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Register a new userPolariton response in the presence of Brownian dissipation from molecular vibrations
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We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed zero-detuning point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to prove results originating from strong coupling, such as vacuum-enhanced chemical reaction rate.
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We construct a model describing the response of a hybrid system where the electromagnetic field - in particular, surface plasmon polaritons - couples strongly with electronic excitations of atoms or molecules. Our approach is based on the input-output theory of quantum optics, and in particular it takes into account the thermal and quantum vibrations of the molecules. The latter is described within the $P(E)$ theory analogous to that used in the theory of dynamical Coulomb blockade. As a result, we are able to include the effect of the molecular Stokes shift on the strongly coupled response of the system. Our model then accounts for the asymmetric emission from upper and lower polariton modes. It also allows for an accurate description of the partial decoherence of the light emission from the strongly coupled system. Our results can be readily used to connect the response of the hybrid modes to the emission and fluorescence properties of the individual molecules, and thus are relevant in understanding any utilization of such systems, like coherent light harvesting.
Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to the bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.
Infrared nanospectroscopy based on Fourier transform infrared near-field spectroscopy (nano-FTIR) is an emerging nanoanalytical tool with large application potential for label-free mapping and identification of organic and inorganic materials with nanoscale spatial resolution. However, the detection of thin molecular layers and nanostructures on standard substrates is still challenged by weak signals. Here, we demonstrate a significant enhancement of nano-FTIR signals of a thin organic layer by exploiting polariton-resonant tip-substrate coupling and surface polariton illumination of the probing tip. When the molecular vibration matches the tip-substrate resonance, we achieve up to nearly one order of magnitude signal enhancement on a phonon-polaritonic quartz (c-SiO2) substrate, as compared to nano-FTIR spectra obtained on metal (Au) substrates, and up to two orders of magnitude when compared to the standard infrared spectroscopy substrate CaF2. Our results will be of critical importance for boosting nano-FTIR spectroscopy towards the routine detection of monolayers and single molecules.
Molecular vibrations underpin important phenomena such as spectral properties, energy transfer, and molecular bonding. However, obtaining a detailed understanding of the vibrational structure of even small molecules is computationally expensive. While several algorithms exist for efficiently solving the electronic structure problem on a quantum computer, there has been comparatively little attention devoted to solving the vibrational structure problem with quantum hardware. In this work, we discuss the use of quantum algorithms for investigating both the static and dynamic vibrational properties of molecules. We introduce a physically motivated unitary vibrational coupled cluster ansatz, which also makes our method accessible to noisy, near-term quantum hardware. We numerically test our proposals for the water and sulfur dioxide molecules.
Quantum pumping, in its different forms, is attracting attention from different fields, from fundamental quantum mechanics, to nanotechnology, to superconductivity. We investigate the crossover of quantum pumping from the adiabatic to the anti-adiabatic regime in the presence of dissipation, and find general and explicit analytical expressions for the pumped current in a minimal model describing a system with the topology of a ring forced by a periodic modulation of frequency omega. The solution allows following in a transparent way the evolution of pumped DC current from much smaller to much larger omega values than the other relevant energy scale, the energy splitting introduced by the modulation. We find and characterize a temperature-dependent optimal value of the frequency for which the pumped current is maximal.
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