Date of Award


Degree Name

Doctor of Philosophy


Material Science and Engineering


Cristian E. Botez


Magnetic nanoparticle ensembles have received a lot of attention, stemming in part from their current and potential applications in biomedicine and in the development of high-density magnetic storage media. Key to the functionality of these systems are microscopic structures and mechanisms that make them exhibit unique properties and behave differently from their bulk counterparts.

We studied microscopic structures and processes that dictate macroscopic properties, behavior and functionality of magnetic nanoparticle ensembles. As the temperature T strongly influences the magnetic behavior of these systems, we studied temperature dependent magnetic properties using AC-susceptibility and DC-magnetization measurements carried out over a broad range of temperatures, between 3 and 300 K. We extracted structural information from X-ray diffraction (XRD) and direct imaging techniques and correlate it with magnetic properties, in an attempt at better understanding the microscopic structures and magnetic mechanisms responsible for the macroscopic magnetic behavior.

We studied ensembles of magnetic nanoparticles: nickel ferrite immobilized in a solid matrix and cobalt ferrite immersed in carrier fluid respectively, in order to explore their potential use in biomedical applications and magnetic recording. For both NiFe2O4(NFO) and Co0.2Fe2.8O4 (CFO) relaxation mechanisms were determined. Structural properties and average particle sizes were derived from XRD, including synchrotron XRD, and direct imaging techniques such as scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Temperature dependent magnetic measurements, FC-ZFC DC magnetometry, as well as AC complex susceptibility measurements at frequencies between 10 and 10,000 Hz were carried out within the temperature range 3K

For NFO, besides the expected blocking of the superspin, observed at T1  45 K, we found that the system undergoes a magnetic transition at T2  6 K. For the latter, frequency- and temperature-resolved dynamic susceptibility data reveal characteristics that are unambiguously related to collective spin freezing: the relative variation (per frequency decade) of the in-phase-susceptibility peak temperature is ~0.025, critical dynamics analysis yields an exponent z = 9.6 and a zero-field freezing temperature TF = 5.8 K, and, in a magnetic field, TF (H) is excellently described by the de Almeida-Thouless line TF  H2/3. Moreover, out-of-phase-susceptibility vs. temperature datasets collected at different frequencies collapse on a universal dynamic scaling curve. All these observations indicate the existence of a spin-glass-like surface layer that surrounds the superparamagnetic core and undergoes a transition to a frozen state upon cooling below 5.8 K.

For the CFO ferrofluid, we used temperature- and frequency-resolved AC-susceptibility measurements to investigate its magnetic relaxation above the freezing point of the liquid carrier. Our data show that both the Néel and the Brown relaxation mechanisms are operative at temperatures in the vicinity of the out-of-phase (imaginary) susceptibility peak. We separate the contributions of the two mechanisms to the overall-relaxation time, and demonstrate that Brownian relaxation plays a dominant role at all temperatures within this high-dissipation regime.




Received from ProQuest

File Size

116 pages

File Format


Rights Holder

Abdul Wazed Bhuiya