arXiv subjects

Eloïse Devaux

Publications and source records attributed to Eloïse Devaux.

5 recordsLinked to original sources

arXiv2023

Submolecular-scale control of phototautomerization

Many natural and artificial reactions including photosynthesis or photopolymerization are initiated by stimulating organic molecules into an excited state, which enables new reaction paths. Controlling light-matter interaction can influence this key concept of photochemistry, however, it remained a challenge to apply this strategy to control photochemical reactions at the atomic scale. Here, we profit from the extreme confinement of the electromagnetic field at the apex of a scanning tunneling microscope (STM) tip to drive and control the rate of a free-base phthalocyanine phototautomerization with submolecular precision. By tuning the laser excitation wavelength and choosing the STM tip position, we control the phototautomerization rate and the relative tautomer population. This sub-molecular optical control can be used to study any other photochemical processes.

cond-mat.mes-hall↗

arXiv2019

Exploring Superconductivity under Strong Coupling with the Vacuum Electromagnetic Field

Light-matter interactions have generated considerable interest as a means to manipulate material properties. Light-induced superconductivity has been demonstrated using pulsed lasers. An attractive alternative possibility is to exploit strong light-matter interactions arising by coupling phonons to the vacuum electromagnetic field of a cavity mode as has been suggested and theoretically studied. Here we explore this possibility for two very different superconductors, namely YBCO (YBa$_2$Cu$_3$O$_{6+x}$) and Rb$_3$C$_{60}$, coupled to surface plasmon polaritons, using a novel cooperative effect based on the presence of a strongly coupled vibrational environment allowing efficient dressing of the otherwise weakly coupled phonon bands of these compounds. By placing the superconductor-surface plasmon system in a SQUID magnetometer, we find that the superconducting transition temperatures ($T_{c}$) for both compounds are modified in the absence of any external laser field. For YBCO, $T_{c}$ decreases from 92 K to 86 K while for Rb$_3$C$_{60}$, it increases from 30 K to 45 K at normal pressures. In the latter case, a simple theoretical framework is provided to understand these results based on an enhancement of the electron-phonon coupling. This proof-of-principle study opens a new tool box to not only modify superconducting materials but also to understand the mechanistic details of different superconductors.

cond-mat.supr-con↗

arXiv2018

Plasmonic interferences of two-particle N00N states

Quantum plasmonics lies at the intersection between nanophotonics and quantum optics. Genuine quantum effects can be observed with non-classical states such as Fock states and with entangled states. A N00N state combines both aspects: it is a quantum superposition state of a Fock state with N excitations in two spatial modes. Here we report the first observation of two-plasmon (N=2) N00N state interferences using a plasmonic beamsplitter etched on a planar interface between gold and air. We analyze in detail the role of losses at the beamsplitter and during the propagation along the metal/air interface. While the intrinsic losses of the beamsplitter are responsible for the emergence of quantum nonlinear absorption, we note that N00N states decay N times faster than classical states due to propagation losses.

quant-ph↗

arXiv2016

Multiple Rabi Splittings under Ultra-Strong Vibrational Coupling

From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies. As a proof of the ultra-strong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the anti-resonant terms in the interaction energy and from the dipolar self-energy of the molecular vibrations themselves. In particular, we measure the opening of a genuine vibrational polaritonic bandgap of ca. $60$ meV. We also demonstrate that the multimode splitting effect defines a whole vibrational ladder of heavy polaritonic states perfectly resolved. These findings reveal the broad possibilities in the vibrational ultra-strong coupling regime which impact both the optical and the molecular properties of such coupled systems, in particular in the context of mode-selective chemistry.

quant-ph↗

arXiv2011

Compact antenna for efficient and unidirectional launching and decoupling of surface plasmons

Controlling the launching efficiencies and the directionality of surface plasmon polaritons (SPPs) and their decoupling to freely propagating light is a major goal for the development of plasmonic devices and systems. Here, we report on the design and experimental observation of a highly efficient unidirectional surface plasmon launcher composed of eleven subwavelength grooves, each with a distinct depth and width. Our observations show that, under normal illumination by a focused Gaussian beam, unidirectional SPP launching with an efficiency of at least 52% is achieved experimentally with a compact device of total length smaller than 8 μm. Reciprocally, we report that the same device can efficiently convert SPPs into a highly directive light beam emanating perpendicularly to the sample.

physics.optics↗