arXiv subjects

Tobias Utikal

Publications and source records attributed to Tobias Utikal.

18 recordsLinked to original sources

arXiv2026

Designing metallo-dielectric antennas for cryogenic applications

We present the design of cryogenic metallo-dielectric antennas tailored to single organic emitters, where the choice of host material imposes specific constraints on the antenna geometry. Using dibenzoterrylene (DBT) in para-dichlorobenzene (p-DCB}) as a model system, we show that photon collection efficiencies exceeding 90% can be achieved for arbitrary dipole orientations of the fluorescent molecule. The antenna design is intrinsically broadband and tolerant to emitter positioning within the structure. We further provide concrete fabrication guidelines for the full antenna architecture, and experimentally demonstrate its operating principle by recording a back-focal-plane image (BFP) of a single molecule inside a fabricated antenna.

physics.optics↗

arXiv2025

Nano-electronvolt Fourier-limited transition of a single surface-adsorbed molecule

High-resolution spectroscopy allows one to probe weak interactions and to detect subtle phenomena. While such measurements are routinely performed on atoms and molecules in the gas phase, spectroscopy of adsorbed species on surfaces is faced with challenges. As a result, previous studies of surface-adsorbed molecules have fallen short of the ultimate resolution, where the transition linewidth is determined by the lifetime of the excited state. In this work, we conceive a new approach to surface deposition and report on Fourier-limited electronic transitions in single dibenzoterrylenes adsorbed onto the surface of an anthracene crystal. By performing spectroscopy and super-resolution microscopy at liquid helium temperature, we shed light on various properties of the adsorbed molecules. Our experimental results pave the way for a new class of experiments in surface science, where high spatial and spectral resolution can be combined.

physics.chem-ph↗

arXiv2024

High-resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals

We perform laser spectroscopy at liquid helium temperatures (T=2 K) to investigate single dibenzoterrylene (DBT) molecules doped in anthracene crystals of nanoscopic height fabricated by electrohydrodynamic dripping. Using high-resolution fluorescence excitation spectroscopy, we show that zero-phonon lines of single molecules in printed nanocrystals are nearly as narrow as the Fourier-limited transitions observed for the same guest-host system in the bulk. Moreover, the spectral instabilities are comparable to or less than one linewidth. By recording super-resolution images of DBT molecules and varying the polarization of the excitation beam, we determine the dimensions of the printed crystals and the orientation of the crystals' axes. Electrohydrodynamic printing of organic nano and microcrystals paves the way for a series of applications, where controlled positioning of quantum emitters with narrow optical transitions is desirable.

quant-ph↗

arXiv2023

Spectral splitting of a stimulated Raman transition in a single molecule

The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T < 2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of the phenomenon at hand. Our study sets the ground for exploiting the intrinsic optomechanical degrees of freedom of molecules for applications in solid-state quantum optics and information processing.

quant-ph↗

arXiv2023

Quantum Efficiency of Single Dibenzoterrylene Molecules in para-Dichlorobenzene at Cryogenic Temperatures

We measure the quantum efficiency (QE) of individual dibenzoterrylene (DBT) molecules embedded in para-dichlorobenzene at cryogenic temperatures. To achieve this, we apply two distinct methods based on the maximal photon emission and on the power required to saturate the zero-phonon line. We find that the outcome of the two approaches are in good agreement, reporting a large fraction of molecules with QE values above 50%, with some exceeding 70%. Furthermore, we observe no correlation between the observed lower bound on the QE and the lifetime of the molecule, suggesting that most of the molecules have a QE exceeding the established lower bound. This confirms the suitability of DBT for quantum optics experiments. In light of previous reports of low QE values at ambient conditions, our results hint at the possibility of a strong temperature dependence of the QE.

quant-ph↗

arXiv2023

On-chip interference of scattering from two individual molecules in plastic

Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of organic molecules embedded in a plastic film to a TiO$_2$ microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the molecules with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8$\,μ$m and an optical phase difference of about $π/2$, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for the coherent coupling of several molecules via a common mode and the realization of polymer-based hybrid quantum photonic circuits.

quant-ph↗

arXiv2022

High-resolution vibronic spectroscopy of a single molecule embedded in a crystal

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at high resolution in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of dibenzoterrylene embedded in an organic crystal made of para-dichlorobenzene. To do this, we use narrow-band continuous-wave lasers and combine spectroscopy methods based on fluorescence excitation and stimulated emission depletion (STED) to assess individual vibrational linewidths in the electronic ground state at a resolution of ~30 MHz dictated by the linewidth of the electronic excited state. In this fashion, we identify several exceptionally narrow vibronic levels with linewidths down to values around 2GHz. Additionally, we sample the distribution of vibronic wavenumbers, relaxation rates, and Franck-Condon factors, both in the electronic ground and excited states for a handful of individual molecules. We discuss various noteworthy experimental findings and compare them with the outcome of DFT calculations. The highly detailed vibronic spectra obtained in our work pave the way for studying the nanoscopic local environment of single molecules. The approach also provides an improved understanding of the vibrational relaxation mechanisms in the electronic ground state, which may help to create long-lived vibrational states for applications in quantum technology.

quant-ph↗

arXiv2021

Single-molecule vacuum Rabi splitting: four-wave mixing and optical switching at the single-photon level

A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this work, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generation and all-optical switching. Our work promotes the use of molecules for applications such as integrated photonic circuits, operating at very low powers.

quant-ph↗

arXiv2020

Nanoscopic charge fluctuations in a gallium phosphide waveguide measured by single molecules

We present efficient coupling of single organic molecules to a gallium phosphide subwavelength waveguide (nanoguide). By examining and correlating the temporal dynamics of various single-molecule resonances at different locations along the nanoguide, we reveal light-induced fluctuations of their Stark shifts. Our observations are consistent with the predictions of a simple model based on the optical activation of a small number of charges in the GaP nanostructure.

quant-ph↗

arXiv2020

Partial cloaking of a gold particle by a single molecule

Extinction of light by material particles stems from losses incurred by absorption or scattering. The extinction cross section is usually treated as an additive quantity, leading to the exponential laws that govern the macroscopic attenuation of light. In this work, we demonstrate that the extinction cross section of a large gold nanoparticle can be substantially reduced, i.e., the particle becomes more transparent, if a single molecule is placed in its near field. This partial cloaking effect results from a coherent plasmonic interaction between the molecule and the nanoparticle, whereby each of them acts as a nano-antenna to modify the radiative properties of the other.

quant-ph↗

arXiv2019

Coherent coupling of single molecules to on-chip ring resonators

We report on cryogenic coupling of organic molecules to ring microresonators obtained by looping sub-wavelength waveguides (nanoguides). We discuss fabrication and characterization of the chip-based nanophotonic elements which yield resonator finesse in the order of 20 when covered by molecular crystals. Our observed extinction dips from single molecules reach 22%, consistent with the expected Purcell enhancements up to 11 folds. Future efforts will aim at efficient coupling of a handful of molecules via their interaction with a ring microresonator mode, setting the ground for the realization of quantum optical cooperative effects.

physics.app-ph↗

arXiv2018

Turning a molecule into a coherent two-level quantum system

Molecules are ubiquitous in natural phenomena and man-made products, but their use in quantum optical applications has been hampered by incoherent internal vibrations and other phononic interactions with their environment. We have now succeeded in turning an organic molecule into a coherent two-level quantum system by placing it in an optical microcavity. This allows several unprecedented observations such as 99\% extinction of a laser beam by a single molecule, saturation with less than 0.5 photon, and nonclassical generation of few-photon super-bunched light. Furthermore, we demonstrate efficient interaction of the molecule-microcavity system with single photons generated by a second molecule in a distant laboratory. Our achievements pave the way for linear and nonlinear quantum photonic circuits based on organic platforms.

quant-ph↗

arXiv2017

On-chip linear and nonlinear control of single molecules coupled to a nanoguide

While experiments with one or two quantum emitters have become routine in various laboratories, scalable platforms for efficient optical coupling of many quantum systems remain elusive. To address this issue, we report on chip-based systems made of one-dimensional subwavelength dielectric waveguides (nanoguides) and polycyclic aromatic hydrocarbon molecules. After discussing the design and fabrication requirements, we present data on coherent linear and nonlinear spectroscopy of single molecules coupled to a nanoguide mode. Our results show that external microelectrodes as well as optical beams can be used to switch the propagation of light in a nanoguide via the Stark effect and a nonlinear optical process, respectively. The presented nanoguide architecture paves the way for the investigation of many-body phenomena and polaritonic states and can be readily extended to more complex geometries for the realization of quantum integrated photonic circuits.

quant-ph↗

arXiv2016

Coherent coupling of a single molecule to a scanning Fabry-Perot microcavity

Organic dye molecules have been used in great many scientific and technological applications, but their wider use in quantum optics has been hampered by transitions to short-lived vibrational levels, which limit their coherence properties. To remedy this, one can take advantage of optical resonators. Here we present the first results on coherent molecule-resonator coupling, where a single polycyclic aromatic hydrocarbon molecule extinguishes 38\% of the light entering a microcavity at liquid helium temperature. We also demonstrate four-fold improvement of single-molecule stimulated emission compared to free-space focusing and set the ground for coherent mechanical manipulation of the molecular transition. Our experimental approach based on a microcavity of low mode volume and low quality factor paves the way for the realization of various nonlinear and collective quantum optical effects with molecules.

quant-ph↗

arXiv2015

Few-photon coherent nonlinear optics with a single molecule

The pioneering experiments of linear spectroscopy were performed using flames in the 1800s, but nonlinear optical measurements had to wait until lasers became available in the twentieth century. Because the nonlinear cross section of materials is very small, usually macroscopic bulk samples and pulsed lasers are used. Numerous efforts have explored coherent nonlinear signal generation from individual nanoparticles or small atomic ensembles with millions of atoms. Experiments on a single semiconductor quantum dot have also been reported, albeit with a very small yield. Here, we report on coherent nonlinear spectroscopy of a single molecule under continuous-wave single-pass illumination, where efficient photon-molecule coupling in a tight focus allows switching of a laser beam by less than a handful of pump photons nearly resonant with the sharp molecular transition. Aside from their fundamental importance, our results emphasize the potential of organic molecules for applications such as quantum information processing, which require strong nonlinearities.

quant-ph↗

arXiv2015

High-resolution spectroscopy of single Pr$^{3+}$ ions on the $^3$H$_4$-$^1$D$_2$ transition

Rare earth ions in crystals exhibit narrow spectral features and hyperfine-split ground states with exceptionally long coherence times. These features make them ideal platforms for quantum information processing in the solid state. Recently, we reported on the first high-resolution spectroscopy of single Pr$^{3+}$ ions in yttrium orthosilicate (YSO) nanocrystals. While in that work we examined the less explored $^3$H$_4$-$^3$P$_0$ transition at a wavelength of 488 nm, here we extend our investigations to the $^3$H$_4$-$^1$D$_2$ transition at 606 nm. In addition, we present measurements of the second-order autocorrelation function, fluorescence lifetime, and emission spectra of single ions as well as their polarization dependencies on both transitions; these data were not within the reach of the first experiments reported earlier. Furthermore, we show that by a proper choice of the crystallite, one can obtain narrower spectral lines and, thus, resolve the hyperfine levels of the excited state. We expect our results to make single-ion spectroscopy accessible to a larger scientific community.

physics.atom-ph↗

arXiv2013

Detection, spectroscopy and state preparation of a single praseodymium ion in a crystal

Solid-state emitters with atom-like optical and magnetic transitions are highly desirable for efficient and scalable quantum state engineering and information processing. Quantum dots, color centers and impurities embedded in inorganic hosts have attracted a great deal of attention in this context, but influences from the matrix continue to pose challenges on the degree of attainable coherence in each system. We report on a new solid-state platform based on the optical detection of single praseodymium ions via 4f intrashell transitions, which are well shielded from their surroundings. By combining cryogenic high-resolution laser spectroscopy with fluorescence microscopy, we were able to spectrally select and spatially resolve individual ions. In addition to elaborating on the essential experimental steps for achieving this long-sought goal, we demonstrate state preparation and read out of the three ground-state hyperfine levels, which are known to have lifetimes of the order of hundred seconds.

quant-ph↗

arXiv2011

Excitonic Fano Resonance in Freestanding Graphene

We investigate the role of electron-hole correlations in the absorption of freestanding monolayer and bilayer graphene using optical transmission spectroscopy from 1.5 to 5.5 eV. Line shape analysis demonstrates that the ultraviolet region is dominated by an asymmetric Fano resonance. We attribute this to an excitonic resonance that forms near the van-Hove singularity at the saddle point of the band structure and couples to the Dirac continuum. The Fano model quantitatively describes the experimental data all the way down to the infrared. In contrast, the common non-interacting particle picture cannot describe our data. These results suggest a profound connection between the absorption properties and the topology of the graphene band structure.

cond-mat.mes-hall↗