arXiv subjects

Michel Orrit

Publications and source records attributed to Michel Orrit.

15 recordsLinked to original sources

arXiv2025

Towards all-optical spin manipulation in single molecules: a refined region for locating a dark resonance

The on-demand manipulation of triplet states in closed-shell single molecules is still out of reach due to a lack of information about the energy of those triplet states. Yet, the access to triplet states would open up a route towards an all-optical single-molecule photonic switch/transistor and, moreover, would provide a way of performing coherent spin operations from the spin-less ground state. In this work, we take an important step towards those aims by measuring the triplet energy from the weak phosphorescence signal of perdeuterated perylene, embedded as a guest molecule in a dibenzothiophene host matrix, which well preserves the coherence properties of the perylene guest. We find that perylene's phosphorescence can be enhanced in this host matrix, when acting as an intermediary for the generation of triplet excitons. The triplet energy that we find can be used to significantly narrow down the search for the ultra-weak spin-forbidden transitions from the ground singlet to the triplet states of a single molecule.

physics.chem-ph↗

arXiv2025

Optical detection of charge defects near a graphene transistor using the Stark shift of fluorescent molecules

Two-dimensional crystals and their heterostructures unlock access to a class of photonic devices, bringing nanophotonics from the nanometer scale down to the atomic level where quantum effects are relevant. Single-photon emitters (SPEs) are central in quantum photonics as quantum markers linked to their electrostatic, thermal, magnetic, or dielectric environment. This aspect is exciting in two-dimensional (2D) crystals and their heterostructures, where the environment can be abruptly modified through vertical stacking or lateral structuring, such as moir\'e or nano-patterned gates. To further develop 2D-based quantum photonic devices, there is a need for quantum markers that are capable of integration into various device geometries, and that can be read out individually, non-destructively, and without additional electrodes. Here, we show how to optically detect charge carrier accumulation using sub-GHz linewidth single-photon emitters coupled to a graphene device. We employ the single molecule Stark effect, sensitive to the electric fields generated by charge puddles, such as those at the graphene edge. The same approach enables dynamic sensing of electronic noise, and we demonstrate the optical read-out of low-frequency white noise in a biased graphene device. The approach described here can be further exploited to explore charge dynamics in 2D heterostructures using quantum emitter markers.

cond-mat.mes-hall↗

arXiv2024

Nano-gap electrode dielectrophoresis for tether-free trapping and interferometric-scattering detection of single 20 nm particles

Accurate detection and characterization of nanoparticles within confined spaces is crucial for applications ranging from nanofluidics to biotechnology. We present a novel approach that combines interferometric scattering (iSCAT) detection with trapping by dielectrophoresis (DEP) to achieve label-free detection of nanoparticles that are trapped and/or actuated between nano-gap electrodes. DEP utilizes the interaction between the induced dipole of the particle and the applied electric field to create a trapping potential. We demonstrate our method by trapping and label-free detection of down to 20 nm polystyrene nanoparticles. Additionally, we demonstrate that the signal-to-noise ratio of our detection can be boosted up to 20-fold by periodic actuation of the nanoparticle in the trap. This is done by a digital lock-in detection scheme on the modulated scattering signal. Our method holds promise for various applications, including assembly of nanoparticles, single-particle property analysis, and nanofluidic devices.

physics.optics↗

arXiv2023

Sharp zero-phonon lines of single organic molecules on a hexagonal boron-nitride surface

Single fluorescent molecules embedded in the bulk of host crystals have proven to be excellent probes of the dynamics in their nano environment, thanks to their narrow (about 0.1 μeV) optical linewidth of the 0-0 zero-phonon line (0-0 ZPL) at cryogenic temperatures. However, the optical linewidths of the 0-0 ZPL have been found to increase dramatically as the single molecules are located closer to a surface or interface, while no 0-0 ZPL has been detected for organic molecules on any surface. Here, we study single fluorescent terrylene molecules adsorbed on the surface of hexagonal boron-nitride (hBN) substrates. Our low-temperature results show for the first time the observation of the 0-0 ZPL of fluorescent molecules on a surface. With resonant excitation, we find 0-0 ZPL linewidths down to values that are about 10 times larger than the Fourier limit of 45 +/- 3 MHz, dictated by the fluorescence lifetime. We compare our results for molecules deposited on the surfaces of annealed and non-annealed hBN flakes and we see a marked improvement in the spectral stability of the emitters after annealing. Our high-resolution spectra obtained on terrylene suggest the possibility of employing hBN in combination with a wide variety of single molecule emitters for investigation of physical phenomena at surfaces or for use in nanophotonic devices.

physics.chem-ph↗

arXiv2020

Label-free Plasmonic Detection of Untethered Nanometer-sized Brownian Particles

Optical detection of individual nanometer-sized analytes, virus particles, and protein molecules holds great promise for understanding and control of biological samples and healthcare applications. As fluorescent labels impose restrictions on detection bandwidth and require lengthy and invasive processes, label-free optical techniques are highly desirable. Powerful label-free optical methods have recently emerged, such as interferometric scattering microscopy, plasmonic nanoparticle-based assays and microcavity-based assays. Although highly sensitive, these methods are so far restricted to integration times in excess of microseconds. This often imposes a requirement to impede analyte motion during these periods via specific molecular tethers, unspecific adsorption or confining arrangements. Here we introduce an optical technique capable of transforming gold nanorods commonly used as photostable labels into highly localized high-speed probes. Our method provides a time resolution well below microseconds. This mitigates the requirement for molecular tethers and allows us to detect single untethered nanoparticles in Brownian motion traversing sub atto-liter sensing volumes. Our method opens a novel gateway for the investigation of highly localized and highly dynamic nanoscale systems and constitutes a first step towards the label-free recognition of single untethered proteins.

physics.optics↗

arXiv2020

Laser-induced frequency tuning of Fourier-limited single-molecule emitters

The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single molecule scale, how a focused laser beam can locally shift by hundreds-time their natural linewidth and in a persistent way the transition frequency of organic chromophores, cooled at liquid helium temperatures in different host matrices. Supported by quantum chemistry calculations, the results are interpreted as effects of a photo-ionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental method is then applied to a common challenge in quantum photonics, i.e. the independent tuning and synchronization of close-by quantum emitters, which is desirable for multi-photon experiments. Five molecules that are spatially separated by about 50 microns and originally 20 GHz apart are brought into resonance within twice their linewidth. Combining this ability with an emission linewidth that is only limited by the spontaneous decay, the system enables fabrication-free, independent tuning of multiple molecules integrated on the same photonic chip.

quant-ph↗

arXiv2020

Effective electron temperature measurement using time-resolved anti-Stokes photoluminescence

Anti-Stokes photoluminescence of metal nanoparticles, in which emitted photons have a higher energy than the incident photons, is an indicator of the temperature prevalent within a nanoparticle. Previous work has shown how to extract the temperature from a gold nanoparticle under continuous-wave monochromatic illumination. We extend the technique to pulsed illumination and introduce pump-probe anti-Stokes spectroscopy. This new technique enables us not only to measure an effective electron temperature in a gold nanoparticle ($\sim 10^3$ K under our conditions), but also to measure ultrafast dynamics of a pulse-excited electron population, through its effect on the photoluminescence, with sub-picosecond time resolution. We measure the heating and cooling, all within picoseconds, of the electrons and find that, with our sub-picosecond pulses, the highest apparent temperature is reached $0.6$ ps before the maximum change in magnitude of the extinction signal

physics.optics↗

arXiv2019

Explosive, oscillatory, and Leidenfrost boiling at the nanoscale

We investigate the different boiling régimes around a single continuously laser-heated 80 nm gold nanoparticle and draw parallels to the classical picture of boiling. Initially, nanoscale boiling takes the form of transient, inertia-driven, unsustainable boiling events characteristic of a nanoscale boiling crisis. At higher heating power, nanoscale boiling is continuous, with a vapor film being sustained during heating for at least up to 20 $μ$s. Only at high heating powers does a substantial stable vapour nanobubble form. At intermediate heating powers, unstable boiling sometimes takes the form of remarkably stable nanobubble oscillations with frequencies between 40 MHz and 60 MHz; frequencies that are consistent with the relevant size scales according to the Rayleigh-Plesset model of bubble oscillation, though how applicable that model is to plasmonic vapor nanobubbles is not clear.

cond-mat.soft↗

arXiv2015

Design and synthesis of aromatic molecules for probing electric-fields at the nanoscale

We propose using halogenated organic dyes as nanoprobes for electric field and show their greatly enhanced Stark coefficients using density functional theory (DFT) calculations. We analyse halogenated variants of three molecules that have been of interest for cryogenic single molecule spectroscopy, perylene, terrylene, and dibenzoterrylene, with the zero-phonon optical transitions at blue, red, and near infrared. Out of all the combinations of halides and binding sites that are calculated, we have found that fluorination of the optimum binding site induces a dipole difference between ground and excited states larger than 0.5 D for all three molecules with the highest value of 0.69 D for fluoroperylene. We also report on synthesis of 3-fluoroterrylene and bulk spectroscopy of this compound in liquid and solid organic environments.

physics.chem-ph↗

arXiv2015

Fast, label-free tracking of single viruses and weakly scattering nanoparticles in a nano-fluidic optical fiber

High-speed tracking of single particles is a gateway to understanding physical, chemical, and biological processes at the nanoscale. It is also a major experimental challenge, particularly for small, nanometer-scale particles. Although methods such as confocal or fluorescence microscopy offer both high spatial resolution and high signal-to-background ratios, the fluorescence emission lifetime limits the measurement speed, while photobleaching and thermal diffusion limit the duration of measurements. Here we present a tracking method based on elastic light scattering that enables long-duration measurements of nanoparticle dynamics at rates of thousands of frames per second. We contain the particles within a single-mode silica fiber containing a sub-wavelength, nano-fluidic channel and illuminate them using the fiber's strongly confined optical mode. The diffusing particles in this cylinderical geometry are continuously illuminated inside the collection focal plane. We show that the method can track unlabeled dielectric particles as small as 20 nm as well as individual cowpea chlorotic mottle virus (CCMV) virions - 4.6 megadaltons in size - at rates of over 2 kHz for durations of tens of seconds. Our setup is easily incorporated into common optical microscopes and extends their detection range to nanometer-scale particles and macromolecules. The ease-of-use and performance of this technique support its potential for widespread applications in medical diagnostics and micro total analysis systems.

physics.optics↗

arXiv2015

Explosive Formation and Dynamics of Vapor Nanobubbles around a Continuously Heated Gold Nanosphere

We form sub-micrometer-sized vapor bubbles around a single laser heating gold nanoparticle in a liquid and monitor them through optical scattering of a probe laser. The fast, inertia-governed expansion is followed by a slower contraction and disappearance after some tens of nanoseconds. In a narrow range of illumination powers, bubble time traces show a clear echo signature. We attribute it to sound waves released upon the initial explosion and reflected by flat interfaces, hundreds of microns away from the particle. Echoes can trigger new explosions. A steady state of nanobubble with a vapor shell surrounding the heated nanoparticle can be reached by a proper time profile of the heating intensity. Stable nanobubbles could have original applications for light modulation and for enhanced optical-acoustic coupling in photoacoustic microscopy.

cond-mat.mes-hall↗

arXiv2014

Optical tracing of multiple charges in single-electron devices

Single molecules that exhibit narrow optical transitions at cryogenic temperatures can be used as local electric-field sensors. We derive the single charge sensitivity of aromatic organic dye molecules, based on first principles. Through numerical modeling, we demonstrate that by using currently available technologies it is possible to optically detect charging events in a granular network with a sensitivity better than $10^{-5}e/\sqrt{\textrm{Hz}}$ and track positions of multiple electrons, simultaneously, with nanometer spatial resolution. Our results pave the way for minimally-invasive optical inspection of electronic and spintronic nanodevices and building hybrid optoelectronic interfaces that function at both single-photon and single-electron levels.

cond-mat.mes-hall↗

arXiv2012

Optical detection of single non-absorbing molecules using the surface plasmon of a gold nanorod

Current optical detection schemes for single molecules require light absorption, either to produce fluorescence or direct absorption signals. This severely limits the range of molecules that can be detected, because most molecules are purely refractive. Metal nanoparticles or dielectric resonators detect non-absorbing molecules by a resonance shift in response to a local perturbation of the refractive index, but neither has reached single-protein sensitivity. The most sensitive plasmon sensors to date detect single molecules only when the plasmon shift is amplified by a highly polarizable label or by a localized precipitation reaction on the particle's surface. Without amplification, the sensitivity only allows for the statistical detection of single molecules. Here we demonstrate plasmonic detection of single molecules in realtime, without the need for labeling or amplification. We monitor the plasmon resonance of a single gold nanorod with a sensitive photothermal assay and achieve a ~ 700-fold increase in sensitivity compared to state-of-the-art plasmon sensors. We find that the sensitivity of the sensor is intrinsically limited due to spectral diffusion of the SPR. We believe this is the first optical technique that detects single molecules purely by their refractive index, without any need for photon absorption by the molecule. The small size, bio-compatibility and straightforward surface chemistry of gold nanorods may open the way to the selective and local detection of purely refractive proteins in live cells.

physics.chem-ph↗

arXiv2006

A Common-Path Interferometer for Time-Resolved and Shot-Noise-Limited Detection of Single Nanoparticles

We give a detailed description of a novel method for time-resolved experiments on single non-luminescent nanoparticles. The method is based on the combination of pump-probe spectroscopy and a common-path interferometer. In our interferometer, probe and reference arms are separated in time and polarization by a birefringent crystal. The interferometer, fully described by an analytical model, allows us to separately detect the real and imaginary contributions to the signal. We demonstrate the possibilities of the setup by time-resolved detection of single gold nanoparticles as small as 10 nm in diameter, and of acoustic oscillations of particles larger than 40 nm in diameter.

physics.optics↗

arXiv2005

Interferometric Time-Resolved Probing of Acoustic Modes in Single Gold Nanospheres

We measure the transient absorption of single gold particles with a common-path interferometer. The prompt electronic part of the signal provides high-contrast images for diameters as small as 10 nm. Mechanical vibrations of single particles appear on a longer timescale (period of 16 ps for 50 nm diameter). They reveal the full heterogeneity of the ensemble, and the intrinsic damping of the vibration. We also observe a lower-frequency mode involving shear. Ultra-fast pump-probe spectroscopy of individual particles opens new insight into mechanical properties of nanometer-sized objects.

cond-mat.other↗