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Fig. 5(Color online) Schematic of timing synchronization andcontrol system for time­resolved PES system at SPring_8
BL07LSU. (Reprinted from M. Ogawa et al., Rev. Sci. In­
strum., 83 (2012) 023109.[6])(Color online) Start trigger signal for the operation of atime­of­ight analyzer in the several bunch mode of SPring_
8. Unequally­spaced start trigger signal (3rd from the top) is
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à¾µ½Æ¨èC|v[U[Év[uúËõÌp{ÍÅÍCäXÌ¤6_9) Ì©çVR\ÊÉCXÍ»ê¼êñ35 fsCñ50 ps ÅéB|v[U[³¹¼±Ì\ÊÌdqóÔâ´q\¢ÍCõGlM[1.55 eVCJèÔµüg 1 kHz ÉÝèð´qxÅnIÉÏ»³¹CõãNLAÌõ½µ½B|võ[U[ÆËÉæèãN³ê½¿ÌdqªÇÌæ¤ÉÏ»·é©ð²×½¤ðÐî·é9)B¼±

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WEiInjðz

ÌðõãNµ½ÛÉ­¶·é\ÊõNdÍøÊÉÂ¢ÄàüúËõðp¢Ä Si2p àkxõdqXyNgðª¾µ½ãCÀ±èCÀ±ÊÉÂ¢Äq×éB

èµj^[µ½B

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Si(111)\ÊÉCWEiInjðz

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Êâ¿Aj[·xð§ä·é¼±Ì\ÊÅÍC\ÊÆoNÌd×ÊÌá¢ðâ¤½±ÆÅClXÈ\Ê´q\¢É\Êdq\¢É\Ê×§ßÉ\ÊßTÉóÔd×wispace charge layer, SCLjª`¬³êCoNohÌGlM[ª\Ê[³ûüÉAxðàÁ½\ÊðÄ»«Ç­ìèª¯é±ÆªÅ«éBÀ±ÅÍCn­type Si(111)(r0.02 Qcmj\ÊÉº·Å In±IÉÏ»·éiohÈªèjBFig. 6(a)É¦·æ¤ÉCðz³¹½BFig. 7 ÉC{¤Åì»µ½lXÈ In/Sin ^¼±ÌÌêCohÍãü«ÉÈªÁÄ¢éB±Ì(111)\ÊÌ¸gl°÷¾ STM ð¦·BIn z¼±Ì\ÊÉoNohMbvÈãÌGlM[ðàOÌ Si(111)´òÊÍCDAS (dimer

adatomstacking­Âõi[U[jðÆË·éÆC¿dqÑ©ç`±ÑÖÌ

faultjf10) ÉæÁÄà¾³êéi7~7jÄ\¬\¢dqJÚªN«ÄdqÆ³Eª¶¬·éBiFig. 6(b)j±ðÆèC\Ê_OO{hÉR·é 2 ³à®

êç 2 íÞÌLAÍóÔd×wÌ|eVÉæ

IÈ\ÊdqóÔðàÂB±Ì Si(111)\ÊÉ0.3 ML (1èóÔIÉª£i³Eª\ÊÖCdqªoNÖÚ®jµC

ML7.8~1014 atoms/cm2 jÌ In ðz³¹éÆCIn ªNdÍª­¶·éB»ÌÊC¼±Ì\ÊßTÌohÈ

3 ~ 3 Ì·üú\¢ðÆé 3 ~ 3 _In/Si(111)\ÊðªèÍ¸­·éB±êð\ÊõNdÍiSurface Photovol­ì»·é±ÆªÅ«éB±Ì

tage, SPVjøÊÆÄÑCõÆËãC

ÍC¼±ÌIÈ\ÊdqóÔðàÂ11)BIn ÌzéèðàÁÄ

3 ~ 3 _In/Si(111)\ÊÊð0.5³ÌóÔÉßÁÄ¢­BSPV øÊÉæé\ÊÌ|eV

ML ÜÅÁ·éÆC 31~ 31_In/Si(111)\Êª¾çêÏ»ÍCõdqªõðp¢éÆàkÊÌs[NVté12) BIn ÌzÊª 1 ML ÉÈéÆCIn Í 1 ³IÈ´gÆµÄÏª·é±ÆªÅ«éB]ÁÄCõdqªõÉæè¼±Ì\ÊÌLA_Ci~NXð²×é±ÆªÅ«éBFig. 6(Color online) Schematics of energy diagrams for n­type
semiconductors with light OFF (a) and with light ON (b).
Ef is the energy of Fermi level. Ec and Ev are the energies ofconduction and valence band edges, respectively. The
amount of band bending (Vs) decreases due to surface pho­
tovoltage (SPV) eect when the light is ON. The region of aspace charge layer (SCL) is indicated with an arrow.

246  úËõ Sept. 2014 Vol.27 No.5

Fig. 7

STM images of various Si(111) surfaces with dierent Indi­um surface coverages: (a) clean Si(111)7~7 (0 ML_In),(b) 3 ~ 3 _In/Si(111) (0.3 ML_In) [16], (c) 31~ 31_
In/Si(111) (0.5 ML_
In) [12], (d) 4~1_
In/Si(111) (1 ML_In) [14]. The unit cell of each superstructure is shown as awhite rectangular in the gures.

ðà ¡ Ôªðî X üõdqªõ@Éæé\ÊLA_Ci~NX¤ÌiW

q½ð`¬µCº·ÅÍ 4~1 ·üú\¢ðÆé13,14)B±Ì 4~1_In/Si(111)\ÊÍC[ 1 ³à®IÈ\ÊdqóÔð¦·13,14) B±êçÌ·üú\¢ðàÂ In/Si(111)\ÊÌì»ÍCº·öµÈªçÌö

ãÌ¿Aj[Ü½Í¿Aj[

ðKvÆ·éB]ÁÄCº·öãÌ¿Aj[ðsíÈ¢ÆCÜ½Í¿Aj[·xðº°éÆC·üú\¢ðà½È¢\Ê×§xªå«¢\Êðì»·é±ÆªÅ«éB{¤ÅÍC·üú\¢ðàÁ½
3 ~ 3 _In/Si(111), 31~ 31_In/Si(111), 4~1_In/Si(111)\ÊÉÁ¦Cº·öÌ0.4 ML, 0.8 ML, 1.2 ML_

In/Si(111)\ÊyÑá·Aj[Ì 4~1_In/Si(111)\Êðì»µ½B±êçÌlXÈ In/Si(111)\ÊÌdq\¢iÁÉ\ÊohÈªèÌÊjÍCõdqªõðp¢ÄèÊIÉ]¿·é±ÆªÅ«éBSi(111)7~7 ´òÊÍCßÌ¤©
çdq\¢ªÇ­ª©ÁÄ¢é½ßC±êðîÆµ½B
Si(111)7~7 ´òÊÅÍC\ÊÅtF~Ê©ç Va­lence band maximum ÌGlM[·ª0.63 eV Åé±Fig. 8Time­resolved PES spectra of Si2p core level on the 3 ~3 _In/Si(111) surface at dierent pump­probe delay times.
The power density of pump laser was 3.1 mJ/cm2/pulse.

Fig. 9(Color online) Energy shift of Si2p3/2 core level on the sur­
In/Si(111)faces of (a) 3 ~ 3 _In/Si(111) and (b) 4~1_
as a function of delay time. The power density of pump laser
was 3.1 mJ/cm2/pulse. (Reprinted from M. Ogawa et al.,Phy. Rev. B, 88 (2013) 165313. [9])ÆªmçêÄ¢é15) BÀ±Ågpµ½ Si îÂi r0.02
QcmjÌêC\ÊÌohÈªèÍC0.37 eV Æ©Ïà
é±ÆªÅ«é9)BlXÈ In/Si(111)\ÊÉ¨¯éohÈªèÍCe\ÊÌ Si2p àkXyNgÌs[NÊuÌSi(111)7~7 ´òÊ©çÌVtgÊ©çßé±ÆªÅ«éBá¦ÎC4~1_In/Si(111)\ÊÌ Si2p àkXyNg
ðªè·éÆ Si(111)7~7 ´òÊÆärµÄ0.31 eV áGlM[¤ÖVtgµÄ¨è9)C\ÊÌohÈªè
Í0.37{0.310.68 eV ÆßçêéB

3.3

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Fig. 8 É

3 ~ 3 _In/Si(111)\ÊÉ¨¯é Si2p àkxÌÔªðõdqªõXyNgð¦·B|vÉv
[uxÔ[ÅÌ|võ[U[ÆËÉæèC
Si2p àkxÍGlM[¤ÉVtgµC»ÌãÔÆ¤É³ÌGlM[ÊuÖßÁÄ¢­±Æªª©
é B ± ± Å C 3 ~ 3 _In / Si ( 111 ) \ Ê y Ñ 4 ~ 1 _In /Si(111)\ÊÉ¨¯é Si2p3/2 àkxÌVtgÊÌÔÏ»ð Fig. 9(a,b)É¦·BVtgÊÍ|võ[U[ÆËOÌ Si2p3/2àkxÌGlM[ÊuðîÆµ½BFig. 9(a,b)©çª©éæ¤ÉC 3 ~ 3 _In/Si(111)\ÊÅÍ SPV øÊÌÉaªñ1000 ns ÅÙÚ®¹µÄ¢
éÌÉÎµC4~1_In/Si(111)\ÊÅÍ7000 ns ÅàÜ¾®¹µÄ¨ç¸C\ÊÉæèõãNLAÌõ½ªå«Fig. 10(a,c)É¦·æ¤ÉC 3 ~ 3 _In/Si(111)\ÊÅÍ­ÙÈé±Æªª©Á½BÜ½Ç¿çÌ\ÊÉ¨¢Äàtfast17 ns, tslow260 ns, 4~1_In/Si(111)\ÊÅÍ tfast

SPV øÊÌÉaßöÍC100 ns ÈºÌ¬¢ßöÆ100 ns

230 ns, tslow6400 ns Æ¢¤èª¾çê½B

ÈãÌx¢ßöÌ 2 ÂÌßö©ç\¬³êé±Æªª©
Á½B±Ì SPV øÊÌÉaßöÍC2 ÂÌwÖ©çÈé( t ){B exp(|t )V(t )A exp |

t

t

fast

slow

(3)

®(3)ðp¢ÄtBbgðs¤±ÆªÅ«C¬¢ßöÆxµ©µC±Ìæ¤ÈwÖðp¢½ðÍ©çßçê¢ßö»ê¼êÌè tfast, tslow ðßé±ÆªÅ«éB½è©çCSPV øÊÌÉaßöÉ¨¯é¨I`úËõ Sept. 2014 Vol.27 No.5  247

Fig. 10

(Color online) Energy shift of Si2p3/2 core level on the surfaces of (a, b) 3 ~ 3 _In/Si(111) and (c, d) 4~1_In/Si(111) as a function of delay time. The power density of pump laser was 3.1 mJ/cm2/pulse. In the panels of(a, c), the data are tted with a double exponential function [Eq. (3)]. The energy shift on the vertical axis isplotted on a logarithmic scale, and the delay time on the horizontal axis is plotted on a linear scale. The time con­stants of double exponential functions are given in the gure. In the panels of (b, d), the black broken and redsolid lines are the results of curve ts using tunneling [Eq. (5)] and thermionic [Eq. (6)] models, respectively.
The energy shift on the vertical axis is plotted on a linear scale, and the delay time on the horizontal axis is plottedon a logarithmic scale. The time constants of the thermionic and tunneling models for the surfaces are given in
the gure.

ð¾é±ÆÍ¢ïÅéB»±Å{¤ÅÍC¨fÉîÃ« SPV øÊÌÉaßöðð·é±ÆðÝ½B

Vtunnel(t )

SPV øÊÌÉaßöÍCoN©ç\ÊÖÌLAÌ[ ( ) (tae 2 2e2
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2ee0
2d
ttunnel)] (5)A¨æÑ\ÊÉ¨¯éLAÄÉæèis·éÆ±±ÅCe ÍdqÌfd×Ce0, e Í»ê¼ê^óÌUdð³êéBoN©ç\ÊÖÌLAÌAÉÍC\¦CäUd¦ÅÊÌ|eVáÇð·è²¯églßöÆ\ÊÌèµ½]èLA§xin ^¼±ÌÌêCz[Ì§|eVáÇðMIÉæèz¦éMdqßöÌ 2 í

xjCd Í|eVáÇÆÈéóÔd×wÌúÝÅ

ÞÌAßöª¶Ý·éBéBglßöfÍCn ^¼±ÌÌêCoNÌdqªóÔd×wÉR·é|eVáÇðgl±êÉÎµCMdqßöÉæéGlM[VtgÍÌ®(6)Å\³êé17)BßöÉæè·è²¯C\ÊÅz[ÆLAÄðN±·fÅ

éB±ÌglßöÉ¨¯éÉa¬x

éBn0 ÍóÔd×wÉ¨¯éêlÆ¼[ () ] (6)

Vthermal(t )|hkT ln 1| 1|e|VSPV(0)/hkT e|t/tsÍCglßöÉ¨¯éoNÌdqÆ\ÊÉ¨¯édqóÔÌg®ÖÌdÈèÉæÁÄÜéBglß±±ÅCh Í_CI[hfÉ¨¯ézWCk ÍöfÉ¨¯éLAÌ¬xûö®ÍC®(4)Ìæ¤{c}èCT Í·xCVSPV(0)Í t0 É¨¯éGlÉ\¹éB

M[VtgÊCts ÍõñÆËiÃd¬jÌLAõ( )dN(z,t )N(z,t )
2z
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|
dt
ae
ttunnel½ð\·B(4)Fig. 10 ( b,d ) É

3 ~ 3 _In / Si ( 111 ) ¨ æ Ñ 4 ~ 1 _In /Si(111)\ÊÉ¨¯é SPV øÊÌÉaßöÉglß±±ÅCz Ígl£Cae ÍoN©çÌLAðöyÑMdqßöÌfðKpµ½Êð¦·BIn/

ßl·é\ÊdqóÔÌ{[A¼aCttunnel ÍglßSi(111)\ÊÌ SPV øÊÌÉaßöÍCglßöÜöÌèÅ

½ÍMdqßöÌÇ¿ç© 1 ÂÌßöÌÝÅÍÄ»·ééBglßöÉæéGlM[VtgÍ®(5)Ìæ¤É\¹éB®(5)Ì±oÉÂ¢ÄÍC_¶9)ðQÆ³ê½¢B±ÆÍÅ«¸C¼ÒÌßöªKvÅ

é±Æªª©Á½B

Ü½ Fig. 10(b,d)É¦·æ¤ÉCZ¢xÔÉ¨¯éGlM[VtgÍglßöÉæèC·¢xÔÉ¨

248  úËõ Sept. 2014 Vol.27 No.5

ðà ¡ Ôªðî X üõdqªõ@Éæé\ÊLA_Ci~NX¤ÌiW

Fig. 11(Color online) Various time constants of (a) tslow, (b) tfast, (c) ts, and (d) ttunnel are plotted as a function of theamount of band bending Vs. The sample surfaces are labeled. The data points of ts in the panel (c) are well tted
with an exponential function (broken line). (Reprinted from M. Ogawa et al., Phy. Rev. B, 88 (2013) 165313.
[9])¯éGlM[VtgÍMdqßöÉæèÇ­Ä»·é±ttunnel ÍimbÈºÅÆªª©Á½BglßöyÑMdqßöÌfðK¢ In/Si(111)\ÊÅÍ10_20imböxÜÅÁµÄ¨

pµ½ÊCeßöÌè ttunnel, ts ªßçêéB
Fig. 11ÉlXÈ In/Si(111)\ÊÉ¨¢Ä 2 ÂÌwÖéÌÉÎµC\Ê·üú\¢ªÈ

èC\Êüú«ÆglßöÉæé SPV øÊÌ¬¢É
aßöÉÖª

é±Æªª©éBglßöÉæéõ

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ãNLAÌÉaÍCoN©ç\ÊÖÌdqÌglqßöÌfðKpµÄß½è ttunnel, ts ðe\ßöÉæéAyÑ\ÊÅÌdqÆz[ÌÄÌ 2

ÊÌ o h Èª è Vs É Î µÄ v bg µ½ B Fig. 11É

iK©çÈéB\Êüú«ÍC\ÊÉA³ê½LA

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3 ~ 3 _In/Si(111)¨æÑ 4~1_ idqjÌdC`±Á«Ée¿ð^¦éÆl¦çêéB\In/Si(111)\ÊÉÁ¦CSi(111)7~7 ´òÊC 31~ 31_

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250  úËõ Sept. 2014 Vol.27 No.5

éBG}ÈNiÞÇæ[ÈwZpåw@åwjÌeÌðà ¡ Ôªðî X üõdqªõ@Éæé\ÊLA_Ci~NX¤ÌiW·Jì@Çæ¶iåwjC^C~O¯úVXeÉÖµÄÍc`læ¶iºÉ§§åwj©ç²¾ð¸¢½BARTOF10k yÑxuÌ§ävOÌJ­ÍÛ´íiåwjÌ²¦Íð¸¢½BIn/Si(111)\11)ÊyÑ»Ì STM ÉÖµÄC·JìCiæ¶iåwj©ç²¾ð¸¢½B±ÌêðØèÄC[­äç\µã°½¢BÜ½C{eÅÐîµ½À±ÍåwúËõAg¤12)

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úËõ Sept. 2014 Vol.27 No.5  251

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E­mail: susumuissp.u­tokyo.ac.jp
êåF\Ê»wmªðn
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E­mail: imatsudaissp.u­tokyo.ac.jp
êåF \Ê¨Cá³¨«C¨»wCúËõÈw
mªðn
2001N 3  åwåw@wn¤È»wêUmÛöC¹CmiwjB
2001N 4  ú{wpU»ïÁÊ¤õ(PD)CXCX` [bqåwÉÄ¤B2001N 9  åwåw@wn¤È³B2006N12 åw¨«¤³ö/y³öC»ÝÉéB

Recent advances in surface carrier dynamics
research by time­resolved soft X­ray photoelec­tron spectroscopy
Susumu YAMAMOTO

The Institute for Solid State Physics, The University of Tokyo,
5_1_
5 Kashiwanoha, Kashiwa 277_
8581

Iwao MATSUDAThe Institute for Solid State Physics, The University of Tokyo,
5_1_
5 Kashiwanoha, Kashiwa 277_
8581

Abstract

Synchrotron radiation is a pulsed light source with a temporal width of about 50 picoseconds.
Time­resolved soft X­ray photoelectron spectroscopy (PES), which combines synchrotron radia­
tion X­ray with ultrashort pulse laser, allows to study the transient variation of electronic struc­tures of materials with a time resolution of 50 picosecond in a wide range of time scale frompicoseconds to milliseconds. In this review article, the experimental details on the time­resolved
soft X­ray photoelectron spectroscopy system developed at SPring_8 BL07LSU will be described.
As an example of experimental results with time­resolved PES, carrier dynamics on semiconduc­
tor surfaces will be presented. In addition, future directions of the time­resolved photoelectron
spectroscopy will be discussed.

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