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1.
J Am Chem Soc ; 146(28): 18999-19008, 2024 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-38736166

RESUMEN

Enhancing the electrical conductance through amorphous nondoped polymers is challenging. Here, we show that vibrational strong coupling (VSC) of intrinsically nonconducting and amorphous polymers such as polystyrene, deuterated polystyrene, and poly(benzyl methacrylate) to the vacuum electromagnetic field of the cavity enhances the electrical conductivity by at least 6 orders of magnitude compared to the uncoupled polymers. Remarkably, the observed extraordinary conductance is vibrational mode selective and occurs only under the VSC of the aromatic C-H(D) out-of-plane bending modes of the polymers. The conductance is thermally activated at the onset of strong coupling and becomes temperature-independent as the collective strong coupling strength increases. The electrical characterizations are performed without external light excitation, demonstrating the role of vacuum electromagnetic field-matter strong coupling in enhancing long-range transport even in amorphous nonconducting polymers.

2.
Phys Rev Lett ; 126(15): 153201, 2021 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-33929231

RESUMEN

Overcoming the detrimental effect of disorder at the nanoscale is very hard since disorder induces localization and an exponential suppression of transport efficiency. Here we unveil novel and robust quantum transport regimes achievable in nanosystems by exploiting long-range hopping. We demonstrate that in a 1D disordered nanostructure in the presence of long-range hopping, transport efficiency, after decreasing exponentially with disorder at first, is then enhanced by disorder [disorder-enhanced transport (DET) regime] until, counterintuitively, it reaches a disorder-independent transport (DIT) regime, persisting over several orders of disorder magnitude in realistic systems. To enlighten the relevance of our results, we demonstrate that an ensemble of emitters in a cavity can be described by an effective long-range Hamiltonian. The specific case of a disordered molecular wire placed in an optical cavity is discussed, showing that the DIT and DET regimes can be reached with state-of-the-art experimental setups.

3.
Nano Lett ; 20(10): 7382-7388, 2020 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-32969667

RESUMEN

Recent experiments by Rainò et al. ( Nature 2018, 563, 671-675) have documented cooperative emission from CsPbBr3 nanocrystal superlattices, exhibiting the hallmarks of low-temperature superradiance. In particular, the optical response is coherent and the radiative decay rate is increased by a factor of 3, relative to that of individual nanocrystals. However, the increase is 6 orders of magnitude smaller than what is theoretically expected from the superradiance of large assemblies, consisting of 106-108 interacting nanocrystals. Here, we develop a theoretical model of superradiance for such systems and show that thermal decoherence is largely responsible for the drastic reduction of the radiative decay rate in nanocrystal superlattices. Our theoretical approach explains the experimental results ( Nature 2018, 563, 671-675), provides insight into the design of small nanocrystal superlattices, and shows a 4 orders of magnitude enhancement in superradiant response. These quantitative predictions pave the path toward observing superradiance at higher temperatures.

4.
J Phys Chem B ; 128(40): 9643-9655, 2024 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-39351757

RESUMEN

Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes containing more than one hundred thousands of chlorophyll molecules, comparable with natural size, have been performed. Photosynthetic antenna complexes present in Green sulfur bacteria and Purple bacteria have been analyzed using a radiative non-Hermitian Hamiltonian, well-known in the field of quantum optics, instead of the widely used dipole-dipole Frenkel Hamiltonian. This approach allows us to study ensembles of emitters beyond the small volume limit (system size much smaller than the absorbed wavelength), where the Frenkel Hamiltonian fails. When analyzed on a large scale, such structures display superradiant states much brighter than their single components. An analysis of the robustness to static disorder and dynamical (thermal) noise shows that exciton coherence in the whole photosynthetic complex is larger than the coherence found in its parts. This provides evidence that the photosynthetic complex as a whole plays a predominant role in sustaining coherences in the system even at room temperature. Our results allow a better understanding of natural photosynthetic antennae and could drive experiments to verify how the response to electromagnetic radiation depends on the size of the photosynthetic antenna.

5.
Nat Phys ; 19(8): 1128-1134, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37575364

RESUMEN

All-to-all interacting, disordered quantum many-body models have a wide range of applications across disciplines, from spin glasses in condensed-matter physics over holographic duality in high-energy physics to annealing algorithms in quantum computing. Typically, these models are abstractions that do not find unambiguous physical realizations in nature. Here we realize an all-to-all interacting, disordered spin system by subjecting an atomic cloud in a cavity to a controllable light shift. Adjusting the detuning between atom resonance and cavity mode, we can tune between disordered versions of a central-mode model and a Lipkin-Meshkov-Glick model. By spectroscopically probing the low-energy excitations of the system, we explore the competition of interactions with disorder across a broad parameter range. We show how disorder in the central-mode model breaks the strong collective coupling, making the dark-state manifold cross over to a random distribution of weakly mixed light-matter, 'grey', states. In the Lipkin-Meshkov-Glick model, the ferromagnetic finite-sized ground state evolves towards a paramagnet as disorder is increased. In that regime, semi-localized eigenstates emerge, as we observe by extracting bounds on the participation ratio. These results present substantial steps towards freely programmable cavity-mediated interactions for the design of arbitrary spin Hamiltonians.

6.
Phys Rev E ; 95(4-1): 042135, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-28505710

RESUMEN

The onset of thermalization in a closed system of randomly interacting bosons at the level of a single eigenstate is discussed. We focus on the emergence of Bose-Einstein distribution of single-particle occupation numbers, and we give a local criterion for thermalization dependent on the eigenstate energy. We show how to define the temperature of an eigenstate, provided that it has a chaotic structure in the basis defined by the single-particle states. The analytical expression for the eigenstate temperature as a function of both interparticle interaction and energy is complemented by numerical data.

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