IEE/CEEM Seminar: Vidvuds Ozolins and Sparse Physics and Its Applications To Energy Materials

Sparse physics via compressive sensing
Vidvuds Ozolins
Department of Materials Science & Engineering
University of California, Los Angeles
DMR-1106024

Supported by:
UCLA Laboratory for the Quantum
Prediction of Advanced Materials
Co-conspirators
Gus Hart
(BYU Provo)
Rogjie Lai
(UC Irvine)
Lance Nelson
(BYU Idaho)
Russ Caflisch
(UCLA)
Fei Zhou
(LLNL)
Stan Osher
(UCLA)
Weston Nielson
(UCLA)
Outline
Premise:
Most physics models are approximately sparse
(i.e., have a few terms) in some basis
Questions:
How do we pick the basis?
How do we determine which terms to pick?
How should we generate fitting data?
How do we systematically improve accuracy?
High-rate charge storage in Nb2O5
V. Augustyn, J. Come, M. A. Lowe, J. W. Kim, P.-L. Taberna, S. H. Tolbert, H. D. Abrua, P. Simon, B.

Dunn, Nature Materials 12, 518522 (2013)
Structure of orthorhombic Nb2O5
Layered structure (stacked along c) 001 layer with octahedra and

pentagonal bipyramids
Acta Cryst. B31, 673 (1975)
Atomic disorder in Nb2O5

Nb (8i): 16 Nb off-center in the c direction
Nb layer
Nb (4g) partial occupancy: 0.8 Nb

between Nb layers
O: distorted close packing within {001} layers
Lithium energy landscape in the (001) plane
Oxygen
C.-P. Liu, F. Zhou, and V. Ozolins (2013)
Li intralayer diffusion map
> 700 meV
50 meV
Configurational problem for Nb2O5
Occupation Si: Vacancy, Li, or Nb
Configurational Ordering in Alloys
Cu3Au
CuAu
All these structures are based on the facecentered cubic (FCC) lattice.
CuAu3
Cluster Expansion
Rewrite as an expansion in clusters of lattice sites:
E = E0 + J1c +
Pairs, Triplets, ...
Jf
if
+ ...
ADVANTAGES:
Very fast can be used in Monte Carlo simulations
Works for any structure based on a given lattice
Cluster selection is difficult
10 000
5-bodies
4-bodies
1000
triplets
100
10.
pairs
1.
0.5
1.0
1.5
2.0
cluster radius
2.5
3.0
Compressive sensing CE
Clusters
Structures
. . . .
1
B 0
B
@ .
.
1
1
.
.
...
...
...
...
...
...
...
S
...
if
10
B
CB
CB
AB
B
B
B
B
B
B
@
?
Jnn
Jnnn
Jtrip
.
.
.
.
.
1 0
C B
C B
C= B
C B
B
C B
C @
C
C
C
C
A
J CS = arg min J 1 : J E 2
J
L. J. Nelson, F. Zhou, G.L.W. Hart, and V. Ozolins, Phys. Rev. B 87, 035125 (2013)
E(
E(
E(
)
)
)
.
.
.
1
C
C
C
C
C
C
A
Why compressive sensing works

x2
x * = arg min x: Ax=b x
x1
a11 x1 + a12 x2 = b1
n
x 1 = xi
i=1
Why Euclidean distance is worse

x2
x * = argmin x: Ax=b x
x1
a11 x1 + a12 x2 = b1
x2=
x
i=1
2
i
Theorem
Probability to find the correct S-sparse solution is
P >1
if the number of data points satisfies
M C S log ( N )
2
Coherence
1N
Sparsity
Size of
basis set
E. Cands, J. Romberg, and T. Tao, Comm. Pure Appl. Math., vol. 59, no. 8, pp. 12071223 (2006).
Ag-Pt cluster expansion

Pairs
Triplets
Cluster radius
L. J. Nelson, F. Zhou, G.L.W. Hart, and V. Ozolins, Phys. Rev. B 87, 035125 (2013).
Quadruplets
Ag-Pt cluster expansion

Pairs
Triplets
Cluster radius
Quadruplets
Discrete Opt.
Compressive sensing
Training set size
kJfit k1 (Dashed Line)
RMS Error (meV) (solid line)
Performance of CSCE
Next step Bayesian CSCE
L. J. Nelson, G. L. W. Hart, S. Reese, F. Zhou, and V. Ozolins, Physical Review B 88, 155105 (2013).
CSCE results for zinc-finger protein
Predicted energy HkcalmolL
10
0
-10
-20
-30
-30
-20
-10
0
Direct energy HkcalmolL
10
Direct conversion of heat to electricity

Up to 30% conversion efficiency with right materials
electrical conductivity
thermopower
S
ZT =
T
total
2
Total thermal conductivity
hot
Power factor
cold
Thermopower S = V/T
PbTe: Standard of excellence
Image from Pei et al. Nature 473, 6669 (2011)
(direct gaps at L point) result from the occurrence of the Pb s band below the top
of the valence band, setting up coupling and level repulsion at the L point.
From Wei & Zunger, Physical Review B 55, 1360513610 (1997)
Giant anharmonicity of PbTe TO mode
Chemical compound space

PbTe
IV-VI
Group I + V
Group VI
I-V-VI2
AgSbTe2, NaSbSe2,
M. Nielsen, V. Ozolins, and J. P. Heremans, Energy & Environ. Sci. 6, 570-578 (2013).
New materials: Search space
ABX2 in cubic D4 (AF-IIb) for A=Cu, Ag, Au

ABX2 in rhombohedral R-3m (AF-II) for A=Na, K, Rb, Cs, Tl
Screened a total of 8 3 3 = 72 compounds
0
AuAsTe2
CuBiSe2
AuBiTe2
CuAsTe2
AgAsTe2
AgSbSe2
CuBiTe2
AuSbTe2
NaSbS2
KAsSe2
AgBiS2
CuSbTe2
AgBiSe2
AgBiTe2
AgSbTe2
NaAsSe2
CsSbSe2
RbSbSe2
NaSbSe2
KSbSe2
CsBiS2
RbBiS2
NaAsTe2
NaBiS2
KBiS2
NaSbTe2
KAsTe2
NaBiSe2
RbAsTe2
CsAsTe2
RbBiSe2
CsBiSe2
NaBiTe2
KBiSe2
RbSbTe2
KSbTe2
CsBiTe2
RbBiTe2
KBiTe2
CsSbTe2
Gruneisen parameter
Calculated Gruneisen parameters
Experimental results from OSU
Cu12Sb4S13: Thermoelectric mineral with ZT=1
Cu
Sb
S
X. Lu, D. T. Morelli, Y. Xia, F. Zhou, V. Ozolins, H. Chi, and C. Uher. Advanced Energy Materials (2013)
Natural tetrahedrite mineral
!
!
!1 cm
!!!!!!!!!!!!!!!!!!!!!!!!!!
Figure of Merit
1
1.2
a)
Figure of Merit zT
Figure of Merit zT
1
0.8
0.6
0.4
0.2
0.8
0.6
0.4
f =1 for Zn (2+)
fb)=2 for Fe (3+)
0.2
0
0
300
400
500
600
Temperature (K)
700
800
0.2
0.4
0.6
0.8
Brillouin Zone Occupation Fraction

!
Lu, Morelli, Xia, Zhou, Ozolins, Chi, Zhou, and Uher, Advanced Energy Materials (2013).
Frustrated Cu(1) bonding environment
Cu(1) (3-fold)
Anharmonic optical mode

50
40
DE HmeVL
30
20
10
0
-10
-0.4
-0.2
0.0
uCu HL
0.2
0.4
CS lattice dynamics
Taylor expansion of the total energy in
terms of the atomic displacements
ua=Ra-R0a:
1
0 + a ua +
2
1
ab ua ub +
6
abc ua ub uc
Forces:
Fa =
@ /@a =
1
( a + ab ub +
2
abc ub uc
Use for: Thermal transport, free energies, phase

transformations, etc.
+ )
Expansion in cluster series

a ua , aa ua2 , aaa ua3,
abua ub , aabua2 ub ,
abc ua ub uc , aabc ua2 ub uc ,
abcd ua ub uc ud ,
How to calculate FCTs from DFT?
Calculate forces Fa
Fa =
Displace atoms ua
1
@ /@a
Fa = @( a/@a
+ =ab u(b +
a+
2
1
uc + abc
)ub uc
abc
ab uubb+
2
Compressive sensing
We need to solve an underdetermined linear system
of equations:
1 u1 u1 u1 a
b
b c
ab
2
2 2
1 ub ub uc
abc

CS

1
Fa
= F 2
a

1
= arg min 1 +
+ F
2
2
Symmetry constraints
Commutativity of derivatives
abc
acb
= ...
Translational invariance (Noethers theorem)
(aa) =
(ab)
Pair ASR
b6=a
X
a
I ({a, b, c })
=0
Multibodies
Dynamical properties of solids, eds. G.K. Horton & A.A. Maradudin (1974)
Symmetry constraints
Space group symmetry
s)
I (
s)
IJ (
J ()
Transformation matrix:
s)
IJ (
i1
j(1)
u1
F3
F2
in
j(n)
Reduces ## of FCTs by a factor

of 10 in cibic crystals
cos
= sin
Dynamical properties of solids, eds. G.K. Horton & A.A. Maradudin (1974)
sin
cos
0
0
0
1
The final CSLD L1 problem

DFT data constraints are imposed via a regular leastsquares norm:
where
CS
1
2
= arg min 1 + + F 2
S
= BT BS BP S.
Trans Rot Perm
are symmetry-distinct FCT components.
DFT tests: NaCl

F
0.15
0.10
0.05
100
200
300
400
500
600
-0.05
Independent FCs by
order, then by distance
Solution is sparse
Force prediction error = 3%
15
FCSLD @eVD
-0.10
20
10
5
0
-5
-10
u/r0=25%
-15
-15 -10 -5
10
FDFT @eVD
Applications
15
20
Performance of CSLD
Applications
Sparsity for PDEs

Classically, sparsity is limited to discrete objects.
[Questions]
What is an analog of the sparsity for continuous
functions?
How to design a tractable method to create
sparse continuous functions?
L1 regularization of DFT
Conventional Kohn-Sham problem:
N
E = minN j H j
{ i }i=1
j =1
s.t. i j = ij
Sparse = localized or short-ranged
1 N
E = minN j H j + j s.t. i j = ij ,
1
{ i }i=1 j =1
j =1
1 (x) dx, x R d
This method converges to spatially localized wave f-ns with compact
support. O(N) becomes possible.
V. Ozolins, R. Lai, R. E. Caflisch, and S. Osher, Compressed modes , PNAS (2013)
Results
Results
Dependence on
1
0.6
1
0.6
3
0.4
4
5
0.2
4
5
0.2
0
0
0
3
0.4
10
15
20
25
30
35
40
45
50
10
15
20
25
30
35
40
45
50
= 50
= 30
1
0.6
0.6
2
3
3
0.4
4
5
0.2
4
5
0.2
0
0
0
0.4
10
15
20
25
30
35
40
45
50
10
15
20
25
30
35
40
45
50
= 300
= 50
1
0.6
0.6
3
0.4
0.2
5
0.2
0
0
3
0.4
0
5
10
15
20
25
30
35
40
45
50
= 500
10
15
20
25
30
35
40
45
50
= 5000
Fig. 4.
Computation results of CMs with dierent values of . The first column: the first 5 CMs of the 1D free-electron model. The second column: the first 5 CMs of the
1D Kronig-Penny model.

electrons in a one-dimensional crystal, where the potential
compact support on , as suggested by general considerations
Fig. 5.
Comparisons of the first 50 eigenvalues of the 1D free electron model (the first row) and
Total energy convergence

M = N = 50
0.1
Potential free
KronigPenney
Relative Error
0.08
0.06
0.04
0.02
0
10
50
100
200
300
400
500
M = 50, = 10
0.1
Potential free
KronigPenney
Relative Error
0.08
0.06
0.04
0.02
0
50
60
70
80
90
100
128
Fig. 6.
Relative eigenvalue error of the 1D free-electron model (red dots) and 1D

KPLai,
model
circles).
relationCompressed
of the relativemodes
error via
dierent
values of
V. Ozolins, R.
R. E.(blue
Caflisch,
andTop:
S. Osher,
,
PNAS (2013)
for fixed M = N = 50. Bottom: relation of the relative error via dierent values
of N for fixed = 10 and M = 50.
compressed mod
Schr
odinger oper
( 1 , , M ) of
KP model and 1D
values ( 1 , ,
ators. Figure 5
small value =
can clearly see t
increasing numb
relative error E =
we speculated in
to zero as ! 1
in the top panel
verge to zero as
is illustrated in t
Moreover, th
also work on dom
ample, Figure. 7
CMs of the free = 30. All the
for 2D cases. In
extended to irre
which will be inv
In conclusion
le with an L1 penalThe trade-o between

acy of the variational
arameter, , without
d spatial cutos. The
d to numerically conthat the CMs can be
provable orthonormal
unctions, energy specto the fact the CMs
onal eort of total enthe number of modes
ation bottleneck limwork by finding the
or.
d variational principle
l component analysis
ver, does not involve
nciple and the sparse
since the component
uum variable.
We expect that CMariety of applications
als science, and other
following directions:
a discrete Laplacian on a network.

Finally, we plan to perform an investigation of the formal
properties of CMs to rigorously analyze their existence and
completeness, including the conjecture that was hypothesized
and numerically tested here.
Higher dimensions, etc.
Fig. 7. The first 25 CMs of freel-electron case on a 2D domain [0, 10]2 with
d basis sets that span
= 30. Each CM is color-coded by its height function.
tor, for instance, the
oncept of plane waves
h multi-resolution caV. Ozolins,
ssed in Ref.
[20]. R. Lai, R. E. Caflisch, and S. Osher, Compressed modes , PNAS (2013)
ated (i.e., O(N )) simACKNOWLEDGMENTS. V.O. gratefully acknowledges financial support from the
National Science Foundation under Award Number DMR-1106024 and use of comal theory (DFT) elec-
Compressed plane waves
Set V=0 to derive general compactly supported basis for the Laplacian:
CPW
1
(x) = arg min + 1 s.t. (x) (x jw) = 0 j
2
V. Ozolins, R. Lai, R. E. Caflisch, and S. Osher, Compressed plane waves , UCLA CAM Report (2013)
Introduction
Compressed Modes (CMs)
Compressed Plane Waves (CPWs)
Numerical algorithm and results
The first six basic CPWs

6
4
0
2
0
5
2
0
10
20
30
40
50
60
70
80
90
100
10
20
30
40
50
5
10
20
30
40
50
60
70
80
90
100
10
20
30
40
50
80
90
100
60
70
80
90
100
5
0
70
60
10
20
30
40
50
60
70
80
90
100
10
20
30
40
50
Figure: From top to the bottom, the first six modes

using L = 100, = 5, w = 5.
60
70
80
90
100
6
1
obtained by Eq. (10 -11)
Introduction
Compressed Modes (CMs)
Compressed Plane Waves (CPWs)
Numerical algorithm and results
Spectral density distribution
0.8
0.6
0.4
0.2
6i=1|i(G)|2
|i(G)|2
0.8
0.6
0.4
0.2
0
0
0.5
1.5
2.5
3
Wave vector G
3.5
4.5
0.5
1.5
2.5
3
Wave vector G
3.5
4.5
Figure: Spectral density distribution of CPWs. Top: the spectral density distribution of
1
, 2 , 3 , 4 , 5 , 6 . Bottom: The total spectral density distribution of the first four modes.
V. Ozolins & R. Lai & R. Caflisch & S. Osher
Compressed Modes for Variational Problems in Math. & Phy.
Summary
CS-based sparse physics is based on rigorous
math, not intuition
Accuracy can be improved systematically
Constraints (symmetry and translational
invariance) can be straightforwardly incorporated
CS automatically picks out important terms
A simple prescription for gathering data

IEE/CEEM Seminar: Vidvuds Ozolins and Sparse Physics and Its Applications To Energy Materials

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Sparse physics via compressive sensing

High-rate charge storage in Nb2O5

V. Augustyn, J. Come, M. A. Lowe, J. W. Kim, P.-L. Taberna, S. H. Tolbert, H. D. Abrua, P. Simon, B.

Structure of orthorhombic Nb2O5

Layered structure (stacked along c) 001 layer with octahedra and

Acta Cryst. B31, 673 (1975)

Atomic disorder in Nb2O5

Nb (4g) partial occupancy: 0.8 Nb

O: distorted close packing within {001} layers

Lithium energy landscape in the (001) plane

C.-P. Liu, F. Zhou, and V. Ozolins (2013)

Li intralayer diffusion map

> 700 meV

C.-P. Liu, F. Zhou, and V. Ozolins (2013)

Configurational problem for Nb2O5

Occupation Si: Vacancy, Li, or Nb

C.-P. Liu, F. Zhou, and V. Ozolins (2013)

Configurational Ordering in Alloys

Pairs, Triplets, ...

Cluster selection is difficult

Why compressive sensing works

x * = arg min x: Ax=b x

Why Euclidean distance is worse

Ag-Pt cluster expansion

Ag-Pt cluster expansion

kJfit k1 (Dashed Line)

RMS Error (meV) (solid line)

Next step Bayesian CSCE

CSCE results for zinc-finger protein

Predicted energy HkcalmolL

Direct conversion of heat to electricity

Total thermal conductivity

PbTe: Standard of excellence

Image from Pei et al. Nature 473, 6669 (2011)

Giant anharmonicity of PbTe TO mode

Chemical compound space

New materials: Search space

ABX2 in cubic D4 (AF-IIb) for A=Cu, Ag, Au

Calculated Gruneisen parameters

Experimental results from OSU

Cu12Sb4S13: Thermoelectric mineral with ZT=1

Natural tetrahedrite mineral

Brillouin Zone Occupation Fraction

Frustrated Cu(1) bonding environment

Anharmonic optical mode

Use for: Thermal transport, free energies, phase

Expansion in cluster series

How to calculate FCTs from DFT?

Translational invariance (Noethers theorem)

Reduces ## of FCTs by a factor

The final CSLD L1 problem

Trans Rot Perm

are symmetry-distinct FCT components.

DFT tests: NaCl

Sparsity for PDEs

Sparse = localized or short-ranged

V. Ozolins, R. Lai, R. E. Caflisch, and S. Osher, Compressed modes , PNAS (2013)

V. Ozolins, R. Lai, R. E. Caflisch, and S. Osher, Compressed modes , PNAS (2013)

compact support on , as suggested by general considerations

Total energy convergence

Relative eigenvalue error of the 1D free-electron model (red dots) and 1D

le with an L1 penalThe trade-o between

a discrete Laplacian on a network.