Photoisomerization transition state manipulation by entangled two-photon absorption

2021 ◽  
Vol 118 (47) ◽  
pp. e2116868118
Author(s):  
Bing Gu ◽  
Daniel Keefer ◽  
Flavia Aleotti ◽  
Artur Nenov ◽  
Marco Garavelli ◽  
...  
Keyword(s):  
Wave Packet ◽  
Transition State ◽  
Product Yield ◽  
Photochemical Reactions ◽  
Photon Absorption ◽  
Conical Intersection ◽  
Two Photon ◽  
Wave Packet Dynamics ◽  
Photon Excitation ◽  
Two Photon Excitation

We demonstrate how two-photon excitation with quantum light can influence elementary photochemical events. The azobenzene trans → cis isomerization following entangled two-photon excitation is simulated using quantum nuclear wave packet dynamics. Photon entanglement modulates the nuclear wave packets by coherently controlling the transition pathways. The photochemical transition state during passage of the reactive conical intersection in azobenzene photoisomerization is strongly affected with a noticeable alteration of the product yield. Quantum entanglement thus provides a novel control knob for photochemical reactions. The distribution of the vibronic coherences during the conical intersection passage strongly depends on the shape of the initial wave packet created upon quantum light excitation. X-ray signals that can experimentally monitor this coherence are simulated.

Two-Photon Excitation Imaging of Glucose Metabolism in Living Tissue

1997 ◽  
Vol 3 (S2) ◽  
pp. 305-306
Author(s):  
David W. Piston
Keyword(s):  
Confocal Microscopy ◽  
Collection Efficiency ◽  
Three Dimensional ◽  
Spatial Filter ◽  
Input Power ◽  
Photon Absorption ◽  
Focal Volume ◽  
Two Photon ◽  
Photon Excitation ◽  
Two Photon Excitation

Two-photon excitation microscopy (TPEM) provides attractive advantages over confocal microscopy for three-dimensionally resolved fluorescence imaging and photochemistry. It provides three-dimensional resolution and eliminates background equivalent to an ideal confocal microscope without requiring a confocal spatial filter, whose absence enhances fluorescence collection efficiency. This results in inherent submicron optical sectioning by excitation alone. In practice, TPEM is made possible by the very high local instantaneous intensity provided by a combination of diffraction-limited focusing of a single laser beam in the microscope and the temporal concentration of 100 femtosecond pulses generated by a mode-locked laser. Resultant peak excitation intensities are 106 times greater than the CW intensities used in confocal microscopy, but the pulse duty cycle of 10−5 limits the average input power to less than 10 mW, only slightly greater than the power normally used in confocal microscopy. Because of the intensity-squared dependence of the two-photon absorption, the excitation is limited to the focal volume.

scholarly journals Two-Photon–NIR-II Antimicrobial Graphene-Nanoagent for Ultraviolet–NIR Imaging and Photoinactivation

2021 ◽  
Author(s):  
WEN-SHUO KUO ◽  
Chia-Yuan Chang ◽  
Ping-Ching Wu ◽  
Jiu-Yao Wang
Keyword(s):  
Photodynamic Therapy ◽  
Quantum Yield ◽  
Chemical Modification ◽  
Near Infrared ◽  
Photon Absorption ◽  
Excitation Wavelength ◽  
Strong Electron ◽  
Two Photon ◽  
Photon Excitation ◽  
Two Photon Excitation

Abstract BackgroundNitrogen doping and amino-group functionalization, which result in strong electron donation, can be achieved through chemical modification. Large π-conjugated systems of graphene quantum dot (GQD)-based materials acting as electron donors can be chemically manipulated with low two-photon excitation energy in a short photoexcitation time for improving the charge transfer efficiency of sorted nitrogen-doped amino acid–functionalized GQDs (sorted amino-N-GQDs). ResultsIn this study, a self-developed femtosecond Ti-sapphire laser optical system (222.7 nJ pixel−1 with 100-170 scans, approximately 0.65-1.11 s of total effective exposure times; excitation wavelength: 960 nm in the near-infrared II region) was used for chemical modification. The sorted amino-N-GQDs exhibited enhanced two-photon absorption, post-two-photon excitation stability, two-photon excitation cross-section, and two-photon luminescence through the radiative pathway. The lifetime and quantum yield of the sorted amino-N-GQDs decreased and increased, respectively. Furthermore, the sorted amino-N-GQDs exhibited excitation-wavelength-independent photoluminescence in the near-infrared region and generated reactive oxygen species after two-photon excitation. An increase in the size of the sorted amino-N-GQDs boosted photochemical and electrochemical efficacy and resulted in high photoluminescence quantum yield and highly efficient two-photon photodynamic therapy. ConclusionThe sorted dots can be used in two-photon contrast probes for tracking and localizing analytes during two-photon imaging in a biological environment and for conducting two-photon photodynamic therapy for eliminating infectious microbes.

Two-photon excitation spectroscopy of photosynthetic light-harvesting complexes and pigments

2019 ◽  
Vol 216 ◽  
pp. 494-506 ◽  
Author(s):  
Alexander Betke ◽  
Heiko Lokstein
Keyword(s):  
Spectral Region ◽  
Protein Complexes ◽  
Photosynthetic Pigment ◽  
Photon Absorption ◽  
Light Harvesting Complexes ◽  
Two Photon Absorption ◽  
Two Photon ◽  
Photon Excitation ◽  
Pigment Protein Complexes ◽  
Two Photon Excitation

Two-photon excitation (TPE) profiles of LHCII samples containing different xanthophyll complements were measured in the presumed 11Ag− → 21Ag− (S0 → S1) transition region of xanthophylls. Additionally, TPE profiles of Chls a and b in solution and of WSCP, which does not contain carotenoids, were measured. The results indicate that direct two-photon absorption by Chls in the presumed S0 → S1 transition spectral region of carotenoids is dominant over that of carotenoids, with negligible contributions of the latter. These results suggest the re-evaluation of previously published TPE data obtained with photosynthetic pigment–protein complexes containing (B)Chls and carotenoids.

Two-Photon Excitation of Potentiometric Probes Enables Optical Recording of Action Potentials From Mammalian Nerve Terminals In Situ

2008 ◽  
Vol 99 (3) ◽  
pp. 1545-1553 ◽  
Author(s):  
Jonathan A. N. Fisher ◽  
Jonathan R. Barchi ◽  
Cristin G. Welle ◽  
Gi-Ho Kim ◽  
Paul Kosterin ◽  
...  
Keyword(s):  
Action Potentials ◽  
Optical Recording ◽  
Photon Absorption ◽  
Nerve Terminals ◽  
Electrode Arrays ◽  
Two Photon ◽  
Photon Excitation ◽  
Mammalian Nerve ◽  
Two Photon Excitation

We report the first optical recordings of action potentials, in single trials, from one or a few (∼1–2 μm) mammalian nerve terminals in an intact in vitro preparation, the mouse neurohypophysis. The measurements used two-photon excitation along the “blue” edge of the two-photon absorption spectrum of di-3-ANEPPDHQ (a fluorescent voltage-sensitive naphthyl styryl-pyridinium dye), and epifluorescence detection, a configuration that is critical for noninvasive recording of electrical activity from intact brains. Single-trial recordings of action potentials exhibited signal-to-noise ratios of ∼5:1 and fractional fluorescence changes of up to ∼10%. This method, by virtue of its optical sectioning capability, deep tissue penetration, and efficient epifluorescence detection, offers clear advantages over linear, as well as other nonlinear optical techniques used to monitor voltage changes in localized neuronal regions, and provides an alternative to invasive electrode arrays for studying neuronal systems in vivo.

scholarly journals Dual Near Infrared Two-Photon Microscopy for Deep-Tissue Dopamine Nanosensor Imaging

2017 ◽  
Author(s):  
Jackson T. Del Bonis-O’Donnell ◽  
Ralph H. Page ◽  
Abraham G. Beyene ◽  
Eric G. Tindall ◽  
Ian McFarlane ◽  
...  
Keyword(s):  
Near Infrared ◽  
Photon Absorption ◽  
Deep Tissue ◽  
Biologically Relevant ◽  
Two Photon Microscopy ◽  
Two Photon ◽  
Tissue Phantom ◽  
Photon Excitation ◽  
Photon Absorption And Scattering ◽  
Two Photon Excitation

A key limitation for achieving deep imaging in biological structures lies in photon absorption and scattering leading to attenuation of fluorescence. In particular, neurotransmitter imaging is challenging in the biologically-relevant context of the intact brain, for which photons must traverse the cranium, skin and bone. Thus, fluorescence imaging is limited to the surface cortical layers of the brain, only achievable with craniotomy. Herein, we describe optimal excitation and emission wavelengths for through-cranium imaging, and demonstrate that near-infrared emissive nanosensors can be photoexcited using a two-photon 1560 nm excitation source. Dopamine-sensitive nanosensors can undergo two-photon excitation, and provide chirality-dependent responses selective for dopamine with fluorescent turn-on responses varying between 20% and 350%. We further calculate the two-photon absorption cross-section and quantum yield of dopamine nanosensors, and confirm a two-photon power law relationship for the nanosensor excitation process. Finally, we show improved image quality of the nanosensors embedded 2 mm deep into a brain-mimetic tissue phantom, whereby one-photon excitation yields 42% scattering, in contrast to 4% scattering when the same object is imaged under two-photon excitation. Our approach overcomes traditional limitations in deep-tissue fluorescence microscopy, and can enable neurotransmitter imaging in the biologically-relevant milieu of the intact and living brain.

Application of two-photon chromophore excitation to laser scanning microscopy

1991 ◽  
Vol 49 ◽  
pp. 404-405
Author(s):  
David W. Piston ◽  
James H. Strickler ◽  
Watt W. Webb
Keyword(s):  
Laser Scanning ◽  
Uv Light ◽  
Excited Electronic State ◽  
Laser Scanning Confocal Microscopy ◽  
Photochemical Reactions ◽  
Laser Scanning Microscopy ◽  
Scanning Confocal Microscopy ◽  
Two Photon ◽  
Photon Excitation ◽  
Two Photon Excitation

The non-linear optical technique of two-photon excitation of fluorescence and photochemical reactions makes possible new applications that are not possible using linear one-photon excitation in laser scanning confocal microscopy. The two-photon excitation effect arises from the simultaneous absorption of two red photons, which causes the transition to an excited electronic state with its normal absorption in the ultraviolet. In our fluorescence experiments, this excited state is the same singlet state, S1, that is populated during a conventional fluorescence experiment, and thus exhibits the same emission properties (e.g. wavelength shifts, environmental sensitivity) that are observed in typical biological microscopy studies. Likewise, photochemical reactions such as light induced polymerization and photolytic uncaging that are normally catalyzed by UV light can be generated using two-photon excitation. In practice, twophoton excitation is made possible by the very high local instantaneous intensity that is provided by a combination of the diffraction limited focusing in the microscope and the temporal concentration of a subpicosecond mode-locked laser.

UV-excited fluorophore images obtained with IR excitation

1996 ◽  
Vol 54 ◽  
pp. 906-907
Author(s):  
D. Wokosin ◽  
V.F. Centonze ◽  
J.G. White
Keyword(s):  
Short Pulse ◽  
Argon Laser ◽  
Confocal Imaging ◽  
Photon Absorption ◽  
Focal Volume ◽  
Two Photon ◽  
Photon Excitation ◽  
Biological Studies ◽  
Short Pulse Lasers ◽  
Two Photon Excitation

The widespread use of two-photon excitation fluorescence imaging has been somewhat inhibited by the necessity to use large, expensive, high-power, short-pulse lasers. These ultra-short pulse lasers are used as an excitation source in a raster scanning configuration to provide sufficient peak power density in a lens focal volume to generate detectable two-photon absorption events for rapid imaging. Biological studies often benefit from multiple fluorescent labels and multi-labelled samples often require different excitation wavelengths for adequate excitation of the various colored fluorophores. This is achieved inexpensively with the three Krypton Argon laser lines in standard confocal imaging systems, but multiple two-photon excitation lasers--if available-- would be a very expensive system. The lasers commonly used for two-photon imaging are tuneable, but this is not a non-trivial and time consuming process. The tuning range on these lasers allows good access to the blue-emitting and green-emitting fluorophores via two-photon excitation; however, we have found that a fixed-wavelength, compact,

Two-Photon Excitation Microscopy in Cellular Biophysics

1996 ◽  
Vol 54 ◽  
pp. 276-277
Author(s):  
David W. Piston
Keyword(s):  
Confocal Microscopy ◽  
Living Cells ◽  
Input Power ◽  
Photon Absorption ◽  
Infrared Light ◽  
Focal Volume ◽  
Excitation Light ◽  
Two Photon ◽  
Photon Excitation ◽  
Two Photon Excitation

Two-photon excitation microscopy (TPEM) provides attractive advantages over confocal microscopy for three-dimensionally resolved fluorescence imaging and photochemistry. Two-photon excitation arises from the simultaneous absorption of two photons in a single quantitized event whose probability is proportional to the square of the instantaneous intensity. For example, two red photons can cause the transition to an excited electronic state normally reached by absorption in the ultraviolet. In practice, two-photon excitation is made possible by the very high local instantaneous intensity provided by a combination of diffraction-limited focusing of a single laser beam in the microscope and the temporal concentration of 100 femtosecond pulses generated by a mode-locked laser. Resultant peak excitation intensities are 106 times greater than the CW intensities used in confocal microscopy, but the pulse duty cycle of 10 5 limits the average input power to less than 10 mW, only slightly greater than the power normally used in confocal microscopy.Three properties TPEM give this method a tremendous advantage over conventional optical sectioning microscopies for the study of thick samples: 1) The excitation is limited to the focal volume because of the intensity-squared dependence of the two-photon absorption. This inherent localization provides three-dimensional resolution and eliminates background equivalent to an ideal confocal microscope without requiring a confocal spatial filter, whose absence enhances fluorescence collection efficiency. Confinement of excitation to the focal volume also minimizes photobleaching and photo damage - the ultimate limiting factors in fluorescence microscopy of living cells and tissues. 2) The two-photon technique allows imaging of UV fluorophores with conventional visible light optics in both the scanning and imaging systems, because both the red excitation light (~700 nm) and the blue fluorescence (>400 nm) are within the visible spectrum. 3) Red or infrared light is far less damaging to most living cells and tissues than bluer light because fewer biological molecules absorb at the higher wavelengths. Longer wavelength excitation also reduces scattering of the incident light by the specimen, thus allowing more of the input power to reach the focal plane. This relative transparency of biological specimens to 700 nm light permits deeper sectioning, since both absorbance and scattering are reduced.

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