arXiv subjects

G. Luca Celardo

Publications and source records attributed to G. Luca Celardo.

13 recordsLinked to original sources

arXiv2026

Relation between structure and functionality in photosynthetic antenna complex of green sulfur bacteria: efficiency under natural sunlight pumping

Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes of the Chlorobium Tepidum green sulfur bacteria (GSB) containing more than one hundred thousand chlorophyll molecules, comparable with natural size, have been performed. Here we have modeled the entire process of the exciton energy transfer, from sunlight absorption to exciton trapping in the reaction centers (RCs) in presence of a thermal bath. The energy transfer has been analyzed using the radiative non-Hermitian Hamiltonian and solving the rate equations for the populations. Sunlight pumping has been modeled as black-body radiation with an attenuation factor that takes the Sun-Earth distance into account. Cylindrical structures typical of GSB antenna complexes, and the dimeric baseplate comparable to natural size have been considered. Our analysis shows that under natural sunlight, in photosynthetic antennae of GSB the number of excitations reaching the RC per unit time matches the RC closure rate and the internal efficiency shows values close to 80%. We also considered cylindrical structures where the orientation of the dipoles does not reflect the natural one. Specifically, we vary continuously the angle of the transition dipole with respect to the cylinder main axis, focusing on the case where all dipoles are parallel to the cylinder axis. We also consider the important case where the dipoles are randomly oriented. In all cases the light-harvesting efficiency is lower than in the natural structure, showing the high sensitivity of light harvesting to the specific orientation of the dipole moments. Our results allow for a better understanding of the relationship between structure and functionality in photosynthetic antennae of GSB and could drive the design of efficient light-harvesting devices.

cond-mat.mes-hall↗

arXiv2023

Enhanced robustness and dimensional crossover of superradiance in cuboidal nanocrystal superlattices

Cooperative emission of coherent radiation from multiple emitters (known as superradiance) has been predicted and observed in various physical systems, most recently in CsPbBr$_3$ nanocrystal superlattices. Superradiant emission is coherent and occurs on timescales faster than the emission from isolated nanocrystals. Theory predicts cooperative emission being faster by a factor of up to the number of nanocrystals ($N$). However, superradiance is strongly suppressed due to the presence of energetic disorder, stemming from nanocrystal size variations and thermal decoherence. Here, we analyze superradiance from superlattices of different dimensionalities (one-, two- and three-dimensional) with variable nanocrystal aspect ratios. We predict as much as a 15-fold enhancement in robustness against realistic values of energetic disorder in three-dimensional (3D) superlattices composed of cuboid-shaped, as opposed to cube-shaped, nanocrystals. Superradiance from small $(N\lesssim 10^3)$ two-dimensional (2D) superlattices is up to ten times more robust to static disorder and up to twice as robust to thermal decoherence than 3D superlattices with the same $N$. As the number of $N$ increases, a crossover in the robustness of superradiance occurs from 2D to 3D superlattices. For large $N\ (> 10^3)$, the robustness in 3D superlattices increases with $N$, showing cooperative robustness to disorder. This opens the possibility of observing superradiance even at room temperature in large 3D superlattices, if nanocrystal size fluctuations can be kept small.

cond-mat.mes-hall↗

arXiv2022

Efficient light harvesting and photon sensing via engineered cooperative effects

Efficient devices for light harvesting and photon sensing are fundamental building blocks of basic energy science and many essential technologies. Recent efforts have turned to biomimicry to design the next generation of light-capturing devices, partially fueled by an appreciation of the fantastic efficiency of the initial stages of natural photosynthetic systems at capturing photons. In such systems extended excitonic states are thought to play a fundamental functional role, inducing cooperative coherent effects, such as superabsorption of light and supertransfer of photoexcitations. Inspired by this observation, we design an artificial light-harvesting and photodetection device that maximally harnesses cooperative effects to enhance efficiency. The design relies on separating absorption and transfer processes (energetically and spatially) in order to overcome the fundamental obstacle to exploiting cooperative effects to enhance light capture: the enhanced emission processes that accompany superabsorption. This engineered separation of processes greatly improves the efficiency and the scalability of the system.

physics.optics↗

arXiv2021

Bio-inspired natural sunlight-pumped lasers

Even though sunlight is by far the most abundant renewable energy source available to humanity, its dilute and variable nature has kept efficient ways to collect, store, and distribute this energy tantalisingly out of reach. Turning the incoherent energy supply provided by the Sun into a coherent laser beam would overcome several of the practical limitations inherent in using sunlight as a source of clean energy: laser beams travel nearly losslessly over large distances, and they are effective at driving chemical reactions which convert sunlight into chemical energy. Here we propose a bio-inspired blueprint for a novel type of laser with the aim of upgrading unconcentrated natural sunlight into a coherent laser beam. Our proposed design constitutes a novel and different path towards sunlight-pumped lasers. In order to achieve lasing with the extremely dilute power provided by natural sunlight, we here propose a laser medium comprised of molecular aggregates inspired by the architecture of natural photosynthetic complexes. Such complexes exhibit a very large internal efficiency in harvesting photons from a power source as dilute as natural sunlight. Specifically, we consider a hybrid structure, where photosynthetic complexes in purple bacteria (Rhodobacter sphaeroides) surround a suitably engineered molecular dimer composed of two strongly coupled chromophores. We show that if pumped by the surrounding photosynthetic complex, which efficiently collects and concentrates solar energy, the core dimer structure can reach population inversion, and reach the lasing threshold under natural sunlight. The design principles proposed here will also pave the way for developing other bio-inspired quantum devices.

quant-ph↗

arXiv2021

Disorder-Enhanced and Disorder-Independent Transport with Long-Range Hopping: Application to Molecular Chains in Optical Cavities

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.

quant-ph↗

arXiv2019

Electric-field assisted optimal quantum transport of photo-excitations in polar heterostructures

Transition-metal-oxide (TMO) heterostructures are promising candidates for building photon-harvesting devices which can exploit optimal quantum transport of charge excitations generated by light absorption. Here we address the explicit role of an electric field on the quantum transport properties of photo-excitations subject to dephasing in one-dimensional chains coupled to a continuum of states acting as a sink. We show that the average transfer time to the sink is optimized for suitable values of both the coupling strength to the sink and the electric field, thus fully exploiting the coherence-enhanced efficiency in the quantum transport regime achievable in few monolayers TMO heterostructures. The optimal coupling to the continuum remains approximately the same as that in absence of electric field and is characterizing the Superradiant Transition. On the other hand, the optimal electric field for which we provide estimates using an analytical expression is dependent on the initial state.

quant-ph↗

arXiv2019

Real and imaginary energy gaps: a comparison between single excitation Superradiance and Superconductivity and robustness to disorder

A comparison between the single particle spectrum of the discrete Bardeen-Cooper-Schrieffer (BCS) model, used for small superconducting grains, and the spectrum of a paradigmatic model of Single Excitation Superradiance (SES) is presented. They are both characterized by an equally spaced energy spectrum (Picket Fence) where all the levels are coupled between each other by a constant coupling which is real for the BCS model and purely imaginary for the SES model. While the former corresponds to the discrete BCS-model describing the coupling of Cooper pairs in momentum space and it induces a Superconductive regime, the latter describes the coupling of single particle energy levels to a common decay channel and it induces a Superradiant transition. We show that the transition to a Superradiant regime can be connected to the emergence of an imaginary energy gap, similarly to the transition to a Superconductive regime where a real energy gap emerges. Despite their different physical origin, it is possible to show that both the Superradiant and the Superconducting gaps have the same magnitude in the large gap limit. Nevertheless, some differences appear: while the critical coupling at which the Superradiant gap appears is independent of the system size $N$, for the Superconductivity gap it scales as $(\ln N)^{-1}$. The presence of a gap in the imaginary energy axis between the Superradiant and the Subradiant states shares many similarities with the "standard" gap on the real energy axis: the superradiant state is protected against disorder from the imaginary gap as well as the superconducting ground state is protected by the real energy gap. Moreover we connect the origin of the gapped phase to the long-range nature of the coupling between the energy levels.

cond-mat.supr-con↗

arXiv2017

Optimal Dephasing for Ballistic Energy Transfer in Disordered Linear Chains

We study the interplay between dephasing, disorder, and openness on transport efficiency in a one-dimensional chain of finite length $N$, and in particular the beneficial or detrimental effect of dephasing on transport. The excitation moves along the chain by coherent nearest-neighbor hopping $Ω$, under the action of static disorder $W$ and dephasing $γ$. The system is open due to the coupling of the last site with an external acceptor system (sink), where the excitation can be trapped with a rate $Γ_{\rm trap}$, which determines the opening strength. While it is known that dephasing can help transport in the localized regime, here we show that dephasing can enhance energy transfer even in the ballistic regime. Specifically, in the localized regime we recover previous results, where the optimal dephasing is independent of the chain length and proportional to $W$ or $W^2/Ω$. In the ballistic regime, the optimal dephasing decreases as $1/N$ or $1/\sqrt{N}$ respectively for weak and moderate static disorder. When focusing on the excitation starting at the beginning of the chain, dephasing can help excitation transfer only above a critical value of disorder $W^{\rm cr}$, which strongly depends on the opening strength $Γ_{\rm trap}$. Analytic solutions are obtained for short chains.

cond-mat.mes-hall↗

arXiv2017

Interplay of different environments in open quantum systems: Breakdown of the additive approximation

We analyze an open quantum system under the influence of more than one environment: a dephasing bath and a probability-absorbing bath that represents a decay channel, as encountered in many models of quantum networks. In our case, dephasing is modeled by random fluctuations of the site energies, while the absorbing bath is modeled with an external lead attached to the system. We analyze under which conditions the effects of the two baths can enter additively the quantum master equation. When such additivity is legitimate, the reduced master equation corresponds to the evolution generated by an effective non-Hermitian Hamiltonian and a Haken-Strobl dephasing super-operator. We find that the additive decomposition is a good approximation when the strength of dephasing is small compared to the bandwidth of the probability-absorbing bath.

cond-mat.mes-hall↗

arXiv2016

Opening-Assisted Coherent Transport in the Deep Classical Regime

We study quantum enhancement of transport in open systems in the presence of disorder and dephasing. Quantum coherence effects may significantly enhance transport in open systems even in the deep classical regime (where the decoherence rate is greater than the inter-site hopping amplitude), as long as the disorder is sufficiently strong. When the strengths of disorder and dephasing are fixed, there is an optimal opening strength at which the coherent transport enhancement is optimized. Analytic results are obtained in two simple paradigmatic tight-binding models of large systems: the linear chain and the fully connected network. The physical behavior is also reflected in the FMO photosynthetic complex, which may be viewed as intermediate between these paradigmatic models.

cond-mat.mes-hall↗

arXiv2016

Optimal efficiency of quantum transport in a disordered trimer

Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of peripheral ring-like structures, where the excitation is initialized, and inner reaction centers (RC), where the excitation is trapped. The peripheral rings display coherent features: their eigenstates can be separated in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In the absence of disorder, superradiant states have an enhanced coupling strength to the RC, while the subradiant ones are basically decoupled from it. Static on-site disorder induces a coupling between subradiant and superradiant states, creating an indirect coupling to the RC. The problem of finding the optimal transfer conditions, as a function of both the RC energy and the disorder strength, is very complex even in the simplest network, namely a three-level system. In this paper we analyze such trimeric structure choosing as initial condition a subradiant state, rather than the more common choice of an excitation localized on a site. We show that, while the optimal disorder is of the order of the superradiant coupling, the optimal detuning between the initial state and the RC energy strongly depends on system parameters: when the superradiant coupling is much larger than the energy gap between the superradiant and the subradiant levels, optimal transfer occurs if the RC energy is at resonance with the subradiant initial state, whereas we find an optimal RC energy at resonance with a virtual dressed state when the superradiant coupling is smaller than or comparable with the gap. The presence of dynamical noise, which induces dephasing and decoherence, affects the resonance structure of energy transfer producing an additional 'incoherent' resonance peak, which corresponds to the RC energy being equal to the energy of the superradiant state.

cond-mat.mes-hall↗

arXiv2015

Optimal efficiency of quantum transport in structured disordered systems with applications to light-harvesting complexes

Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of antenna structures where the light is captured and inner structures (reaction centers) where the excitation is transferred. Antennae often display distinguished coherent features: their eigenstates can be separated, with respect to the transfer of excitation, in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In absence of disorder superradiant states have an enhanced coupling strength to the RC, while subradiant ones are basically decoupled from it. Disorder induces a coupling between subradiant and superradiant states, thus creating an indirect coupling to the RC. We consider the problem of finding the maximal excitation transfer efficiency as a function of the RC energy and the disorder strength, first in a paradigmatic three-level system and then in a realistic model for the light-harvesting complex of purple bacteria. Specifically, we focus on the case in which the excitation is initially on a subradiant state, showing that the optimal disorder is of the order of the superradiant coupling. We also determine the optimal detuning between the initial state and the RC energy. We show that the efficiency remains high around the optimal detuning in a large energy window, proportional to the superradiant coupling. This allows for the simultaneous optimization of excitation transfer from several initial states with different optimal detuning.

cond-mat.mes-hall↗

arXiv2015

Non-Hermitian Hamiltonian approach to quantum transport in disordered networks with sinks: validity and effectiveness

We investigate the validity of the non-Hermitian Hamiltonian approach in describing quantum transport in disordered tight-binding networks connected to external environments, acting as sinks. Usually, non-Hermitian terms are added, on a phenomenological basis, to such networks to summarize the effects of the coupling to the sinks. Here we consider a paradigmatic model of open quantum network for which we derive a non-Hermitian effective model, discussing its limit of validity by a comparison with the analysis of the full Hermitian model. Specifically, we consider a ring of sites connected to a central one-dimensional lead. The lead acts as a sink which absorbs the excitation initially present in the ring. The coupling strength to the lead controls the opening of the ring system. This model has been widely discussed in literature in the context of light-harvesting systems. We analyze the effectiveness of the non-Hermitian description both in absence and in presence of static disorder on the ring. In both cases, the non-Hermitian model is valid when the energy range determined by the eigenvalues of the ring Hamiltonian is smaller than the energy band in the lead. Under such condition, we show that results about the interplay of opening and disorder, previously obtained within the non-Hermitian Hamiltonian approach, remain valid when the full Hermitian model in presence of disorder is considered. The results of our analysis can be extended to generic networks with sinks, leading to the conclusion that the non-Hermitian approach is valid when the energy dependence of the coupling to the external environments is sufficiently smooth in the energy range spanned by the eigenstates of the network.

cond-mat.mes-hall↗