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Spectroscopy with Free Electron Lasers David Bernstein SASS Talk January 28 th , 2009

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Page 1: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Spectroscopy with Free Electron Lasers

David BernsteinSASS Talk

January 28th, 2009

Page 2: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Overview

• Who am I?!• What is FLASH?!• The promise of Free Electron Lasers

(FELs)• The Trouble with Spectroscopy• Sample Fabrication• The Actual Experiment• Data Analysis

Page 3: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Who am I?!

Page 4: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Who am I?!

Page 5: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Who am I?!

Page 6: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Who am I?!

Page 7: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

What is FLASH?!Free election LASer at Hamburg

BOGUS ACRONYM

Page 8: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The promise of FELs

• Intense pulses containing upto 1012

photons• Short temporal pulse widths, on the order

of 50-100 fs• Represents a 108 improvement in peak

intensity over 3rd generation synchrotron sources

Page 9: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The promise of FELs

H. Chapman, et.al., Nature Physics, 2, 839 (2006)

Page 10: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The trouble with Spectroscopy

• Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy:– Commonly used at synchrotrons– X-rays excite a core electron into a valence

state– Element Specific– Sensitive to bond angle and length– Can probe subsystems such as spin

(magnetic) and charge (electric) subsystems independently

Page 11: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The trouble with Spectroscopy

http://unicorn.mcmaster.ca/research/stxm-intro/STXM_poly3.JPG http://ssrl.slac.stanford.edu/stohr/xmcd.htm

Page 12: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The trouble with Spectroscopy• So whats the problem?

– FELs are difficult to tune (sort of…)

– FEL radiation is produced by Self-Amplified Spontaneous Emission. This process is inherently stochastic.

– FEL radiation is therefore characterized by humungous fluctuations in relevant beam parameters such as energy, position, intensity and mode profile.

http://hasylab.desy.de/facilities/flash/machine/how_it_works/sase_self_amplified_spontaneous_emission/index_eng.html

Page 13: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The trouble with Spectroscopy

To deal with these problems… we need to capture as much information as possible on a shot-by-shot basis.

Page 14: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The experiment!

Grating disperses the beam by 0.3-0.4eV/mm in the vertical direction

Different parts of the sample get hit with different energy photons

We record an entire spectrum in each shot

Page 15: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

The experiment!

Page 16: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Sample Fab

• In order to do this, we designed a sample with large silicon nitride windows in a silicon wafer.

• Half of the window is covered by the metal, the other half is blank nitride. This records the “Io” information

METAL Si3N4 membrane

Page 17: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Sample Fab

• Samples consist of 100nm thick silicon nitride windows sitting on top of silicon wafers

• 100nm of metal (LaMnO or Aluminum) deposited via shadow mask

Page 18: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Analytical Challenges• We need to linearize

the detector• We need to normalize

the transmitted intensity by the incident intensity based on the information we have from a little sliver of window next to the sample.

Page 19: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Linearizing the DetectorWe recorded a run with no sample in the beamline. A gold mesh upstream of the sample chamber recorded total pulse intensity:

We also have the intensity on each pixel recorded by the (very nonlinear) detection scheme consisting of a Ce:YAG crystal imaged by an intensified CCD camera.

What we want to know is the true intensity incident on a given pixel,

Page 20: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Linearizing the DetectorTo do this, we use the ansatz:

We then construct an error function summed over all images,

…and iteratively adjust our parameters, ai, until the error function reaches an acceptable value.

Page 21: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Linearizing the Detector

Page 22: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Normalizing the DataWe calculate the mode intensity in the x-direction by summing over y for each value of x.

Now the spectra are flat in the x-direction. We then normalize by the average value at each y point to get the full normalized spectrum.

Page 23: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Normalizing the DataFor this to work, we can only accept images with a single mode in the x-direction. In other words, we have good shots and bad shots.

GOOD SHOT BAD SHOT

Page 24: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Finally… the spectra!

Page 25: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Finally… more spectra!

Page 26: Spectroscopy with Free Electron Lasers · The trouble with Spectroscopy • Near Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy: – Commonly used at synchrotrons –

Acknowledgements

• Stanford/SSRL/Pulse– Yves Acremann– Andreas Scherz– Mark Burkhard– Jo Stohr

• Stanford Nanofabrication Laboratory– Mahnaz Mansourpour

• DESY/UH– Bill Schlotter– Martin Beye, – Torben Beeck– F. Sorgenfrei– Annette Pietzch– Wilfred Wurth– A Foehlisch