Proprietary | Lake Shore Cryotronics, Inc.
Terahertz Materials Characterization
in Extreme Environments
Emerging Tools for Materials Research
David R. Daughton
Applications Scientist
Proprietary | Lake Shore Cryotronics, Inc.
THz Systems
Probe Stations
Hall Effect
Measurement
Systems (HMS)
Magnetometers
(VSM/AGM)
Permanent Magnets
High Density Recording Media
Mineral Magnetism
Electronic thin films
Organic Electronics
Spintronics
Nanowires
Magnetoresistance
Organic electronics
Thermoelectrics
Solar Cells
HEMTS
Materials Characterization Systems
2
Systems
Measure electrical
properties of devices and
materials in temperature-
controlled environment
AC/DC measurements:
 Hall mobilities
 Carrier concentration
 Carrier type
Measure magnetic properties:
 Hysteresis M(H) loops
 FORC curves
 Temperature dependencies
Fully integrated for material properties:
 Electronic
 Magnetic
 Chemical
Proprietary | Lake Shore Cryotronics, Inc.
Why THz?
3
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
5
1012 Hz
2.5 THz ~ 10 meV
 Alignment of THz energy levels
with phenomena of interest
– Vibrational resonances
– Novel spin resonances
– Free carrier motion in
semiconductors
Proprietary | Lake Shore Cryotronics, Inc.
Materials Phenomena
6
The Electromagnetic Spectrum
D. N. Basov, et al.
“Electrodynamics of correlated electron materials”
Rev. Mod. Phys. 85(2), 471 (2011).
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
 THz wavelengths match the feature
sizes of development-grade
electronic materials
– Non-contact electronic characterization
– Novel magnetic materials
7
1012 Hz
0.6 THz ~ 0.5 mm
2”
10 mm
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
 Coupling to spin-based
materials at THz frequencies
– High speed computing
paradigms
– May require large fields
8
1012 Hz
0.2 THz ~7 T
Nagashima, T.; Nishitani, J.; Kozuki, Kohei, "Lasers & Electro Optics & The Pacific
Rim Conference on Lasers and Electro-Optics, 2009. CLEO/PACIFIC RIM '09.
Conference on , vol., no., pp.1,2, 30-3 Aug. 2009
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
9
1012 Hz
6.5 THz ~ 300 K
480 500 520 540 560 580
0.1
1
THzTransmission
Frequency (GHz)
5.8 K
75 K
150 K
a-Lactose
THzTransmission
 Cryogenic temperatures
– Homogeneous broadening of
vibrational resonances
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
10
1012 Hz
 Cryogenic temperatures
– Homogeneous broadening of
vibrational resonances
– Temperature dependent carrier
concentration and mobility
6.5 THz ~ 300 K
Proprietary | Lake Shore Cryotronics, Inc.
Equivalent Scales for THz
11
1012 Hz
10 meV7 T 300 K0.5 mm
 Alignment of THz energy levels with phenomena of interest
 THz wavelengths match the feature sizes of development-
grade electronic materials
 Coupling to spin-based materials at THz frequencies
 Cryogenic temperatures
Proprietary | Lake Shore Cryotronics, Inc.
THz System Product Challenges
 THz performance suitable for materials characterization
– Continuous tuning over bandwidth
– Spectral resolution
 Ability to characterize samples while exposed to variable
cryogenic temperatures and magnetic fields
 Affordable THz-based measurement platform
 Robust design
 Proceduralized experimental methods and reliable
analysis of the spectral results
– Convenient sample insertion without complicated alignment
– Enable materials developers to rapidly begin productive research
12
Proprietary | Lake Shore Cryotronics, Inc.
Filling the THz Gap
13
The Electromagnetic Spectrum
0 10 20 30 40 50
0
ElectricField(a.u.)
Time (ps)
Proprietary | Lake Shore Cryotronics, Inc.
THz with cryogenics & magnetics
14
 Many materials of interest for THz
require variable temperature
and/or high magnetic fields
 Optical cryostats are the standard
approach
– THz generation outside the
environment
– Must pass optical energy through
windows, cutting signal power and
spectral distortion
 Not ideal for THz spectroscopies
Proprietary | Lake Shore Cryotronics, Inc.
Variable Temperature and
High Magnetic Field THz Platform
15
Cryostat Sample space
±9 T magnet
Removable
sample insert
Cryo-compatible
THz emitter with
collimating optics
Rotatable
sample stage
(10 mm × 10 mm)
Thermally stable
optical
alignment stages
Proprietary | Lake Shore Cryotronics, Inc.
Application software
for turnkey operation
 Experiment setup/run
 Analysis of spectral data
 Calculation of material properties
Integrated THz System Details
16
Fiber-based optical
platform for CW THz
spectroscopy
 CW THz spectrometer instrument
 Amplitude and phase detection from
200 GHz to 1.5 THz
 Spectral resolution under 500 MHz
 Circularly polarized light
Integrated controls
 Model 336 cryogenic
temperature controller
 Model 625 superconducting
magnet power supply
Superconducting magnet
 High magnetic fields to ±9 Tesla
Integrated cryostat & insert
 Variable temperatures from 5 K to 300 K
 Sample size – 10 mm
 Measurement – THz transmission
Proprietary | Lake Shore Cryotronics, Inc.
Photoconductive THz Emitter
17
Photoconductive
device
-10 -5 0 5 10
-40
-20
0
20
40
Current(A)
Bias (V)
Dark
Fiber illuminated device
Room Temperature
Proprietary | Lake Shore Cryotronics, Inc.
Photoconductive THz Emitter
18
 THz-frequency transient current
oscillations induced by amplitude
modulated IR laser light
 Current oscillations in the antenna
structure radiate propagating EM
waves.
 A high resistivity Si lens is attached
to the emitter device to couple the
THz emission to free space.
Photoconductive
device
Proprietary | Lake Shore Cryotronics, Inc.
THz Time Domain Spectroscopy
19
fs
I
Proprietary | Lake Shore Cryotronics, Inc.
THz Time Domain Spectroscopy
20
fs
IA
0 10 20 30 40
0
ElectricField(a.u.)
Time (ps)
E
Proprietary | Lake Shore Cryotronics, Inc.
THz Time Domain Spectroscopy
21
ps
fs
Dispersion
Proprietary | Lake Shore Cryotronics, Inc.
THz Time Domain Spectroscopy
22
Dispersion
Compensation
fs
Proprietary | Lake Shore Cryotronics, Inc.
THz Time Domain Spectroscopy
23
Dispersion
Compensation
ps
Proprietary | Lake Shore Cryotronics, Inc.
Continuous-Wave THz Spectroscopy
24
DFB Laser 1
DFB Laser 2
f1
f2
Proprietary | Lake Shore Cryotronics, Inc.
Continuous-Wave THz Spectroscopy
- Generation
25
f1-f2
f1-f2
Proprietary | Lake Shore Cryotronics, Inc.26
Detected current No detected current
Continuous-Wave THz Spectroscopy
- Detection
Proprietary | Lake Shore Cryotronics, Inc.
Continuous-Wave THz Spectroscopy
- Frequency Tuning
27
DFB Laser 1
DFB Laser 2
f1
f2
Proprietary | Lake Shore Cryotronics, Inc.28
DFB Laser 1
DFB Laser 2
f1
f2
| Confidential Lake Shore Cryotronics, Inc.
Integrated Software for Turn-key Operation
29
| Confidential Lake Shore Cryotronics, Inc.
Integrated Software for Turn-key Operation
30
| Confidential Lake Shore Cryotronics, Inc.
Integrated Software for Turn-key Operation
31
Sample Reference Background
BLOCK
| Confidential Lake Shore Cryotronics, Inc.
Integrated Software for Turn-key Operation
32
| Confidential Lake Shore Cryotronics, Inc.
Integrated Software for Turn-key Operation
33
Proprietary | Lake Shore Cryotronics, Inc.
Case Study: Sr2CrReO6 Thin Films
34
In-plane
 Double-perovskite ferrimagnet (Tc = 635 K)
 Ms = 1.29 B per f.u.
 Predicted 90% spin polarization
 Large anisotropy
 Stoichiometric, epitaxial, and well ordered
 Well ordered films on STO and LSAT
substrates
Proprietary | Lake Shore Cryotronics, Inc.
Case Study: Sr2CrReO6 Thin Films
35
Stoichiometric, epitaxial, and well ordered
 Grown with off-axis magnetron sputtering
1 µm thickness ~ 20 hours
Low material yields
 10 to 200 nm thick film on 10 × 10 mm substrate
 After characterization, wafer is diced & distributed for
device manufacturing
Wafer real estate is at a premium
 Electrical contacts for material evaluation reduce
number of devices — non contact evaluation
 Cryogenic characterization elucidates conduction
mechanisms
Proprietary | Lake Shore Cryotronics, Inc.
CW-THz Transmission
36
0.5 1.0 1.5
0.0
0.5
1.0
THzTransmission
Frequency (THz)
Proprietary | Lake Shore Cryotronics, Inc.
CW-THz Spectroscopy of
Conductive Thin Films
37
Thickness
Conductivity
Ga-doped ZnO on ZnO
Proprietary | Lake Shore Cryotronics, Inc.
SCRO Film DC Conductivity
38
0.0
0.2
0.4
0.6
0.8
1.0
200 400 600 800 1000
0.0
0.2
0.4
0.6
0.8
1.0
120 m LSAT
5 K
50 K
100 K
300 K
1.4 mSCRO on 120 m LSAT
THzTransmission
Frequency (GHz)
300 K
0.0
0.2
0.4
0.6
0.8
1.0
200 400 600 800 1000
0.0
0.2
0.4
0.6
0.8
1.0
120 m LSAT
5 K
50 K
100 K
300 K
1.4 mSCRO on 120 m LSAT
THzTransmission
Frequency (GHz)
300 K
Proprietary | Lake Shore Cryotronics, Inc.
Variable Range Hopping Conductivity
39
Variable Range Hopping
5 K
5 K
Proprietary | Lake Shore Cryotronics, Inc.
What’s Next
40
– Turn-key acquisition of temperature
and field dependent THz spectra
Taking orders March 2014!
Model 8500
THz System for
Material Characterization
 Customer applications
— samples
 Sponsored research
program to develop
turn-key analysis
software for CW-THz
spectra

Terahertz materials characterization in extreme environments

  • 1.
    Proprietary | LakeShore Cryotronics, Inc. Terahertz Materials Characterization in Extreme Environments Emerging Tools for Materials Research David R. Daughton Applications Scientist
  • 2.
    Proprietary | LakeShore Cryotronics, Inc. THz Systems Probe Stations Hall Effect Measurement Systems (HMS) Magnetometers (VSM/AGM) Permanent Magnets High Density Recording Media Mineral Magnetism Electronic thin films Organic Electronics Spintronics Nanowires Magnetoresistance Organic electronics Thermoelectrics Solar Cells HEMTS Materials Characterization Systems 2 Systems Measure electrical properties of devices and materials in temperature- controlled environment AC/DC measurements:  Hall mobilities  Carrier concentration  Carrier type Measure magnetic properties:  Hysteresis M(H) loops  FORC curves  Temperature dependencies Fully integrated for material properties:  Electronic  Magnetic  Chemical
  • 3.
    Proprietary | LakeShore Cryotronics, Inc. Why THz? 3
  • 4.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz 5 1012 Hz 2.5 THz ~ 10 meV  Alignment of THz energy levels with phenomena of interest – Vibrational resonances – Novel spin resonances – Free carrier motion in semiconductors
  • 5.
    Proprietary | LakeShore Cryotronics, Inc. Materials Phenomena 6 The Electromagnetic Spectrum D. N. Basov, et al. “Electrodynamics of correlated electron materials” Rev. Mod. Phys. 85(2), 471 (2011).
  • 6.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz  THz wavelengths match the feature sizes of development-grade electronic materials – Non-contact electronic characterization – Novel magnetic materials 7 1012 Hz 0.6 THz ~ 0.5 mm 2” 10 mm
  • 7.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz  Coupling to spin-based materials at THz frequencies – High speed computing paradigms – May require large fields 8 1012 Hz 0.2 THz ~7 T Nagashima, T.; Nishitani, J.; Kozuki, Kohei, "Lasers & Electro Optics & The Pacific Rim Conference on Lasers and Electro-Optics, 2009. CLEO/PACIFIC RIM '09. Conference on , vol., no., pp.1,2, 30-3 Aug. 2009
  • 8.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz 9 1012 Hz 6.5 THz ~ 300 K 480 500 520 540 560 580 0.1 1 THzTransmission Frequency (GHz) 5.8 K 75 K 150 K a-Lactose THzTransmission  Cryogenic temperatures – Homogeneous broadening of vibrational resonances
  • 9.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz 10 1012 Hz  Cryogenic temperatures – Homogeneous broadening of vibrational resonances – Temperature dependent carrier concentration and mobility 6.5 THz ~ 300 K
  • 10.
    Proprietary | LakeShore Cryotronics, Inc. Equivalent Scales for THz 11 1012 Hz 10 meV7 T 300 K0.5 mm  Alignment of THz energy levels with phenomena of interest  THz wavelengths match the feature sizes of development- grade electronic materials  Coupling to spin-based materials at THz frequencies  Cryogenic temperatures
  • 11.
    Proprietary | LakeShore Cryotronics, Inc. THz System Product Challenges  THz performance suitable for materials characterization – Continuous tuning over bandwidth – Spectral resolution  Ability to characterize samples while exposed to variable cryogenic temperatures and magnetic fields  Affordable THz-based measurement platform  Robust design  Proceduralized experimental methods and reliable analysis of the spectral results – Convenient sample insertion without complicated alignment – Enable materials developers to rapidly begin productive research 12
  • 12.
    Proprietary | LakeShore Cryotronics, Inc. Filling the THz Gap 13 The Electromagnetic Spectrum 0 10 20 30 40 50 0 ElectricField(a.u.) Time (ps)
  • 13.
    Proprietary | LakeShore Cryotronics, Inc. THz with cryogenics & magnetics 14  Many materials of interest for THz require variable temperature and/or high magnetic fields  Optical cryostats are the standard approach – THz generation outside the environment – Must pass optical energy through windows, cutting signal power and spectral distortion  Not ideal for THz spectroscopies
  • 14.
    Proprietary | LakeShore Cryotronics, Inc. Variable Temperature and High Magnetic Field THz Platform 15 Cryostat Sample space ±9 T magnet Removable sample insert Cryo-compatible THz emitter with collimating optics Rotatable sample stage (10 mm × 10 mm) Thermally stable optical alignment stages
  • 15.
    Proprietary | LakeShore Cryotronics, Inc. Application software for turnkey operation  Experiment setup/run  Analysis of spectral data  Calculation of material properties Integrated THz System Details 16 Fiber-based optical platform for CW THz spectroscopy  CW THz spectrometer instrument  Amplitude and phase detection from 200 GHz to 1.5 THz  Spectral resolution under 500 MHz  Circularly polarized light Integrated controls  Model 336 cryogenic temperature controller  Model 625 superconducting magnet power supply Superconducting magnet  High magnetic fields to ±9 Tesla Integrated cryostat & insert  Variable temperatures from 5 K to 300 K  Sample size – 10 mm  Measurement – THz transmission
  • 16.
    Proprietary | LakeShore Cryotronics, Inc. Photoconductive THz Emitter 17 Photoconductive device -10 -5 0 5 10 -40 -20 0 20 40 Current(A) Bias (V) Dark Fiber illuminated device Room Temperature
  • 17.
    Proprietary | LakeShore Cryotronics, Inc. Photoconductive THz Emitter 18  THz-frequency transient current oscillations induced by amplitude modulated IR laser light  Current oscillations in the antenna structure radiate propagating EM waves.  A high resistivity Si lens is attached to the emitter device to couple the THz emission to free space. Photoconductive device
  • 18.
    Proprietary | LakeShore Cryotronics, Inc. THz Time Domain Spectroscopy 19 fs I
  • 19.
    Proprietary | LakeShore Cryotronics, Inc. THz Time Domain Spectroscopy 20 fs IA 0 10 20 30 40 0 ElectricField(a.u.) Time (ps) E
  • 20.
    Proprietary | LakeShore Cryotronics, Inc. THz Time Domain Spectroscopy 21 ps fs Dispersion
  • 21.
    Proprietary | LakeShore Cryotronics, Inc. THz Time Domain Spectroscopy 22 Dispersion Compensation fs
  • 22.
    Proprietary | LakeShore Cryotronics, Inc. THz Time Domain Spectroscopy 23 Dispersion Compensation ps
  • 23.
    Proprietary | LakeShore Cryotronics, Inc. Continuous-Wave THz Spectroscopy 24 DFB Laser 1 DFB Laser 2 f1 f2
  • 24.
    Proprietary | LakeShore Cryotronics, Inc. Continuous-Wave THz Spectroscopy - Generation 25 f1-f2 f1-f2
  • 25.
    Proprietary | LakeShore Cryotronics, Inc.26 Detected current No detected current Continuous-Wave THz Spectroscopy - Detection
  • 26.
    Proprietary | LakeShore Cryotronics, Inc. Continuous-Wave THz Spectroscopy - Frequency Tuning 27 DFB Laser 1 DFB Laser 2 f1 f2
  • 27.
    Proprietary | LakeShore Cryotronics, Inc.28 DFB Laser 1 DFB Laser 2 f1 f2
  • 28.
    | Confidential LakeShore Cryotronics, Inc. Integrated Software for Turn-key Operation 29
  • 29.
    | Confidential LakeShore Cryotronics, Inc. Integrated Software for Turn-key Operation 30
  • 30.
    | Confidential LakeShore Cryotronics, Inc. Integrated Software for Turn-key Operation 31 Sample Reference Background BLOCK
  • 31.
    | Confidential LakeShore Cryotronics, Inc. Integrated Software for Turn-key Operation 32
  • 32.
    | Confidential LakeShore Cryotronics, Inc. Integrated Software for Turn-key Operation 33
  • 33.
    Proprietary | LakeShore Cryotronics, Inc. Case Study: Sr2CrReO6 Thin Films 34 In-plane  Double-perovskite ferrimagnet (Tc = 635 K)  Ms = 1.29 B per f.u.  Predicted 90% spin polarization  Large anisotropy  Stoichiometric, epitaxial, and well ordered  Well ordered films on STO and LSAT substrates
  • 34.
    Proprietary | LakeShore Cryotronics, Inc. Case Study: Sr2CrReO6 Thin Films 35 Stoichiometric, epitaxial, and well ordered  Grown with off-axis magnetron sputtering 1 µm thickness ~ 20 hours Low material yields  10 to 200 nm thick film on 10 × 10 mm substrate  After characterization, wafer is diced & distributed for device manufacturing Wafer real estate is at a premium  Electrical contacts for material evaluation reduce number of devices — non contact evaluation  Cryogenic characterization elucidates conduction mechanisms
  • 35.
    Proprietary | LakeShore Cryotronics, Inc. CW-THz Transmission 36 0.5 1.0 1.5 0.0 0.5 1.0 THzTransmission Frequency (THz)
  • 36.
    Proprietary | LakeShore Cryotronics, Inc. CW-THz Spectroscopy of Conductive Thin Films 37 Thickness Conductivity Ga-doped ZnO on ZnO
  • 37.
    Proprietary | LakeShore Cryotronics, Inc. SCRO Film DC Conductivity 38 0.0 0.2 0.4 0.6 0.8 1.0 200 400 600 800 1000 0.0 0.2 0.4 0.6 0.8 1.0 120 m LSAT 5 K 50 K 100 K 300 K 1.4 mSCRO on 120 m LSAT THzTransmission Frequency (GHz) 300 K 0.0 0.2 0.4 0.6 0.8 1.0 200 400 600 800 1000 0.0 0.2 0.4 0.6 0.8 1.0 120 m LSAT 5 K 50 K 100 K 300 K 1.4 mSCRO on 120 m LSAT THzTransmission Frequency (GHz) 300 K
  • 38.
    Proprietary | LakeShore Cryotronics, Inc. Variable Range Hopping Conductivity 39 Variable Range Hopping 5 K 5 K
  • 39.
    Proprietary | LakeShore Cryotronics, Inc. What’s Next 40 – Turn-key acquisition of temperature and field dependent THz spectra Taking orders March 2014! Model 8500 THz System for Material Characterization  Customer applications — samples  Sponsored research program to develop turn-key analysis software for CW-THz spectra