Visualizing Quantum Coherence Based on Single-Molecule Coherent Modulation Microscopy

Abstract

Massive magical phenomena in nature are closely related to quantum effects at the microscopic scale. However, the lack of straightforward methods to observe the quantum coherent dynamics in integrated biological systems limits the study of essential biological mechanisms. In this work, we developed a single-molecule coherent modulation (SMCM) microscopy by combining the superior features of single-molecule microscopy with ultrafast spectroscopy. By introducing the modem technology and defining the coherent visibility, we realized visualization and real-time observation of the decoherence process of a single molecule influenced by the microenvironment for the first time. In particular, we applied this technique to observe the quantum coherent properties of the entire chlorella cells and found the correlation between the coherent visibility and metabolic activities, which may have potential applications in molecular diagnostics and precision medicine.

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

“…It is worthwhile to consider the two-pulse variant of populationdetected spectroscopy, that is phase-locked double-pump population-detected spectroscopy, in some detail. This technique, pioneered in femtosecond ensemble molecular spectroscopy by Scherer and co-workers, 674 was extended to single-molecule spectroscopy by van Hulst and co-workers 540,675 and to single-molecule microscopy by Fujiwara 676 and Zhou et al 677,678 Double-pump population-detected signals were simulated for a number of systems, from molecules 552−554,679−682 to antenna complexes. 683−685 These signals can be calculated via eq 44 through the numerical solution of driven TDSEs or MEs with a system−field interaction Hamiltonian containing two pump pulses separated by the time delay τ.…”

“…It is worthwhile to consider the two-pulse variant of population-detected spectroscopy, that is phase-locked double-pump population-detected spectroscopy, in some detail. This technique, pioneered in femtosecond ensemble molecular spectroscopy by Scherer and co-workers, was extended to single-molecule spectroscopy by van Hulst and co-workers , and to single-molecule microscopy by Fujiwara and Zhou et al , Double-pump population-detected signals were simulated for a number of systems, from molecules − ,− to antenna complexes. − These signals can be calculated via eq through the numerical solution of driven TDSEs or MEs with a system–field interaction Hamiltonian containing two pump pulses separated by the time delay τ. It is not necessary to perform a phase decomposition of the double-pump population-detected signal, because it can be conveniently decomposed into population and coherence contributions. , If, for example, the pump pulses are temporally well separated and contributions from the states of manifold {II} can be neglected, the DW approximation yields the double-pump population-detected signal in the form S ( τ ) = A ( τ ) + ( B false( τ false) e i φ + B * false( τ false) e − i φ ) e − γ τ Here A (τ) is the contribution which results from the evolution of the chromophore in electronic population, B (τ) is the coherence contribution, φ is the relative phase of the pump pulses, and γ is the electronic dephasing rate.…”

Computer Vision Analysis on Material Characterization Images

“…The optical system of OM uses the visible light and lens coefficient to magnify and image tiny objects. [1][2][3] The object passes through the objective lens to form a magnified real image, and then passes through the eyepiece to form a magnified virtual image. OM observe selected cross sections of transparent materials without slicing the samples.…”

“…It can be real-time and dynamic observation, and occupies a dominant position in the field of biology. [2,3] However, the diffraction limit of an OM is limited to 1000Â amplification and 200 nm resolution.…”

“…OM takes advantage of visible-light imaging, whose resolution is at the micrometer level and sample preparation is fast and simple. [1][2][3] The electron microscopes use shorter wavelength electron beam imaging, and its resolution can reach the nanometer level. Among them, SEM fine electron beam imaging can obtain the surface morphology and composition information of samples.…”