Photoisomerization transition state manipulation by entangled two-photon absorption

Gu, Bing; Keefer, Daniel; Aleotti, Flavia; Nenov, Artur; Garavelli, Marco; Mukamel, Shaul

doi:10.1073/pnas.2116868118

Title: Photoisomerization transition state manipulation by entangled two-photon absorption

Abstract

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.

Authors:

Gu, Bing ^[1];

^[1];

^[2]; Nenov, Artur ^[2];

^[2];

^[1]

Department of Chemistry, University of California, Irvine, CA 92697,, Department of Physics &, Astronomy, University of California, Irvine, CA 92697,
Dipartimento di Chimica Industriale “Toso Montanari”, Università degli studi di Bologna, 40136 Bologna, Italy

Publication Date:: Fri Nov 19 00:00:00 EST 2021

Research Org.:: Univ. of California, Irvine, CA (United States)

Sponsoring Org.:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF); Alexander von Humboldt Foundation

OSTI Identifier:: 1831557

Alternate Identifier(s):: OSTI ID: 1979164

Grant/Contract Number:: SC0019484; CHE-1953045

Resource Type:: Published Article

Journal Name:: Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:: Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 118 Journal Issue: 47; Journal ID: ISSN 0027-8424

Publisher:: Proceedings of the National Academy of Sciences

Country of Publication:: United States

Language:: English

Subject:: 54 ENVIRONMENTAL SCIENCES; entangled photons; two-photon absorption; photoisomerization; azobenzene; wave packets

Citation Formats


                    Gu, Bing, Keefer, Daniel, Aleotti, Flavia, Nenov, Artur, Garavelli, Marco, and Mukamel, Shaul. Photoisomerization transition state manipulation by entangled two-photon absorption.  United States: N. p., 2021. 
Web.  doi:10.1073/pnas.2116868118.

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                    Gu, Bing, Keefer, Daniel, Aleotti, Flavia, Nenov, Artur, Garavelli, Marco, & Mukamel, Shaul. Photoisomerization transition state manipulation by entangled two-photon absorption.  United States.  https://doi.org/10.1073/pnas.2116868118

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                    Gu, Bing, Keefer, Daniel, Aleotti, Flavia, Nenov, Artur, Garavelli, Marco, and Mukamel, Shaul. Fri .  
"Photoisomerization transition state manipulation by entangled two-photon absorption".  United States.  https://doi.org/10.1073/pnas.2116868118.

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@article{osti_1831557,

  title        = {Photoisomerization transition state manipulation by entangled two-photon absorption},

  author       = {Gu, Bing and Keefer, Daniel and Aleotti, Flavia and Nenov, Artur and Garavelli, Marco and Mukamel, Shaul},

  abstractNote = {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.},

  doi          = {10.1073/pnas.2116868118},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 47,

  volume       = 118,

  place        = {United States},

  year         = {Fri Nov 19 00:00:00 EST 2021},

  month        = {Fri Nov 19 00:00:00 EST 2021}

}

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Title: Photoisomerization transition state manipulation by entangled two-photon absorption

Abstract

Citation Formats

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Quantum interference in the presence of a resonant medium journal, September 2017

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Functional patterned multiphoton excitation deep inside scattering tissue journal, February 2013

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Squeezed light induced two-photon absorption fluorescence of fluorescein biomarkers journal, June 2020

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Two-Photon Fluorescence Microscopy at Extremely Low Excitation Intensity: The Power of Quantum Correlations journal, July 2020

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Entangled Photon-Pair Two-Dimensional Fluorescence Spectroscopy (EPP-2DFS) journal, September 2013

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Theory of two-photon entanglement in type-II optical parametric down-conversion
journal, December 1994

Terahertz quantum plasmonics at nanoscales and angstrom scales
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Enlightening Materials with Photoswitches
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journal, September 2017

Designing high-power, octave spanning entangled photon sources for quantum spectroscopy
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Nonadiabatic Dynamics Simulation of the Wavelength-Dependent Photochemistry of Azobenzene Excited to the nπ* and ππ* Excited States
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journal, April 1989

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journal, July 2020

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journal, January 2021

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journal, January 2020

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journal, April 2015

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journal, February 2015

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Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
journal, January 2021

Manipulating Two-Photon-Absorption of Cavity Polaritons by Entangled Light
journal, September 2020

Mechanism and Dynamics of Azobenzene Photoisomerization
journal, July 2003

Investigations of Thienoacene Molecules for Classical and Entangled Two-Photon Absorption
journal, September 2018

Femtosecond photoisomerization of cis-azobenzene
journal, July 1997

Multidimensional Potential Energy Surfaces Resolved at the RASPT2 Level for Accurate Photoinduced Isomerization Dynamics of Azobenzene
journal, October 2019

Spontaneous parametric down-conversion
journal, July 2018

Observing the transition from quantum to classical energy correlations with photon pairs
journal, June 2018

Entangled Two-Photon Absorption Spectroscopy
journal, August 2018

Two-photon absorption and two-photon-induced isomerization of azobenzene compounds
journal, January 2020

Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating
journal, September 1997

Imaging conical intersection dynamics during azobenzene photoisomerization by ultrafast X-ray diffraction
journal, January 2021

Enhanced Two‐Photon Absorption of Organic Chromophores: Theoretical and Experimental Assessments
journal, December 2008

Spatial correlations in parametric down-conversion
journal, October 2010

Intrapulse Dynamical Effects in Multiphoton Processes: Theoretical Analysis
journal, June 1998

Entangling Macroscopic Oscillators Exploiting Radiation Pressure
journal, March 2002

Entangled Photon-Pair Two-Dimensional Fluorescence Spectroscopy (EPP-2DFS)
journal, September 2013

Two-photon laser scanning fluorescence microscopy
journal, April 1990