Related papers: Optical cycling in polyatomic molecules with compl…
We investigated the optical cycling effect of the $\mathrm{X}^2\Sigma(v=0,\ N=1^-) - \mathrm{A}^2\Pi_{1/2}(v'=0,\ J'=1/2^+)$ band of MgF molecules, specifically the $\mathrm{P_1/Q_{12}(1)}$ transition, which serves as the main transition in…
The rotational and hyperfine spectrum of the $X^1\Sigma^+ \rightarrow B^3\Pi_1$ transition in TlF molecules was measured using laser-induced fluorescence from both a thermal and a cryogenic molecular beam. Rotational and hyperfine constants…
An optical cycling center (OCC) is a recently coined term to indicate two electronic states within a complex quantum object that can repeatedly experience optical laser excitation and spontaneous decay, while being well isolated from its…
We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra,…
Polyatomic molecules equipped with optical cycling centers (OCCs), enabling continuous photon scattering during optical excitation, are exciting candidates for advancing quantum information science. However, as these molecules grow in size…
Because molecules can have their orientation locked when embedded into a solid rare-gas matrix, their hyperfine structure is strongly perturbed relative to the freely rotating molecule. The addition of an electric field further perturbs the…
Precise measurement of the particle number, spatial distribution and internal state is fundamental to all proposed experiments with ultracold molecules both in bulk gases and optical lattices. Here, we demonstrate in-situ detection of…
Molecular polaritons are hybrid states of photonic and molecular character that form when molecules strongly interact with light. Strong coupling tunes energy levels and importantly, can modify molecular properties (e.g. photoreaction…
Herein, we show that single molecules containing multiple optical cycling centers (CaO moieties) can exhibit superradiant phenomena. We demonstrate the accuracy of the Frenkel exciton model at describing these superradiant states via…
A study of the intensity-borrowing mechanisms important to optical cycling transitions in laser-coolable polyatomic molecules arising from non-adiabatic coupling, contributions beyond the Franck-Condon approximation, and Fermi resonances is…
Photonic molecules - particular systems composed of coupled optical resonators - emulate the behavior of complex physical systems exhibiting discrete energy levels. In this work, we present a novel photonic molecule composed of two strongly…
Polyatomic molecules have been identified as sensitive probes of charge-parity violating and parity-violating physics beyond the Standard Model (BSM). For example, many linear triatomic molecules are both laser-coolable and have parity…
We present a spectroscopic investigation of $^{169}\mathrm{Tm}^+$ that provides two key foundations for its use as a platform for advanced quantum applications. First, we establish the complete spectroscopic road map for optical cycling…
We present an opto-electrical cooling scheme for polar molecules based on a Sisyphus-type cooling cycle in suitably tailored electric trapping fields. Dissipation is provided by spontaneous vibrational decay in a closed level scheme found…
Driven by recent developments in time-resolved photoemission spectroscopy, we extend the successful method of photoemission orbital tomography (POT) to excitons. Our theory retains the intuitive orbital picture of POT, while respecting both…
Polyatomic molecules provide complex internal structures that are ideal for applications in quantum information science, quantum simulation, and precision searches for physics beyond the Standard Model. A key feature of polyatomic molecules…
Understanding the quantum dynamics of strongly coupled molecule-cavity systems remains a significant challenge in molecular polaritonics. This work develops a comprehensive self-consistent model simulating electromagnetic interactions of…
We use state- and time-resolved coherent Raman spectroscopy to study the rotational dynamics of oxygen molecules in ultra-high rotational states. While it is possible to reach rotational quantum numbers up to $N \approx 50$ by increasing…
We present a computer program to calculate the quantised rotational and hyperfine energy levels of $^{1}\Sigma $ diatomic molecules in the presence of dc electric, dc magnetic, and off-resonant optical fields. Our program is applicable to…
We propose a scheme to transfer molecules from a slow beam into an optical trap using only a single photon absorption and emission cycle. The efficiency of such a scheme is numerically explored for BaF using realistic experimental…