A high-frequency electron paramagnetic resonance spectrometer for multi-dimensional, -frequency and -phase pulsed measurements

TL;DR

This paper presents a versatile high-frequency EPR spectrometer capable of multi-dimensional, multi-frequency, and multi-phase pulsed measurements, enabling advanced spin dynamics studies in solid-state systems.

Contribution

The paper introduces a novel high-frequency EPR instrument with integrated multi-frequency and pulsed capabilities, enhancing experimental flexibility and sensitivity.

Findings

Successful implementation of multi-frequency pulsed EPR measurements

Demonstration of PELDOR spectroscopy for spin correlation analysis

Extension of spin coherence times using dynamical decoupling techniques

Abstract

We describe instrumentation for a high-frequency electron paramagnetic resonance (EPR) and pulsed electron-electron double resonance (PELDOR) spectroscopy. The instrumentation is operated in the frequency range of 107$-$120 GHz and 215$-$240 GHz and in the magnetic field range of 0$-$12.1 Tesla. The spectrometer consisting of a high-frequency high-power solid-state source, a quasioptical system, a phase-sensitive detection system, a cryogenic-free superconducting magnet and a $^4$He cryostat enables multi-frequency continuous-wave EPR spectroscopy as well as pulsed EPR measurements with a few hundred nanosecond pulses. Here we discuss the details of the design and the pulsed EPR sensitivity of the instrumentation. We also present performance of the instrumentation in unique experiments including PELDOR spectroscopy to probe correlations in an insulating electronic spin system and application of dynamical decoupling techniques to extend spin coherence of electron spins in an insulating solid-state system.