Non-Bloch-Siegert-type power-induced shift of two-photon electron paramagnetic resonances of charge-carrier spin states in an OLED

We present Floquet theory-based predictions and electrically detected magnetic resonance (EDMR) experiments scrutinizing the nature of two-photon magnetic resonance shifts of charge-carrier spin states in the perdeuterated \(\pi\)-conjugated polymer poly[2-methoxy-5-(2'-ethylhexyloxy)-1,4-pheny...

Full description

Saved in:
Bibliographic Details
Published in:arXiv.org 2023-10
Main Authors: Atwood, S I, Hosseinzadeh, S, Mkhitaryan, V V, Tennahewa, T H, Malissa, H, Jiang, W, Darwish, T A, Burn, P L, Lupton, J M, Boehme, C
Format: Article
Language:English
Subjects:
Amplitudes
Circular polarization
Current carriers
Electron spin
Helicity
Linear polarization
Organic light emitting diodes
Paramagnetic resonance
Photons
Polyphenylene vinylene
Radiation
Robustness (mathematics)
Room temperature
Spin resonance
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:We present Floquet theory-based predictions and electrically detected magnetic resonance (EDMR) experiments scrutinizing the nature of two-photon magnetic resonance shifts of charge-carrier spin states in the perdeuterated \(\pi\)-conjugated polymer poly[2-methoxy-5-(2'-ethylhexyloxy)-1,4-phenylene vinylene] (d-MEH-PPV) under strong magnetic resonant drive conditions (radiation amplitude \(B_1\) ~ Zeeman field \(B_0\)). Numerical calculations show that the two-photon resonance shift with power is nearly drive-helicity independent. This is in contrast to the one-photon Bloch-Siegert shift that only occurs under non-circularly polarized strong drive conditions. We therefore treated the Floquet Hamiltonian analytically under arbitrary amplitudes of the co- and counter-rotating components of the radiation field to gain insight into the nature of the helicity dependence of multi-photon resonance shifts. In addition, we tested Floquet-theory predictions experimentally by comparing one-photon and two-photon charge-carrier spin resonance shifts observed through room-temperature EDMR experiments on d-MEH-PPV-based bipolar injection devices [i.e., organic light emitting diode structures (OLEDs)]. We found that under the experimental conditions of strong, linearly polarized drive, our observations consistently agree with theory, irrespective of the magnitude of \(B_1\), and therefore underscore the robustness of Floquet theory in predicting nonlinear magnetic resonance behaviors.
ISSN:2331-8422
DOI:10.48550/arxiv.2310.14180