Publications by authors named "Jean-Sebastien Lauret"

Recent advancements in materials science have shed light on the potential of exploring hierarchical assemblies of molecules on surfaces, driven by both fundamental and applicative challenges. This field encompasses diverse areas including molecular storage, drug delivery, catalysis, and nanoscale chemical reactions. In this context, the utilization of nanotube templates (NTs) has emerged as promising platforms for achieving advanced one-dimensional (1D) molecular assemblies.

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Perovskite nanocrystals have attracted much attention in the last ten years due to their different applications, especially in the photovoltaic domain and LED performance. In this large family of perovskite nanocrystals, CsPbBr nanocrystals are attractive nanomaterials because they are good candidates for obtaining green emissions and exploring new synthesis routes. In this context, controlling the nanometric scale's morphology, particularly the size and monodispersity, is fundamental for exploring their photophysical properties and final applications.

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We report on speeding-up equilibrium recovery in the previously unexplored general case of the underdamped regime using an optically levitated particle. We accelerate the convergence toward equilibrium by an order of magnitude compared to the natural relaxation time. We then discuss the efficiency of the studied protocols, especially for a multidimensional system.

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Nanographene materials are promising building blocks for the growing field of low-dimensional materials for optics, electronics and biophotonics applications. In particular, bottom-up synthesized 0D graphene quantum dots show great potential as single quantum emitters. To fully exploit their exciting properties, the graphene quantum dots must be of high purity; the key parameter for efficient purification being the solubility of the starting materials.

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A new synthetic method for preparing highly calibrated CsPbBr nanocrystal perovskites is described and analyzed using high-resolution scanning transmission electron microscopy. This new method based on soft chemistry leads to the large-scale production of nanocrystals. Such monodisperse nanocrystals allow for the deposition of homogeneous films, which provides new opportunities for the next generation of optoelectronic devices.

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Atomically precise graphene quantum dots synthesized by bottom-up chemistry are promising versatile single emitters with potential applications for quantum photonic technologies. Toward a better understanding and control of graphene quantum dot (GQD) optical properties, we report on single-molecule spectroscopy at cryogenic temperature. We investigate the effect of temperature on the GQDs' spectral linewidth and vibronic replica, which we interpret building on density functional theory calculations.

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Graphene quantum dots, atomically precise nanopieces of graphene, are promising nano-objects with potential applications in various domains such as photovoltaics, quantum light emitters and bio-imaging. Despite their interesting prospects, precise reports on their photophysical properties remain scarce. Here, we report on a study of the photophysics of CH(CH) graphene quantum dots.

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Using femtosecond transient absorption (fs-TA), we investigate the hot exciton relaxation dynamics in strongly confined lead iodide perovskite nanoplatelets (NPLs). The large quantum and dielectric confinement leads to discrete excitonic transitions and strong Stark features in the TA spectra. This prevents the use of conventional relaxation analysis methods extracting the carrier temperature or measuring the buildup of the band-edge bleaching.

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Taking advantage of an innovative design concept for layered halide perovskites with active chromophores acting as organic spacers, we present here the synthesis of two novel two-dimensional (2D) hybrid organic-inorganic halide perovskites incorporating for the first time 100% of a photoactive tetrazine derivative as the organic component. Namely, the use of a heterocyclic ring containing a nitrogen proportion imparts a unique electronic structure to the organic component, with the lowest energy optical absorption in the blue region. The present compound, a tetrazine, presents several resonances between the organic and inorganic components, both in terms of single particle electronic levels and exciton states, providing the ideal playground to discuss charge and energy transfer mechanisms at the organic/inorganic interface.

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Sensitization of graphene with inorganic semiconducting nanostructures has been demonstrated as a powerful strategy to boost its optoelectronic performance. However, the limited tunability of optical properties and toxicity of metal cations in the inorganic sensitizers prohibits their widespread applications, and the in-depth understanding of the essential interfacial charge-transfer process within such hybrid systems remains elusive. Here, we design and develop high-quality nanographene (NG) dispersions with a large-scale production using high-shear mixing exfoliation.

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The synthesis of π-extended porphyrins containing anthracenyl moieties still represents an important challenge. Here, we report on the synthesis of a series of unsubstituted naphthyl-, pyrenyl- and anthracenyl-fused zinc porphyrin derivatives. To this aim, meso-substitued porphyrins are synthesized and the fusion of the PAHs (Polycyclic Aromatic Hydrocarbon) on the β-positions are performed through thermally induced dehydro-aromatization.

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Random lasing is an intriguing phenomenon occurring in disordered structures with optical gain in which light scattering provides the necessary feedback for lasing action. Unlike conventional lasers, random lasing systems emit in all directions due to light scattering. While this property can be desired in some cases, directional emission remains required for most applications.

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Negatively curved nanographene (NG) , having two heptagons and a [5]helicene, was unexpectedly obtained by aryl rearrangement and stepwise cyclodehydrogenations. X-ray crystallography confirmed the saddle-shaped structures of intermediate and NG . The favorability of rearrangement over helicene formation following radical cation or arenium cation mechanisms is supported by theoretical calculations.

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Recently, Ruddlesden-Popper 2D perovskite (RPP) solar cells and light-emitting diodes (LEDs) have shown promising efficiencies and improved stability in comparison to 3D halide perovskites. Here, the exciton recombination dynamics is investigated at room temperature in pure-phase RPP crystals (CHCHNH)(CHNH)PbI ( = 1, 2, 3, and 4) by time-resolved photoluminescence (TRPL) in a large range of power excitations. As the number of perovskite layers increases, we detect the presence of an increasing fraction of out-of-equilibrium free carriers just after photoexcitation, on a picosecond time scale, while the dynamics is characterized by the recombination of excitons with long lifetime spanning several tens of nanoseconds.

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Graphene being a zero-gap material, considerable efforts have been made to develop semiconductors whose structure is compatible with its hexagonal lattice. Size reduction is a promising way to achieve this objective. The reduction of both dimensions of graphene leads to graphene quantum dots.

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Among organic electronic materials, graphene nanoribbons (GNRs) offer extraordinary versatility as next-generation semiconducting materials for nanoelectronics and optoelectronics due to their tunable properties, including charge-carrier mobility, optical absorption, and electronic bandgap, which are uniquely defined by their chemical structures. Although planar GNRs have been predominantly considered until now, nonplanarity can be an additional parameter to modulate their properties without changing the aromatic core. Herein, we report theoretical and experimental studies on two GNR structures with "cove"-type edges, having an identical aromatic core but with alkyl side chains at different peripheral positions.

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We study the ability of porphyrin molecules to cooperate upon adsorption on the sp curved surface of carbon nanotube. We discuss the role of the phenyl substituents in the cooperativity of the functionalization reaction. Moreover, a specific spatial organization of the molecules around the nanotube is unveiled through polarization sensitive experiments.

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Understanding the surface properties of organic-inorganic lead-based perovskites is of high importance to improve the device's performance. Here, we have investigated the differences between surface and bulk optical properties of CHNHPbBr single crystals. Depth-resolved cathodoluminescence was used to probe the near-surface region on a depth of a few microns.

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Structural identification of double-walled carbon nanotubes (DWNTs) is presented through a robust procedure based on the latest generation of transmission electron microscope, making possible a statistical analysis based on numerous nano-objects. This approach reveals that inner and outer tubes of DWNTs are not randomly oriented, suggesting the existence of a mechanical coupling between the two concentric walls. With the support of atomic-scale modeling, we attribute it to the presence of incommensurate domains whose structures depend on the diameters and helicities of both tubes and where inner tubes try to achieve a local stacking orientation to reduce strain effects.

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We investigate the origin of the slow kinetics of functionalization processes in micellar environments. We show that the ionic nature of the surfactants used to solubilize small molecules and nano-objects plays a central role in the slowness of the kinetics. In order to solve this issue, we have developed an innovative method that we apply to the hybrid compound porphyrin molecule/carbon nanotube.

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Hybrid perovskite thin films have demonstrated impressive performance for solar energy conversion and optoelectronic applications. However, further progress will benefit from a better knowledge of the intrinsic photophysics of materials. Here, the temperature-dependent emission properties of CHNHPbI single crystals are investigated and compared to those of thin polycrystalline films by means of steady-state and time-resolved photoluminescence spectroscopy.

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Investigating the stability and evaluating the quality of the CH₃NH₃PbI₃ perovskite structures is quite critical both to the design and fabrication of high-performance perovskite devices and to fundamental studies of the photophysics of the excitons. In particular, it is known that, under ambient conditions, CH₃NH₃PbI₃ degrades producing some PbI₂. We show here that low temperature Photoluminescence (PL) spectroscopy is a powerful tool to detect PbI₂ traces in hybrid perovskite layers and single crystals.

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Solutions of calibrated nanographenides (negatively charged nanographenes) are obtained by dissolution of graphite nanofibre intercalation compounds (GNFICs). Deposits show homogeneous unfolded nanographene platelets of 1 to 2 layers thickness and 10 nm lateral size, evidenced by atomic force microscopy and Raman spectroscopy. Upon oxidation, nanographenide solutions exhibit strong photoluminescence.

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A great advantage of the hybrid organic-inorganic perovskites is the chemical flexibility and the possibility of a molecular engineering of each part of the material (the inorganic part and the organic part respectively) in order to improve or add some functionalities. An adequately chosen organic luminophore has been introduced inside a lead bromide type organic-inorganic perovskite, while respecting the two-dimensional perovskite structure. A substantial increase of the brilliance of the perovskite is obtained.

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We focus here our attention on a particular family of 2D-layered and 3D hybrid perovskite molecular crystals, the mixed perovskites (C6H5-C2H4-NH3)2PbZ4(1-x)Y4x and (CH3-NH3)PbZ3(1-x)Y3x, where Z and Y are halogen ions such as I, Br, and Cl. Studying experimentally the disorder-induced effects on the optical properties of the 2D mixed layered materials, we demonstrate that they can be considered as pseudobinary alloys, exactly like Ga1-xAlxAs, Cd1-xHgxTe inorganic semiconductors, or previously reported 3D mixed hybrid perovskite compounds. 2D-layered and 3D hybrid perovskites afford similar continuous optical tunability at room temperature.

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