stfc corporate powerpoint template · •then, in the incoherent approximation, the real phonon...
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Good Vibrations Studying phonons with momentum resolved
spectroscopy
D.J. Voneshen
20/6/2018
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Overview
• What probe to use?
• Types of instruments.
• Single crystals example
• Powder example
• Thing I didn’t talk about because they were tricky.
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Select your probe.
• Lets say we want to measure the phonons in Aluminium.
• We need ~1 meV resolution.
• We also want information at many wavevectors.
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Select your probe.
Image pinched from:
http://www2.lbl.gov/MicroWorlds/ALSTool/EM
Spec/EMSpec2.html
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So, x-rays it is.
• Good news, we can produce lots!
• Bad news, for 1 Å wavelength the energy is around 107 meV.
• So for 1 meV resolution we wont have many left.
• Anything else?
Image pinched from: http://www.esrf.eu/
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Neutrons!
• Typical energy 10-100 meV.
• 1 Å wavelength.
• Hard to produce, but we wont have to waste many.
Image pinched from: http://www.esrf.eu/
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Where can we find neutrons?
Nuclear reactors Spallation sources
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Nuclear reactor, now what?
• Neutrons from reactor have many energies following some profile. Emitted continuously.
• Profile depends on what bit of the reactor you look at.
• For spectroscopy, we need to know how much energy was transferred so we need to know incident and final energies.
Image pinched from:
http://pd.chem.ucl.ac.uk/pdnn/inst3/reactors.htm
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In diffraction we use a monochromator for Ei….
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So why not use another!
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The triple axis spectrometer
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Spallation, what is different?
• Most spallation sources are pulsed.
• So time integrated flux is much lower.
• But, the pulsed nature gives a big advantage. We can use the neutron Time-Of-Flight (TOF) to determine either Ei or Ef.
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Chopper spectrometers
• For phonons we normally use the TOF to give us Ef.
• To get Ei we use a neutron absorber with a hole cut in it.
• By spinning this we get a “chopper”.
Chopper
Sample
Detector
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Chopper spectrometers
• For phonons we normally use the TOF to give us Ef.
• To get Ei we use a neutron absorber with a hole cut in it.
• By spinning this we get a “chopper”.
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A chopper spectrometer
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A return to x-rays
• We can do inelastic x-ray scattering.
• It’s basically a TAS.
• But, instead of varying angles, we vary the temperature of the monochromator!
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Doing a single crystal measurement
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Where do we look?
• We have two options.
– We could use diffuse scattering to tell us where the signal should be strong.
– We can think about the phonon scattering cross section.
• Lets go with the second.
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One phonon scattering cross section
𝐼 𝑄, 𝐸 =𝑁ℏ
2
1
𝜔 𝑄, 𝜈𝜈
𝑏𝑗
𝑚𝑗1 2
𝑗
𝑄 ∙ 𝑒𝑗 𝑘, 𝜈 𝑒𝑖𝑄∙𝑅𝑗𝑇𝑗 𝑄
2
× 𝑛 𝜔 𝑄, 𝜈 , 𝑇 + 1 𝛿 𝐸 + ℏ𝜔(𝑄, 𝜈)
+ 𝑛 𝜔 𝑄, 𝜈 , 𝑇 𝛿 𝐸 − ℏ𝜔(𝑄, 𝜈) .
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One phonon scattering cross section
𝐼 𝑄, 𝐸 =𝑁ℏ
2
1
𝜔 𝑄, 𝜈𝜈
𝑏𝑗
𝑚𝑗1 2
𝑗
𝑄 ∙ 𝑒𝑗 𝑘, 𝜈 𝑒𝑖𝑄∙𝑅𝑗𝑇𝑗 𝑄
2
× 𝑛 𝜔 𝑄, 𝜈 , 𝑇 + 1 𝛿 𝐸 + ℏ𝜔(𝑄, 𝜈)
+ 𝑛 𝜔 𝑄, 𝜈 , 𝑇 𝛿 𝐸 − ℏ𝜔(𝑄, 𝜈) .
We know this bit, its just the normal elastic scattering equation.
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One phonon scattering cross section
𝐼 𝑄, 𝐸 =𝑁ℏ
2
1
𝜔 𝑄, 𝜈𝜈
𝑏𝑗
𝑚𝑗1 2
𝑗
𝑄 ∙ 𝑒𝑗 𝑘, 𝜈 𝑒𝑖𝑄∙𝑅𝑗𝑇𝑗 𝑄
2
× 𝑛 𝜔 𝑄, 𝜈 , 𝑇 + 1 𝛿 𝐸 + ℏ𝜔(𝑄, 𝜈)
+ 𝑛 𝜔 𝑄, 𝜈 , 𝑇 𝛿 𝐸 − ℏ𝜔(𝑄, 𝜈) .
This looks horrible, but its just telling us that we have more phonons at
high temperatures (they follow Bose-Einstein statistics).
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One phonon scattering cross section
𝐼 𝑄, 𝐸 =𝑁ℏ
2
1
𝜔 𝑄, 𝜈𝜈
𝑏𝑗
𝑚𝑗1 2
𝑗
𝑄 ∙ 𝑒𝑗 𝑘, 𝜈 𝑒𝑖𝑄∙𝑅𝑗𝑇𝑗 𝑄
2
× 𝑛 𝜔 𝑄, 𝜈 , 𝑇 + 1 𝛿 𝐸 + ℏ𝜔(𝑄, 𝜈)
+ 𝑛 𝜔 𝑄, 𝜈 , 𝑇 𝛿 𝐸 − ℏ𝜔(𝑄, 𝜈) .
Phonons at higher energy are weaker.
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One phonon scattering cross section
𝐼 𝑄, 𝐸 =𝑁ℏ
2
1
𝜔 𝑄, 𝜈𝜈
𝑏𝑗
𝑚𝑗1 2
𝑗
𝑄 ∙ 𝑒𝑗 𝑘, 𝜈 𝑒𝑖𝑄∙𝑅𝑗𝑇𝑗 𝑄
2
× 𝑛 𝜔 𝑄, 𝜈 , 𝑇 + 1 𝛿 𝐸 + ℏ𝜔(𝑄, 𝜈)
+ 𝑛 𝜔 𝑄, 𝜈 , 𝑇 𝛿 𝐸 − ℏ𝜔(𝑄, 𝜈) .
This is the only “complicated” bit. 𝑒 is the phonon eigenvector,
physically, you can think of this as the direction atoms are
moving in.
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Things to remember
• Phonons are strong when 𝑄 is parallel to direction of atomic motion.
• Phonon intensity goes up with 𝑄2.
• Phonons are weaker at high energy.
• Strong Bragg reflections often have strong phonons around them.
• Phonons can be stronger at high temperature (but care needed here).
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Measuring a longitudinal acoustic phonon
We want to measure a longitudinal phonon along 00L.
Which peak would be best to measure around?
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Measuring a longitudinal acoustic phonon
We want to measure a longitudinal phonon along 00L.
Which peak would be best to measure around?
𝑄
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Measuring a transverse acoustic phonon
What about a transverse phonon?
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Measuring a transverse acoustic phonon
What about a transverse phonon? 𝑄
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Exploiting 𝑸 ∙ 𝒆, an example
• We were looking for a
phonon around 12
meV.
• However, the
background from the
cryostat/mount was
huge.
• Rotate sample 90°.
Suppresses, phonon
but background
unchanged
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Exploiting 𝑸 ∙ 𝒆, an example
• We were looking for a
phonon around 12
meV.
• However, the
background from the
cryostat/mount was
huge.
• Rotate sample 90°.
Suppresses phonon
but background
unchanged
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TOF, what do we get?
• With TOF we get an excellent survey.
• However, we are normally struggling for statistics.
• Data here was at 300 K counted for two days.
• Need at least 1 cm3 single crystal.
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Comparison to DFT
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A quick example of this with IXS and INS
• We were interested in Na0.8CoO2 as a thermoelectric.
• We wanted to show that the Na vacancy order has a big impact on the phonons.
• We also wanted to relate this to the thermal conductivity.
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A quick example of this with IXS and INS
• We were interested in Na0.8CoO2 as a thermoelectric.
• We wanted to show that the Na vacancy order has a big impact on the phonons.
• We also wanted to relate this to the thermal conductivity.
Voneshen, D.J. et al. Nature Mater. 12, 1028 (2013).
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A quick example of this with IXS and INS
• We were interested in Na0.8CoO2 as a thermoelectric.
• We wanted to show that the Na vacancy order has a big impact on the phonons.
• We also wanted to relate this to the thermal conductivity.
Voneshen, D.J. et al. Nature Mater. 12, 1028 (2013).
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A quick example of this with IXS and INS
• We were interested in Na0.8CoO2 as a thermoelectric.
• We wanted to show that the Na vacancy order has a big impact on the phonons.
• We also wanted to relate this to the thermal conductivity.
Voneshen, D.J. et al. Nature Mater. 12, 1028 (2013).
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A quick example of this with IXS and INS
• We were interested in Na0.8CoO2 as a thermoelectric.
• We wanted to show that the Na vacancy order has a big impact on the phonons.
• We also wanted to relate this to the thermal conductivity.
Voneshen, D.J. et al. Nature Mater. 12, 1028 (2013).
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Powders!
• Good news, powders are simpler!
• Much simpler.
• With them we can extract the neutron weighted phonon density of states.
• But, going beyond that is hard.
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Powders, what are we doing? • We are averaging over a
sphere at some 𝑄 .
• So, for small values of 𝑄
we are covering just a few
(or even 1) Brillouin zones.
• But, for large 𝑄 we are
covering many zones,
essentially capturing
everything in 1 shot.
• This means for high 𝑄 we
can no longer see the effect
of 𝑸 ∙ 𝒆 and the signal is the
same as incoherent
scattering.
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Powders, what are we doing? • We are averaging over a
sphere at some 𝑄 .
• So, for small values of 𝑄
we are covering just a few
(or even 1) Brillouin zones.
• But, for large 𝑄 we are
covering many zones,
essentially capturing
everything in 1 shot.
• This means for high 𝑄 we
can no longer see the effect
of 𝑸 ∙ 𝒆 and the signal is the
same as incoherent
scattering.
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The neutron weighted phonon density of states
• We normally correct the data for the effects of Bose statistics, 1 𝜔 and 𝑄2.
• Then, in the incoherent approximation, the real Phonon Density of States (PDOS) is related to the PDOS we see via the above.
• This means we cannot obtain the true PDOS for anything other than a monoatomic system.
𝑃𝐷𝑂𝑆𝑛𝑒𝑢𝑡 𝐸 = 𝐴 𝑏𝑗2
𝑚𝑗𝑗
𝑃𝐷𝑂𝑆𝑗 𝐸 ,
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A quick powder example
• Another thermoelectric.
• This time, the idea was that superionic diffusion would dramatically change the phonons, leading to a very low thermal conductivity.
• It doesn’t. Instead the low thermal conductivity is caused by regular anharmonic effects.
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A quick powder example
• Another thermoelectric.
• This time, the idea was that superionic diffusion would dramatically change the phonons, leading to a very low thermal conductivity.
• It doesn’t. Instead the low thermal conductivity is caused by regular anharmonic effects.
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A quick powder example
• Another thermoelectric.
• This time, the idea was that superionic diffusion would dramatically change the phonons, leading to a very low thermal conductivity.
• It doesn’t. Instead the low thermal conductivity is caused by regular anharmonic effects.
![Page 45: STFC Corporate PowerPoint Template · •Then, in the incoherent approximation, the real Phonon Density of States (PDOS) is related to the PDOS we see via the above. •This means](https://reader034.vdocuments.us/reader034/viewer/2022050312/5f73eca5a559d60ed00c81c5/html5/thumbnails/45.jpg)
A quick powder example
• Another thermoelectric.
• This time, the idea was that superionic diffusion would dramatically change the phonons, leading to a very low thermal conductivity.
• It doesn’t. Instead the low thermal conductivity is caused by regular anharmonic effects.
Phys. Rev. Lett. 118, 145901
![Page 46: STFC Corporate PowerPoint Template · •Then, in the incoherent approximation, the real Phonon Density of States (PDOS) is related to the PDOS we see via the above. •This means](https://reader034.vdocuments.us/reader034/viewer/2022050312/5f73eca5a559d60ed00c81c5/html5/thumbnails/46.jpg)
The thing I was scared to talk about
• Measuring phonon dispersions from time resolved diffuse scattering.
• Still very early, but really cool.
Nature Communications, 7, 12291
(2016)
![Page 47: STFC Corporate PowerPoint Template · •Then, in the incoherent approximation, the real Phonon Density of States (PDOS) is related to the PDOS we see via the above. •This means](https://reader034.vdocuments.us/reader034/viewer/2022050312/5f73eca5a559d60ed00c81c5/html5/thumbnails/47.jpg)
The thing I was scared to talk about
• Measuring phonon dispersions from time resolved diffuse scattering.
• Still very early, but really cool.
Nature Communications, 7, 12291
(2016)
![Page 48: STFC Corporate PowerPoint Template · •Then, in the incoherent approximation, the real Phonon Density of States (PDOS) is related to the PDOS we see via the above. •This means](https://reader034.vdocuments.us/reader034/viewer/2022050312/5f73eca5a559d60ed00c81c5/html5/thumbnails/48.jpg)
Summary
• Momentum resolved spectroscopy is great!
• We have options, TOF for surveys, TAS for focussed studies and x-rays for tiny samples.
• Remember that the intensity of phonons depends on
𝑄 ∙ 𝑒 2
.
• If you have questions, email me! [email protected]