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Papers by Roberto Rosati
Nano Letters, Sep 18, 2019
The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic... more The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.
arXiv (Cornell University), May 21, 2021
ACS Photonics, Sep 4, 2020
arXiv (Cornell University), Feb 6, 2023
Nature Communications
The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral hetero... more The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe2-WSe2 heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. We show that for hBN-encapsulated heterostructures, CT excitons exhibi...
Nanoscale, 2021
Combining microscopic theory and spatiotemporal photoluminescence experiments we reveal an unconv... more Combining microscopic theory and spatiotemporal photoluminescence experiments we reveal an unconventional, time-dependent exciton diffusion in atomically thin semiconductors. This behavior originates from hot dark excitons with large excess energies.
Physical Review Letters, 2021
Applied Physics Letters, 2015
We investigate the propagation of electron wavepackets in single-walled carbon nanotubes via a Li... more We investigate the propagation of electron wavepackets in single-walled carbon nanotubes via a Lindblad-based density-matrix approach that enables us to account for both dissipation and decoherence effects induced by various phonon modes. We show that, while in semiconducting nanotubes the wavepacket experiences the typical dispersion of conventional materials, in metallic nanotubes its shape remains essentially unaltered, even in the presence of the electron-phonon coupling, up to micron distances at room temperature.
2014 International Workshop on Computational Electronics (IWCE), 2014
Nature Communications, 2021
Transport of charge carriers is at the heart of current nanoelectronics. In conventional material... more Transport of charge carriers is at the heart of current nanoelectronics. In conventional materials, electronic transport can be controlled by applying electric fields. Atomically thin semiconductors, however, are governed by excitons, which are neutral electron-hole pairs and as such cannot be controlled by electrical fields. Recently, strain engineering has been introduced to manipulate exciton propagation. Strain-induced energy gradients give rise to exciton funneling up to a micrometer range. Here, we combine spatiotemporal photoluminescence measurements with microscopic theory to track the way of excitons in time, space and energy. We find that excitons surprisingly move away from high-strain regions. This anti-funneling behavior can be ascribed to dark excitons which possess an opposite strain-induced energy variation compared to bright excitons. Our findings open new possibilities to control transport in exciton-dominated materials. Overall, our work represents a major advance...
Nano Letters, Sep 18, 2019
The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic... more The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.
arXiv (Cornell University), May 21, 2021
ACS Photonics, Sep 4, 2020
arXiv (Cornell University), Feb 6, 2023
Nature Communications
The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral hetero... more The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe2-WSe2 heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. We show that for hBN-encapsulated heterostructures, CT excitons exhibi...
Nanoscale, 2021
Combining microscopic theory and spatiotemporal photoluminescence experiments we reveal an unconv... more Combining microscopic theory and spatiotemporal photoluminescence experiments we reveal an unconventional, time-dependent exciton diffusion in atomically thin semiconductors. This behavior originates from hot dark excitons with large excess energies.
Physical Review Letters, 2021
Applied Physics Letters, 2015
We investigate the propagation of electron wavepackets in single-walled carbon nanotubes via a Li... more We investigate the propagation of electron wavepackets in single-walled carbon nanotubes via a Lindblad-based density-matrix approach that enables us to account for both dissipation and decoherence effects induced by various phonon modes. We show that, while in semiconducting nanotubes the wavepacket experiences the typical dispersion of conventional materials, in metallic nanotubes its shape remains essentially unaltered, even in the presence of the electron-phonon coupling, up to micron distances at room temperature.
2014 International Workshop on Computational Electronics (IWCE), 2014
Nature Communications, 2021
Transport of charge carriers is at the heart of current nanoelectronics. In conventional material... more Transport of charge carriers is at the heart of current nanoelectronics. In conventional materials, electronic transport can be controlled by applying electric fields. Atomically thin semiconductors, however, are governed by excitons, which are neutral electron-hole pairs and as such cannot be controlled by electrical fields. Recently, strain engineering has been introduced to manipulate exciton propagation. Strain-induced energy gradients give rise to exciton funneling up to a micrometer range. Here, we combine spatiotemporal photoluminescence measurements with microscopic theory to track the way of excitons in time, space and energy. We find that excitons surprisingly move away from high-strain regions. This anti-funneling behavior can be ascribed to dark excitons which possess an opposite strain-induced energy variation compared to bright excitons. Our findings open new possibilities to control transport in exciton-dominated materials. Overall, our work represents a major advance...