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Proportional-Derivative (PD) control is a widely used control method in various engineering systems to enhance stability and performance. In a system with only proportional control, common issues include high maximum overshoot and oscillation, observed in both the error signal and its rate of change. This behavior can be divided into three distinct phases: initial overshoot, subsequent undershoot, and gradual stabilization.
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Longitudinal Pulsed Dynamic Nuclear Polarization Transfer via Periodic Optimal Control.

José P Carvalho1, Anders Bodholt Nielsen1, David L Goodwin1

  • 1Interdisciplinary Nanoscience Center (iNANO) and Department of Chemistry, Aarhus University, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.

The Journal of Physical Chemistry Letters
|February 23, 2026
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Summary
This summary is machine-generated.

New pulsed dynamic nuclear polarization (DNP) sequences called LOOP achieve efficient polarization transfer. These sequences overcome limitations of previous methods, enhancing NMR sensitivity with broad bandwidths.

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Area of Science:

  • Magnetic Resonance Spectroscopy
  • Physical Chemistry
  • Quantum Control

Background:

  • Pulsed dynamic nuclear polarization (DNP) enhances Nuclear Magnetic Resonance (NMR) sensitivity by transferring electron polarization to nuclear spins.
  • Current pulsed DNP methods often rely on transverse spin-locking and Hartmann-Hahn matching, which can be limited by excitation pulse imperfections.
  • Continuous-wave DNP is the prevailing method, but pulsed DNP offers potential for improved performance and flexibility.

Purpose of the Study:

  • To develop a new family of broadband pulsed DNP pulse sequences to overcome the limitations of existing methods.
  • To achieve efficient longitudinal polarization transfer, mitigating challenges associated with excitation pulses in DNP.
  • To enhance NMR sensitivity through advanced DNP techniques.

Main Methods:

  • Application of optimal control theory and effective Hamiltonian theory to design novel DNP pulse sequences.
  • Development of the Longitudinally Optimized with Overarching Periodicity (LOOP) pulse sequences.
  • Characterization of sequence performance under microwave field inhomogeneity and at a specific magnetic field (0.35 T).

Main Results:

  • The LOOP sequences enable robust single-spin effective z rotations, demonstrating effective longitudinal polarization transfer.
  • These sequences exhibit significant compensation for microwave field inhomogeneity.
  • Achieved DNP transfer bandwidths exceeding 100 MHz with a modest peak microwave field amplitude of 32 MHz.

Conclusions:

  • The LOOP pulse sequences represent a significant advancement in pulsed DNP, offering enhanced performance and robustness.
  • These sequences effectively address the challenge of excitation pulse limitations in DNP applications.
  • The demonstrated broadband capability and efficiency open new avenues for high-sensitivity NMR spectroscopy.