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1.
Phys Rev Lett ; 132(4): 043805, 2024 Jan 26.
Article in English | MEDLINE | ID: mdl-38335338

ABSTRACT

Ring quantum cascade lasers have recently gained considerable attention, showing ultrastable frequency comb and soliton operation, thus opening a way to integrated spectrometers in the midinfrared and terahertz fingerprint regions. Thanks to a self-consistent Maxwell-Bloch model, we demonstrate, in excellent agreement with the experimental data, that a small but finite coupling between the counterpropagating waves arising from distributed backscattering is essential to stabilize the soliton solution.

2.
Science ; 382(6669): 434-438, 2023 Oct 27.
Article in English | MEDLINE | ID: mdl-37883562

ABSTRACT

Synthetic lattices in photonics enable the exploration of light states in new dimensions, transcending phenomena common only to physical space. We propose and demonstrate a quantum walk comb in synthetic frequency space formed by externally modulating a ring-shaped semiconductor laser with ultrafast recovery times. The initially ballistic quantum walk does not dissipate into low supermode states of the synthetic lattice; instead, the state stabilizes in a broad frequency comb, unlocking the full potential of the synthetic frequency lattice. Our device produces a low-noise, nearly flat broadband comb (reaching 100 per centimeter bandwidth) and offers a promising platform to generate broadband, tunable, and stable frequency combs.

3.
Angew Chem Int Ed Engl ; 62(12): e202216729, 2023 Mar 13.
Article in English | MEDLINE | ID: mdl-36652344

ABSTRACT

Organic semiconductors are promising for efficient, printable optoelectronics. However, strong excited-state quenching due to uncontrolled aggregation limits their use in devices. We report on the self-assembly of a supramolecular pseudo-cube formed from six perylene diimides (PDIs). The rigid, shape-persistent cage sets the distance and orientation of the PDIs and suppresses intramolecular rotations and vibrations, leading to non-aggregated, monomer-like properties in solution and the solid state, in contrast to the fast fluorescence quenching in the free ligand. The stabilized excited state and electronic purity in the cage enables the observation of delayed fluorescence due to a bright excited multimer, acting as excited-state reservoir in a rare case of benign inter-chromophore interactions in the cage. We show that self-assembly provides a powerful tool for retaining and controlling the electronic properties of chromophores, and to bring molecular electronics devices within reach.

4.
J Am Chem Soc ; 144(34): 15862-15870, 2022 Aug 31.
Article in English | MEDLINE | ID: mdl-35977424

ABSTRACT

Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M2+) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understanding of the universal working mechanism for such doping is still missing. Here, we directly compare the optical properties of nanocrystals containing the most commonly employed dopants, fabricated under identical synthesis conditions. We show for the first time unambiguously, and supported by first-principles calculations and molecular orbital theory, that element-unspecific symmetry-breaking rather than element-specific electronic effects dominate these properties under device-relevant conditions. The impact of most dopants on the perovskite electronic structure is predominantly based on local lattice periodicity breaking and resulting charge carrier localization, leading to enhanced radiative recombination, while dopant-specific hybridization effects play a secondary role. Our results suggest specific guidelines for selecting a dopant to maximize the performance of perovskite emitters in the desired optoelectronic devices.

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