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Nanosecond super-resolved imaging of a single cold atom by stimulated emission depletion microscopy

Zhong-Hua Qian, Jin‐Ming Cui, Xi-Wang Luo, Yong-Xiang Zheng, Yun‐Feng Huang, Ming-Zhong Ai, Ran He, Chuan‐Feng Li, Guang‐Can Guo

Published Apr 20, 2021• 1 citation
OpenAlex

Abstract

As one of the most critical methods for optical super-resolved microscopy, stimulated emission depletion (STED) microscopy has been widely applied in biological and chemical fields, leading to the Nobel prize of 2014 in chemistry. In cold atomic systems, fast and high-resolution microscopy of individual atoms is crucial since it can provide direct information on the dynamics and correlations of the system. Here, we demonstrate nanosecond two-dimensional snapshots of a single trapped ion beyond the optical diffraction limit, by combining the main idea of STED with the quantum state transition control in cold atoms. We achieve a spatial resolution up to 175 nm and a time resolution up to 50 ns simultaneously using a NA=0.1 objective in the experiment, which is improved over ten times compared to direct fluorescence imaging. To show the potential of this method, we applied it to record the motion of the trapped ion and observe one cycle of the secular motion of the ion with a displacement detection sensitivity of 10 nm. Our method provides a powerful tool for probing particles' positions, momenta and correlations, as well as their dynamics in cold atomic systems.

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Ultrahigh-contrast imaging by temporally modulated stimulated emission depletion

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Stimulated emission depletion (STED) is the key optical technology enabling super-resolution microscopy below the diffraction limit. Here, we demonstrate that modulation of STED in the time domain, combined with properly designed lock-in detection, can radically enhance the contrast of fluorescent images of strongly autofluorescent biotissues. In our experiments, the temporally modulated STED technique, implemented with low-intensity continuous-wave laser sources, is shown to provide an efficient all-optical suppression of a broadband fluorescent background, allowing the contrast of fluorescent images of mammal brain tissues tagged with nitrogen-vacancy diamond to be increased by five orders of magnitude.

Optics Letters•Feb 13, 2015•16 citations
As one of the most critical methods for optical super-resolved microscopy, stimulated emission depletion (STED) microscopy has been widely applied in biological and chemical fields, leading to the Nobel prize of 2014 in chemistry. In cold atomic systems, fast and high-resolution microscopy of individual atoms is crucial since it can provide direct information on the dynamics and correlations of the system. Here, we demonstrate nanosecond two-dimensional snapshots of a single trapped ion beyond the optical diffraction limit, by combining the main idea of STED with the quantum state transition control in cold atoms. We achieve a spatial resolution up to 175 nm and a time resolution up to 50 ns simultaneously using a NA=0.1 objective in the experiment, which is improved over ten times compared to direct fluorescence imaging. To show the potential of this method, we applied it to record the motion of the trapped ion and observe one cycle of the secular motion of the ion with a displacement detection sensitivity of 10 nm. Our method provides a powerful tool for probing particles' positions, momenta and correlations, as well as their dynamics in cold atomic systems.
In cold atomic systems, fast and high-resolution microscopy of individual atoms is crucial, since it can provide direct information on the dynamics and correlations of the system. Here, we demonstrate nanosecond-scale two-dimensional stroboscopic pictures of a single trapped ion beyond the optical diffraction limit, by combining the main idea of ground-state depletion microscopy with quantum-state transition control in cold atoms. We achieve a spatial resolution up to 175 nm using a NA=0.1 objective in the experiment, which represents a more than tenfold improvement compared with direct fluorescence imaging. To show the potential of this method, we apply it to observe the secular motion of the trapped ion; we demonstrate a temporal resolution up to 50 ns with a displacement detection sensitivity of 10 nm. Our method provides a powerful tool for probing particle positions, momenta, and correlations, as well as their dynamics in cold atomic systems.
Abstract Nonlinear depletion of fluorescence states by stimulated emission constitutes the basis of stimulated emission depletion (STED) microscopy. Despite significant efforts over the past decade, achieving super-resolution at low saturation intensities by STED remains a major technical challenge. By harnessing the surface quenching effect in NaGdF 4 :Yb/Tm nanocrystals, we report here high-efficiency emission depletion through surface migration. Using a dual-beam, continuous-wave laser manipulation scheme (975-nm excitation and 730-nm de-excitation), we achieved an emission depletion efficiency of over 95% and a low saturation intensity of 18.3 kW cm −2 . Emission depletion by surface migration through gadolinium sublattices enables super-resolution imaging with sub-20 nm lateral resolution. Our approach circumvents the fundamental limitation of high-intensity STED microscopy, providing autofluorescence-free, re-excitation-background-free imaging with a saturation intensity over three orders of magnitude lower than conventional fluorophores. We also demonstrated super-resolution imaging of actin filaments in Hela cells labeled with 8-nm nanoparticles. Combined with the highly photostable lanthanide luminescence, surface-migration emission depletion (SMED) could provide a powerful mechanism for low-power, super-resolution imaging or biological tracking as well as super-resolved optical sensing/writing and lithography.
This thesis presents the first application of the stimulated emission depletion (STED) technique to the field of single-molecule fluorescence spectroscopy. It is demonstrated that fluorescence quenching induced by STED is reversible and can be repeated a large number of cycles on a single molecule. Being ideal point-like probes, single molecules can therefore be used to characterize the resolution of STED microscopes. In a spectroscopic study, two simplifed models of the photophysical processes involved in STED are analyzed and applied to the experimental determination of the stimulated emission cross sections on a single-molecule level. In addition, the STED concept as applied in subdiffraction-resolution microscopy is transferred to fluorescence fluctuation spectroscopy. A successful implementation promises to expand the possibilities particularly of fluorescence correlation spectroscopy (FCS) which is already the most widely used fluctuation technique today but is restricted to concentrations on the nanomolar scale. Reducing the detection volume beyond the diffraction limit could render the micromolar range accessible and could thus open up new applications in the life sciences.
Nitrogen-vacancy (NV) color centers in nanodiamonds are highly promising for bioimaging and sensing. However, resolving individual NV centers within nanodiamond particles and the controlled addressing and readout of their spin state has remained a major challenge. Spatially stochastic super-resolution techniques cannot provide this capability in principle, whereas coordinate-controlled super-resolution imaging methods, like stimulated emission depletion (STED) microscopy, have been predicted to fail in nanodiamonds. Here we show that, contrary to these predictions, STED can resolve single NV centers in 40-250 nm sized nanodiamonds with a resolution of ≈10 nm. Even multiple adjacent NVs located in single nanodiamonds can be imaged individually down to relative distances of ≈15 nm. Far-field optical super-resolution of NVs inside nanodiamonds is highly relevant for bioimaging applications of these fluorescent nanolabels. The targeted addressing and readout of individual NV(-) spins inside nanodiamonds by STED should also be of high significance for quantum sensing and information applications.
Sub-micrometer light patterns play a pivotal role in biology, biophysics, and AMO physics, yet their in situ characterization is limited in spatial resolution and sensitivity. Here, we present an atom camera with a single ultracold atom in an optical tweezer as a scanning probe. Measuring the energy shift on the spin states with the long coherence time and polarization-sensitive transitions yields highly sensitive, high-resolution 2D imaging of both intensity and polarization ellipticity. We characterize the polarization of a tightly-focused beam, observing its non-trivial profile. The spatial resolution is fundamentally limited by the atom’s position uncertainty, suppressed down to quantum fluctuations (~25 nm) in the motional ground state of the tweezer, with an experimentally obtained upper bound of σ ≤ 96(4) nm. This method enables imaging beyond the diffraction limit, surpassing previous approaches limited by thermal fluctuations of the atom, and provides a powerful tool for designing and analyzing submicron-scale light patterns. In situ super-resolution imaging of light has inherent limitations when applied to the polarization profile. Here, the authors introduce an “atom camera” approach by means of a single tweezer-trapped 87Rb atom measuring the field-induced shifts at sub-micrometer steps, achieving resolution beyond the optical diffraction limit.
Stimulated emission depletion (STED) is the key optical technology enabling super-resolution microscopy below the diffraction limit. Here, we demonstrate that modulation of STED in the time domain, combined with properly designed lock-in detection, can radically enhance the contrast of fluorescent images of strongly autofluorescent biotissues. In our experiments, the temporally modulated STED technique, implemented with low-intensity continuous-wave laser sources, is shown to provide an efficient all-optical suppression of a broadband fluorescent background, allowing the contrast of fluorescent images of mammal brain tissues tagged with nitrogen-vacancy diamond to be increased by five orders of magnitude.