Ilja Gerhardt, Gert Wrigge, Vahid Sandoghdar
We study the influence of a scanning nano-electrode on fluorescence excitation spectra of single terrylene molecules embedded in thin p-terphenyl films at cryogenic temperatures. We show that applied voltages less than 10 V can result in reversible Stark shifts of up to 100 times and linewidth increase greater than 10 times the natural linewidth. We discuss the potential of our experimental scheme for direct imaging of individual two-level systems (TLS) in the nanometer vicinity of single molecules.
P. Kukura, M. Celebrano, A. Renn, V. Sandoghdar
Room temperature detection of single quantum emitters has had a broad impact in fields ranging from biophysics to material science, photophysics, or even quantum optics. These experiments have exclusively relied on the efficient detection of fluorescence. An attractive alternative would be to employ direct absorption, or more correctly expressed "extinction" measurements. Indeed, small nanoparticles have been successfully detected using this scheme in reflection and transmission. Coherent extinction detection of single emitters has also been reported at cryogenic temperatures, but their room temperature implementation has remained a great laboratory challenge owing to the expected weak signal-to-noise ratio. Here we report the first extinction study of a single quantum emitter at ambient condition. We obtain a direct measure for the extinction cross section of a single semiconductor nanocrystal both during and in the absence of fluorescence, for example in the photobleached state or during blinking off-times. Our measurements pave the way for the detection and absorption spectroscopy of single molecules or clusters of atoms even in the quenched state.
Johannes Zirkelbach, Masoud Mirzaei, Irena Deperasinska, Boleslaw Kozankiewicz, Burak Gurlek, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Hsuan-Wei Liu, Michael A. Becker, Korenobu Matsuzaki, Randhir Kumar, Stephan Götzinger, Vahid Sandoghdar
Mar 10, 2022·quant-ph·PDF Scanning probe microscopes scan and manipulate a sharp tip in the immediate vicinity of a sample surface. The limited bandwidth of the feedback mechanism used for stabilizing the separation between the tip and the sample makes the fragile nanoscopic tip very susceptible to mechanical instabilities. We propose, demonstrate and characterize a new alternative device based on bulging a thin substrate against a second substrate and rolling them with respect each other. We showcase the power of this method by placing gold nanoparticles and semiconductor quantum dots on the two opposite substrates and positioning them with nanometer precision to enhance the fluorescence intensity and emission rate. We exhibit the passive mechanical stability of the system over more than one hour. The design concept presented in this work holds promise in a variety of other contexts, where nanoscopic features have to be positioned and kept near contact with each other.
Daqing Wang, Hrishikesh Kelkar, Diego Martin-Cano, Dominik Rattenbacher, Alexey Shkarin, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Sep 20, 2018·quant-ph·PDF 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.
Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Rasoul Alaee, Akbar Safari, Vahid Sandoghdar, Robert W. Boyd
We study scattering phenomena such as the Kerker effect, superscattering, and scattering dark states in a subwavelength atomic antenna consisting of atoms with only electric dipole transitions. We show that an atomic antenna can exhibit arbitrarily large or small scattering cross sections depending on the geometry of the structure and the direction of the impinging light. We also demonstrate that atoms with only an electric dipole transition can exhibit a directional radiation pattern with zero backscattering when placed in a certain configuration. This is a special case of a phenomenon known as the Kerker effect, which typically occurs in the presence of both electric and magnetic transitions. Our findings open a pathway to design highly directional emitters, nonradiating sources, and highly scattering objects based on individually controlled atoms.
Korenobu Matsuzaki, Simon Vassant, Hsuan-Wei Liu, Anke Dutschke, Björn Hoffmann, Xuewen Chen, Silke Christiansen, Matthew R. Buck, Jennifer A. Hollingsworth, Stephan Götzinger, Vahid Sandoghdar
Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other non-radiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60% and 70%, respectively, in very good agreement with the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.
Sanli Faez, Pierre Türschmann, Vahid Sandoghdar
Cavity-free efficient coupling between emitters and guided modes is of great current interest for nonlinear quantum optics as well as efficient and scalable quantum information processing. In this work, we extend these activities to the coupling of organic dye molecules to a highly confined mode of a nanofiber, allowing mirrorless and low-threshold laser action in an effective mode volume of less than 100 femtoliters. We model this laser system based on semi-classical rate equations and present an analytic compact form of the laser output intensity. Despite the lack of a cavity structure, we achieve a coupling efficiency of the spontaneous emission to the waveguide mode of 0.07(0.01), in agreement with our calculations. In a further experiment, we also demonstrate the use of a plasmonic nanoparticle as a dispersive output coupler. Our laser architecture is promising for a number of applications in optofluidics and provides a fundamental model system for studying nonresonant feedback stimulated emission.
Pu Zhang, Igor Protsenko, Vahid Sandoghdar, Xue-Wen Chen
We theoretically demonstrate the generation and radiation of coherent nanoplasmons powered by a single three-level quantum emitter on a plasmonic nanoresonator. By pumping the three-level emitter in a Raman configuration, we show a pathway to achieve macroscopic accumulation of nanoplasmons due to stimulated emission in the nanoresonator despite their fast relaxation. Thanks to the antenna effect of the nanoresonator, the system acts as an efficient and bright nanoscopic coherent light source with a photon emission rate of hundreds of Terahertz and could be realized with solid-state emitters at room temperatures in pulse mode. We provide physical interpretations of the results and discuss their realization and implications for ultra-compact integration of optoelectronics.
Nassiredin M. Mojarad, Vahid Sandoghdar, Mario Agio
We study the modification of the far-field cross sections and the near-field enhancement for gold and silver nanospheres illuminated by a tightly focused beam. Using a multipole-expansion approach we obtain an analytical solution to the scattering problem and provide insight on the effects of focusing on the optical response. Large differences with respect to Mie theory are found especially when the nanoparticle supports quadrupole or higher-order resonances.
Daqing Wang, Hrishikesh Kelkar, Diego Martin-Cano, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
Dec 15, 2016·quant-ph·PDF 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.
Masoud Mirzaei, Alexey Shkarin, Burak Gurlek, Johannes Zirkelbach, Ashley J. Shin, Irena Deperasińska, Boleslaw Kozankiewicz, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar
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.
Jahangir Nobakht, André Pscherer, Jan Renger, Stephan Götzinger, Vahid Sandoghdar
Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.
Marek Piliarik, Vahid Sandoghdar
More than twenty years ago, scientists succeeded in pushing the limits of optical detection to single molecules using fluorescence. This breakthrough has revolutionized biophysical measurements, but restrictions in photophysics and labeling protocols have motivated many efforts to achieve fluorescence-free single-molecule sensitivity in biological studies. Although several interesting mechanisms using vibrational spectroscopy, photothermal detection, plasmonics or microcavities have been proposed for biosensing at the single-protein level, no method has succeeded in direct label-free detection of single proteins. Here, we present the first results using interferometric detection of scattering (iSCAT) from single proteins without the need for any label, optical nanostructure or microcavity. Furthermore, we demonstrate super-resolution imaging of protein binding with nanometer localization precision. The ease of iSCAT instrumentation promises a breakthrough for industrial usage as well as fundamental laboratory experiments.
Burak Gurlek, Vahid Sandoghdar, Diego Martín-Cano
We show that a broadband Fabry-Perot microcavity can assist an emitter coupled to an off-resonant plasmonic nanoantenna to inhibit the nonradiative channels that affect the quenching of fluorescence. We identify the interference mechanism that creates the necessary enhanced couplings and bandwidth narrowing of the hybrid resonance and show that it can assist entering into the strong coupling regime. Our results provide new possibilities for improving the efficiency of solid-state emitters and accessing diverse realms of photophysics with hybrid structures that can be fabricated using existing technologies.
Xue-Wen Chen, Vahid Sandoghdar, Mario Agio
Jun 20, 2009·quant-ph·PDF Successful exploitations of strongly confined surface plasmon-polaritons critically rely on their efficient and rapid conversion to lossless channels. We demonstrate a simple, robust, and broad-band butt-coupling technique for connecting a metallic nanowire and a dielectric nanofiber. Conversion efficiencies above 95% in the visible and close to 100% in the near infrared can be achieved with realistic parameters. Moreover, by combining butt-coupling with nanofocusing, we propose a broad-band high-throughput near-field optical microscope.
Ahmad Mohammadi, Franziska Kaminski, Vahid Sandoghdar, Mario Agio
We investigate the properties of finite gold nanocones as optical antennas for enhancing molecular fluorescence. We compute the modification of the excitation rate, spontaneous emission rate, and quantum efficiency as a function of the nanocone base and length, showing that the maximum field and fluorescence enhancements do not occur for the same nanocone parameters. We compare the results with those for nanorods and nanospheroids and find that nanocones perform better.
Xue-Wen Chen, Mario Agio, Vahid Sandoghdar
We devise new optical antennas that reduce the excited-state radiative lifetimes of emitters to the order of 100 femtoseconds while maintaining quantum efficiencies of about 80% at a broadband operation. Here, we combine metallic nanoparticles with planar dielectric structures and exploit design strategies from plasmonic nanoantennas and concepts from Cavity Quantum Electrodynamics to maximize the local density of states and minimize the nonradiative losses incurred by the metallic constituents. The proposed metallo-dielectric hybrid antennas promise important impact on various fundamental and applied research fields, including photophysics, ultrafast plasmonics, bright single photon sources and Raman spectroscopy.
Kiarash Kasaian, Mahdi Mazaheri, Vahid Sandoghdar
Tracking nanoparticle movement is highly desirable in many scientific areas, and various imaging methods have been employed to achieve this goal. Interferometric scattering (iSCAT) microscopy has been particularly successful in combining very high spatial and temporal resolution for tracking small nanoparticles in all three dimensions. However, previous works have been limited to an axial range of only a few hundred nanometers. Here, we present a robust and efficient strategy for localizing nanoparticles recorded in high-speed iSCAT videos in three dimensions over tens of micrometers. We showcase the performance of our algorithm by tracking gold nanoparticles as small as 10 nm diffusing in water while maintaining 5 μs temporal resolution and nanometer axial localization precision. Our results hold promise for applications in cell biology and material science, where the three-dimensional motion of nanoparticles in complex media is of interest.