Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy

Kobayashi, Yuki; Leone, Stephen R.

doi:10.1063/5.0119942

Title: Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy

Abstract

Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials, and so with the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.

Authors:

^[1];

^[2]

SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford University, CA (United States); University of California, Berkeley, CA (United States)
University of California, Berkeley, CA (United States):Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Publication Date:: Tue Nov 08 00:00:00 EST 2022

Research Org.:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); Stanford University; USDOE

OSTI Identifier:: 1908925

Alternate Identifier(s):: OSTI ID: 1897585

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; FA9550-19-1-0314; FA9550-20-1-0334; CHE-1951317

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 157; Journal Issue: 18; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Kobayashi, Yuki, and Leone, Stephen R. Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy.  United States: N. p., 2022. 
Web.  doi:10.1063/5.0119942.

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                    Kobayashi, Yuki, & Leone, Stephen R. Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy.  United States.  https://doi.org/10.1063/5.0119942

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                    Kobayashi, Yuki, and Leone, Stephen R. Tue .  
"Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy".  United States.  https://doi.org/10.1063/5.0119942.  https://www.osti.gov/servlets/purl/1908925.

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@article{osti_1908925,

  title        = {Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy},

  author       = {Kobayashi, Yuki and Leone, Stephen R.},

  abstractNote = {Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials, and so with the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.},

  doi          = {10.1063/5.0119942},

  journal      = {Journal of Chemical Physics},

  number       = 18,

  volume       = 157,

  place        = {United States},

  year         = {Tue Nov 08 00:00:00 EST 2022},

  month        = {Tue Nov 08 00:00:00 EST 2022}

}

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Catching Conical Intersections in the Act: Monitoring Transient Electronic Coherences by Attosecond Stimulated X-Ray Raman Signals
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Kowalewski, Markus; Bennett, Kochise; Dorfman, Konstantin E.
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Kobayashi, Yuki; Reduzzi, Maurizio; Chang, Kristina F.
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Attosecond state-resolved carrier motion in quantum materials probed by soft x-ray XANES
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Buades, Bárbara; Picón, Antonio; Berger, Emma
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Peng, Peng; Mi, Yonghao; Lytova, Marianna
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Attosecond XUV probing of vibronic quantum superpositions in ${Br}_{2}^{+}$
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Real-time observation of electronic, vibrational, and rotational dynamics in nitric oxide with attosecond soft x-ray pulses at 400 eV
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Title: Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy

Abstract

Citation Formats

Real‐time femtosecond probing of ‘‘transition states’’ in chemical reactions journal, August 1987

Probing electron-hole coherence in strongly driven 2D materials using high-harmonic generation journal, May 2022

Attosecond transient-absorption dynamics of xenon core-excited states in a strong driving field journal, March 2017

Attosecond molecular dynamics: fact or fiction? journal, February 2014

Essential entanglement for atomic and molecular physics journal, September 2011

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Colloquium : Excitons in atomically thin transition metal dichalcogenides journal, April 2018

Colloquium : Strong-field phenomena in periodic systems journal, April 2018

Wave‐packet dynamics in the Li2 E(1Σ+g) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state journal, November 1995

Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses journal, September 2021

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Attosecond science based on high harmonic generation from gases and solids journal, June 2020

Revealing electronic state-switching at conical intersections in alkyl iodides by ultrafast XUV transient absorption spectroscopy journal, August 2020

Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal, April 2007

Ultrafast dynamics in van der Waals heterostructures journal, November 2018

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration journal, February 2022

Measurement and laser control of attosecond charge migration in ionized iodoacetylene journal, October 2015

Comparison of Electronic and Vibrational Coherence Measured by Two-Dimensional Electronic Spectroscopy journal, July 2011

De- and Recoherence of Charge Migration in Ionized Iodoacetylene journal, July 2019

Coupled valence carrier and core-exciton dynamics in WS 2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy journal, August 2021

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium journal, June 2017

Conical intersection and coherent vibrational dynamics in alkyl iodides captured by attosecond transient absorption spectroscopy journal, March 2022

Characterization of vibrational wave packets by core-level high-harmonic transient absorption spectroscopy journal, August 2013

Extreme-ultraviolet refractive optics journal, November 2018

Elucidating the origins of multimode vibrational coherences of polyatomic molecules induced by intense laser fields journal, September 2017

Control of Nuclear Dynamics through Conical Intersections and Electronic Coherences journal, March 2018

Quantum coherences reveal excited-state dynamics in biophysical systems journal, June 2019

Attosecond spectroscopy of liquid water journal, August 2020

Charge Migration in Propiolic Acid: A Full Quantum Dynamical Study journal, November 2018

Generation of deep ultraviolet sub-2-fs pulses journal, March 2019

Generation of optical Schrödinger cat states in intense laser–matter interactions journal, August 2021

What will it take to observe processes in 'real time'? journal, February 2014

Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study journal, May 2021

Adaptive strong-field control of chemical dynamics guided by three-dimensional momentum imaging journal, December 2013

State-resolved attosecond reversible and irreversible dynamics in strong optical fields journal, February 2017

Quantum coherence in molecular photoionization journal, January 2022

Real-time observation of valence electron motion journal, August 2010

Probing coherently excited optical phonons by extreme ultraviolet radiation with femtosecond time resolution journal, July 2008

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide journal, May 2020

Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy journal, November 2019

BEYOND BORN-OPPENHEIMER: Molecular Dynamics Through a Conical Intersection journal, June 2004

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction journal, April 2017

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe 2 with Femtosecond Core-Level Spectroscopy journal, October 2020

Visualizing coherent vibrational motion in the molecular iodine B3Π0+u state using ultrafast XUV transient-absorption spectroscopy journal, August 2021

Atomically Thin MoS2 A New Direct-Gap Semiconductor journal, September 2010

Sub-7-femtosecond conical-intersection dynamics probed at the carbon K-edge journal, January 2021

Charge migration and charge transfer in molecular systems journal, November 2017

Charge directed reactivity: journal, March 1998

The Birth of Attochemistry journal, January 2019

Entanglement and coherence in photoionization of H2 by an ultrashort XUV laser pulse journal, July 2019

Coherent ultrafast charge transfer in an organic photovoltaic blend journal, May 2014

Excited-state vibronic wave-packet dynamics in H 2 probed by XUV transient four-wave mixing journal, February 2018

Origin of Long-Lived Coherences in Light-Harvesting Complexes journal, June 2012

Attosecond band-gap dynamics in silicon journal, December 2014

NaI revisited: Theoretical investigation of predissociation via ultrafast XUV transient absorption spectroscopy journal, November 2019

High-harmonic generation from solids journal, November 2018

Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy journal, July 2019

Translational, rotational and vibrational relaxation dynamics of a solute molecule in a non-interacting solvent journal, July 2016

Ab initio investigation of Br-3 d core-excited states in HBr and HBr + toward XUV probing of photochemical dynamics journal, January 2019

Observation of high-order harmonic generation in a bulk crystal journal, December 2010

Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source journal, January 2017

Control of Electron Localization in Molecular Dissociation journal, April 2006

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Using coherence to enhance function in chemical and biophysical systems journal, March 2017

Spin–Orbit State-Selective C–I Dissociation Dynamics of the CH 3 I + X̃ Electronic State Induced by Intense Few-Cycle Laser Fields journal, December 2017

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Attosecond physics journal, February 2009

Entanglement between electronic and vibrational degrees of freedom in a laser-driven molecular system journal, December 2013

Attosecond chirp compensation in water window by plasma dispersion journal, January 2018

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond journal, August 2016

Theoretical Analysis of High-Harmonic Generation in Solids journal, August 2014

Isomerization Through Conical Intersections journal, May 2007

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Pumping and probing vibrational modulated coupled electronic coherence in HCN using short UV fs laser pulses: a 2D quantum nuclear dynamical study journal, January 2017

Femtosecond real-time alignment in chemical reactions journal, July 1989

Real‐time femtosecond probing of ‘‘transition states’’ in chemical reactions
journal, August 1987

Probing electron-hole coherence in strongly driven 2D materials using high-harmonic generation
journal, May 2022

Attosecond transient-absorption dynamics of xenon core-excited states in a strong driving field
journal, March 2017

Attosecond molecular dynamics: fact or fiction?
journal, February 2014

Essential entanglement for atomic and molecular physics
journal, September 2011

Theory of attosecond transient absorption spectroscopy of strong-field-generated ions
journal, March 2011

Attosecond science
journal, June 2007

Search for long-lasting electronic coherence using on-the-fly ab initio semiclassical dynamics
journal, January 2022

Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018

Colloquium : Strong-field phenomena in periodic systems
journal, April 2018

Wave‐packet dynamics in the Li₂ E(¹Σ⁺_g) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state
journal, November 1995

Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses
journal, September 2021

Vibrational Beatings Conceal Evidence of Electronic Coherence in the FMO Light-Harvesting Complex
journal, October 2014

Attosecond science based on high harmonic generation from gases and solids
journal, June 2020

Revealing electronic state-switching at conical intersections in alkyl iodides by ultrafast XUV transient absorption spectroscopy
journal, August 2020

Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
journal, April 2007

Ultrafast dynamics in van der Waals heterostructures
journal, November 2018

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration
journal, February 2022

Measurement and laser control of attosecond charge migration in ionized iodoacetylene
journal, October 2015

Comparison of Electronic and Vibrational Coherence Measured by Two-Dimensional Electronic Spectroscopy
journal, July 2011

De- and Recoherence of Charge Migration in Ionized Iodoacetylene
journal, July 2019

Coupled valence carrier and core-exciton dynamics in ${WS}_{2}$ probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy
journal, August 2021

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium
journal, June 2017

Conical intersection and coherent vibrational dynamics in alkyl iodides captured by attosecond transient absorption spectroscopy
journal, March 2022

Characterization of vibrational wave packets by core-level high-harmonic transient absorption spectroscopy
journal, August 2013

Extreme-ultraviolet refractive optics
journal, November 2018

Elucidating the origins of multimode vibrational coherences of polyatomic molecules induced by intense laser fields
journal, September 2017

Control of Nuclear Dynamics through Conical Intersections and Electronic Coherences
journal, March 2018

Quantum coherences reveal excited-state dynamics in biophysical systems
journal, June 2019

Attosecond spectroscopy of liquid water
journal, August 2020

Charge Migration in Propiolic Acid: A Full Quantum Dynamical Study
journal, November 2018

Generation of deep ultraviolet sub-2-fs pulses
journal, March 2019

Generation of optical Schrödinger cat states in intense laser–matter interactions
journal, August 2021

What will it take to observe processes in 'real time'?
journal, February 2014

Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study
journal, May 2021

Adaptive strong-field control of chemical dynamics guided by three-dimensional momentum imaging
journal, December 2013

State-resolved attosecond reversible and irreversible dynamics in strong optical fields
journal, February 2017

Quantum coherence in molecular photoionization
journal, January 2022

Real-time observation of valence electron motion
journal, August 2010

Probing coherently excited optical phonons by extreme ultraviolet radiation with femtosecond time resolution
journal, July 2008

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide
journal, May 2020

Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy
journal, November 2019

BEYOND BORN-OPPENHEIMER: Molecular Dynamics Through a Conical Intersection
journal, June 2004

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction
journal, April 2017

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe ₂ with Femtosecond Core-Level Spectroscopy
journal, October 2020

Visualizing coherent vibrational motion in the molecular iodine B3Π0+u state using ultrafast XUV transient-absorption spectroscopy
journal, August 2021

Atomically Thin ${MoS}_{2}$ A New Direct-Gap Semiconductor
journal, September 2010

Sub-7-femtosecond conical-intersection dynamics probed at the carbon K-edge
journal, January 2021

Charge migration and charge transfer in molecular systems
journal, November 2017

Charge directed reactivity:
journal, March 1998

The Birth of Attochemistry
journal, January 2019

Entanglement and coherence in photoionization of H2 by an ultrashort XUV laser pulse
journal, July 2019

Coherent ultrafast charge transfer in an organic photovoltaic blend
journal, May 2014

Excited-state vibronic wave-packet dynamics in $H_{2}$ probed by XUV transient four-wave mixing
journal, February 2018

Origin of Long-Lived Coherences in Light-Harvesting Complexes
journal, June 2012

Attosecond band-gap dynamics in silicon
journal, December 2014

NaI revisited: Theoretical investigation of predissociation via ultrafast XUV transient absorption spectroscopy
journal, November 2019

High-harmonic generation from solids
journal, November 2018

Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
journal, July 2019

Translational, rotational and vibrational relaxation dynamics of a solute molecule in a non-interacting solvent
journal, July 2016

Ab initio investigation of Br-3 d core-excited states in HBr and HBr ⁺ toward XUV probing of photochemical dynamics
journal, January 2019

Observation of high-order harmonic generation in a bulk crystal
journal, December 2010

Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source
journal, January 2017

Control of Electron Localization in Molecular Dissociation
journal, April 2006

Unravelling the intertwined atomic and bulk nature of localised excitons by attosecond spectroscopy
journal, February 2021

Using coherence to enhance function in chemical and biophysical systems
journal, March 2017

Spin–Orbit State-Selective C–I Dissociation Dynamics of the CH ₃ I ⁺ X̃ Electronic State Induced by Intense Few-Cycle Laser Fields
journal, December 2017

Attosecond electronic dynamics of core-excited states of N2O in the soft x-ray region
journal, December 2021

Attosecond physics
journal, February 2009

Entanglement between electronic and vibrational degrees of freedom in a laser-driven molecular system
journal, December 2013

Attosecond chirp compensation in water window by plasma dispersion
journal, January 2018

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond
journal, August 2016

Theoretical Analysis of High-Harmonic Generation in Solids
journal, August 2014

Isomerization Through Conical Intersections
journal, May 2007

Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy
journal, July 2019

Pumping and probing vibrational modulated coupled electronic coherence in HCN using short UV fs laser pulses: a 2D quantum nuclear dynamical study
journal, January 2017

Femtosecond real-time alignment in chemical reactions
journal, July 1989

Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes
journal, September 2012

The measurement of ultrafast electronic and structural dynamics with X-rays
journal, April 2019

Vibronic coherence unveiled
journal, February 2014