Ultrafast electron diffraction : source development, diffractometer design and pulse characterisation

Kassier, Gunther Horst (2010-12)

Thesis (PhD (Physics))--University of Stellenbosch, 2010.

Thesis

ENGLISH ABSTRACT: Ultrafast Electron Diffraction (UED) is a rapidly maturing field which allows investigation of the evolution of atomic arrangement in solids on timescales comparable to the vibrational period of their constituent atoms (~10-13 s). The technique is an amalgamation of conventional high energy electron diffraction methods and pump-probe spectroscopy with femtosecond (1 fs = 10-15 s) laser pulses. Ultrafast pulsed electron sources generally suffer from limitations on the attainable electron number per pulse (brightness) due to Coulomb repulsion among the electrons. In this dissertation, the design and construction of a compact UED source capable of delivering sub-300 fs electron pulses suitable for diffraction experiments and containing about 5000 electrons per shot is described. The setup has been characterised by measurement of the transverse beam size and angular spread, and through recording and analyzing an electron diffraction pattern from a titanium foil. Measurement of the temporal duration of fs electron pulses is not trivial, and a specialised compact streak camera operating in accumulation mode has been developed as part of this study. A sub-200 fs temporal resolution has been achieved, and the dependence of temporal duration on electron number per pulse was investigated for the current UED source. The observed trends correlate well with detailed electron bunch simulations. In order to investigate ultrafast processes on samples that cannot be probed repeatedly, it becomes necessary to significantly increase the brightness of current state of the art compact sources such as the one constructed in the present study. UED sources employing electron pulse compression techniques offer this possibility. Traditional pulse compression schemes based on RF cavities, while simple in principle, pose significant technical challenges in their realisation. The current thesis describes two novel UED pulse compression methods developed by the author: achromatic reflectron compression and pulsed cavity compression. Both concepts are expected to be easier to realise than conventional RF compression. Detailed simulations predict that such sources can attain a brightness improvement of more than one order of magnitude over compact sources that do not employ compression techniques. In addition, such sources show much promise for the attainment of pulse durations in the sub-100 fs range.

AFRIKAANSE OPSOMMING: Ultra vinnige elektron diffraksie is ‘n meettegniek wat tans in die proses is om vinnige ontwikkeling te ondergaan. Die tegniek het ten doel om strukturele omsettingsprosesse op ‘n lengteskaal van atoombindings en ‘n tydskaal van die vibrasie periode van atome in materie, ongeveer 10-13 s, te ondersoek. Dit word bewerkstellig deur die spasieresolusievermoë van gewone hoë energie elektron diffraksie met die tydresolusievermoë van femtosekonde (1 fs = 10-15 s) laserspektroskopie te kombineer. Die aantal elektrone per puls (intensiteit) van ultravinnige gepulsde elektronbronne word beperk deur die Coulomb afstootingskragte tussen die elektrone. Hierdie dissertasie beskryf die ontwerp en konstruksie van ‘n kompakte ultravinnige elektron bron. Die elektronpulse wat geproduseer word bevat tot 5000 elektrone per puls met ‘n tyd durasie van minder as 300 fs, en is geskik vir diffraksie eksperimente. Die aparaat is gekarakteriseer deur die volgende metings: elektronpulsdiameter, straaldivergensie, en ‘n titaan foelie se statiese diffraksie patroon. Dit is nie triviaal om die durasie van femtosekonde elektronpulse te meet nie, en n spesiale kompakte akkumulerende “streak camera” is vir die doeleindes van hierdie projek onwikkel. Die tydresolusie van hierdie “streak camera” is beter as 200 fs, en die afhanklikheid van die pulsdurasie wat deur die ultravinnige elektron bron geproduseer word as n funksie van die elektrongetal per puls is met behulp van hierdie toestel bepaal. Die resultate klop redelik goed met gedetaileerde simulasies van die elektron puls dinamika. Die karakterisasie van monsters wat nie herhaaldelik gemeet kan word nie vereis verkieslik ‘n nog hoër pulsintensiteit as wat met huidige bronne bereik kan word. ‘N verdere doelstelling is dus om ultravinnige elektron bronne te ontwikkel wat pulse met meer elektrone per puls kan genereer. Dit kan bewerkstellig word deur bronne wat van elektron puls kompressie tegnieke gebruik maak. Die tradisionele manier waarop dít gedoen word is deur middel van n kontinu gedrewe radio frekwensie holte. Hierdie metode gaan egter gepaard met aanmerklik hoë tegniese uitdagings. Om hierdie rede het die outeur twee alternatiewe puls kompressie konsepte ontwikkel: akromatiese reflektron kompressie and gepulsde holte kompressie. Albei konsepte sal waarskeinlik makliker wees om te realiseer as die tradisionele radio frekwensie kompressie, en is deur middel van gedetaileerde simulasies geverifiseer. Hierdie simulasies voorspel dat die intensiteit van genoemde bronne met ten minste n grooteorde meer kan wees as wat tans met kompakte ultravinnige elektron bronne moontlik is. Verder blyk dit dat sulke bronne n pulsdurasie van minder as 100 fs kan bereik.

Please refer to this item in SUNScholar by using the following persistent URL: http://hdl.handle.net/10019.1/5359
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