Electron Spin Relaxation and 39K Pulsed ENDOR Studies on Cr5+ doped K3NbO8 at 9.7 and 240 GHz

TL;DR

This study investigates electron spin relaxation and hyperfine interactions in Cr^5+ doped K3NbO8 using pulsed EPR and ENDOR at 9.7 and 240 GHz, revealing frequency-dependent relaxation rates and detailed nuclear couplings relevant for spin qubit applications.

Contribution

It provides the first detailed high-frequency ENDOR analysis of 39K and 93Nb hyperfine interactions in Cr^5+ doped K3NbO8, highlighting frequency effects on relaxation and hyperfine couplings.

Findings

Spin-lattice relaxation rate 1/T_1 is 250 times faster at 240 GHz than at 9.7 GHz.

Spin-spin relaxation rate 1/T_2 is largely frequency independent.

Largest 39K hyperfine coupling is positive, with isotropic 0.522 MHz.

Abstract

Cr^5+ doped K_3NbO_8, considered to be useful as a electron spin qubit, has been investigated by pulsed X-band (~9.7 GHz) and 240 GHz electron paramagnetic resonance and electron nuclear double resonance (ENDOR). Comparison of the low temperature electronic spin-lattice relaxation rate 1/T_1 at 9.7 and 240 GHz shows that it is 250 times faster at 240 GHz than at X-band. On the other hand, the spin-spin relaxation rate 1/T_2 appears largely frequency independent and is very likely related to the superhyperfine (SHF) coupling of the Cr^5+ electron with the surrounding potassium and niobium nuclei. This coupling was investigated by HYSCORE at 9.7 GHz and pulsed Mims ENDOR at 240 GHz. The high frequency and field enabled us to unambiguously measure the hyperfine and quadrupole couplings of the 39K in spite of its small magnetic moment. We find that the largest 39K SHF coupling is positive, with 0.522 MHz and 0.20 MHz as its isotropic and dipolar parts respectively. 93Nb ENDOR was dominantly due to its quadrapolar interaction, with a coupling of about 0.8 MHz, and a SHF coupling of about 0.08 MHz. The significance of these data to spin qubit studies is pointed out.