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Related Concept Videos

Radical Reactivity: Overview01:11

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Radicals, the highly reactive species, gain stability by undergoing three different reactions. The first reaction involves a radical-radical coupling, in which a radical combines with another radical, forming a spin‐paired molecule. The second reaction is between a radical and a spin‐paired molecule, generating a new radical and a new spin‐paired molecule. The third reaction is radical decomposition in a unimolecular reaction, forming a new radical and a spin‐paired...
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Atomic Nuclei: Nuclear Relaxation Processes01:23

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In the absence of an external magnetic field, nuclear spin states are degenerate and randomly oriented. When a magnetic field is applied, the spins begin to precess and orient themselves along (lower energy) or against (higher energy) the direction of the field. At equilibrium, a slight excess population of spins exists in the lower energy state. Because the direction of the magnetic field is fixed as the z-axis,  the precessing magnetic moments are randomly oriented around the z-axis.
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Radical Reactivity: Steric Effects01:10

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The presence of electron-donating, electron-withdrawing, or conjugating groups adjacent to a radical center, imparts electronic stabilization to the radicals. Examples of such electronically-stabilized radicals are triphenylmethyl, tetramethylpiperidine‐N‐oxide, and 2,2‐diphenyl‐1‐picrylhydrazyl. These radicals are remarkably stable and are known as persistent radicals. Some of the persistent radicals can even be isolated and purified.
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Nuclear Overhauser Enhancement (NOE)01:06

Nuclear Overhauser Enhancement (NOE)

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Irradiation of a spin-active nucleus causes an increase or decrease in the signal intensity of neighboring nuclei that are not necessarily chemically bonded or involved in J-coupling. This phenomenon, called the nuclear Overhauser enhancement (NOE), results from through-space interactions between the nuclear spins. The NOE effect decreases with increasing internuclear distance and is generally not observed beyond 4 angstroms. In NOE, dipole-dipole interactions between neighboring spin-active...
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Radical Reactivity: Nucleophilic Radicals01:16

Radical Reactivity: Nucleophilic Radicals

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Radicals adjacent to electron-donating groups are called nucleophilic radicals. These radicals readily react with electrophilic alkenes. The SOMO–LUMO interactions are the driving force for the reaction, where the high-energy SOMO of the electron-rich, nucleophilic radicals interacts with the low-energy LUMO of the electron-deficient, electrophilic alkenes. Such SOMO–LUMO interactions are the basis of reactive radical traps, affecting the selectivity in radical reactions. For...
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Radical Formation: Homolysis00:54

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A bond is formed between two atoms by sharing two electrons. When this bond is broken by supplying sufficient energy, either two electrons can be taken up by one atom forming ions by the cleavage called heterolysis, or the two electrons are shared by two atoms, with one each creating radicals by the cleavage called homolysis.
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Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
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Coherent Control over Nuclear Hyperpolarization Using an Optically Initializable Chromophore-Radical System.

Hoang M Le, Joshua S Straub, Quentin Stern

  • 1Department of Chemistry, New York University, Abu-Dhabi, PO Box 129188, Abu Dhabi, United Arab Emirates.

Journal of the American Chemical Society
|September 17, 2025
PubMed
Summary
This summary is machine-generated.

Chromophore radicals (CRs) enable coherent manipulation of electron and nuclear spins for quantum information science. Optically amplified electron hyperpolarization was transferred to nuclear spins and back, demonstrating CRs

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Area of Science:

  • Molecular quantum information science (QIS)
  • Quantum sensing
  • Spin physics

Background:

  • Chromophore radicals (CRs) are key components in molecular quantum information science (QIS) and quantum sensing.
  • Efficient manipulation of electron and nuclear spins is crucial for QIS applications.

Purpose of the Study:

  • To demonstrate coherent manipulation of optically hyperpolarized electrons in CRs for spin polarization transfer.
  • To investigate the use of pulsed dynamic nuclear polarization (DNP) methods for initializing and reading out nuclear spin states.

Main Methods:

  • Utilized a covalently linked system of tpPDI and BDPA-d16 chromophore radicals.
  • Applied pulsed dynamic nuclear polarization (DNP) methods, including nuclear orientation via electron spin-locking (NOVEL) and reverse-NOVEL.
  • Investigated electron hyperpolarization under light illumination at 85 K.

Main Results:

  • Achieved a 2.1- to 2.4-fold enhancement of electron hyperpolarization in BDPA under illumination, lasting over 100 ms.
  • Demonstrated efficient (65%) transfer of hyperpolarization from electrons to a 1H nuclear spin using NOVEL DNP.
  • Showcased reversible hyperpolarization transfer, achieving a 688-fold nuclear spin hyperpolarization.

Conclusions:

  • CR systems allow for reversible coherent manipulation of spin polarization at moderate cryogenic temperatures.
  • These findings highlight the potential of nuclear spins within CRs for QIS applications like quantum sensing and memory.
  • CRs offer environmental compatibility, tunability, and precise state initialization for advanced QIS.