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Optical Spectroscopy of Condensed Matter
Dmitry Smirnov Maglab Users Summer School May 2016
Optical Spectroscopy of Condensed Matter
Dmitry Smirnov Maglab Users Summer School May 2016
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Outline
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Study of interaction of matter with light (or photons)Spectrum : response of matter to EM radiation as a function of energy
Electromagnetic spectrum, after a diagram from SURA(D.Tanner, Optical Effects in Solids)
P&9%2'*)&(%-"+)%+&.*/*01.3*P&9%2'*)&(%-"+)%+&.*/*01.3*
Study of interaction of matter with light (or photons)Spectrum : response of matter to EM radiation as a function of E (or wn, or !)
!" #" !$" !#" %$" %#" !$$"
0.5 1 1.5 2
UV Near IR
THz Mid IR Far IR
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!""#$"% &'% ('% !'% )*% )!% (%
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),(+$% !+$$% ),(+% "&'% $!'% *$*% ),,%L(8&("2-7"(*CTE
P&9%2'*)&(%-"+)%+&.*/*01.3*
Study of interaction of matter with light (or photons)Spectrum : response of matter to EM radiation as a function of E (or wn, or !)
P&9%2'*)&(%-"+)%+&.*/*01.3*
Study of interaction of matter with light (or photons)Spectrum : response of matter to EM radiation as a function of E (or wn, or !)
Visiblelight
Pene
tratio
n de
pth
into
wat
er
Wavelength1 km 1 m 1 mm 1 µm 1 nm
UVX-ray
Radio Microwave
IR
1 mm
1 km
1 µm
1 m Proto-ocean protected early life from the Sun’s UV
Photosynthesis harvesting Vis range photons
Vision in the visible range
Spectroscopist’s take on life’s development on Earth
U"2&1($(*U"2&1#-(
!1+$+$)*
?2$>27*'(D(')
Probe various structural, electronic and magnetic states/excitations in matter
P&9%2'*)&(%-"+)%+&.*/*01.3*
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Probe various structural, electronic and magnetic states/excitations in matter
introduce tunable length scale
-
+
B
lB
!
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EZ
introduce length scale tunable
lm ��
�eB
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Bnm 10T ! 8 nm
40T ! 4 nm
1T ! 25 nm
!
m* m0 ~ 0.1
… tunable orbital and electron spin energy scales
m* m ~ 0.1
��c = � eB
m�
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⇠ 1 meV/T
!
m* m0 ~ 0.1
X((82$*($("<.F*
⇠ 0.1 meV/T
!
EZ = gµBB
… interaction energy scale
!
Ee"e #e2
$lB#50meV$
B 10T ! 15 meV !=10
breaks time-reversal symmetrybreaks time-reversal symmetry !5*/(.'#NO%;4+,!!!?7
High magnetic fields in condensed matter physics
High magnetic fields in condensed matter physics
introduces tunable length scale
-
+
B
lB
!
g
ELL
EZ
introduces tunable length scale
lm ��
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=25.6⇥
Bnm 10T ! 8 nm
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!
m* m0 ~ 0.1
… tunable orbital and electron spin energy scales
m* m ~ 0.1
��c = � eB
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⇠ 1 meV/T
!
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⇠ 0.1 meV/T
!
EZ = gµBB
… interaction energy scale
!
Ee"e #e2
$lB#50meV$
B 10T ! 15 meV !=10
breaks time-reversal symmetrybreaks time-reversal symmetry !5*/(.'#NO%;4+,!!!?7
5*/(.;4!P.8@!$.@34.+!!'&.!(Y(%9D(*>#8($)#+$2'#-.
DO
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Energy
DO
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Energy
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QZI'#[(B
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Raman scatteringPhoto-Luminescence (PL)
Reflection and Transmission Uv, Vis, IR, THz
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Temperature
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Excitation spectroscopy
Broad-band spectroscopy
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Vis spectroscopy
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Physics spectroscopic probe of structural, electronic and magnetic states or excitations
Physics:
Chemistry
analytical tool to determine composition, structure, ...Biology…
http://www.cryst.ehu.es/html/lekeitio-docs/mihailova-presentation.pdf
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P&9%2'**)&(%-"+)%+&.*/*L(%1$#B7()
• Frequency domain spectroscopy (dispersive spectrometers)
UV-Vis-NIR spectral region : ~ 1 eV scale
• Raman spectroscopy
• Fourier transform infrared (FTIR) spectroscopyIR-THz spectral region ~ 1-1000 meV
UV-Vis-NIR (~ 1eV) probe of low energy excitations (~meV)
Conventional (dispersive) optical spectrometer based on a broadband source and dispersive elements (prism, grating)
^<!%$#43$.@!6.!*!'$9*(/38*$!/8*++!%$9+6!'#!'$0!'&.$.B9'&!'&.!4.8.Q$*'.@!%&.(#6.(*!#1!4#8#$+F^!"_.B'#(G!K]]\)
Price in 1704: £1Price today: $62,000
Frequency domain spectroscopy (UV-VIS-NIR)
Frequency domain spectroscopy (UV-VIS-NIR)
Conventional (dispersive) optical spectrometer based on a broadband source and dispersive elements (prism, grating)
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s(") - complex transmission/reflection coefficient
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Isample(!) / |s(!)|2|E(!)|2
|s(!)|2 =Isample(!)
Iref (!)
Frequency domain spectroscopy (UV-VIS-NIR)
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Czerny-Turner spectrometer for Vis spectroscopy, Raman scattering and PL
William Herschel, February 11th 1800
F.W. Herschel, Phil. Trans. Royal Soc. London 90, 49 (1800).
Birth of IR spectroscopy
Infrared spectroscopy
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ion
700 600 500 400 300 200 100wavenumber (cm-1)
Tran
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ion
700 600 500 400 300 200 100wavenumber (cm-1)
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3.Referencing
1. Interferogram
T (⌫) =Sair(⌫)
Svac(⌫)
Fourier transform infrared (FTIR) spectroscopy
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1. Interferogram
Fourier transform infrared (FTIR) spectroscopy
T (⌫) =Sair(⌫)
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What is special about IR spectroscopy ?
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Timeline
1923 – Inelastic light scattering is predicted by A. Smekel1928 – Landsberg and Mandelstam see unexpected frequency shifts in scattering from quartz1928 – C.V. Raman and K.S. Krishnan see “feeble fluorescence” from neat solvents 1930 – C.V. Raman wins Nobel Prize in Physics
4<*2"%*'28&?]d]!+4*C.$9(/
"A new type of Secondary Radiation", Nature, 1928
1960 – Invention of laser made Raman experiments more effective and meaningful
1964 – Townes, Basov, Prochorov win Nobel Prize in Physics for the invention of the maser and the laser
Here again, Ted Maiman was the first to have a first working laser!
Raman spectroscopy
What is special about Raman spectroscopy ?
H(".*'+5*)#<$2'*a*Q**#$**Qbc*I**QbQd*&1+-+$)*#)*)%2O("(>*#$('2)9%2''.
Devereaux and Hackl,RMP. 79, 175 (2007)10-7
< 10-9Ram
an e
ffici
ency
What is special about Raman spectroscopy ?
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CW optical magneto-spectroscopy @ MagLab
FTIR Magneto-Spectroscopy
d.($9R+.(!!"#$%G!!7He!Qbd!"])G!M]JIMI!"LMKM)
Interaction-induced Shift of the CR in Monolayer Graphene
CW optical magneto-spectroscopy @ MagLab
Spatially resolved PL and Raman spectroscopy
Sample plate
x-y travel : ~2.5mmPiezo-stages
z travel : ~3mm
Excitationfiber
Collectionfiber
Working distance:~1.5mm
CW optical magneto-spectroscopy @ MagLab
Spatially resolved PL and Raman spectroscopy
!"#$%&'()*+&
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J<:*+&<$-6/&%0C6'*&K</>&(&LM&A<'/*+& Magnet Temperatures Techniques
45T 1.5K-300K PL, Raman,
35T 1.5K-300K PL, Raman,
31T (cell#9)
300mK-70K 1.5K-300K
PL, Raman, spatially resolved
18T (SCM2)
300mK-70K 1.5K-300K
PL, Raman, spatially resolved
17.5T (SCM3)
4K-100K PL, Raman, spatially resolved
14.5T (EMR)
4.5K-300K PL, Raman, spatially resolved
Semiconducting monolayer TMDs
hνi
E
k
Photoluminescence (PL)
EPL
Neutral exciton
Charged exciton (trion)
e-h+
e-h+ EPL
e-
h+
Charged exciton (trion)
e-
h+
e-EPL
TMDs: Strongly bond excitons ! EX0: ~ 500 meVEX!: ~ 30 meV
h"excit
h"PL
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Charged excitons: MoSe2 vs. WSe2
MoSe2
WSe2
-30
-15
0
15
30
Fiel
d (T
)
1.681.661.641.621.60Energy (eV)
B
!+ X0X! MoSe2: intervalley
WSe2: intravalley
-30
-20
-10
0
10
20
30
Field(
T)
1.761.721.68Energy(eV)
>i >M
I\h
B
CW optical magneto-spectroscopy @ MagLab
Magnet-Raman spectroscopy: Examples
Charge-lattice-spin coupling in Co[N(CN)2]2
Brinzari, T. V. et al. Phys. Rev. Lett. 111, 047202 (2013).
LAB PRACTICALS - Optical spectroscopy of Al203
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LAB PRACTICALS - Optical spectroscopy of Al203
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Two Al2O3 groups per unit cell
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LAB PRACTICALS - Optical spectroscopy of Al203
Raman scattering
H*6*(!*4;E.!6#@.+,!J
LWK/!![!\-/!!k!!WK/!![!WK/!![!\-/!
!4"4 "4
LAB PRACTICALS - Optical spectroscopy of Al203
IR spectroscopy1.0
0.8
0.6
0.4
0.2
0.0
Tran
smiss
ion
1500 1000 500 0wavenumber (cm-1)
Restrahlen band
<H!*4;E.!6#@.+,!]
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!4 "4
1500 1000 500 0wavenumber (cm-1)
1.0
0.8
0.6
0.4
0.2
0.0
Reflection
LAB PRACTICALS - Optical spectroscopy of Al203
Photoluminescence
250x103
200
150
100
50
0
inte
nsity
(co
unts
/sec
)
45004450440043504300
wavenumber (cm-1)
250x103
200
150
100
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0
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(co
unts
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)
45004450440043504300
wavenumber (cm-1)
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LAB PRACTICALS - Optical spectroscopy of Al203
Excitation spectroscopy : PL vs. Raman
250x103
200
150
100
50
0
inte
nsity
(co
unts
/sec
)
50004000300020001000
wavenumber (cm-1)
250x103
200
150
100
50
0
inte
nsity
(co
unts
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)
50004000300020001000
wavenumber (cm-1)
\VL(6!.>49'*;#(
450
400
350
300
250
200
650600550500450400350rel wavenumbers (cm-1)
Optical Spectroscopy of Condensed Matter
Dmitry Smirnov Maglab Users Summer School May 2016
Optical Spectroscopy of Condensed Matter
Dmitry Smirnov Maglab Users Summer School May 2016
• !"#$%#&'()*+,*)&(%-"+)%+&.*/*012-3*01.3*4+53*• 6$)-"78($-29+$*
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Outline
@ A"(B7($%.*>+82#$*)&(%-"+)%+&.*C>#)&(")#D(*)&(%-"+8(-(")EF**GHIH#)IJ6K*@ A+7"#("*-"2$),+"8*#$,"2"(>*CAL6KE*)&(%-"+)%+&.F*J6KI;6KIA6KML4N*@ K282$*)%2O("#$<*2$>*!1+-+'78#$()%($%(