This dissertation presents the investigation of magnetic exchange and anisotropy in novel metal-organic complexes containing minimum number of magnetic ions. Such complexes can serve as a model system to understand the exciting magnetic phenomena in such class of materials and also can put forward as candidates for the so called molecular nanomagnets. A direct assessment of the effective magnetic moment and the effective interaction between the metal ions in the complex can be done using magnetization measurements. Here the magnetization studies are performed as a function of temperature and field using a SQUID magnetometer. Yet another powerful tool to characterize and determine the spin levels, the ESR spectroscopic methods, has also been exploited. The study of the dynamical properties of this class of materials was relevant to understand the relaxation mechanism in the low temperatures. For this a new ac susceptometer has been built in house which was another main objective of this dissertation work. The design, fabrication, calibration and automation done on this device is presented in this thesis. The device has been tested using the known molecular magnet Mn12 acetate, and the antiferromagnet Dy2PdSi3. The present work is mainly focused on the magnetic properties of Mn, Ni and Fe based organometallic complexes. The studied Mn dimer with different acceptor and donor ligands exhibit the fine tuning of the electron density at the core of molecular complex by variation in ligands. This in turn shows that the change in peripheral ligands can control the magnetism of the molecule. The influence of the change in Ni-S-Ni bond angle in the magnetic exchange interaction is studied in a Ni(2) dimer and a Ni(2) trimer complex. The Ni dimer complex shows a ferromagnetic interaction (J = -42K) whereas trimer shows an antiferromagnetic interaction (J = 140K). Another Ni based complex bridged via phosphorous has been studied which shows the existence of glassy nature at low temperature. Also a polymeric chain compound based on Fe is studied and presented. All these phosphorous or sulphur bridged complexes are novel materials and these are the first data on these complexes.

This dissertation presents the investigation of magnetic exchange and anisotropy in novel metal-organic complexes containing minimum number of magnetic ions. Such complexes can serve as a model system to understand the exciting magnetic phenomena in such class of materials and also can put forward as candidates for the so called molecular nanomagnets. A direct assessment of the effective magnetic moment and the effective interaction between the metal ions in the complex can be done using magnetization measurements. Here the magnetization studies are performed as a function of temperature and field using a SQUID magnetometer. Yet another powerful tool to characterize and determine the spin levels, the ESR spectroscopic methods, has also been exploited. The study of the dynamical properties of this class of materials was relevant to understand the relaxation mechanism in the low temperatures. For this a new ac susceptometer has been built in house which was another main objective of this dissertation work. The design, fabrication, calibration and automation done on this device is presented in this thesis. The device has been tested using the known molecular magnet Mn12 acetate, and the antiferromagnet Dy2PdSi3. The present work is mainly focused on the magnetic properties of Mn, Ni and Fe based organometallic complexes. The studied Mn dimer with different acceptor and donor ligands exhibit the fine tuning of the electron density at the core of molecular complex by variation in ligands. This in turn shows that the change in peripheral ligands can control the magnetism of the molecule. The influence of the change in Ni-S-Ni bond angle in the magnetic exchange interaction is studied in a Ni(2) dimer and a Ni(2) trimer complex. The Ni dimer complex shows a ferromagnetic interaction (J = -42K) whereas trimer shows an antiferromagnetic interaction (J = 140K). Another Ni based complex bridged via phosphorous has been studied which shows the existence of glassy nature at low temperature. Also a polymeric chain compound based on Fe is studied and presented. All these phosphorous or sulphur bridged complexes are novel materials and these are the first data on these complexes.

Foi desenvolvido uma ponte de indutâncias mútuas, auto-balanceada, para medidas automáticas e simultâneas das partes real (x\') e imaginária (x\") da susceptibilidade magnética AC, na faixa de freqüências de 20 Hz e 1 KHz e temperaturas de 2K a 300K. O sistema é balanceado em um elo de realimentação digital que assegura um sinal, em fase e quadratura, continuamente nulo. A amplificação do sinal é feita através de um amplificador \"lock-in\" de duas fases, cujas saídas comandam dois DAC multiplicadores, gerando o sinal composto que é usado para balancear a ponte. O valor absoluto da susceptibilidade é medida movendo as bobinas primária e secundárias de tal forma que a amostra fique posicionada ora em um dos secundários, ora em outro. A resolução da parte numérica é 1 em 4000. A sensibilidade alcançada foi de 10-7 emu para amostras de 10-2cm-3 em um campo de excitação de amplitude 15 Gauss. A interface com um microcomputador ainda não foi desenvolvida. / An automatic self-balanced mutual inductance bridge has been designed to measure the real (x\') and imaginary (x\") parts of the magnetic AC susceptibility simultaneously in the frequency range 20 Hz to 1 KHz and temperatures between 2K to 30OK. The system is based on a digitally controlled feedback loop, which ensures continuous balanced operation, in phase as well in quadrature. The signal amplification chain is made of a dual-phase lock-in amplifier, whose outputs command two DAC multipliers, generating the composite balance signal for nulling the bridge. The absolute value of the susceptibility is measured by moving the primary and secondary coils in such a way to place the sample in the center of both secondary coils. The resolution of the numerical part is 1 in 4000. Sensivities of the order of 10-7 emu for samples of 10-2cm-3 in a primary field of 15 gauss have been obtained. The interface with a desktop computer has not been developed yet.

Foi desenvolvido uma ponte de indutâncias mútuas, auto-balanceada, para medidas automáticas e simultâneas das partes real (x\') e imaginária (x\") da susceptibilidade magnética AC, na faixa de freqüências de 20 Hz e 1 KHz e temperaturas de 2K a 300K. O sistema é balanceado em um elo de realimentação digital que assegura um sinal, em fase e quadratura, continuamente nulo. A amplificação do sinal é feita através de um amplificador \"lock-in\" de duas fases, cujas saídas comandam dois DAC multiplicadores, gerando o sinal composto que é usado para balancear a ponte. O valor absoluto da susceptibilidade é medida movendo as bobinas primária e secundárias de tal forma que a amostra fique posicionada ora em um dos secundários, ora em outro. A resolução da parte numérica é 1 em 4000. A sensibilidade alcançada foi de 10-7 emu para amostras de 10-2cm-3 em um campo de excitação de amplitude 15 Gauss. A interface com um microcomputador ainda não foi desenvolvida. / An automatic self-balanced mutual inductance bridge has been designed to measure the real (x\') and imaginary (x\") parts of the magnetic AC susceptibility simultaneously in the frequency range 20 Hz to 1 KHz and temperatures between 2K to 30OK. The system is based on a digitally controlled feedback loop, which ensures continuous balanced operation, in phase as well in quadrature. The signal amplification chain is made of a dual-phase lock-in amplifier, whose outputs command two DAC multipliers, generating the composite balance signal for nulling the bridge. The absolute value of the susceptibility is measured by moving the primary and secondary coils in such a way to place the sample in the center of both secondary coils. The resolution of the numerical part is 1 in 4000. Sensivities of the order of 10-7 emu for samples of 10-2cm-3 in a primary field of 15 gauss have been obtained. The interface with a desktop computer has not been developed yet.