Neutron Scattering Studies of Magnetic and Non-Magnetic Correlated Systems

Author:
Hu, Xiao, Physics - Graduate School of Arts and Sciences, University of Virginia
Advisor:
Lee, Seung-Hun, AS-Physics, University of Virginia
Abstract:

The field of correlated electron systems has been one of the most widely studied areas of research in condensed-matter physics. Due to the Coulomb interactions between electrons in these systems, the collective states cannot be understood via one-electron approximation that one electron is embedded in a static mean field generated by other electrons. To theoretically describe correlated electron systems, the Hubbard model was proposed based on the tight-binding approximation from condensed-matter physics, which describes particles in a periodic potential. According to the ratio of the hopping integral t and on-site interaction U defined in the Hubbard model, correlated electron systems can be categorized as strongly and weakly correlated systems.
For this thesis, we have performed elastic and inelastic neutron scattering measurements on one strongly correlated magnetic system, Sr2CuTe0.5W0.5O6, and two weakly correlated non-magnetic systems, (BA)2PbI4 (butylammonium lead iodide) and (PEA)2PbI4 (phenethyl-ammonium lead iodide).
For Sr2CuTe0.5W0.5O6, using sub-K temperature and 20 μeV energy resolution neutron scattering experiments, we show that the system below Tf=1.7(1) K exhibits an extremely weak frozen moment of 〈S〉/S~0.1. Below Tf, the imaginary part of the dynamical susceptibility, χ''(ℏω), behaves linearly with ℏω for ℏω275 K). Whereas in (PEA)2PbI4, only the C3 rotational of the NH3 group was identified.
Based on the characterized rotational dynamics of both samples, we determined and separated the rotational contributions from the measured phonon intensities. We find that the low-energy inorganic modes of both samples have similar scattering intensities and temperature dependence, which is consistent with the fact that regardless of the different organic molecule configurations, the Pb-I networks of both samples are similar and hence the vibrational responses to the incident neutrons are expected to be similar. On the other hand, the scattering intensities of hybrid modes are quite different for the two samples. The much lower intensities of hybrid modes in (PEA)2PbI4 than in (BA)2PbI4 suggests that the tight stacking of PEA+ cations probably restricts their vibrational degrees of freedom and hence suppresses the vibrational response of hybrid modes to the incident neutrons. The temperature dependence of either inorganic phonon modes or hybrid phonon modes does not show predominant correlations with photoluminescence quantum yield (PLQY) indicated by their bromide equivalents that we assume to be similar with or same as the iodides. However, the rotational dynamics exhibits an excellent correspondence to PLQY that: below ~ 150 K when the rotational dynamics of both samples are frozen, both of their bromide equivalents’ PLQY stay at high levels (> 90%); while above 150 K, the rotational motion of organic molecules in (BA)2PbI4 get enhanced much faster than that in (PEA)2PbI4, which coincides with the faster decay of PLQY observed in (BA)2PbBr4. This correspondence indicates that the rotational dynamics of organic molecules in 2D HOIPs may dominate the optoelectronic performance such as PLQY.

Degree:
PHD (Doctor of Philosophy)
Keywords:
Frustrated Magnets, Hybrid Organic-Inorganic Perovskites, Neutron Scattering
Sponsoring Agency:
U.S. Department of Energy
Language:
English
Issued Date:
2021/11/05