Huygens Institute for History and Culture of the Netherlands

We present a method to efficiently sort orbital angular momentum (OAM) states of light using two static optical elements. The optical elements perform a Cartesian to log-polar coordinate transformation, converting the helically phased light beam corresponding to OAM states into a beam with a transverse phase gradient. A subsequent lens then focuses each input OAM state to a different lateral position. We demonstrate the concept experimentally by using two spatial light modulators to create the desired optical elements, applying it to the separation of eleven OAM states.

Ambient optical detection of labeled molecules is limited for fluorescent dyes by photobleaching and for semiconducting nanoparticles by "blinking" effects. Because nanometer-sized metal particles do not optically bleach, they may be useful optical labels if suitable detection signals can be found. We demonstrate far-field optical detection of gold colloids down to diameters of 2.5 nanometers with a photothermal method that combines high-frequency modulation and polarization interference contrast. The photothermal image is immune to the effects of scattering background, which limits particle imaging through Rayleigh scattering to diameters larger than 40 nanometers.

International audience

We create mechanical metamaterials whose response to uniaxial compression can be programmed by lateral confinement, allowing monotonic, nonmonotonic, and hysteretic behavior. These functionalities arise from a broken rotational symmetry which causes highly nonlinear coupling of deformations along the two primary axes of these metamaterials. We introduce a soft mechanism model which captures the programmable mechanics, and outline a general design strategy for confined mechanical metamaterials. Finally, we show how inhomogeneous confinement can be explored to create multistability and giant hysteresis.

Low-temperature single-molecule spectroscopic techniques were applied to a light-harvesting pigment-protein complex (LH2) from purple photosynthetic bacteria. The properties of the electronically excited states of the two circular assemblies (B800 and B850) of bacteriochlorophyll a (BChl a) pigment molecules in the individual complexes were revealed, without ensemble averaging. The results show that the excited states of the B800 ring of pigments are mainly localized on individual BChl a molecules. In contrast, the absorption of a photon by the B850 ring can be consistently described in terms of an excitation that is completely delocalized over the ring. This property may contribute to the high efficiency of energy transfer in these photosynthetic complexes.

The performance of an optoelectronic terahertz (THz) beam system is described. The transmitter operation is based on the repetitive, subpicosecond laser excitation of a Hertzian dipole antenna embedded in a charged coplanar line. With this transmitter electromagnetic beams of 1/2 cycle THz pulses at a repetition rate of 100 MHz are produced. The associated optoelectronic receiver is gated in synchronism with the excitation of the transmitter by subpicosecond pulses from the same laser source. With this receiver, the 10-nW beams of THz pulses were observed with a signal-to-noise ratio greater than 10000:1. Several sources contributing to the noise of the receiver are discussed, together with ways to reduce them. With an integration time of 125 ms, a signal-to-noise ratio of 1 is obtained for a THz beam with an average power of 10/sup -16/ W. The receiver operates in the sampling mode and has a time resolution of 0.5 ps.< <ETX xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">&gt;</ETX>

The primary light-induced charge separation in reaction centers from Rhodopseudomonas sphaeroides R-26 has been investigated after excitation with laser pulses of 150 fsec duration within the longwave absorption band of the primary donor at 850 nm. An excited state of the primary donor, characterized by a broad absorption spectrum extending over the whole spectral range investigated (545-1240 nm), appeared within 100 fsec and gave rise to stimulated emission in the 870- to 1000-nm region with a 2.8-psec lifetime. The photooxidation of the primary donor, as measured at 1240 nm, and the photoreduction of the bacteriopheophytin acceptor, monitored at 545 nm and 675 nm, have been found to proceed simultaneously with a time constant of 2.8 +/- 0.2 psec. Kinetics of absorbance changes at other probe wavelengths gave no indication that an accessory bacteriochlorophyll is involved as a transient electron acceptor.

A critical overview of the theory of the chirality-induced spin selectivity (CISS) effect, that is, phenomena in which the chirality of molecular species imparts significant spin selectivity to various electron processes, is provided. Based on discussions in a recently held workshop, and further work published since, the status of CISS effects-in electron transmission, electron transport, and chemical reactions-is reviewed. For each, a detailed discussion of the state-of-the-art in theoretical understanding is provided and remaining challenges and research opportunities are identified.

We show that the simplest building blocks of origami-based materials-rigid, degree-four vertices-are generically multistable. The existence of two distinct branches of folding motion emerging from the flat state suggests at least bistability, but we show how nonlinearities in the folding motions allow generic vertex geometries to have as many as five stable states. In special geometries with collinear folds and symmetry, more branches emerge leading to as many as six stable states. Tuning the fold energy parameters, we show how monostability is also possible. Finally, we show how to program the stability features of a single vertex into a periodic fold tessellation. The resulting metasheets provide a previously unanticipated functionality-tunable and switchable shape and size via multistability.

Enhancing the fluorescence of a weak emitter is important to further extend the reach of single-molecule fluorescence imaging to many unexplored systems. Here we study fluorescence enhancement by isolated gold nanorods and explore the role of the surface plasmon resonance (SPR) on the observed enhancements. Gold nanorods can be cheaply synthesized in large volumes, yet we find similar fluorescence enhancements as literature reports on lithographically fabricated nanoparticle assemblies. The fluorescence of a weak emitter, crystal violet, can be enhanced more than 1000-fold by a single nanorod with its SPR at 629 nm excited at 633 nm. This strong enhancement results from both an excitation rate enhancement of ∼130 and an effective emission enhancement of ∼9. The fluorescence enhancement, however, decreases sharply when the SPR wavelength moves away from the excitation laser wavelength or when the SPR has only a partial overlap with the emission spectrum of the fluorophore. The reported measurements of fluorescence enhancement by 11 nanorods with varying SPR wavelengths are consistent with numerical simulations.

Electronic transport is localized in low-dimensional disordered media. The addition of gauge fields to disordered media leads to fundamental changes in the transport properties. We implement a synthetic gauge field for photons using silicon-on-insulator technology. By determining the distribution of transport properties, we confirm that waves are localized in the bulk and localization is suppressed in edge states. Our system provides a new platform for investigating the transport properties of photons in the presence of synthetic gauge fields.

Since the first report on the far-field optical detection of single metal nanoparticles in the late 1990s, the field has rapidly developed and new methods and concepts have been introduced. Eliminating averaging over the broad size, shape and crystallinity distributions produced by even the best of current synthesis methods, these techniques have proven extremely useful for gaining a deeper insight into many of the properties of metal nanoparticles. These techniques have already led to the first applications specifically directed at using single particles. In this review we describe far-field optical techniques (both linear and nonlinear) that have sufficient sensitivity to detect single metal particles. We further discuss emerging applications, and emphasize the importance of single-particle detection techniques in their development.

Quantum data are susceptible to decoherence induced by the environment and to errors in the hardware processing it. A future fault-tolerant quantum computer will use quantum error correction to actively protect against both. In the smallest error correction codes, the information in one logical qubit is encoded in a two-dimensional subspace of a larger Hilbert space of multiple physical qubits. For each code, a set of non-demolition multi-qubit measurements, termed stabilizers, can discretize and signal physical qubit errors without collapsing the encoded information. Here using a five-qubit superconducting processor, we realize the two parity measurements comprising the stabilizers of the three-qubit repetition code protecting one logical qubit from physical bit-flip errors. While increased physical qubit coherence times and shorter quantum error correction blocks are required to actively safeguard the quantum information, this demonstration is a critical step towards larger codes based on multiple parity measurements.

We present an efficient method for probing the orbital angular momentum of optical vortices of arbitrary sizes. This method, based on a multipoint interferometer, has its most important application in measuring the orbital angular momentum of light from astronomical sources, opening the way to interesting new astrophysics. We demonstrate its viability by measuring the orbital angular momentum of Laguerre-Gaussian laser beams.

We observe the unconventional photon blockade effect in quantum dot cavity QED, which, in contrast to the conventional photon blockade, operates in the weak coupling regime. A single quantum dot transition is simultaneously coupled to two orthogonally polarized optical cavity modes, and by careful tuning of the input and output state of polarization, the unconventional photon blockade effect is observed. We find a minimum second-order correlation g^{(2)}(0)≈0.37, which corresponds to g^{(2)}(0)≈0.005 when corrected for detector jitter, and observe the expected polarization dependency and photon bunching and antibunching; close by in parameter space, which indicates the abrupt change from phase to amplitude squeezing.

We review recent developments in single-molecule spectroscopy and microscopy. New optical methods provide access to the absorption, emission, or excitation spectra of single nano-objects and can determine either the positions of these objects with subwavelength accuracy or the full three-dimensional orientation of their transition dipole moments. Recent work aims at using single molecules as nanoparts or nanoelements in a variety of molecular-scale devices, from triggered sources of single photons to single-molecular switches. A prominent new direction explores the various interactions between molecules within individual multichromophoric systems obtained by chemical synthesis. These systems are the models for natural self-assembled systems such as the light-harvesting proteins of bacteria and green plants, which are currently studied on a single-molecule basis. Another important class of multichromophoric systems are conjugated polymers. The combination of microscopy with time- and frequency-resolved spectroscopy is opening a wide field of new and exciting applications to individual nano-objects.

The photothermal (PT) signal arises from slight changes of the index of refraction in a sample due to absorption of a heating light beam. Refractive index changes are measured with a second probing beam, usually of a different color. In the past two decades, this all-optical detection method has reached the sensitivity of single particles and single molecules, which gave birth to original applications in material science and biology. PT microscopy enables shot-noise-limited detection of individual nanoabsorbers among strong scatterers and circumvents many of the limitations of fluorescence-based detection. This review describes the theoretical basis of PT microscopy, the methodological developments that improved its sensitivity toward single-nanoparticle and single-molecule imaging, and a vast number of applications to single-nanoparticle imaging and tracking in material science and in cellular biology.

Isolating single molecules in the solid state has allowed fundamental experiments in basic and applied sciences. When cooled down to liquid helium temperature, certain molecules show transition lines that are tens of megahertz wide, limited by only the excited-state lifetime. The extreme flexibility in the synthesis of organic materials provides, at low costs, a wide palette of emission wavelengths and supporting matrices for such single chromophores. In the past few decades, their controlled coupling to photonic structures has led to an optimized interaction efficiency with light. Molecules can hence be operated as single-photon sources and as nonlinear elements with competitive performance in terms of coherence, scalability and compatibility with diverse integrated platforms. Moreover, they can be used as transducers for the optical read-out of fields and material properties, with the promise of single-quanta resolution in the sensing of charges and motion. We show that quantum emitters based on single molecules hold promise to play a key role in the development of quantum science and technologies. This Review discusses the photophysical properties and nonlinear behaviour of single molecules, and their use as single-photon sources and in single-molecule sensing and quantum-sensing applications.

It is known that the porphyrin free base (H2P) can be incorporated in an n-octane Shpol'skii matrix. In slowly grown crystals the solute molecules occur in two orientations, which are co-planar and have their N-H … H-N axes at right angles; in the S 1↔S 0 ‘quasi-line’ absorption and fluorescence spectra they can be distinguished by a relative shift of 65 cm-1 of their spectral features. By irradiation with light the two species are transformed into one another via a shift of the two inner protons. Here a study is presented of the photoisomerism following selective excitation with a dye laser into the 0-0 band of the S 1←S 0 transition of either of the two forms, for H2P and D2P (two inner hydrogens replaced by deuterium). At 4·2 K the reaction proceeds in both directions; for H2P the reaction in one direction appears to be 10 per cent faster than in the other, for D2P the absolute rates are nearly ten times lower than for H2P and not measurably different in the two directions. The reactions are not significantly enhanced when the experiment is carried out at 77 K, or by excitation into the Soret band, i.e. via absorption of photons that are 8000 cm-1 more energetic. A possible reaction mechanism is discussed: the intersystem crossing from S 1 into the triplet manifold may lead to a displacement of the inner hydrogens because of vibronic coupling between the two lower triplet states. Finally the isotope effect on the T 0→S 0 decay rate has been determined: for H2P =92 s-1, for D2P =46 s-1.

Hubble Space Telescope images of 3CR radio galaxies at redshifts 0.6 < z < 1.8 have shown a remarkable variety of structures, generally aligned along the radio axis, indicating that the radio source strongly influences the optical appearance of these galaxies. In this paper we investigate the host galaxies underlying this aligned emission, combining the HST data with ground-based infrared images.