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

Sun, Shichao; Yong, Haiwang; Chen, Feng; Mukamel, Shaul

doi:10.1039/d2sc02768b

Cited by 7 publications

(7 citation statements)

References 54 publications

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“…Concurrently, Mukamel et al , theoretically explored the utility of chiral optical cavity designs to magnesium-porphyrin compounds, known for their coherent ring currents that exhibit variable X-ray circular dichroism signals due to their aromatic structure , (Figure c). The ring current of the Mg-porphyrin was intricately linked to the molecular electronic structure, characterized by a distinctive time scale of 150 fs . Consequently, the strong coupling between Mg-porphyrin electronic transition and chiral optical cavity mode holds the potential to significantly amplify the X-ray circular dichroism effect. , …”

Section: Polarization Properties Under Strong-coupling Regimementioning

confidence: 99%

Section: Polarization Properties Under Strong-coupling Regimementioning

confidence: 99%

“…Concurrently, Mukamel et al 133,134 theoretically explored the utility of chiral optical cavity designs to magnesiumporphyrin compounds, known for their coherent ring currents that exhibit variable X-ray circular dichroism signals due to their aromatic structure 250,251 (Figure 34c). The ring current of the Mg-porphyrin was intricately linked to the molecular electronic structure, characterized by a distinctive time scale of 150 fs.…”

Section: Theoretical Development Of Polarized Polaritonic Effectmentioning

confidence: 99%

“…The ring current of the Mg-porphyrin was intricately linked to the molecular electronic structure, characterized by a distinctive time scale of 150 fs. 250 Consequently, the strong coupling between Mgporphyrin electronic transition and chiral optical cavity mode holds the potential to significantly amplify the X-ray circular dichroism effect. 133,134 Vu and colleagues 235 harnessed an optical cavity to enhance the diastereocontrol in the context of the excited-state proton transfer (ESPT)-driven diastereomeric enrichment between a chiral diene and a chiral dienophile, based on their quantum electrodynamics (QED) generalization of time-dependent density functional theory.…”

Section: Theoretical Development Of Polarized Polaritonic Effectmentioning

confidence: 99%

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Molecular Polaritons for Chemistry, Photonics and Quantum Technologies

Xiang,

Xiong

2024

Chem. Rev.

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Molecular polaritons are quasiparticles resulting from the hybridization between molecular and photonic modes. These composite entities, bearing characteristics inherited from both constituents, exhibit modified energy levels and wave functions, thereby capturing the attention of chemists in the past decade. The potential to modify chemical reactions has spurred many investigations, alongside efforts to enhance and manipulate optical responses for photonic and quantum applications. This Review centers on the experimental advances in this burgeoning field. Commencing with an introduction of the fundamentals, including theoretical foundations and various cavity architectures, we discuss outcomes of polariton-modified chemical reactions. Furthermore, we navigate through the ongoing debates and uncertainties surrounding the underpinning mechanism of this innovative method of controlling chemistry. Emphasis is placed on gaining a comprehensive understanding of the energy dynamics of molecular polaritons, in particular, vibrational molecular polaritons�a pivotal facet in steering chemical reactions. Additionally, we discuss the unique capability of coherent twodimensional spectroscopy to dissect polariton and dark mode dynamics, offering insights into the critical components within the cavity that alter chemical reactions. We further expand to the potential utility of molecular polaritons in quantum applications as well as precise manipulation of molecular and photonic polarizations, notably in the context of chiral phenomena. This discussion aspires to ignite deeper curiosity and engagement in revealing the physics underpinning polariton-modified molecular properties, and a broad fascination with harnessing photonic environments to control chemistry.

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Section: Polarization Properties Under Strong-coupling Regimementioning

confidence: 99%

Section: Polarization Properties Under Strong-coupling Regimementioning

confidence: 99%

Section: Theoretical Development Of Polarized Polaritonic Effectmentioning

confidence: 99%

Section: Theoretical Development Of Polarized Polaritonic Effectmentioning

confidence: 99%

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Molecular Polaritons for Chemistry, Photonics and Quantum Technologies

Xiang,

Xiong

2024

Chem. Rev.

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“…Alternatively, optical methods based on femtosecond laser pulses have made substantial progress in producing shorter magnetic bursts through laser-induced currents in plasmas, − plasmonic nanostructures, , semiconductors, − molecules, ,,− or atoms . Interestingly, additional control over the magnetic field features can be gained by shaping the spatial structure of the laser beams. ,,− ,, Nevertheless, to our knowledge the perspective of attosecond time scales has only been theoretically foreseen in relation to the attosecond electromagnetic pulses, ,, where the dominance of the electric field overshadows the magnetic component.…”

mentioning

confidence: 99%

Tunable Tesla-Scale Magnetic Attosecond Pulses through Ring-Current Gating

de las Heras,

Bonafé,

Hernández-García

et al. 2023

J. Phys. Chem. Lett.

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Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, “current-gating” schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

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