Monitoring aromatic ring-currents in Mg-porphyrin by time-resolved circular dichroism

Nam, Yeonsig; Rouxel, Jérémy R.; Lee, Jin Yong; Mukamel, Shaul

doi:10.1039/d0cp04815a

Monitoring aromatic ring-currents in Mg-porphyrin by time-resolved circular dichroism

Journal Article · Mon May 11 00:00:00 EDT 2020 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d0cp04815a· OSTI ID:1849505

^[1]; ^[2]; ^[3]; ^[2]

Univ. of California, Irvine, CA (United States); Sungkyunkwan Univ., Suwon (South Korea); OSTI
Univ. of California, Irvine, CA (United States)
Sungkyunkwan Univ., Suwon (South Korea)

We report time-resolved circular dichroism signals (TRCD) in the X-ray regime can directly probe the magnitude and the direction of ring currents in molecules. The electronic ring currents in Mg-porphyrin, generated by a coherent superposition of electronic states induced by a circularly polarized UV pulse, are tracked by a time-delayed circularly polarized attosecond X-ray pulse. The signals are calculated using the minimal coupling Hamiltonian, which directly makes use of transition current densities. The TRCD signals obtained from the left and right circularly polarized light pump have opposite signs, revealing the direction of the ring current. Molecular aromaticity and its role in photochemical reactions such as ring opening or closure can be studied using this technique.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Research Foundation (NRF); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-04ER15571

OSTI ID:: 1849505

Alternate ID(s):: OSTI ID: 1716551

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 45 Vol. 22; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Periodic Electron Circulation Induced by Circularly Polarized Laser Pulses: Quantum Model Simulations for Mg Porphyrin Barth, Ingo; Manz, Jörn Angewandte Chemie International Edition, Vol. 45, Issue 18 https://doi.org/10.1002/anie.200504147	journal	April 2006
Control of π-Electron Rotation in Chiral Aromatic Molecules by Nonhelical Laser Pulses Kanno, Manabu; Kono, Hirohiko; Fujimura, Yuichi Angewandte Chemie International Edition, Vol. 45, Issue 47 https://doi.org/10.1002/anie.200602479	journal	December 2006
Aromaticity Switching in Porphyrinoids Pawlicki, Miłosz; Latos-Grażyński, Lechosław Chemistry - An Asian Journal, Vol. 10, Issue 7 https://doi.org/10.1002/asia.201500170	journal	April 2015
The Induced Magnetic Field in Cyclic Molecules Merino, Gabriel; Heine, Thomas; Seifert, Gotthard Chemistry - A European Journal, Vol. 10, Issue 17 https://doi.org/10.1002/chem.200400457	journal	September 2004
Photoelectron angular distributions from strong-field coherent electronic excitation Wollenhaupt, M.; Krug, M.; Köhler, J. Applied Physics B, Vol. 95, Issue 2 https://doi.org/10.1007/s00340-009-3431-1	journal	February 2009
Ground and excited states of Mg porphin studied by the SAC/SAC-CI method Hasegawa, J.; Hada, M.; Nonoguchi, M. Chemical Physics Letters, Vol. 250, Issue 2 https://doi.org/10.1016/0009-2614(95)01406-3	journal	February 1996
Optical Spectra and Electronic Structure of Porphyrins and Related Rings Gouterman, Martin The Porphyrins https://doi.org/10.1016/B978-0-12-220103-5.50008-8	book	January 1978
Density functional theory study of the electronic absorption spectrum of Mg-porphyrin and Mg-etioporphyrin-I Sundholm, D. Chemical Physics Letters, Vol. 317, Issue 3-5 https://doi.org/10.1016/S0009-2614(99)01422-0	journal	February 2000
A DFT/TDDFT interpretation of the ground and excited states of porphyrin and porphyrazine complexes Baerends, E. J.; Ricciardi, G.; Rosa, A. Coordination Chemistry Reviews, Vol. 230, Issue 1-2 https://doi.org/10.1016/S0010-8545(02)00093-0	journal	August 2002
Vibrational effects on UV/Vis laser-driven π-electron ring currents in aromatic ring molecules Mineo, H.; Lin, S. H.; Fujimura, Y. Chemical Physics, Vol. 442 https://doi.org/10.1016/j.chemphys.2014.02.011	journal	October 2014
The effect of twisted light on the ring-shaped molecules: The manipulation of the photoinduced current and the magnetic moment by transferring spin and orbital angular momentum of high frequency light Köksal, Koray; Koç, Fatih Computational and Theoretical Chemistry, Vol. 1099 https://doi.org/10.1016/j.comptc.2016.11.031	journal	January 2017
Aromaticity, polarisability and ring current Fowler, P. W.; Soncini, A. Chemical Physics Letters, Vol. 383, Issue 5-6 https://doi.org/10.1016/j.cplett.2003.11.081	journal	January 2004
Ring-current aromaticity in open-shell systems Soncini, A.; Fowler, P. W. Chemical Physics Letters, Vol. 450, Issue 4-6 https://doi.org/10.1016/j.cplett.2007.11.053	journal	January 2008
Quantum Design of π-Electron Ring Currents in Polycyclic Aromatic Hydrocarbons: Parallel and Antiparallel Ring Currents in Naphthalene Mineo, Hirobumi; Fujimura, Yuichi The Journal of Physical Chemistry Letters, Vol. 8, Issue 9 https://doi.org/10.1021/acs.jpclett.7b00704	journal	April 2017
Attosecond Dynamics of Molecular Electronic Ring Currents Yuan, Kai-Jun; Shu, Chuan-Cun; Dong, Daoyi The Journal of Physical Chemistry Letters, Vol. 8, Issue 10 https://doi.org/10.1021/acs.jpclett.7b00877	journal	May 2017
Aromaticity and Ring Currents Gomes, J. A. N. F.; Mallion, R. B. Chemical Reviews, Vol. 101, Issue 5 https://doi.org/10.1021/cr990323h	journal	May 2001
Diamagnetic susceptibility exaltation in hydrocarbons Dauben, Hyp J.; Wilson, James Dennis; Laity, John L. Journal of the American Chemical Society, Vol. 91, Issue 8 https://doi.org/10.1021/ja01036a022	journal	April 1969
Unidirectional Electronic Ring Current Driven by a Few Cycle Circularly Polarized Laser Pulse: Quantum Model Simulations for Mg−Porphyrin Barth, Ingo; Manz, Jörn; Shigeta, Yasuteru Journal of the American Chemical Society, Vol. 128, Issue 21 https://doi.org/10.1021/ja057197l	journal	May 2006
Correlated Electron Dynamics: How Aromaticity Can Be Controlled Ulusoy, Inga S.; Nest, Mathias Journal of the American Chemical Society, Vol. 133, Issue 50 https://doi.org/10.1021/ja206193t	journal	December 2011
Nucleus-Independent Chemical Shifts: A Simple and Efficient Aromaticity Probe Schleyer, Paul von Ragué; Maerker, Christoph; Dransfeld, Alk Journal of the American Chemical Society, Vol. 118, Issue 26 https://doi.org/10.1021/ja960582d	journal	January 1996
A bond order approach to ring current and aromaticity Jug, Karl The Journal of Organic Chemistry, Vol. 48, Issue 8 https://doi.org/10.1021/jo00156a038	journal	April 1983
1H chemical shifts in NMR. Part 18.1 Ring currents and π-electron effects in hetero-aromatics Abraham, Raymond J.; Reid, Matthew Journal of the Chemical Society, Perkin Transactions 2, Issue 6 https://doi.org/10.1039/B201789J	journal	April 2002
Magnetic criteria of aromaticity Gershoni-Poranne, Renana; Stanger, Amnon Chem. Soc. Rev., Vol. 44, Issue 18 https://doi.org/10.1039/C5CS00114E	journal	January 2015
Detection of a weak ring current in a nonaromatic porphyrin nanoring using magnetic circular dichroism Kowalska, Patrycja; Peeks, Martin D.; Roliński, Tomasz Physical Chemistry Chemical Physics, Vol. 19, Issue 48 https://doi.org/10.1039/C7CP07348H	journal	January 2017
Ab initio determination of the induced ring current in aromatic molecules Juse´lius, Jonas; Sundholm, Dage Physical Chemistry Chemical Physics, Vol. 1, Issue 15 https://doi.org/10.1039/a903847g	journal	January 1999
The gauge including magnetically induced current method Fliegl, Heike; Taubert, Stefan; Lehtonen, Olli Physical Chemistry Chemical Physics, Vol. 13, Issue 46 https://doi.org/10.1039/c1cp21812c	journal	January 2011
Zeeman shift of two-dimensional optical signals of Mg-porphyrin dimers with circularly polarized beams Rodriguez, Justo J.; Mukamel, Shaul The Journal of Chemical Physics, Vol. 137, Issue 20 https://doi.org/10.1063/1.4767066	journal	November 2012
Theoretical study of the electronic spectrum of magnesium-porphyrin Rubio, Mercedes; Roos, Björn O.; Serrano-Andrés, Luis The Journal of Chemical Physics, Vol. 110, Issue 15 https://doi.org/10.1063/1.478624	journal	April 1999
Non-linear non-local molecular electrodynamics with nano-optical fields Chernyak, Vladimir Y.; Saurabh, Prasoon; Mukamel, Shaul The Journal of Chemical Physics, Vol. 143, Issue 16 https://doi.org/10.1063/1.4934231	journal	October 2015
Electric ring currents in atomic orbitals and magnetic fields induced by short intense circularly polarized π laser pulses Barth, Ingo; Manz, Jörn Physical Review A, Vol. 75, Issue 1 https://doi.org/10.1103/PhysRevA.75.012510	journal	January 2007
Photoinduced electric currents in ring-shaped molecules by circularly polarized laser pulses Nobusada, Katsuyuki; Yabana, Kazuhiro Physical Review A, Vol. 75, Issue 3 https://doi.org/10.1103/PhysRevA.75.032518	journal	March 2007
Attosecond-magnetic-field-pulse generation by intense few-cycle circularly polarized UV laser pulses Yuan, Kai-Jun; Bandrauk, André D. Physical Review A, Vol. 88, Issue 1 https://doi.org/10.1103/PhysRevA.88.013417	journal	July 2013
Background-Free Measurement of Ring Currents by Symmetry-Breaking High-Harmonic Spectroscopy Neufeld, Ofer; Cohen, Oren Physical Review Letters, Vol. 123, Issue 10 https://doi.org/10.1103/PhysRevLett.123.103202	journal	September 2019
Optimal Control of Quantum Rings by Terahertz Laser Pulses Räsänen, E.; Castro, A.; Werschnik, J. Physical Review Letters, Vol. 98, Issue 15 https://doi.org/10.1103/PhysRevLett.98.157404	journal	April 2007
Watching a Protein as it Functions with 150-ps Time-Resolved X-ray Crystallography Schotte, F. Science, Vol. 300, Issue 5627 https://doi.org/10.1126/science.1078797	journal	June 2003
Laser-Control of Ultrafast π-Electron Ring Currents in Aromatic Molecules: Roles of Molecular Symmetry and Light Polarization Kanno, Manabu; Kono, Hirohiko; Fujimura, Yuichi Applied Sciences, Vol. 8, Issue 12 https://doi.org/10.3390/app8122347	journal	November 2018

Similar Records

Coherent ring-current migration of Mg-phthalocyanine probed by time-resolved X-ray circular dichroism

Journal Article · Wed Aug 10 20:00:00 EDT 2022 · Chemical Science · OSTI ID:1882452

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS

Monitoring aromatic ring-currents in Mg-porphyrin by time-resolved circular dichroism

Citation Formats

References (36)

Similar Records

Related Subjects