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Introducing organic molecular crystals into ultrafast electron diffractionRohwer, Andrea Berenike 12 1900 (has links)
Thesis (MSc)--Stellenbosch University, 2014. / ENGLISH ABSTRACT: Organic molecular salts have a wide range of physical properties which can be chemically tailored
by minor variations of their substituents. These characteristics include high degrees of anisotropy,
electrical conductivity ranging from superconducting to insulating, and structural changes in the
crystal lattice during first order phase transitions brought about by minimal changes in temperature,
effective pressure, and in some cases even light. Hence, these materials are particularly interesting
for the development of molecular electronics and also as study materials in solid state physics.
The family of copper-dimethyl-dicyanoquinone-diimine (Cu(DMe-DCNQI)2) salts forms part of the
radical anion salt subclass of organic molecular crystals and is of particular interest due to its extraordinarily
high conductivity compared to other quasi one-dimensional organic conductors. Its
metal-to-insulator phase transition is characterised by conductivity jumps across several orders of
magnitude within a few kelvin. Over the past three decades the metallic and insulating phases,
as well as the transition behaviour have been investigated extensively utilising a broad spectrum
of methods amongst others electrical conductivity, electron spin resonance, and re
ectivity measurements,
x-ray photoelectron and infrared spectroscopy, x-ray diffraction, and dilatometry. Fast
light-switching between phases has been observed in partially deuterated forms of Cu(DCNQI)2 on
sub-100-ps time scales. Furthermore, the phase transition is believed to be induced by a deformation
of the crystalline lattice and a charge density wave formation which are detectable in diffraction
images. Therefore we want to investigate this metal-to-insulator phase transition structurally and
temporally via ultrafast electron diffraction. The technique of ultrafast electron diffraction employs
the fundamentals of pump-probe spectroscopy: One of the two femtosecond pulsed laser beams
excites the thin, crystalline sample, while the other - after being converted into a pulsed electron
beam via the photoelectric effect - forms a diffraction image of the sample's lattice structure. The
arrival time of the two pulses at the sample can be varied by a few femtoseconds with respect to
each other enabling the resolution of ultrafast structural dynamics of the crystal's atomic lattice via electron diffraction. During the work presented in this thesis the sample preparation and characterisation
leading to a successful introduction of Cu(DCNQI)2 into our ultrafast electron diffraction
setup is presented. A diffraction pattern of comparable quality to that of a commercially available
transmission electron microscope was recorded of the metallic state of partially deuterated d6
Cu(DCNQI)2. Subsequent analysis of the obtained diffraction data and further studies of the low temperature state { including simulations as well as experiments { have narrowed down the factors
still making the diffraction pattern
evasive. Possible solutions to experimental challenges are proposed to make the documentation of
structural ultrafast dynamics in these organic molecular salts an attainable goal in the future. / AFRIKAANSE OPSOMMING: Organiese molekulêre soute het `n wye verskeidenheid van fisiese eienskappe wat chemies verander
kan word deur geringe variasie in die samestelling van die sout. Hierdie eienskappe sluit in `n hoë
graad van anisotropie, elektriese geleidingsvermoë wat strek van supergeleiding tot elektriese isolasie,
en strukturele veranderinge in die kristalstruktuur tydens eerste orde fase-oorgange wat veroorsaak
word deur geringe veranderinge in temperature, effektiewe druk en in sommige gevalle selfs lig.
Gevolglik is hierdie material besonder interessant vir die ontwikkeling van molekulêre elektronika
en ook as studiemateriaal in vastetoestandfisika. Die familie van koperdimetieldisianokinoondiimien
(Cu(DMe-DCNQI)2) soute vorm `n deel van die radikaal-anioon-sout subklas van organiese
molekulêre kristalle en is van besondere belang as gevolg van hulle buitengewone hoë elektriese
geleidingsvermoë in vergelyking met ander kwasi-eendimensionele organiese geleiers. Die metaal-na-isolator fase-oorgang van hierdie kristal word gekenmerk deur die verandering van die geleidingsvermoë met verskeie ordegroottes binne `n paar kelvin. Gedurende die laaste drie dekades is
die metaal en isolator fases, asook die oorgangsgedrag deeglik ondersoek met behulp van `n wye
verskeidenheid van metodes wat onder andere elektriese geleidingsvermoë, elektron-spin resonans
en reeksiemetings, x-straal fotoelektron en infrarooi spektroskopie, x-straal diffraksie en dilatometrie
insluit. Vinnige skakeling tussen fases is waargeneem in gedeeltelik gedeuteerde vorms van
Cu(DCNQI)2 op `n sub-100-ps tydskaal. Daar word verder geglo dat die fase-oorgang geïnduseer
word deur `n deformasie van die kristalstruktuur en die vorming van `n ladingsdigtheidgolf wat
meetbaar is in elektrondiffraksiebeelde. Om hierdie rede wil ons die metaal-na-isolator fase-oorgang
se struktuur- en tydafhanklikheid ondersoek deur gebruik te maak van ultra-vinnige elektron diffraksie.
Die tegniek van ultra-vinnige elektron diffraksie maak gebruik van die beginsels van pomp-toets
spektroskopie: Een van die twee femtosekonde laserpulse wek die dun kristallyne monster op, terwyl
die ander na omskakeling in `n elektronpuls via die foto-elektriese effek `n diffraksiebeeld van die
monster se kristalstruktuur vorm. Die aankomtyd van die twee pulse by die monster kan met `n
paar femtosekondes ten opsigte van mekaar verander word om die tydresolusie van die ultra-vinnige
strukturele dinamika van die kristal se atoomstruktuur deur elektrondiffraksie moontlik te maak. In
hierdie tesis word die monstervoorbereiding en karakterisering wat gelei het tot suksesvolle eksperimente
op Cu(DCNQI)2 in ons ultra-vinnige elektron diffraksie opstelling behandel. `n Diffraksie
patroon waarvan die kwaliteit vergelykbaar is met die van `n kommersiëel beskikbare transmissie
elektron mikroskoop is gemeet vir die metaalfase van gedeeltelik gedeuteerde d6 Cu(DCNQI)2.
Daaropvolgende analiese van die gemete diffraksiedata en verdere studies van die lae temperatuur
toestand wat simulasies sowel as eksperimente insluit het `n klein aantal faktore uitgewys wat
steeds die deteksie van die isolatorfase se ladingsdigtheidgolf se kenmerkende diffraksiepatroon verhoed.
Moontlike oplossings tot eksperimentele uitdagings word voorgestel om die dokumentering
van strukturele ultra-vinnige dinamika in hierdie organiese molekulêre soute `n haalbare toekomstige
doelwit te maak.
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Magneto-transporte no limite quântico em grafite e bismuto / Magnet transport in the quantum limit in graphite and bismuthMedina Pantoja, Juan Carlos 11 August 2018 (has links)
Orientadores: Iakov Veniaminovitch Kopelevitch, George Gershon Kleiman / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-08-11T13:15:15Z (GMT). No. of bitstreams: 1
MedinaPantoja_JuanCarlos_D.pdf: 3933664 bytes, checksum: 33f9dc730779c11f8c3d83b7ee0e56b4 (MD5)
Previous issue date: 2007 / Resumo: Esta tese é o resultado da investigação das propriedades elétricas e magnéticas de dois semimetais: bismuto (Bi) policristalino romboédrico e grafite pirolítica altamente orientada (HOPG). Inicialmente nós discutimos o efeito Hall no limite quântico, que acontece em amostras de grafite HOPG com certo grau de desordem e onde a desordem é reduzida. Em particular, a resistência Hall R xy (B) exibe platôs em amostras HOPG menos desordenadas que possuem uma característica quase-bidimensional e uma forte anisotropia. Em amostras com maior desordem é observada a ocorrência de picos em lugar de platôs, evidenciando, experimentalmente, a predição de T. Ando.
A condutância Hall reduzida Rxy (v) G0xy . fornece uma evidencia experimental para a coexistência de ambos os tipos de férmions de Dirac, normais e sem massa. Este resultado revela que o efeito Hall quântico inteiro e semi-inteiro tomam lugar simultaneamente na amostra HOPG. Nós encontramos as transições metal¿isolante (MIT) e isolante¿metal (IMT) induzidas por campo magnético em amostras de bismuto (Bi), quando o campo é aplicado paralelo ao eixo-c cristalográfico e observamos que estas transições têm enormes semelhanças com o MIT e IMT achados em HOPG e amostras monocristalinas Kish. As análises destes resultados experimentais sugerem que estas transições devem estar associadas à transição entre o estado metal de Bose (líquido não superfluido de pares de Cooper) e isolante excitônico. O aumento do momento diamagnético em bismuto e sua supressão próxima do campo crítico do MIT evidenciam a existência de correlações supercondutoras (metal de Bose) e excitônicas.
Nós reportamos a observação experimental do efeito Hall anômalo Hall (AHE) em amostras de bismuto e de grafite HOPG. Os resultados indicam que este AHE pode ser compreendido, autoconsistentemente, através de modelos de pareamento excitônico induzido pelo campo magnético, possivelmente, devido ao surgimento de ferromagnetismo / Abstract: This thesis is the result of the investigation of the electric and magnetic properties of two semimetals: highly oriented pyrolitic graphite (HOPG) and polycrystalline bismuth (Bi), rhomboedral. Initially we discuss the Hall effect in the quantum limit that occurs in HOPG samples with a certain degree of disorder and with reduced disorder. In particular, the Hall resistance R xy (B) exhibits plateaus in less disordered HOPG samples, which present characteristic quasi-bidimensional and strongly anisotropic. In more disordered samples there occur peaks instead of plateaus, experimentally evidencing the T. Ando's prediction. The reduced Hall conductance G xy (v)/ G 0xy gives evidence experimental for the coexistence of both massless and massive Dirac fermions. This result reveals that the integer- and semi-integer QHE take place simultaneously in HOPG samples. We observed magnetic field induced metal-insulator (MIT) and insulator-metal (IMT) transitions, when this field is in the crystallographic c-axis direction, and observed that these transitions are very similar to the MIT and IMT observed in HOPG and monocrystalline samples (Kish). The analysis of the experimental results suggests that these transitions must be associated with the transition from the Bose metal state (a non superfluid liquid of Cooper pairs) to the excitonic insulator. The increase of the diamagnetic momentum in bismuth and its suppression in the vicinity of the critical field of the MIT evidences the existence of superconducting (Bose metal) and excitonic correlations. We report the experimental observation of the anomalous Hall effect (AHE) in HOPG samples. This AHE may be autoconsistently understood by means of magnetic field induced excitonic pairing models, possibly, due to the onset of ferromagnetism / Doutorado / Física da Matéria Condensada / Doutor em Ciências
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