Photon correlation spectroscopy as a witness for quantum coherence

The development of spectroscopic techniques able to detect and verify quantum coherence is a goal of increasing importance given the rapid progress of new quantum technologies, the advances in the field of quantum thermodynamics, and the emergence of new questions in chemistry and biology regarding the possible relevance of quantum coherence in biochemical processes. Ideally, these tools should be able to detect and verify the presence of quantum coherence in both the transient dynamics and the steady state of driven-dissipative systems, such as light-harvesting complexes driven by thermal photons in natural conditions. This requirement poses a challenge for standard laser spectroscopy methods. Here, we propose photon correlation measurements as a new tool to analyse quantum dynamics in molecular aggregates in driven-dissipative situations. We show that the photon correlation statistics on the light emitted by a molecular dimer model can signal the presence of coherent dynamics. Deviations from the counting statistics of independent emitters constitute a direct fingerprint of quantum coherence in the steady state. Furthermore, the analysis of frequency resolved photon correlations can signal the presence of coherent dynamics even in the absence of steady state coherence, providing direct spectroscopic access to the much sought-after site energies in molecular aggregates

Two-photon absorption cross sections of pulsed entangled beams

Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a 'classical' quadratic scaling which dominates the signal at large photon fluxes and thus recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even to very large photon numbers. To this end, we use a minimal model for quantum light, which can interpolate continuously between the entangled pair and a high-photon-flux limit, to derive analytically ETPA cross sections and the intensity crossover regime. We investigate the interplay between spectral and spatial degrees of freedom, how linewidth broadening of the sample impacts the experimentally achievable enhancement.Comment: 18 pages, 7 figure

Bunching and anti-bunching of localised particles in disordered media

We consider pairs of non-interacting quantum particles transmitted through a disordered medium, with emphasis on the role of their quantum statistics. It is shown that particle-number correlations measured in transmission are strikingly sensitive to the quantum nature of the particles when they undergo Anderson localisation, due to bosonic bunching and fermionic anti-bunching in the scattering channels of the medium. The case of distinguishable particles is also discussed.Comment: 5 pages, 3 figure

Cavity-mediated electron-photon superconductivity

We investigate electron paring in a two-dimensional electron system mediated by vacuum fluctuations inside a nanoplasmonic terahertz cavity. We show that the structured cavity vacuum can induce long-range attractive interactions between current fluctuations which lead to pairing in generic materials with critical temperatures in the low-Kelvin regime for realistic parameters. The induced state is a pair density wave superconductor which can show a transition from a fully gapped to a partially gapped phase - akin to the pseudogap phase in high-$T_c$ superconductors. Our findings provide a promising tool for engineering intrinsic electron interactions in two-dimensional materials.Comment: 11 page

Nonlinear optical signals and spectroscopy with quantum light

Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties - known as "time-energy entanglement". Nonlinear optical signals induced by quantized light fields are expressed using time ordered multipoint correlation functions of superoperators. These are different from Glauber's g- functions for photon counting which use normally ordered products of ordinary operators. Entangled photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multi-level model systems

Optical control of the current-voltage relation in stacked superconductors

We simulate the current-voltage relation of short layered superconductors, which we model as stacks of capacitively coupled Josephson junctions. The system is driven by external laser fields, in order to optically control the voltage drop across the junction. We identify parameter regimes in which supercurrents can be stabilised against thermally induced phase slips, thus reducing the effective voltage across the superconductor. Furthermore, single driven Josephson junctions are known to exhibit phase-locked states, where the superconducting phase is locked to the driving field. We numerically observe their persistence in the presence of thermal fluctuations and capacitive coupling between adjacent Josephson junctions. Our results indicate how macroscopic material properties can be manipulated by exploiting the large optical nonlinearities of Josephson plasmons.Comment: 7 pages, 7 figure

Mott polaritons in cavity-coupled quantum materials

We show that strong electron-electron interactions in cavity-coupled quantum materials can enable collectively enhanced light-matter interactions with ultrastrong effective coupling strengths. As a paradigmatic example we consider a Fermi-Hubbard model coupled to a single-mode cavity and find that resonant electron-cavity interactions result in the formation of a quasi-continuum of polariton branches. The vacuum Rabi splitting of the two outermost branches is collectively enhanced and scales with $g_{\text{eff}}\propto\sqrt{2L}$, where $L$ is the number of electronic sites, and the maximal achievable value for $g_{\text{eff}}$ is determined by the volume of the unit cell of the crystal. We find that $g_{\text{eff}}$ for existing quantum materials can by far exceed the width of the first excited Hubbard band. This effect can be experimentally observed via measurements of the optical conductivity and does not require ultra-strong coupling on the single-electron level. Quantum correlations in the electronic ground state as well as the microscopic nature of the light-matter interaction enhance the collective light-matter interaction compared to an ensemble of independent two-level atoms interacting with a cavity mode.Comment: 11 pages, 4 figures. arXiv admin note: text overlap with arXiv:1806.0675

Terahertz field control of interlayer transport modes in cuprate superconductors

We theoretically show that terahertz pulses with controlled amplitude and frequency can be used to switch between stable transport modes in layered superconductors, modelled as stacks of Josephson junctions. We find pulse shapes that deterministically switch the transport mode between superconducting, resistive and solitonic states. We develop a simple model that explains the switching mechanism as a destablization of the centre of mass excitation of the Josephson phase, made possible by the highly non-linear nature of the light-matter coupling

How to optimize the absorption of two entangled photons

We investigate how entanglement can enhance two-photon absorption in a three-level system. First, we employ the Schmidt decomposition to determine the entanglement properties of the optimal two-photon state to drive such a transition, and the maximum enhancement which can be achieved in comparison to the optimal classical pulse. We then adapt the optimization problem to realistic experimental constraints, where photon pairs from a down-conversion source are manipulated by local operations such as spatial light modulators. We derive optimal pulse shaping functions to enhance the absorption efficiency, and compare the maximal enhancement achievable by entanglement to the yield of optimally shaped, separable pulses.Comment: 25 pages, 8 figure