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Ruben Esteban

Publications and source records attributed to Ruben Esteban.

At least 19 recordsLinked to original sources

Utility-scale quantum experiments using dynamic circuits to address collective dissipation in interacting qubits

Open quantum systems are central to quantum optics, condensed matter, and chemistry, yet their simulation remains challenging for both classical and near-term quantum hardware. In this work we implement and execute utility-scale quantum circuits that accurately reproduce the dissipative dynamics of interacting qubits. We consider a one-dimensional chain of many qubits weakly coupled to a common Markovian bath. The Markovian time evolution of the system is implemented through Trotterized evolution with the introduction of ancilla-assisted dissipative channels, including single-qubit and two-qubit dissipators to capture collective decay. Mid-circuit measurements, conditional gates, and hardware-aware transpilation significantly reduce circuit depth. We further implement a biased Clifford data regression (biased CDR), an error mitigation strategy that outperforms the uniform Cliffordization baseline and a variety of zero-noise extrapolation protocols. We execute large-scale quantum experiments of the dynamics of chains comprising up to 86 emitters on the IBM System Two \texttt{ibm\_basquecountry}. In order to do so, we use 129 total qubits (including ancillas), with the largest circuits contain about 8000 two-qubit gates. To validate these experiments we develop a classical Monte Carlo-Time-Evolving Block-Decimation (MC-TEBD) tensor-network method that incorporates reset operations through stochastic pure-state trajectories, obtaining very good agreement. The approach presented here opens a practical route for utility-scale quantum simulation of dissipative dynamics, enabled by dynamic circuits, targeted error mitigation, and tensor-network validation, and enables to tackle complex dynamics of systems such as quantum emitters in dissipative optical cavities.

quant-ph

Extreme Optical Field Confinement and Enhancement in a Plasmonic Picopatch within a Nanoparticle-on-Mirror Resonator

Plasmonic resonances in metallic nanogaps can confine light into nanometric regions, but reaching modes of volume $\approx 1$ nm$^3$ remains challenging. We present a detailed theoretical analysis of the optical modes of an experimentally-motivated nanoresonator configuration that contains a picopatch formed by the lifting of a few gold atoms in the gap of a Nanoparticle-on-Mirror (NPoM) structure. Classical simulations indicate that the plasmonic modes associated with the picopatch geometry can confine light to extremely small regions and are highly sensitive to the picopatch size and shape, enabling broad tunability. Furthermore, these modes can couple strongly with other nanocavity modes of the structure, as identified from a clear anti-crossing behavior of the polaritonic resonances. Remarkably, up to $\approx 2000$-fold electric field enhancement inside the picopatch and tiny effective mode volumes approaching $\approx 1$ nm$^3$ are obtained. Further, changing the morphology of the picopatch does not modify the qualitative findings, and increasing the absorption losses in the classical simulations, to mimic quantum (non-local) effects in the metal permittivity, decreases the electric field enhancement only moderately. Compared to the standard picocavities formed by single-atom protrusions, picopatches are an intriguing alternative to reach extreme optical field confinement and enhancement in plasmonic cavities.

physics.optics

Atomic-scale Stark-shift spectroscopy and microscopy of organic molecules

In conventional optical Stark-shift spectroscopy, molecules are exposed to spatially homogeneous static electric fields that shift the energies of their spectral lines. These shifts are attributed to the molecular electronic properties, such as variation of dipolar moment and polarizability of the molecule associated with photo(de)excitation. In realistic environments containing structural defects and nanoscale heterogeneities, however, molecules experience internal electric fields that vary strongly on the molecular scale, rendering the standard Stark selection rules inapplicable. Here we develop an extended theory of atomic-scale Stark shift, addressing such scenarios. Specifically, we present a detailed theoretical analysis of an experimentally relevant configuration where the atomically sharp tip of a light-assisted scanning tunneling microscope is used to controllably apply inhomogeneous electrostatic fields to representative molecular dyes spanning several molecular families. We decompose the total Stark shift into linear and quadratic contributions and show that they contain different information about the molecular properties. Concretely, spatial variations of the linear Stark shift as the tip scans across the molecule enable subnanometric mapping of the charge redistribution between ground and excited electronic states, with high sensitivity to molecular composition and chemical functionalization. The quadratic Stark contribution, in contrast, reflects changes in the conventional dipolar polarizability upon excitation. Together, these results establish nanoscale Stark-shift spectroscopy as a powerful tool for resolving excited-state charge dynamics in single molecules under realistic, strongly inhomogeneous electric fields.

physics.optics

Addressing intramolecular vibrational redistribution in a single molecule through pump and probe surface-enhanced vibrational spectroscopy

The development of accurate tools to characterize Intramolecular Vibrational Redistribution (IVR) is of major interest in chemistry. In this context, surface-enhanced vibrational spectroscopies stand up as well-established techniques to study molecular vibrational lines and populations with a sensitivity that can reach the single-molecule level. However, to date, this possibility has not been fully developed to address IVR. Here, we establish a quantum mechanical framework based on molecular optomechanics that accounts for IVR, and we adopt it to analyze strategies to optimize IVR characterization by surface-enhanced vibrational spectroscopy. In particular, we model two different pump-and-probe configurations where the vibrational pumping is provided either by infrared laser illumination or by Stokes scattering processes in surface-enhanced Raman spectroscopy (SERS). We show for the two pumping configurations the existence of clear signatures on the anti-Stokes SERS spectra of population transfer between coupled vibrational modes in a molecule. Our calculations adopt realistic molecular and SERS parameters, suggesting that these signatures of IVR could be accessible at the single-molecule level within realistic experimental platforms.

physics.optics

Generation of polarization-entangled photon pairs from two interacting quantum emitters

Entangled photon pairs are key elements in quantum communication and quantum cryptography. State-of-the-art sources of entangled photons are mainly based on parametric down-conversion from nonlinear crystals, which is probabilistic in nature, and on cascade emission from biexciton quantum dots, which finds difficulties in generating entangled photons in the visible regime. Here, we use the Wigner-Weisskopf theory to provide a demonstration that polarization-entangled photon pairs can be emitted from two interacting quantum emitters with two-level-system behavior and perpendicular transition dipole moments. These emitters can represent a large variety of systems (e.g., organic molecules, quantum dots, and diamond color centers) offering a large technological versatility, for example, in the spectral regime of the emission. We show that a highly entangled photon pair can be postselected from this system by including optical filters. Additionally, we verify that the photon entanglement is not significantly affected by small changes in the detection directions and in the orientation between the dipole moments.

quant-ph

Addressing the correlation of Stokes-shifted photons emitted from two quantum emitters

In resonance fluorescence excitation experiments, light emitted from solid-state quantum emitters is typically filtered to eliminate the laser photons, ensuring that only red-shifted Stokes photons are detected. However, theoretical analyses of the fluorescence intensity correlation often model emitters as two-level systems, focusing on light emitted exclusively from the purely electronic transition (the zero-phonon line), or they rely on statistical approaches based on conditional probabilities that neglect the quantum coherence between the emitters and the coherence between the electric fields they generate. Here, we propose a model to characterize the correlation of either zero-phonon line photons or Stokes-shifted photons. This model successfully reproduces the experimental correlation of Stokes-shifted photons emitted from two interacting molecules and predicts that this correlation is affected by quantum coherence. Besides, we analyze the role of quantum coherence in the Stokes-shifted emission from two distant emitters, showing a sharp peak at zero time delay due to the Hanbury Brown--Twiss effect.

quant-ph

Giant Purcell broadening and Lamb shift for DNA-assembled near-infrared quantum emitters

Controlling the light emitted by individual molecules is instrumental to a number of novel nanotechnologies ranging from super-resolution bio-imaging and molecular sensing to quantum nanophotonics. Molecular emission can be tailored by modifying the local photonic environment, for example by precisely placing a single molecule inside a plasmonic nanocavity with the help of DNA origami. Here, using this scalable approach, we show that commercial fluorophores experience giant Purcell factors and Lamb shifts, reaching values on par with those recently reported in scanning tip experiments. Engineering of plasmonic modes enables cavity-mediated fluorescence far detuned from the zero-phonon-line (ZPL) - at detunings that are up to two orders of magnitude larger than the fluorescence linewidth of the bare emitter and reach into the near-infrared. Our results evidence a regime where the emission linewidth is dominated by the excited state lifetime, as required for indistinguishable photon emission, baring relevance to the development of nanoscale, ultrafast quantum light sources and to the quest toward single-molecule cavity-QED. In the future, this approach may also allow to design efficient quantum emitters at infrared wavelengths, where standard organic sources have a reduced performance.

physics.optics

Uncovering low-frequency vibrations in surface-enhanced Raman of organic molecules

Accessing the terahertz (THz) spectral domain through surface-enhanced Raman spectroscopy (SERS) is challenging and opens up the study of low-frequency molecular and electronic excitations. Compared to direct THz probing of heterogenous ensembles, the extreme plasmonic confinement of visible light to deep sub-wavelength scales allows the study of hundreds or even single molecules. We show that self-assembled molecular monolayers of a set of simple aromatic thiols confined inside single-particle plasmonic nanocavities can be distinguished by their low-wavenumber spectral peaks below 200 cm-1, after removal of a bosonic inelastic contribution and an exponential background from the spectrum Developing environment-dependent density-functional-theory simulations of the metal-molecule configuration enables the assignment and classification of their THz vibrations as well as the identification of intermolecular coupling effects and of the influence of the gold surface configuration Furthermore, we show dramatically narrower THz SERS spectra from individual molecules at picocavities, which indicates the possibility to study intrinsic vibrational properties beyond inhomogeneous broadening further supporting the key role of local environment.

physics.optics

Description of ultrastrong light-matter interaction through coupled harmonic oscillator models and their connection with cavity-QED Hamiltonians

Classical coupled harmonic oscillator models are capable of describing the optical and infrared response of nanophotonic systems where a cavity photon couples to dipolar matter excitations. The distinct forms of coupling adopted in these classical models leads to different results in the ultrastrong coupling regime. To clarify the specific classical model required to address particular configurations, we establish a connection between each oscillator model and the equivalent cavity Quantum Electrodynamics description. We show that the proper choice of coupled harmonic oscillator model depends on the presence or absence of the diamagnetic term in the quantum models, linked to whether transverse or longitudinal electromagnetic fields mediate the coupling. This analysis also shows how to exploit the classical oscillator models to extract measurable information of the optical response, as demonstrated in three canonical photonic systems, and to describe the opening of the Reststrahlen band in the bulk dispersion of phononic materials

quant-ph

Influence of direct dipole-dipole interactions on the optical response of 2D materials in strongly inhomogeneous infrared cavity fields

A two-dimensional (2D) material, formed for example by a self-assembled molecular monolayer or by a single layer of a van der Walls material, can couple efficiently with photonic nanocavities, potentially reaching the strong coupling regime. The coupling can be modelled using classical harmonic oscillator models or cavity quantum electrodynamics Hamiltonians that often neglect the direct dipole-dipole interactions within the monolayer. Here, we diagonalize the full Hamiltonian of the system, including these direct dipole-dipole interactions. The main effect on the optical properties of a typical 2D system is simply to renormalize the effective energy of the bright collective excitation of the monolayer that couples with the nanophotonic mode. On the other hand, we show that for situations of extreme field confinement, large transition dipole moments and low losses, fully including the direct dipole-dipole interactions is critical to correctly capture the optical response, with many collective states participating in it. To quantify this result, we propose a simple equation that indicates the condition for which the direct interactions strongly modify the optical response.

quant-ph

Preservation and destruction of the purity of two-photon states in the interaction with a nanoscatterer

The optical resonances supported by nanostructures offer the possibility to enhance the interaction between matter and the quantum states of light. In this work, we provide a framework to study the scattering of quantum states of light with information encoded in their helicity by a nanostructure. We analyze the purity of the scattered output quantum state, and we find that the purity of the incident state can be lost, when it interacts with the optical resonances of the nanostructure. To explain the loss of quantum purity, we develop a physical picture based on time delays and frequency shifts between the output two-photon modes. The framework and analysis proposed in this work establishes a tool to address the interaction between quantum light and nanoenvironments.

quant-ph

Identifying unbound strong bunching and the breakdown of the Rotating Wave Approximation in the quantum Rabi model

We use a recently derived gauge-invariant formulation of the problem of a two-level system coupled to an optical cavity, to explore the transition between the weak, and the ultra-strong coupling regimes of light-matter interaction. We explore this transition using the intensity correlations $g^{(2)}(\tau)$ of the emitted light, and find strong, unbounded bunching of the emission from systems governed by the Rabi Hamiltonian. Surprisingly, this effect is observed not only in the ultra-strong coupling regime, but also for weakly coupled systems, where the Jaynes-Cummings Hamiltonian would predict the opposite, antibunched emission. This suggests that the higher-order correlations are a particularly sensitive probe of the divergence between the Jaynes-Cummings and Rabi Hamiltonians, and can serve as an indicator of the breakdown of the rotating wave approximation. Our findings indicate also that the boundary between the weakly, strongly, and ultra-strongly coupled dynamics, is much richer than currently accepted.

quant-ph

Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering

Molecular vibrations couple to visible light only weakly, have small mutual interactions, and hence are often ignored for non-linear optics. Here we show the extreme confinement provided by plasmonic nano- and pico-cavities can sufficiently enhance optomechanical coupling so that intense laser illumination drastically softens the molecular bonds. This optomechanical pumping regime produces strong distortions of the Raman vibrational spectrum related to giant vibrational frequency shifts from an optical spring effect which is hundred-fold larger than in traditional cavities. The theoretical simulations accounting for the multimodal nanocavity response and near-field-induced collective phonon interactions are consistent with the experimentally-observed non-linear behavior exhibited in the Raman spectra of nanoparticle-on-mirror constructs illuminated by ultrafast laser pulses. Further, we show indications that plasmonic picocavities allow us to access the optical spring effect in single molecules with continuous illumination. Driving the collective phonon in the nanocavity paves the way to control reversible bond softening, as well as irreversible chemistry.

physics.optics

Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity

Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features in photoluminescence spectra point to the contribution of multiple excited states. Using model simulations based on an extended Jaynes Cummings Hamiltonian, we find that the involvement of a dark state of the quantum dots explains the experimental findings. The coupling of quantum emitters to plasmonic cavities thus exposes complex relaxation pathways and emerges as an unconventional means to control dynamics of quantum states.

cond-mat.mes-hall

Microcavity phonon polaritons from weak to ultrastrong phonon-photon coupling

Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the much less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ultrastrong coupling in fully filled cavities yields a cavity polariton dispersion matching that of phonon polaritons in bulk hBN, highlighting that the maximum light-matter coupling in microcavities is limited to the coupling strength between photons and the bulk material. The tunable cavity phonon polaritons could become a versatile platform for studying how the coupling strength between photons and phonons may modify the properties of polar crystals.

physics.optics

Frequency-resolved photon correlations in cavity optomechanics

Frequency-resolved photon correlations have proven to be a useful resource to unveil nonlinearities hidden in standard observables such as the spectrum or the standard (color-blind) photon correlations. In this manuscript, we analyze the frequency-resolved correlations of the photons being emitted from an optomechanical system where light is nonlinearly coupled to the quantized motion of a mechanical mode of a resonator, but where the quantum nonlinear response is typically hard to evidence. We present and unravel a rich landscape of frequency-resolved correlations, and discuss how the time-delayed correlations can reveal information about the dynamics of the system. We also study the dependence of correlations on relevant parameters such as the single-photon coupling strength, the filtering linewidth, or the thermal noise in the environment. This enriched understanding of the system can trigger new experiments to probe nonlinear phenomena in optomechanics, and provide insights into dynamics of generic nonlinear systems.

quant-ph

Optomechanical Collective Effects in Surface-Enhanced Raman Scattering from Many Molecules

The interaction between molecules is commonly ignored in surface-enhanced Raman scattering (SERS). Under this assumption, the total SERS signal is described as the sum of the individual contributions of each molecule treated independently. We adopt here an optomechanical description of SERS within a cavity quantum electrodynamics framework to study how collective effects emerge from the quantum correlations of distinct molecules. We derive analytical expressions for identical molecules and implement numerical simulations to analyze two types of collective phenomena: (i) a decrease of the laser intensity threshold to observe strong non-linearities as the number of molecules increases, within intense illumination, and (ii) identification of superradiance in the SERS signal, namely a quadratic scaling with the number of molecules. The laser intensity required to observe the latter in the anti-Stokes scattering is relatively moderate, which makes it particularly accessible to experiments. Our results also show that collective phenomena can survive in the presence of moderate homogeneous and inhomogeneous broadening.

physics.optics

Quantum description of surface-enhanced resonant Raman scattering within a hybrid-optomechanical model

Surface-Enhanced Raman Scattering (SERS) allows for detection and identification of molecular vibrational fingerprints in minute sample quantities. The SERS process can be also exploited for optical manipulation of molecular vibrations. We present a quantum description of Surface-Enhanced Resonant Raman scattering (SERRS), in analogy to hybrid cavity optomechanics, and compare the resonant situation with the off-resonant SERS. Our model predicts the existence of a regime of coherent interaction between electronic and vibrational degrees of freedom of a molecule, mediated by a plasmonic nanocavity. This coherent mechanism can be achieved by parametrically tuning the frequency and intensity of the incident pumping laser and is related to the optomechanical pumping of molecular vibrations. We find that vibrational pumping is able to selectively activate a particular vibrational mode, thus providing a mechanism to control its population and drive plasmon-assisted chemistry.

physics.optics