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The Journal of Physical Chemistry Letters

Quantum Coherent Modulation-Enhanced Single-Molecule Imaging Microscopy

Haitao Zhou, Chengbing Qin, Ruiyun Chen, Yaoming Liu, Wenjin Zhou, Guofeng Zhang, Yan Gao, Liantuan Xiao, Suotang Jia

Published Jan 1, 2019• 17 citations
Publisher

Abstract

In fluorescence imaging and detection, undesired fluorescence interference (such as autofluorescence) often hampers the contrast of the image and even prevents the identification of structures of interest. Here, we develop a quantum coherent modulation-enhanced (QCME) single-molecule imaging microscopy (SMIM) to substantially eliminate the strong fluorescence interference, based on manipulation of the excited-state population probability of a single molecule. By periodically modulating the phase difference between the ultrashort pulse pairs and performing a discrete Fourier transform of the arrival time of emitted photons, the decimation of single molecules from strong interference in QCME-SMIM has been clearly determined, where the signal-to-interference ratio is enhanced by more than 2 orders of magnitude. This technique, confirmed to be universal to organic dyes and linked with biomacromolecules, paves the way to high-contrast bioimaging under unfavorable conditions.

DOI
10.1021/acs.jpclett.8b03606

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In fluorescence imaging and detection, undesired fluorescence interference (such as autofluorescence) often hampers the contrast of the image and even prevents the identification of structures of interest. Here, we develop a quantum coherent modulation-enhanced (QCME) single-molecule imaging microscopy (SMIM) to substantially eliminate the strong fluorescence interference, based on manipulation of the excited-state population probability of a single molecule. By periodically modulating the phase difference between the ultrashort pulse pairs and performing a discrete Fourier transform of the arrival time of emitted photons, the decimation of single molecules from strong interference in QCME-SMIM has been clearly determined, where the signal-to-interference ratio is enhanced by more than 2 orders of magnitude. This technique, confirmed to be universal to organic dyes and linked with biomacromolecules, paves the way to high-contrast bioimaging under unfavorable conditions.
The classical optical diffraction limit can be overcome by exploiting the quantum properties of light in several theoretical studies; however, they mostly rely on an entangled light source. Recent experiments have demonstrated that quantum properties are preserved in many fluorophores, which makes it possible to add a new dimension of information for super-resolution fluorescence imaging. Here, we developed a statistical quantum coherence model for fluorescence emitters and proposed a new super-resolution method using fluorescence quantum coherence in fluorescence microscopy. In this study, by exploiting a single-photon avalanche detector (SPAD) array with a time-correlated single-photon-counting technique to perform spatial-temporal photon statistics of fluorescence coherence, the subdiffraction-limited spatial separation of emitters is obtained from the determined coherence. We numerically demonstrate an example of two-photon interference from two common fluorophores using an achievable experimental procedure. Our model provides a bridge between the macroscopic partial coherence theory and the microscopic dephasing and spectral diffusion mechanics of emitters. By fully taking advantage of the spatial-temporal fluctuations of the emitted photons as well as coherence, our quantum-enhanced imaging method has the significant potential to improve the resolution of fluorescence microscopy even when the detected signals are weak.
ObjectiveCellular temperature imaging can assist scientists in studying and comprehending the temperature distribution within cells, revealing critical information about cellular metabolism and biochemical processes. Currently, cell temperature imaging techniques based on fluorescent temperature probes suffer from limitations such as low temperature resolution and a limited measurement range. This paper aims to develop a single-cell temperature imaging and real-time monitoring technique by leveraging the temperature-dependent properties of single-molecule quantum coherence processes.MethodsUsing femtosecond pulse lasers, we prepare delayed and phase-adjustable pairs of femtosecond pulses. These modulated pulse pairs excite fluorescent single molecules labeled within cells through a microscopic system, followed by the collection and recording of the arrival time of each fluorescent photon. By defining the quantum coherence visibility (V) of single molecules in relation to the surrounding environmental temperature, a correspondence between V and environmental temperature is established. By modulating and demodulating the arrival times of fluorescent photons, we obtain the local temperature of single molecules. Combined with scanning imaging, we finally achieve temperature imaging and real-time detection of cells.ResultsThis method achieves high precision (temperature resolution <0.1°C) and a wide temperature range (10-50°C) for temperature imaging and measurement, and it enables the observation of temperature changes related to individual cell metabolism.ConclusionThis research contributes to a deeper understanding of cellular metabolism, protein function, and disease mechanisms, providing a valuable tool for biomedical research.
Technological advancements in the creation, manipulation and detection of quantum states of light have motivated the application of such states to overcome classical limits in sensing and imaging. In particular, there has been a surge of recent interest in super-resolution imaging based on principles of quantum optics. However, the application of such schemes for practical imaging of biological samples is demanding in terms of signal-to-noise ratio, speed of acquisition and robustness with respect to sample labeling. Here, we re-introduce the concept of quantum image scanning microscopy (Q-ISM), a super-resolution method that enhances the classical image scanning microscopy (ISM) method by measuring photon correlations. Q-ISM was already utilized to achieve super-resolved images of a biological sample labeled with fluorescent nanoscrystals whose contrast is based entirely on a quantum optical phenomenon, photon antibunching. We present here an experimental demonstration of the method and discuss with further details its prospects for application in life science microscopy.
Nonlinear optical microscopy techniques have emerged as a set of successful tools for biological imaging. Stimulated emission microscopy belongs to a small subset of pump–probe techniques, which can image non-fluorescent samples without requiring fluorescent labeling. However, its sensitivity has been shown to be ultimately limited by the quantum fluctuations in the probe beam. We propose and experimentally implement sub-shot-noise limited stimulated emission microscopy by preparing the probe pulse in an intensity-squeezed state. This technique paves the way for imaging delicate biological samples that have no detectable fluorescence with sensitivity beyond standard quantum fluctuations.
Nonlinear optical microscopy techniques have emerged as a set of successful tools for biological imaging. Stimulated emission microscopy belongs to a small subset of pump-probe techniques which can image non-fluorescent samples without requiring fluorescent labelling. However, its sensitivity has been shown to be ultimately limited by the quantum fluctuations in the probe beam. We propose and experimentally implement sub-shot-noise limited stimulated emission microscopy by preparing the probe pulse in an intensity-squeezed state. This technique paves the way for imaging delicate biological samples that have no detectable fluorescence with sensitivity beyond standard quantum fluctuations.