Time-Dependent Density Functional Theory in Optical Sciences

Transcription

1 Exenal Revew on Cene fo Compuaonal Scences Unvesy of Tsuuba Tme-Dependen Densy Funconal Theoy n Opcal Scences K. YABANA Cene fo Compuaonal Scences Unvesy of Tsuuba Collaboaos: G.F. Besch Unv. Washngon T. Oobe JAEA J.-I. Iwaa Unv. Toyo S. Shnohaa Unv. Tsuuba/MPI T. Sugyama Unv. Tsuuba S.A. Sao Unv. Tsuuba

2 Fs-pncples elecon dynamcs smulaon based on Tme-Dependen Densy Funconal Theoy (TDDFT) Real-me and eal-space soluon of me-dependen Kohn-Sham equaon + Von ( Ra ) + e m a n( ) d + µ xc n( ) = ψ ( ) ( n( )) + V ex ( ) ψ ( ) = ψ ( ) Developmen of mehodology and ou own sofwea ARTED = Ab-no Real-Tme Elecon Dynamcs smulao 1996 Isolaed sysem (molecules cluses) K. Yabana G.F. Besch Phys. Rev. B (1996). ψ m ( x y z ) j l 000 Infnely peodc sysem (cysallne solds) G.F. Besch J.-I. Iwaa A. Rubo K. Yabana Phys. Rev. B (000). 01 Couplng o macoscopc Maxwell equaon K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01).

3 Lnea opcal absopon n molecules K. Yabana Y. Kawasha T. Naasuasa J.-I. Iwaa Chaged Pacle and Phoon Ineacons wh Mae: Recen Advances Applcaons and Inefaces Chape 4 Taylo & Fancs 010. Elecon dynamcs n cysallne solds unde femosecond lase pulses - Opcal beadown of deleccs T. Oobe M. Yamagwa J.-I. Iwaa K. Yabana T. Naasuasa G.F. Besch Phys. Rev. B (008). - Coheen phonon geneaon Y. Shnohaa K. Yabana Y. Kawasha J.-I. Iwaa T. Oobe G.F. Besch Phys. Rev. B (010) Y. Shnohaa S.A. Sao K. Yabana J.-I. Iwaa T. Oobe G.F. Besch J. Chem. Phys. 137 A57 (01). Coupled dynamcs of macoscopc elecomagnec felds and mcoscopc elecon dynamcs K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01). 3

4 Lnea opcal absopon n molecules K. Yabana Y. Kawasha T. Naasuasa J.-I. Iwaa Chaged Pacle and Phoon Ineacons wh Mae: Recen Advances Applcaons and Inefaces Chape 4 Taylo & Fancs 010. Elecon dynamcs n cysallne solds unde femosecond lase pulses - Opcal beadown of deleccs T. Oobe M. Yamagwa J.-I. Iwaa K. Yabana T. Naasuasa G.F. Besch Phys. Rev. B (008). - Coheen phonon geneaon Y. Shnohaa K. Yabana Y. Kawasha J.-I. Iwaa T. Oobe G.F. Besch Phys. Rev. B (010) Y. Shnohaa S.A. Sao K. Yabana J.-I. Iwaa T. Oobe G.F. Besch J. Chem. Phys. 137 A57 (01). Coupled dynamcs of macoscopc elecomagnec felds and mcoscopc elecon dynamcs K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01). 4

5 Wong n wo felds Nuclea Physcs and Condensed Mae Physcs has bough us ognal developmens poon neuon Nucle Nucleon many-body sysem Aoms Molecules Solds Elecon many-body sysems Common heoes and compuaonal mehods ae useful. 5

6 In nuclea physcs 3D smulaon solvng TDHF eq. has long hsoy. One of he oldes 3D quanum-mechancal smulaon Nuclea fuson eacon of 16 O- 16 O Spaal gd: 30x8x16 (10-15 m) Tme-sep 4x10 (10 - s) H. Flocad S.E. Koonn M.S. Wess Phys. Rev. 17(1978)168.

7 Elecon dynamcs n meallc cluses by TDDFT K. Yabana G.F. Besch Phys. Rev. B (1996). Assume Icosahedal shape L Densy change nduced by mpulsve foce 30 0 Dpole momen Tme [ev -1 ] Dpole momen as funcon of me

8 Real-me calculaon fo opcal absopon specum of L K. Yabana G.F. Besch Phys. Rev. B (1996). Real-me calculaon fo auocoelaon funcon zˆ ( ) zˆ ( 0) [ev -1 ] Exp:L TDDFT Foue ansfomaon oscllao sengh dsbuon σ 1 ω ( ω) d e zˆ ( ) zˆ ( 0)

9 Phooabsopon of molecules by TDDFT (LB94 funconal) Connuum RPA calculaon fo defomed sysem K. Yabana Y. Kawasha T. Naasuasa J.-I. Iwaa Chaged Pacle and Phoon Ineacons wh Mae: Recen Advances Applcaons and Inefaces Chape 4 Taylo & Fancs 010. N H O C 6 H 6 C 60

10 Lnea opcal absopon n molecules K. Yabana Y. Kawasha T. Naasuasa J.-I. Iwaa Chaged Pacle and Phoon Ineacons wh Mae: Recen Advances Applcaons and Inefaces Chape 4 Taylo & Fancs 010. Elecon dynamcs n cysallne solds unde femosecond lase pulses - Opcal beadown of deleccs T. Oobe M. Yamagwa J.-I. Iwaa K. Yabana T. Naasuasa G.F. Besch Phys. Rev. B (008). - Coheen phonon geneaon Y. Shnohaa K. Yabana Y. Kawasha J.-I. Iwaa T. Oobe G.F. Besch Phys. Rev. B (010) Y. Shnohaa S.A. Sao K. Yabana J.-I. Iwaa T. Oobe G.F. Besch J. Chem. Phys. 137 A57 (01). Coupled dynamcs of macoscopc elecomagnec felds and mcoscopc elecon dynamcs K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01). 10

11 Tme-dependen exenson of Bloch s band heoy ( ) ( ) ( ) ( ) [ ] ( ) ( ) ( ) 1 = = n n n xc n u n u n n e d A c e p m u µ ( ) ( ) u a u n n = + Compuaonal aspecs - 3D unfom gd fo space hgh-ode fne dffeence fo dffeenaon - Taylo expanson fo me evoluon Elecon dynamcs n cysallne sold (aomc posons ae fxed)

12 Elecon dynamcs n bul S unde song lase pulse I= W/cm T=50 fs ħω=0.5 ev Lase phoon enegy s much lowe han dec bandgap. Elecc Feld (a.u.) Tme (fs) 40 Densy change fom he gound sae (110) Gound sae densy (110) Red + Geen 0 Blue - 1

13 Delecc funcon of S fom eal-me TDDFT-ALDA Insananeous c a =0 hen calculae cuen J() σ 1 = ω ( ω) d e J ( ) ε ( ω) = 1+ 4 ( ω) ω π σ J ( ) τ fs 13 No vey good n qualy.

14 Inense and ulasho lase pulse on S: Mul-phoon o unnel/feld onzaons ω = 1.55eV ( dec bandgap.4 ev n LDA) I = W/cm Elecc feld E I Elecon excaon enegy Tunnelng/feld onzaon Cuen Mulphoon onzaon Numbe densy of exced elecons Enegy pe elecon Elecon excaon enegy phoons 14

15 Lase-Mae neacon: Song and Ula-Sho Lase Pulse Song lgh feld Magnude of lgh elecc feld compaable o ha bound elecons n maes. Nonlnea nonequlbum Elecon Dynamcs Ula-sho pulse Pulse me duaon compaable o a peod of elecon moon n maes. Femo-echnology Ao-second scence ee()z z Real-me obsevaon of lase elecc feld usng ao-second seang echnque Jon LMU-MPQ Laboaoy of Aosecond

16 Nonhemal Lase Machney Melng ablaon flamenaon on bul suface R.R. Gaass E. Mazu Naue Phooncs 0 (008). Mcomachnng wavegude- Nanosugey Opcal mcoscope mage of wavegudes wen nsde bul glass by a 5-MHz an of 5-nJ sub-100-fs pulses C.B. Schaffe e.al OPTICS LETTERS 6 93 (001) Ablaon of a sngle mochondon n a lvng cell. N. Shen e.al Mech. Chem. Bosysems 17 (005). 16

17 Lnea opcal absopon n molecules K. Yabana Y. Kawasha T. Naasuasa J.-I. Iwaa Chaged Pacle and Phoon Ineacons wh Mae: Recen Advances Applcaons and Inefaces Chape 4 Taylo & Fancs 010. Elecon dynamcs n cysallne solds unde femosecond lase pulses - Opcal beadown of deleccs T. Oobe M. Yamagwa J.-I. Iwaa K. Yabana T. Naasuasa G.F. Besch Phys. Rev. B (008). - Coheen phonon geneaon Y. Shnohaa K. Yabana Y. Kawasha J.-I. Iwaa T. Oobe G.F. Besch Phys. Rev. B (010) Y. Shnohaa S.A. Sao K. Yabana J.-I. Iwaa T. Oobe G.F. Besch J. Chem. Phys. 137 A57 (01). Coupled dynamcs of macoscopc elecomagnec felds and mcoscopc elecon dynamcs K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01). 17

18 Odnay macoscopc elecomagnesm Elecomagnesm: Maxwell equaon fo macoscopc felds E D B H Lnea consuve elaon D = [ ] = ε ( ω)e D E Quanum Mechancs: Peubaon heoy o calculae lnea suscepbles ε(ω) D α As he feld sengh becomes lage nonlnea opcs becomes mpoan. = αβ β ( ( ) ( ) ( ) ) d ε E + 4π d d χ ( ) E ( ) E ( ) + αβγ β γ A exeme nense lm EM and QM no moe sepaae. Coupled dynamcs of macoscopc elecomagnec felds and mcoscopc elecon dynamcs K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01).

19 Mulscale smulaon ( ) ( ) ( ) J c A A c 4 1 π = Macoscopc gd pons(μm) o descbe macoscopc veco poenal { } e on xc en en n E e A c e m 4 1 = + + = π φ ψ δ δ φ ψ ψ ψ ( ) A n c e m j j d J e e e * * 4 ) ( π ψ ψ ψ ψ = = Ω A each macoscopc pons Kohn-Sham obals ae pepaed and descbed n mcoscopc gds. Exchange of nfomaon by macoscopc cuen and macoscopc veco poenal. ( ) A ( ) J ψ A each macoscopc gd pon We consde a un cell and pepae mcoscopc gd. K. Yabana T. Sugyama Y. Shnohaa T. Oobe G.F. Besch Phys. Rev. B (01).

20 Popagaon of wea pulse Odnay elecomagnesm s OK. A/c Lase fequency:1.55ev: lowe han dec bandgap.4ev(lda) I=10 10 W/cm Vacuum S [µm] =0 [µm] =0.8 [µm] =1.6 [µm] Coupled Maxwell + TDDFT smulaon 0

21 Moe nense lase pulse Dynamcs of elecons and macoscopc EM felds ae no moe sepaable. I =5 x 10 1 W/cm Vacuum S [µm] =0 [µm] =0.8 [µm] =1.6 [µm] 1

22 Compuaonally scalable smulaon 1000 coes 10 hous coes 0 mn (K-compue Kobe) Pefomance a K-Compue n Kobe (n ealy access) Compuaonal me ganed a K-compue fo 014 yea. - Geneal use s admed (4M node-hous) - Use n saegc pogam s planned We also have compuaonal me a SupeMUC (LR Gemany)

23 Lage-scale compuaon s ndspensable A pesen 1-dm popagaon (macoscopc gd) S damond: 1000 coes 10 hous 0000 coes 0 mn (K-compue Kobe) SO (α-quaz) coes hous Oblque ncdence -dm 50 3-dm - Self focusng - Ccula polazaon A mllon of maco-gd pons 1000 need o wa nex geneaon supecompues

24 Inenaonal/Domesc Collaboaons F. Kausz V. Yaovlev (MPQ) K.M. Lee (APRI Koea) G.F. Besch (Washngon) J. Bugdöfe (Venna Tech.) M. Schulze (UCB) K. Vaga (Vandebl) JSPS Blaeal jon eseach 4

25 Inenaonal/Domesc Collaboaons F. Kausz V. Yaovlev (MPQ) K.M. Lee (APRI Koea) G.F. Besch (Washngon) J. Bugdöfe (Venna Tech.) M. Schulze (UCB) K. Vaga (Vandebl) JSPS Blaeal jon eseach 5

26 Fs-pncples calculaon of ablaon deph of α-quaz (SO ) Enegy ansfe fom Lase pulse o elecons ω = 1.55eV ( λ = 800nm) E gap = 6.5eV (LDA) T = 10fs Ablaon heshold nensy W/cm Ablaon deph : 100nm E coheson = 9eV Melng heshold nensy W/cm Melhng deph 600nm E = 3T Mel 6 Typcal compuaonal me: node-hous

27 HA-PACS: Mul-GPU calculaon fo hybd funconal ( ) ( ) ( ) ( ) * 4 K e f e u w u u e d K n n K K n n n n n n + = π Hybd funconal povdes a bee pefomance fo solds. Calculaon of he nonlocal exchange s he bole nec. ( ) ( ) w u de f n n K K n n * 1 Ω Ω = We acceleae usng HA-PACS mul-gpu machne: Un cell: cubc 8 aoms/cell -pons:1 3 downsampled -pons:4 3 spaal gd: GPU(K090) cufft 15 hous Compason wh CPU (FFTW) In one node 4 GPUs s 4 mes fase han 16 CPU coes S delecc funcon

28 Code developmens (ARTED): Y. Shnohaa (Ph.D 013 now JSPS fellowshp MPI-Halle) S.A. Sao (M JSPS followshp fom Apl) Y. Tanguch (PD suppoed by he Cene developng GPU code) Compue esouces: ISSP Unv. of Toyo CCS Unv. of Tsuuba K-Compue ( Geneal pojec Saegc pogam) Exenal fnancal suppo: KAKENHI (Gans-n-Ad fo Scenfc Reseach MEXT) KIBAN(B) M Shn-gaujyusu (Koubo) M Shn-gaujyusu (Koubo) M Shn-gaujyusu (Keau) unde applcaon JSPS Blaeal Inenaonal Collaboaon beween US-Japan M 8