopy to detect nonlinear photophysical dynamics in two distinct semiconductor classes through time-integrated photolumi…
Chain Conformation and Exciton Delocalization in a Push-Pull Conjugated Polymer
Yulong Zheng, Rahul Venkatesh, Connor P. Callaway +6
Linear and nonlinear optical lineshapes reveal details of excitonic structure in semiconductor polymers. We implement absorption, photoluminescence, and transient absorption spectr…
Formation of a highly ordered red phase in a MEH-PPV: polystyrene pseudogels
Elham Rezasoltani, Jaime Martin, Sophia C. Hayes +5
In this work, we demonstrate the formation of a "red-phase" poly[2-methoxy, 5-(2'- ethyl-hexoxy)-1,4-phenylene vinylene-PPV] (MEH-PPV) embedded into a host matrix of highly entangl…
Frenkel biexcitons in hybrid HJ photophysical aggregates
Elizabeth Gutiérrez Meza, Ravyn Malatesta, Hongmo Li +9
Frenkel excitons, the primary photoexcitations in organic semiconductors that are unequivocally responsible for the optical properties of this materials class, are predicted to for…
Probing polaron excitation spectra in organic semiconductors by photoinduced-absorption-detected two-dimensional coherent spectroscopy
Hao Li, Aurelie Gauthier-Houle, Pascal Gregoire +3
We report a theoretical description and experimental implementation of a novel two-dimensional coherent excitation spectroscopy based on quasi-steady-state photoinduced absorption…
Do ultrafast exciton-polaron decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells?
E. Vella, H. Li, P. Gregoire +7
All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dis…
Multi-phase semicrystalline microstructures drive exciton dissociation in neat plastic semiconductors
Francis Paquin, Jonathan Rivnay, Alberto Salleo +2
The optoelectronic properties of macromolecular semiconductors depend fundamentally on their solid-state microstructure. For example, the molecular-weight distribution influences p…