Ultrafast structural dynamics in 4Hb-TaSe2 observed by femtosecond electron diffraction

Erasmus, Nicolas (2013-03)

Thesis (PhD)--Stellenbosch University, 2013.

Thesis

ENGLISH ABSTRACT: In this thesis the structural dynamics, upon photo-excitation, of the charge-densitywave (CDW) material 4Hb-TaSe2 is investigated on the time-scale of atomic motion and simultaneously on the spatial-scale of atomic dimensions. CDW materials have been of interest since their discovery in the 1970’s because of their remarkable non-linear and anisotropic electrical properties, gigantic dielectric constants, unusual elastic properties and rich dynamical behaviour. Some of these exotic properties were extensively investigated in thermal equilibrium soon after their discovery but only recently have ultrafast techniques like femtosecond spectroscopy become available to study their out-of-equilibrium behaviour on the time-scale of atomic motion. By studying their behaviour on this time-scale a more in-depth understanding of their macroscopic properties can be gained. However, to do investigations on the atomic time-scale and simultaneously directly observe the evolution of the atomic arrangements is another challenge. One approach is through the previously mentioned technique of femtosecond pump-probe spectroscopy but converting the usual ultrashort optical probing source to an ultrashort electron or x-ray source that can diffract off the sample and reveal structural detail on the atomic level. Here, the femto-to-picosecond out-of-equilibrium behaviour upon photo-excitation in 4Hb-TaSe2 is investigated using an ultrashort electron probe source. Two variations of using an electron probe source are used: conventional scanning Femtosecond Electron Diffraction (FED) and a new approach namely Femtosecond Streaked Electron Diffraction (FSED). The more established FED technique, based on femtosecond pumpprobe spectroscopy, is used as the major investigating tool while the FSED technique, based on ultrafast streak camera technology, is an attempt at broadening the scope of available techniques to study structural dynamics in crystalline material on the subpicosecond time-scale. With these two techniques, the structural dynamics during the phase transition from the commensurate- to incommensurate-CDW phase in 4Hb-TaSe2 is observed through diffraction patterns with a temporal resolution of under 500 fs. The study reveals strong coupling between the electronic and lattice systems of the material and several time-constants of under and above a picosecond are extracted from the data. Using these time-constants, the structural evolution during the phase transition is better understood and with the newly gained knowledge, a model of all the processes involved after photo-excitation is proposed.

AFRIKAANSE OPSOMMING: In hierdie tesis word die strukturele dinamika van die lading-digtheid-golf (LDG) materiaal 4Hb-TaSe2 ondersoek op die tydskaal van atomiese bewegings en gelyktydig op die ruimtelikeskaal van atomiese dimensies. LDG materie is al van belang sedert hul ontdekking in die 1970’s as gevolg van hul merkwaardige nie-lineêre en anisotrope elektriese eienskappe, reuse diëlektriese konstantes, ongewone elastiese eienskappe en ryk dinamiese gedrag. Sommige van hierdie eksotiese eienskappe is omvattend ondersoek in termiese ewewig kort na hul ontdekking, maar eers onlangs is dit moontlik deur middle van ultravinnige tegnieke soos femtosekonde spektroskopie om hulle uit-ewewigs gedrag te bestudeer op die tydskaal van atomiese beweging. Deur die gedrag op hierdie tydskaal te bestudeer kan ’n meer insiggewende begrip van hul makroskopiese eienskappe verkry word. Om ondersoeke in te stel op die atomiese tydskaal en gelyktydig direk die evolusie van die atoom posisie te waarneem is egter ’n moeilike taak. Een benadering is deur middle van femtosekonde “pump-probe” spektroskopie maar dan die gewone optiese “probe” puls om te skakel na ’n electron of x-straal puls wat van die materiaal kan diffrak en dus strukturele inligting op die atomiese vlak kan onthul. Hier word die femto-tot-pico sekonde uit-ewewig gedrag in 4Hb-TaSe2 ondersoek met behulp van elektron pulse. Twee variasies van die gebruik van ’n elektron bron word gebruik: konvensionele “Femtosecond Electron Diffraction” (FED) en ’n nuwe benadering, naamlik, “Femtosecond Streaked Electron Diffraction” (FSED). Die meer gevestigde FED tegniek, wat gebaseer is op femtosekonde “pump-probe” spektroskopie, word gebruik as die hoof ondersoek metode terwyl die FSED tegniek, wat gebaseer is op die ultra vinnige “streak camera” tegnologie, ’n poging is om beskikbare tegnieke uit te brei wat gebruik kan word om strukturele dinamika in materie te bestudeer op die sub-picosekonde tydskaal. Met behulp van hierdie twee tegnieke, word die strukturele dinamika tydens die fase oorgang van die ooreenkomstige tot nie-ooreenkomstige LDG fase in 4Hb-TaSe2 deur diffraksie patrone met ’n tydresolusie van minder as 500 fs waargeneem. Die studie toon ’n sterk korrelasie tussen die elektroniese sisteem en kristalrooster. Verskeie tydkonstantes van onder en bo ’n picosekonde kon ook uit die data onttrek word en gebruik word om die strukturele veranderinge beter te verstaan. Hierdie nuwe kennis het ons in staat gestel om ’n model van al die betrokke prosesse voor te stel.

Please refer to this item in SUNScholar by using the following persistent URL: http://hdl.handle.net/10019.1/79934
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