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"Conte, Stefano"
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Optical parametric amplification by monolayer transition metal dichalcogenides
by
Curreli Nicola
,
Yao Kaiyuan
,
Ciattoni Alessandro
in
Amplification
,
Chalcogenides
,
First principles
2021
Optical parametric amplification is a second-order nonlinear process whereby an optical signal is amplified by a pump via the generation of an idler field1. This mechanism is inherently related to spontaneous parametric down-conversion, which currently constitutes the building block for entangled photon pair generation2, a process that is exploited in modern quantum technologies. Here we demonstrate single-pass optical parametric amplification at the ultimate thickness limit; using semiconducting transition metal dichalcogenides3,4, we show that amplification can be attained over propagation through a single atomic layer. Such a second-order nonlinear interaction at the two-dimensional limit bypasses phase-matching requirements5 and achieves ultrabroad amplification bandwidths. In agreement with first-principle calculations, we observe that the amplification process is independent of the in-plane polarization of signal and pump fields. By the use of AA-stacked multilayers, we present a clear pathway towards the scaling of conversion efficiency. Our results pave the way for the development of atom-sized tunable sources of radiation with potential applications in nanophotonics and quantum information technology.Single-pass optical parametric amplification is demonstrated following propagation though an atomically thin semiconducting transition metal dichalcogenide. The demonstration may lead to atom-sized tunable light sources.
Journal Article
The ultrafast onset of exciton formation in 2D semiconductors
by
Katsch, Florian
,
Trovatello, Chiara
,
Conte, Stefano Dal
in
140/125
,
639/624/1107/527
,
639/925/357/1018
2020
The equilibrium and non-equilibrium optical properties of single-layer transition metal dichalcogenides (TMDs) are determined by strongly bound excitons. Exciton relaxation dynamics in TMDs have been extensively studied by time-domain optical spectroscopies. However, the formation dynamics of excitons following non-resonant photoexcitation of free electron-hole pairs have been challenging to directly probe because of their inherently fast timescales. Here, we use extremely short optical pulses to non-resonantly excite an electron-hole plasma and show the formation of two-dimensional excitons in single-layer MoS
2
on the timescale of 30 fs via the induced changes to photo-absorption. These formation dynamics are significantly faster than in conventional 2D quantum wells and are attributed to the intense Coulombic interactions present in 2D TMDs. A theoretical model of a coherent polarization that dephases and relaxes to an incoherent exciton population reproduces the experimental dynamics on the sub-100-fs timescale and sheds light into the underlying mechanism of how the lowest-energy excitons, which are the most important for optoelectronic applications, form from higher-energy excitations. Importantly, a phonon-mediated exciton cascade from higher energy states to the ground excitonic state is found to be the rate-limiting process. These results set an ultimate timescale of the exciton formation in TMDs and elucidate the exceptionally fast physical mechanism behind this process.
The formation dynamics of excitons in 2D transition metal dichalcogenides are challenging to probe directly because of their inherently fast timescales. Here, the authors use extremely short optical pulses to excite an electron-hole plasma, and show the formation of 2D excitons in MoS
2
on the timescale of 30 fs.
Journal Article
Exciton–phonon coupling strength in single-layer MoSe2 at room temperature
by
Soavi, Giancarlo
,
Trovatello, Chiara
,
Dal Conte, Stefano
in
140/125
,
639/624/1107/527/1819
,
639/925/357/1018
2021
Single-layer transition metal dichalcogenides are at the center of an ever increasing research effort both in terms of fundamental physics and applications. Exciton–phonon coupling plays a key role in determining the (opto)electronic properties of these materials. However, the exciton–phonon coupling strength has not been measured at room temperature. Here, we use two-dimensional micro-spectroscopy to determine exciton–phonon coupling of single-layer MoSe
2
. We detect beating signals as a function of waiting time induced by the coupling between A excitons and
A
′
1
optical phonons. Analysis of beating maps combined with simulations provides the exciton–phonon coupling. We get a Huang–Rhys factor ~1, larger than in most other inorganic semiconductor nanostructures. Our technique offers a unique tool to measure exciton–phonon coupling also in other heterogeneous semiconducting systems, with a spatial resolution ~260 nm, and provides design-relevant parameters for the development of optoelectronic devices.
The exciton–phonon coupling (EXPC) affects the opto-electronic properties of atomically thin semiconductors. Here, the authors develop two-dimensional micro-spectroscopy to determine the EXPC of monolayer MoSe
2
.
Journal Article
Ultrafast hot carrier transfer in WS2/graphene large area heterostructures
2022
Charge transfer processes in two-dimensional van der Waals heterostructures enable upconversion of low energy photons and efficient charge carriers extraction. Here we use broadband ultrafast optical spectroscopy to track charge transfer dynamics in large-area 2D heterostructures made of epitaxial single-layer tungsten disulfide (WS2) grown by chemical vapour deposition on graphene. Selective carrier photoexcitation in graphene, with tunable near-infrared photon energies as low as 0.8 eV (i.e. lower than half of the optical bandgap of WS2), results in an almost instantaneous bleaching of the WS2 excitonic peaks in the visible range, due to the interlayer charge transfer process. We find that the charge transfer signal is strongly non-linear with the pump fluence and it becomes progressively more linear at increasing pump photon energies, while the interlayer photoinjection rate is constant in energy, reflecting the spectrally flat absorbance of graphene. We ascribe the interlayer charge transfer to a fast transfer of hot carriers, photogenerated in graphene, to the semiconducting layer. The measured sub-20-fs hot-carrier transfer sets the ultimate timescale for this process. Besides their fundamental interest, our results are technologically relevant because, given the capability of large-area deterministic growth of the heterostructure, they open up promising paths for novel 2D photodetectors, also potentially scalable to industrial platforms.
Journal Article
Broadband, electrically tunable third-harmonic generation in graphene
by
Celebrano, Michele
,
Soavi, Giancarlo
,
Rostami, Habib
in
Broadband
,
Data processing
,
Electrical resistivity
2018
Optical harmonic generation occurs when high intensity light (>1010 W m–2) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong light–matter interaction and electrically and broadband tunable third-order nonlinear susceptibility. Here, we show that the third-harmonic generation efficiency in graphene can be increased by almost two orders of magnitude by controlling the Fermi energy and the incident photon energy. This enhancement is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from resonant multiphoton transitions. Thanks to the linear dispersion of the massless Dirac fermions, gate controllable third-harmonic enhancement can be achieved over an ultrabroad bandwidth, paving the way for electrically tunable broadband frequency converters for applications in optical communications and signal processing.
Journal Article
Revealing the high-energy electronic excitations underlying the onset of high-temperature superconductivity in cuprates
by
Coslovich, Giacomo
,
Conte, Stefano Dal
,
Raichle, Markus
in
639/301/119/1003
,
639/301/119/995
,
639/766/400/1119
2011
In strongly correlated systems the electronic properties at the Fermi energy (
E
F
) are intertwined with those at high-energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high-energy scale physics associated with Mott-like excitations (|
E
−
E
F
|>1 eV) is involved in the condensate formation. Here, we report the interplay between the many-body high-energy CuO
2
excitations at 1.5 and 2 eV, and the onset of HTSC. This is revealed by a novel optical pump-supercontinuum-probe technique that provides access to the dynamics of the dielectric function in Bi
2
Sr
2
Ca
0.92
Y
0.08
Cu
2
O
8+
δ
over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (
T
c
).
Understanding how the high-energy physics of Mott-like excitations affects condensate formation is a key challenge in high-temperature superconductivity. Giannetti
et al
. clarify the relationship of many-body CuO
2
excitations and the onset of superconductivity using a new optical pump supercontinuum-probe technique.
Journal Article
Time-domain observation of interlayer exciton formation and thermalization in a MoSe2/WSe2 heterostructure
by
Policht, Veronica R.
,
Zhu, Xiaoyang
,
Katzer, Manuel
in
639/624/1107/527
,
639/766/119/1000/1018
,
Absorption spectroscopy
2023
Vertical heterostructures of transition metal dichalcogenides (TMDs) host interlayer excitons with electrons and holes residing in different layers. With respect to their intralayer counterparts, interlayer excitons feature longer lifetimes and diffusion lengths, paving the way for room temperature excitonic optoelectronic devices. The interlayer exciton formation process and its underlying physical mechanisms are largely unexplored. Here we use ultrafast transient absorption spectroscopy with a broadband white-light probe to simultaneously resolve interlayer charge transfer and interlayer exciton formation dynamics in a MoSe
2
/WSe
2
heterostructure. We observe an interlayer exciton formation timescale nearly an order of magnitude (~1 ps) longer than the interlayer charge transfer time (~100 fs). Microscopic calculations attribute this relative delay to an interplay of a phonon-assisted interlayer exciton cascade and thermalization, and excitonic wave-function overlap. Our results may explain the efficient photocurrent generation observed in optoelectronic devices based on TMD heterostructures, as the interlayer excitons are able to dissociate during thermalization.
Here, the authors use ultrafast transient absorption spectroscopy with a broadband white-light probe to simultaneously resolve interlayer charge transfer and interlayer exciton formation dynamics in a MoSe
2
/WSe
2
heterostructure.
Journal Article
Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS2 homobilayers
by
David G. Lidzey
,
Xuerong Hu
,
Kenji Watanabe
in
639/301/357/1018
,
639/624/399/1097
,
639/766/119/1000/1018
2023
Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS
2
to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS
2
monolayers, both hIX and dipolaritons exhibit ≈ 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.
In semiconductors, accessing nonlinear interactions between excitons strongly coupled to light will be key for quantum technologies. Here, in atomic bilayers of MoS
2
, new types of excitons are discovered showing strong inter-excitonic interactions.
Journal Article
Targeting Progression in Pulmonary Fibrosis: An Overview of Underlying Mechanisms, Molecular Biomarkers, and Therapeutic Intervention
by
Mariniello, Domenica Francesca
,
Perrotta, Fabio
,
Conte, Stefano
in
antifibrotics
,
Apoptosis
,
Biological markers
2024
Interstitial lung diseases comprise a heterogenous range of diffuse lung disorders, potentially resulting in pulmonary fibrosis. While idiopathic pulmonary fibrosis has been recognized as the paradigm of a progressive fibrosing interstitial lung disease, other conditions with a progressive fibrosing phenotype characterized by a significant deterioration of the lung function may lead to a burden of significant symptoms, a reduced quality of life, and increased mortality, despite treatment. There is now evidence indicating that some common underlying biological mechanisms can be shared among different chronic fibrosing disorders; therefore, different biomarkers for disease-activity monitoring and prognostic assessment are under evaluation. Thus, understanding the common pathways that induce the progression of pulmonary fibrosis, comprehending the diversity of these diseases, and identifying new molecular markers and potential therapeutic targets remain highly crucial assignments. The purpose of this review is to examine the main pathological mechanisms regulating the progression of fibrosis in interstitial lung diseases and to provide an overview of potential biomarker and therapeutic options for patients with progressive pulmonary fibrosis.
Journal Article
Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons
by
Soavi, Giancarlo
,
Müllen, Klaus
,
Dal Conte, Stefano
in
639/301/119
,
639/766/400/385
,
639/925/357/918
2016
Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.
Graphene nanoribbons confine electrons to just one dimension and this gives rise to strong electron–hole interactions. Here, the authors investigate the creation and recombination of biexcitons in these structures by ultrafast optical pulses using femtosecond transient absorption spectroscopy.
Journal Article