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.

Thermal Decoherence of Superradiance in Lead Halide Perovskite Nanocrystal Superlattices.

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.

Opening-assisted coherent transport in the semiclassical 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 semiclassical regime (where the decoherence rate is greater than the intersite 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 Fenna-Matthews-Olson (FMO) photosynthetic complex, which may be viewed as intermediate between these paradigmatic models.

Optimal dephasing for ballistic energy transfer in disordered linear chains.

We study the interplay between dephasing, disorder, and coupling to a sink 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 last site is coupled to an external acceptor system (sink), where the excitation can be trapped with a rate Γ_{trap}. 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^{cr}, which strongly depends on the sink coupling strength Γ_{trap}. Analytic solutions are obtained for short chains.

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.

Optimal efficiency of quantum transport in a disordered trimer.

Disordered quantum networks, such as those describing light-harvesting complexes, are often characterized by the presence of peripheral ringlike structures, where the excitation is initialized, and inner structures and reaction centers (RCs), where the excitation is trapped and transferred. The peripheral rings often display distinguished coherent features: Their eigenstates can be separated, with respect to the transfer of excitation, into 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, thus 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 the initial condition an excitation on a subradiant state, rather than the more common choice of an excitation localized on a single 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 to 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.