Selective reflection spectroscopy at normal incidence provides signals with sub-Doppler resolution, linear with optical intensity. Frequency modulated (FM) selective reflection probes atomic vapours at distances comparable to the excitation wavelength (~λ/2π) and is used extensively to probe the Casimir-Polder interactions between an excited state atom and a macroscopic surface. Extending selective reflection spectroscopy to molecular gases allows probing a thin layer of molecular gas next to a surface. This is a very attractive prospect that allows envisaging high-resolution molecular spectroscopy and molecular frequency references in a compact and miniaturised apparatus, such as a thin cell [1] or a photonic crystal [2]. Additionally, it paves the way for spectroscopic probing of the Casimir-Polder interaction with molecules. The molecule-surface interaction has been the object of extensive theoretical investigations, focusing on the effects of molecular orientation and chirality. However, experimental tests are few and comparison with theoretical predictions has been challenging [3].
Selective reflection spectroscopy at normal incidence provides signals with sub-Doppler resolution, linear with optical intensity. Frequency modulated (FM) selective reflection probes atomic vapours at distances comparable to the excitation wavelength (~λ/2π) and is used extensively to probe the Casimir-Polder interactions between an excited state atom and a macroscopic surface. Extending selective reflection spectroscopy to molecular gases allows probing a thin layer of molecular gas next to a surface. This is a very attractive prospect that allows envisaging high-resolution molecular spectroscopy and molecular frequency references in a compact and miniaturised apparatus, such as a thin cell [1] or a photonic crystal [2]. Additionally, it paves the way for spectroscopic probing of the Casimir-Polder interaction with molecules. The molecule-surface interaction has been the object of extensive theoretical investigations, focusing on the effects of molecular orientation and chirality. However, experimental tests are few and comparison with theoretical predictions has been challenging [3].
Selective reflection is a high-resolution spectroscopic method that allows the probing of atomic and molecular gases in the near field of dielectric cell windows. It is a sensitive technique for measuring interactions between excited atoms and surfaces, thus providing a unique tool to probe resonant effects in Casimir-Polder physics. The theoretical modelling of selective reflection spectra has thus far employed the infinite Doppler approximation which assumes that the Doppler shift dominates over the atom-surface interactions as well as the homogeneous transition linewidth. Here we extend the theoretical treatment of selective reflection spectra to include the effects of finite Doppler width. This allows us to analyse the regime of very large Casimir-Polder interactions, relevant for Rydberg atom spectroscopy, and revisit previous analyses of experiments with low-lying excited states. Further, this will aid in determining the signatures of quantum friction in vapor cell spectroscopy.
In this habilitation thesis, I briefly present my work at Imperial College London on trapping atomic clouds in micro-pyramids fabricated on silicon chips, which led to the fabrication of an on-chip integrated atom source. Next, I describe the research carried out at the Laboratoire de Physique des Lasers in the SAI group. Our experiments demonstrated the temperature dependence of near-field Casimir-Polder interactions due to thermal excitation of surface waves, thus advancing our understanding of the dielectric properties of matter and the quantum vacuum that surrounds it. I also present spectroscopic experiments with atomic vapors confined in nanostructures (nano-sphere opals) aiming at the fabrication of miniature frequency references. Finally, I explore the possibility of performing spectroscopic experiments on molecular gases close to surfaces.
Up to now, Doppler-free nonlinear spectroscopy has been applied to atoms inside a gas medium (volume spectroscopy). We have extended these methods to atoms in the vicinity of a surface. The basic principle consists of monitoring reflectivity changes produced when a laser beam, incident on a glass–vapor interface, is brought into resonance with an atomic transition. For Doppler-free spectroscopy, two counterpropagating beams are used to operate velocity selection. If these two beams are under normal incidence in the glass—velocity selection perpendicular to the surface—one observes saturated dispersion (selective reflection sensitive to the real index). For incidence angles in the glass (prism) larger than the critical angle (total internal reflection), a standing evanescent wave is produced in the gas (velocity selection along the surface), and saturated absorption is detected. Experimental demonstration was performed on the Na resonance line; high sensitivity (10−4 relative reflectivity change) and spectral resolution as good as 20 MHz were obtained. The main limitation to better resolution comes from the short atomic transit time in the evanescent wave (typical extension ~λ). Relevant applications of these techniques should also concern the diagnostics of optically thick media, as analysis of interaction between gas-phase atoms and the surface, notably atom–wall collisions, and modification of the spontaneous emission characteristics.
Selective reflection spectroscopy at an interface with a low-density resonant vapor, especially when combined with a frequency modulation technique, is a high-resolution Doppler-free tool for probing atoms interacting with a surface. We analyze different types of relevant surface interaction, emphasizing the spectral consequences of a van der Waals surface attraction associated to a z−3 potential dependence (z: distance to the wall). We present detailed results of two series of experiments at a Cs vapor/dielectric window interface on the 6S1/2-6P3/2 (λ=852 nm) resonance line and on the 6S1/2-7P second resonance line (λ=455 nm and 459 nm). Lineshape analysis at various pressures consistently shows that a van der Waals-type surface attraction has to be considered to interpret strong lineshape distortions and resonance shift. The attractive strengths are found to be equal respectively to ≈2 kHz μm3 and ≈20 kHz μm3, independently of the considered hyperfine component, within the experimental accuracy. It yields also typical parameters of pressure broadening and shift, which are shown to originate in collisional processes, at densities where the medium is opaque. Theoretical expectations for the VW strength are discussed on the basis of the results of atomic theory. The predicted values are smaller, by a typical factor of 2, than those deduced from the experiments. The validity of the theory, when applied to a dielectric interface, is discussed and seems questionable when the frequency of virtual atomic transitions involved in the van der Waals attraction potential lies in the dielectric window absorption range.
We calculate the modulation of the reflection coefficient for a frequency-modulated (FM) light beam incident on the interface between a dielectric and an atomic vapor. The vapor is described as a gas of resonant, Doppler-broadened, two-level systems, with transition frequency and linewidth arbitrarily depending on the atom-dielectric distance. The atoms are supposed to get deexcited at collisions with the surface. The transient atomic response is calculated to first order in the incident field, for both incoming and desorbed atoms. The reflection coefficient, evaluated to first order in the vapor dipole polarization, leads to a formal expression of the reflectivity modulation, valid for arbitrary atom-surface interaction potentials. One first discusses the reflection signal in absence of wall interactions, for arbitrary modulation frequencies. At large frequencies, it allows one to monitor both vapor absorption and dispersion. Second, the formal theory is applied to the case of a Van der Waals-London surface attraction exerted on the atomic vapor. Both normal and oblique beam incidences are considered. One shows how the vapor dispersion signal is red-shifted and strongly distorted by the appearance of vapor-surface long-range interactions, and how it can be used to monitor these interactions. At non-normal incidences, the lineshapes get Doppler-broadened.
Highly excited (Rydberg) atoms have exaggerated properties making them extremely sensitive to external electromagnetic fields and interacting strongly with their environment. Atomic vapor cells represent an attractive platform for studying Rydberg atoms and fabricating quantum devices. For example, Rydberg atoms in vapor cells have been used as sensitive detectors of electric fields of frequencies ranging from DC up to the THz range but also as single photon sources for quantum technology applications exploiting collective phenomena due to the Rydberg blockade effect [1]. Rydberg atoms also find applications in fundamental physics, in particular for the measurement of dispersive interactions of the Casimir-Polder type (atom-surface interactions) [2]. One major advantage of Rydberg atoms is that they expose limitations in the traditional perturbative approach of Casimir-Polder (CP) theory [3, 4]. Indeed, in the extreme near-field, the dipole approximation breaks down and higher-order terms need to be considered. We report on extensive experimental measurements of the Rydberg-surface interaction using spectroscopy in cesium vapor nanocells of a thickness ranging roughly from 200-700nm, as well as selective reflection spectroscopy on a macroscopic cesium all-sapphire cell. Atoms are first excited to the Cs(6P) level with a 894nm pump laser and subsequently a green laser ≈ 510nm probes Rydberg nD or nS states, where the principal quantum number n ranges between 15-17. Our experiments evidence the dipole-dipole term of the Casimir-Polder interaction providing a measurement of the C3 coefficient for cesium Rydberg states. Furthermore, our experiment clearly evidences an additional interaction that induces shifts and broadens the linewidth of the probed transitions in the vicinity of the dielectric windows of our cells. We believe that this interaction is due to electric fields that are either generated by patch charges (trapped on the surface or induced by the excitation lasers), or by cesium adsorbants. We show that the different polarizability (of opposing sign) between S and D Rydberg states can be exploited to extract quantitative measurements of the strength and distance scaling (z-dependence) of such parasitic electrostatic interactions.Our experiments suggest that the sensitivity of Rydberg atoms to external electric fields could provide a unique tool for probing electrostatic interactions in the vicinity of surfaces. This could allow systematic error corrections in Casimir-Polder experiments with excited or even ground state atoms that aim at putting bounds on the existence of non-Newtonian gravity [5]. We are currently exploring the possibility of coating the internal window interfaces with conducting 2D material such as graphene to reduce the influence of parasitic charges. This could allow us to probe atoms closer to the surface, where quadrupole interactions could be experimentally attainable for the first time [4].References[1] H. Kubler, J. P. Shaffer, T. Baluktsian, R. Loew, T. Pfau, Nat. Photon., 4, 112–116 (2013).[2] V. Sandoghdar et al., Phys. Rev. Lett 68, 3432–3435 (1993).[3] J. A. Crosse et al., Phys. Rev. A 82, 3010901 (2010).[4] B. Dutta et al., Phys. Rev. Res. 6, L022035 (2024).[5] A. Laliotis, B-S. Lu, M. Ducloy, D. Wilkowski, AVS Quantum Sci. 3, 043501 (2021).