ERL ࠿ࡽᚓࡽࢀࡿ◳ X ⥺ࢆ⏝࠸ࡓඛ➃ⓗ฼⏝◊✲┤㠃ࡍࡿㄢ㢟ࢆゎỴࡋᑗ᮶ࡢ⏕άࢆࢧ࣏࣮ࢺࡍ
ࡿ࡛࠶ࢁ࠺ࠋ
୍᪉ࠊ⏕࿨⣔ࡶᮏ㉁ⓗ࡟୙ᆒ୍࡛ືⓗ࡞ࢩࢫࢸ࣒࡛࠶ࡿࠋ᪤Ꮡࡢᨺᑕගᢏ⾡࡟ᇶ࡙࠸ࡓᵓ㐀⏕≀1. ࡣࡌࡵ࡟

Ꮫࡣྜ⌮ⓗ࡞๰⸆ࡢࡓࡵࡢ᭷⏝࡞᝟ሗ࡛࠶ࡿ㟼

ERL ࡣ᭱᪂ࡢ㉸ఏᑟ⥺ᙧຍ㏿ჾᢏ⾡ࢆ⏝࠸ࡓⓗ࡞ཎᏊᗙᶆࢆ୚࠼ࡿࡇ࡜࡟኱ࡁࡃ㈉⊩ࡋ࡚ࡁḟୡ௦㹖⥺ග※࡛࠶ࡾࠊ᪤Ꮡࡢᨺᑕගࢆ㐶࠿࡟෽

ࡓࠋERL ࡣࠊࡇࢀࡽ࡟ຍ࠼ࠊ⣽⬊ᶵ⬟ࡢ୙ᆒ୍ᛶ

㥙ࡍࡿග※ᛶ⬟ࢆᣢࡘࠋ㧗⧞ࡾ㏉ࡋࠊ▷ࣃࣝࢫࠊ

ࡸ」㞧ᛶࢆゎ᫂ࡍࡿࡇ࡜࡛⏕࿨⛉Ꮫࡸࣂ࢖࢜ᢏ

㧗✵㛫ࢥࣄ࣮ࣞࣥࢫࠊࡑࡋ࡚㧗㍤ᗘࡢ≉ᚩࡣ㉸㧗⾡࡟᭦࡞ࡿ㈉⊩ࢆᯝࡓࡍ࡛࠶ࢁ࠺ࠋ

㏿ࡢཎᏊື⏬᧜ᙳࢆྍ⬟࡜ࡋࠊ୙ᆒ୍⣔࡟࠾ࡅࡿࢼࣀࢫࢣ࣮ࣝࡢᵓ㐀Ỵᐃࡀྍ⬟࡜࡞ࡿࠋ
ERL ࡀᣢࡘ≉ᚩⓗ࡞ࡇࢀࡽࡢ⬟ຊࡣࠊX ⥺⛉Ꮫࡢ◊✲ᑐ㇟ࢆ“㟼ⓗ࡛ᆒ୍”ࡢ⣔࠿ࡽ“ືⓗ࡛୙ᆒ2. ࡞ࡐ ERL ࡀᚲせ࠿㸽
2.1. X ⥺※ࡢኚ㑄୍”ࡢ⣔࡬ኚ࠼ࡿࡼ࠺࡞᫂☜࡞ࣃࣛࢲ࢖࣒ࢩࣇࢺ

20 ୡ⣖ึ㢌ࡼࡾࠊX ⥺Ⳣࡣඛ㥑⪅ࣦ࢕ࣝ࣊ࣝ

ࢆࡶࡓࡽࡍ࡛࠶ࢁ࠺ࠋ࠸ࢃࡤ ERL ࠿ࡽᚓࡽࢀࡿ

࣒࣭ࣞࣥࢺࢤࣥ㸦1901 ᖺึ௦ࣀ࣮࣋ࣝ㈹ཷ㈹⪅㸧ග࡟ࡼࡗ࡚ࠊࡇࢀࡲ࡛୺࡜ࡋ࡚⾜ࢃࢀ࡚ࡁࡓ“᫬࡟ࡼࡗ࡚ X ⥺᧜ᙳࡢࡓࡵ࡟ࠊࡲࡓ࣮ࣟࣞࣥࢫ࣭ࣈ

㛫࣭✵㛫㸫ᖹᆒゎᯒ”࠿ࡽࠊ᪂ࡓ࡟“᫬㛫࣭✵㛫㸫ศࣛࢵࢢ㸦1915 ᖺࣀ࣮࣋ࣝ㈹ཷ㈹⪅㸧࡟ࡼࡗ࡚⤖ᬗ

ゎゎᯒ”ࡀᐇ⌧ྍ⬟࡜࡞ࡿ࡜ゝ࠼ࡿࠋᵓ㐀ゎᯒࡢࡓࡵ࡟୙ྍḞ࡞ࢶ࣮ࣝ࡜ࡋ࡚ᶵ⬟ࢆࡑࢀࡽࡢ୙ᆒ୍⣔≀㉁ࡣ௒ᚋࡶࠊゐ፹࣭ࣂࢵࢸ

ᯝࡓࡋ࡚ࡁࡓࠋ20 ୡ⣖༙ࡤ࡟ࡣࠊ1947 ᖺ࡟ࢮࢿ࣮࣭ࣜ㉸ఏᑟ࣭ࣂ࢖࢜⇞ᩱ࣭ࣛࣥࢲ࣒࢔ࢡࢭࢫ࣓

࣭࢚ࣛࣝࣞࢡࢺࣜࢵࢡ♫࡛ึࡵ࡚ᨺᑕගࡀほ ࡉ࣭ࣔࣜࢫࣆࣥࢺࣟࢽࢡࢫࢹࣂ࢖ࢫࠊගࢫ࢖ࢵࢳ➼ࢀࠊࡑࢀࡼࡾᨺᑕග᪋タࡣ X ⥺Ⳣࡼࡾᩘ᱆௨ୖࡶ

ࡢ୰࡛ᚲせ୙ྍḞ࡞ᢏ⾡࡜ࡋ࡚౑ࢃࢀ⥆ࡅࡿ࡜

㍤ᗘࡀ㧗࠸ࣅ࣮࣒ࢆᥦ౪ࡋ࡚࠾ࡾࠋX ⥺⛉Ꮫࠊ࠾⪃࠼ࡽࢀࡿࠋࡑࡇ࡛ࠊ୙ᆒ୍ᶵ⬟ᮦᩱࡀ࡝ࡢࡼ࠺

ࡼࡧࠊ࢖࣓࣮ࢪࣥࢢ࣭ཎᏊᵓ㐀ゎᯒ࣭ศගᏛ࡜࠸

࡟✌ാࡍࡿ࠿ࠊ᫬㛫ⓗ࣭✵㛫ⓗ࡞┤᥋᝟ሗ࡜ࡋ࡚

ࡗࡓᗈ࠸⠊ᅖࡢᛂ⏝࡟࠾࠸࡚ᩘከࡃࡢࣈ࣮ࣞࢡ

▱ࡿࡇ࡜ࡣࠊࡑࢀࡽࡢᮦᩱ࡟ࠊࡼࡾⰋ࠸ᶵ⬟ࢆᣢࢫ࣮ࣝᘬࡁ㉳ࡇࡋ࡚ࡁࡓࠋ21 ୡ⣖࡟࠾࠸࡚ ERLࡓࡏࡿࡓࡵࡢタィᣦ㔪ࢆ୚࠼ࠊ᭱⤊ⓗ࡟ࡣே㢮ࡀ

Fig. 1: ERL ࡟ࡼࡿࢼࣀࢫࢣ࣮ࣝࡢ✵㛫ศゎ⬟࠿ࡘࠊࡑࡢ⣔ࡀᣢࡘ⮬↛࡞᫬㛫ࢫࢣ࣮࡛ࣝࡢࠊ୙ᆒ୍ᶵ⬟ᛶᮦᩱ࡟࠾ࡅࡿືస≧ែࡢ㏣㊧[1] 㸫 

ࡣ᪂ࡋ࠸᫬௦ࡢ⛉Ꮫ◊✲ࢆඛᑟࡋࠊ᪤Ꮡࡢ᪋タ࡛

100 fs ࠿ࡽ 1ps ࡟ಖࡓࢀ࡚࠸ࡿࠋERL ࡢࣂࣥࢳࡣ୙ྍ⬟࡞Ⓨぢࢆࡶࡓࡽࡍ⬟ຊࢆᣢࡗ࡚࠸ࡿࠋ

㛗ࡣ⵳✚ࣜࣥࢢࡢ඾ᆺⓗ࡞ࣂࣥࢳ㛗㸦100 ps㸧ࡼ
ࡾ 2 ᱆▷ࡃࠊࢧࣥࣉࣝ࡟ࢲ࣓࣮ࢪࢆ୚࠼ࡿࡇ࡜࡞

2.2. X ⥺⛉Ꮫ࡟ࡼࡿᣢ⥆ྍ⬟࡞♫఍ࡢᐇ⌧ࡃࠊࡑࡢ⣔ࡢࡶࡘ⮬↛࡞᫬㛫ࢫࢣ࣮࡛ࣝ㉸㧗㏿⌧ᨻᗓࡣࠊࡼࡾᣢ⥆ྍ⬟࡞♫఍ࢆᐇ⌧ࡍࡿࡓࡵ࡟

㇟࡟࠾ࡅࡿືⓗ㐣⛬ࡢほ ࢆྍ⬟࡜ࡍࡿࠋᐇ㦂ࡢࢢ࣮ࣜࣥ㸭ࣛ࢖ࣇ࣭࢖ࣀ࣮࣋ࢩࣙࣥࡢಁ㐍ࢆ᪥ᮏᑐ㇟ࡣࠊゐ፹໬Ꮫ཯ᛂࠊගྜᡂ⣔ࠊᶵ⬟ᮦᩱࡢ┦ࡢᡂ㛗ᡓ␎࡜ࡋ࡚᣺⯆ࡋ࡚࠸ࡿࡀࠊ໬▼⇞ᩱࡢῶ㌿⛣࡜࠸ࡗࡓࠊᗈ⠊ᅖࡢືⓗ㐣⛬ࡀྵࡲࢀࡿࠋ

ᑡࠊ෌⏕ྍ⬟࢚ࢿࣝࢠ࣮ࡢ⏕ᡂࠊඛ㐍ࡢᮦᩱࡢ㛤Ⓨࠊ㔜⑓ࡢண㜵ࠊ೺ᗣⓗ࡞ࣛ࢖ࣇࢫࢱ࢖ࣝࡢ㐩ᡂ

2.5. ERL ࡢග※ᛶ⬟ϩϩ㸸✵㛫ࢥࣄ࣮ࣞࣥࢫ

࡜࠸ࡗࡓࠊᡃࠎࡢ♫఍ࡀ┤㠃ࡋ࡚࠸ࡿ㔜せ࡞ၥ㢟

ERL ࠿ࡽࡢᨺᑕග࡟࠾ࡅࡿ 2 ࡘ┠ࡢ㔜せ࡞≉ࢆゎỴࡍࡿࡓࡵ࡟ࡣ⛉Ꮫⓗ࡞ࣈ࣮ࣞࢡࢫ࣮ࣝࡀ

Ⰽࡣࠊࡑࡢ࡜࡚ࡶᑠࡉ࠸㟁Ꮚࣅ࣮࣒ࢧ࢖ࢬ࡜ࠊᚲせ୙ྍḞ࡛࠶ࡿࠋERL ࡣ㉸ఏᑟ✵Ὕࢆ⏝࠸ࡓ⥺

ERL ࡛㐩ᡂࡉࢀࡿࣅ࣮࣒Ⓨᩓᗘࡢ⤖ᯝᚓࡽࢀࡿࠊ

ᙧຍ㏿ჾᢏ⾡࡟ᇶ࡙ࡁࠊ㟼ⓗ࣭ᆒ୍⣔ࡢࡳ࡞ࡽࡎ

㧗࠸✵㛫ࢥࣄ࣮ࣞࣥࢫ࡛࠶ࡿࠋ୍⯡ⓗ࡟⵳✚ࣜࣥືⓗ࣭୙ᆒ୍⣔ࡢほ ࢆྍ⬟࡜ࡍࡿࠋࡇࡢࠊ୙ᆒ

ࢢ࠿ࡽࡢᨺᑕගࡢ✵㛫ࢥࣄ࣮ࣞࣥࢫࡣᮏ᮶࡜࡚

୍࡞ᶵ⬟ᮦᩱࡀᐇ᫬㛫ࢫࢣ࣮࣭ࣝࢼࣀࢫࢣ࣮࡛ࣝ

ࡶప࠸ࠋࡋࡓࡀࡗ࡚ࠊࡑࡢࡼ࠺࡞ప࠸✵㛫ࢥࣄ࣮࡝ࡢࡼ࠺࡟ືసࡍࡿ࠿ゎࡁ᫂࠿ࡍ⬟ຊࠊࡍ࡞ࢃ

ࣞࣥࢫࡢ X ⥺ࣅ࣮࣒ࢆ⏝࠸࡚ཎᏊศゎ⬟࡛ᵓ㐀Ỵࡕࠊືసୗ࡟࠾ࡅࡿࢼࣀࢫࢣ࣮࡛ࣝࡢཎᏊ࣭㟁Ꮚᐃࢆ⾜࠺ࡓࡵ࡟ࡣࠊ ᐃ≀㉁୰ࡢ✵㛫ࢥࣄ࣮ࣞࣥ

ᵓ㐀ࠊ໬Ꮫ⤌ᡂࠊ☢Ẽⓗᛶ㉁ࢆ≉ᚩ࡙ࡅࡿࡓࡵࡢ

ࢫ㸦⤖ᬗ⛛ᗎ㸧ࡀᚲ㡲࡜࡞ࡾࠊࡇࢀࡀ⌮⏤࡛ࠊཎ᪂ࡋ࠸ᡭẁࡣࠊୖグࡢ㞴ၥゎỴࡢࡓࡵࡢࣈ࣮ࣞࢡ

Ꮚࣞ࣋ࣝࡢᵓ㐀Ỵᐃ࡟࠾ࡅࡿ㐺ᛂᛶࡣ࿘ᮇⓗ࡞ࢫ࣮ࣝ࡜ᡂࡾ࠼ࡿ X ⥺⛉Ꮫࡢ㠉᪂ⓗ࡞㐍Ṍ࡛࠶ࡿᆒ୍ࢧࣥࣉࣝࡢࡳ࡟ไ㝈ࡉࢀ࡚࠸ࡿࠋࡇࡢ≧ἣࡣ

㸦Fig. 1㸧ࠋ

ERL ࡟ࡼࡗ࡚๻ⓗ࡟ኚࢃࡿࠋERL ࡢ㧗࠸✵㛫ࢥࣄ࣮ࣞࣥࢫ࡟ࡼࡗ࡚ࠊ㠀࿘ᮇ࡛୙ᆒ୍࡞≀㉁࠿ࡽ

2.3. ERL ࡟࠾ࡅࡿ㟁Ꮚࣅ࣮࣒ࡢᖹ⾮ᛶ⬟࡛ࡶࠊᩓ஘ࡉࢀࡿ X ⥺ࣅ࣮࣒ࡢᖸ΅ࢆグ㘓ࡍࡿࡇ᪤Ꮡࡢ⵳✚ࣜࣥࢢᢏ⾡ࡢ᭱ࡶỴᐃⓗ࡞ไ㝈ࡣࠊ࡜ࡀྍ⬟࡜࡞ࡾࠊࡋࡓࡀࡗ࡚ࠊཎ⌮ⓗ࡟ࡣ X ⥺ࡢ㟁Ꮚࣅ࣮࣒ࡢᖹ⾮ᛶ㉁࡛࠶ࡿࠋ㟁Ꮚࣂࣥࢳࡀ⵳✚Ἴ㛗࣮࢜ࢲ࣮㸦~0.1 nm㸧ࡢ✵㛫ศゎ⬟࡛୙ᆒ୍ࣜࣥࢢෆࢆఱᅇࡶ࿘ᅇࡍࡿࡓࡵࠊ㟁Ꮚࣅ࣮࣒ࡢࢧ

≀㉁ࡢᵓ㐀ゎᯒࡀྍ⬟࡜࡞ࡿࠋࡇࡢ≉ᚩ࡟ࡼࡾᐇ

࢖ࢬࠊⓎᩓࠊࣂࣥࢳ㛗ࡣᖹ⾮໬ࡉࢀࠊ᭱⤊ⓗ࡟ึ⌧ࡉࢀࡿࠊ୙ᆒ୍࡞ᶵ⬟ᮦᩱ࡟ᗈࡃ㐺ᛂ࡛ࡁࡿᵓ

ᮇ㟁Ꮚࣅ࣮࣒ࡢࣃ࣓࣮ࣛࢱ࣮ࡣᗈࡀࡗࡓࡶࡢ࡜

㐀ゎᯒࡣ X ⥺࡟ࡼࡿཎᏊྍど໬ᢏ⾡࡟኱ᖜ࡞ᨵ㠉࡞ࡿࠋ୍᪉ࠊERL ࡣᇶᮏⓗ࡟⥺ᙧຍ㏿ჾ࡛࠶ࡾࠊ

ࢆࡶࡓࡽࡍࠋ

㟁Ꮚࣂࣥࢳࡣຍ㏿ࡉࢀࠊࣜࣥࢢࢆ 1 ᅇ࿘ᅇࡋࡓᚋ
ῶ㏿ࡉࢀࠊࢲࣥࣉࡍࡿࠋࡇࡢ≉ᚩࡣ ERL ࡟ᅛ᭷ࡢϪ㸸ࢼࣀࣅ࣮࣒
2.6. ERL ࡢග※ᛶ⬟Ϫ

฼Ⅼ࡛࠶ࡿࠋࡇࡢ᭱ඛ➃ࡢ┤⥺ຍ㏿ჾᢏ⾡ࡣ᪤Ꮡྠ᫬࡟㟁Ꮚࣅ࣮࣒ࡢⓎᩓゅࡣ 17 pmrad ⛬ᗘ࡜ࡢ⵳✚ࣜࣥࢢᆺග※࡜ẚ࡭࡚᱁ẁ࡟㧗࠸ᛶ⬟ࢆ࡞ࡿࠋࡇࢀࡣ᪤Ꮡࡢ⵳✚ࣜࣥࢢࡢⓎᩓゅ㸦㹼1⏕ࡳฟࡋࠊḟୡ௦ X ⥺ග※ࡢᇶ♏ᢏ⾡࡜ࡋ࡚ࡢᑗ

nmrad㸧࡜ẚ࡭࠾ࡼࡑ 60 ศࡢ 1 ࡢ್࡛ࠊ㌾ X ⥺᮶ⓗ࡞ᣑᙇᛶࡶಖドࡍࡿࡶࡢ࡛࠶ࡿࠋ

ࡢᅇᢡ㝈⏺㸦O = 0.2 nm㸧࡜࡯࡜ࢇ࡝➼ࡋ࠸್࡛࠶ࡾࠊᅇᢡ㝈⏺ࡢ X ⥺ࣅ࣮࣒ࢆ⏝࠸ࡿ࡜ࢼࣀ࣓࣮

Ϩ㸸▷ࣃࣝࢫ
2.4. ERL ࡢග※ᛶ⬟Ϩࢺࣝࢧ࢖ࢬ㞟ගࡀྍ⬟࡜࡞ࡿࠋࡇࢀࡀ ERL ࡢ 3

ERL ࡢ୺せ࡞≉ᚩࡣ▷ࣃࣝࢫࠊ✵㛫ࢥࣄ࣮ࣞࣥ

ࡘ┠ࡢ≉ᚩ࡛࠶ࡿࠋX ⥺㟁Ꮚศග㸦XPS㸧ࠊX ⥺྾ࢫࠊࢼࣀࣅ࣮࣒࡛࠶ࡿࠋ▷ࣃࣝࢫᛶ⬟࡟㛵ࡋ࡚ࡣࠊ཰ศග㸦XAS㸧ࠊX ⥺Ⓨගศග㸦XES㸧ࠊX ⥺☢Ẽ㟁Ꮚࣂࣥࢳࡀࣜࣥࢢࢆ㸯࿘ࡋࣂࣥࢳ㛗ࡀఙࡧࡿ஧Ⰽᛶ㸦XMCD㸧ࠊඹ㬆㠀ᙎᛶ X ⥺ᩓ஘㸦RIXS㸧ࡇ࡜↓ࡃࢲࣥࣉࡍࡿ㛫࡟ ERL ࡢ㟁Ꮚࣂࣥࢳ㛗ࡣ࡜࠸ࡗࡓ X ⥺ࡢศගᏛⓗᡭἲࡣࠊࢼࣀ࣓࣮࣮ࣝ࢜ 㸫 

ࢲ࣮ࡢ✵㛫ศゎ⬟࡟࠾࠸࡚୙ᆒ୍≀㉁ࡢ㟁Ꮚⓗ࣭ࡀྍ⬟࡜࡞ࡿࠋ㏆ᖺࠊ⣸እ࠿ࡽ㉥እἼ㛗ᇦࡢ㉸▷☢Ẽⓗᛶ㉁ࢆㄪᰝࡍࡿࡢ࡟ᙉຊ࡞ᡭἲ࡜࡞ࡿࠋ

ࣃࣝࢫ࣮ࣞࢨ࣮ࢆ⏝࠸ࡓ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲ࡟ࡼ
ࡾࠊࣇ࢙࣒ࢺ⛊࣮࢜ࢲ࣮ࡢศᏊ᣺ືࡸ㟁Ꮚ㑄⛣ࢆ

2.7. ERL ࡜ SASE--XFEL ࡢẚ㍑ࣜ࢔ࣝࢱ࢖࣒࡛ほ ࡛ࡁࡿࡼ࠺࡟࡞ࡗࡓࡀࠋࡑࢀ

SASE-XFEL ࡜ẚ㍑ࡍࡿ࡜ࠊSASE-XFEL ࡜࡜ࡣ┦⿵ⓗ࡟ࣉ࣮ࣟࣈග࡟ࣃࣝࢫ X ⥺ࢆ⏝࠸ࡓ᫬

ERL ࡢග※≉ᛶࡣ␗࡞ࡗ࡚࠾ࡾࠊ࠸ࡃࡘ࠿ࡢⅬ࡛㛫ศゎ X ⥺ ᐃࢆᐇ᪋ࡍࢀࡤࠊཎᏊࢫࢣ࣮ࣝࡢື

┦⿵ⓗ࡛࠶ࡿࠋSASE-XFEL ࡣẚ㍑ⓗప⧞ࡾ㏉ࡋⓗᵓ㐀᝟ሗࢆ┤᥋ⓗ࡟ᚓࡿࡇ࡜ࡀྍ⬟࡜࡞ࡿࠋ࡛ࠊ㧗࠸ࣆ࣮ࢡࣃ࣮࣡ࡢ X ⥺ࣃࣝࢫࢆ᭷ࡍࡿࠋ୍᪉ࠊERL ࡣẚ㍑ⓗప࠸ࣆ࣮ࢡࣃ࣮࣡࡜㠀ᖖ࡟㧗⧞

3.2. ⵳ ✚ࣜࣥࢢᆺᨺᑕග࡟࠾ࡅࡿࣆࢥ⛊ࣃࣝࢫX ⥺Ⓨ⏕

ࡾ㏉ࡋ㸦1.3 GHz㸧ࡢ X ⥺ࣃࣝࢫࢆ⏕ᡂࡍࡿࠋ⥲ィ࡛ࡇࢀࡽࡢ᫬㛫ᖹᆒࡉࢀࡓගᏊ᮰㸦༢఩᫬㛫ᙜ⌧ᅾࠊࣃࣝࢫ X ⥺ࢆⓎ⏕ࡉࡏࡿ᪉ἲ࡜ࡋ࡚ࡣࠊ

ࡓࡾࡢගᏊᩘ㸧ࡣ 2 ࡘࡢග※࡛ྠ➼࡛࠶ࡿࠋ
SASE-ᨺᑕගࡸ X ⥺⮬⏤㟁Ꮚ࣮ࣞࢨ࣮㸦XFEL㸧࡜࠸ࡗ

XFEL ࡛ࡣࡑࡢ㧗࠸ࣆ࣮ࢡࣃ࣮࣡ࡢࡓࡵࢼࣀ࣓࣮

ࡓຍ㏿ჾග※ࢆ⏝࠸ࡿ᪉ἲࡸࠊ࣮ࣞࢨ࣮ࣉࣛࢬ࣐

ࢱɆࢧ࢖ࢬࡲ࡛㞟ගࡋ࡚ᐇ㦂ࢆ⾜࠺࡜ࢧࣥࣉࣝࡢ

ࢆ⏝࠸ࡿ᪉ἲ࡞࡝ࡀ࠶ࡿࡀࠊࡇࡇ࡛ࡣࠊ୺࡟ຍ㏿◚ቯࢆక࠺ᐃ࡜࡞ࡿࠋࡇࡢព࿡࡛ࡣࠊSASE-ჾග※ࡢࣃࣝࢫ X ⥺࡟ࡘ࠸࡚ゎㄝࢆ⾜࠺ࠋᨺᑕගXFEL ࡣᴟ㝈⎔ቃ࡟࠾ࡅࡿ≀㉁◊✲ࡢ඲ࡃ᪂ࡋ࠸

ࡣࠊ㟁Ꮚ⵳✚ࣜࣥࢢ୰ࡢ㟁Ꮚࡢ㌶㐨ࡀ☢ሙ࡟ࡼࡗᶵ఍ࢆ୚࠼࡚࠸ࡿ࡜ࡶゝ࠼ࡿࠋ୍᪉ࠊERL ࣃࣝࢫ࡚᭤ࡆࡽࢀࡿࡇ࡜࡛෇㐠ືࡢ᥋⥺᪉ྥ࡟ᨺฟࡉ

ࡢࣆ࣮ࢡࣃ࣮࣡ࡣከࡃࡢ≀㉁ࡢࢲ࣓࣮ࢪ㜈್ࢆࢀࡿ㟁☢ሙ࡛࠶ࡿࡀࠊ㟁ᏊࡣᨺᑕගⓎ⏕࡟ࡼࡗ࡚㉸࠼࡞࠸ࡓࡵࠊᩘከࡃࡢࣅ࣮࣒ࣛ࢖ࣥ࡜࣮ࣘࢨ࣮

ኻ࠺࢚ࢿࣝࢠ࣮ࢆຍ㏿✵Ὕࡢ㧗࿘Ἴᩘ㟁ሙ࠿ࡽ࡟✵㛫ࢥࣄ࣮ࣞࣥࢫ࣭ࢼࣀࣅ࣮࣒࣭▷ࣃࣝࢫࢆᣢ

⿵ࡗ࡚࠸ࡿࠋࡇࡢຍ㏿✵Ὕࢆ≉ᐃࡢ఩┦࿘ࡾ࡛㏻

ࡗࡓ㧗ရ㉁࡞ࣅ࣮࣒ࢆᥦ౪ࡍࡿࡇ࡜ࡀྍ⬟࡜࡞㐣ࡍࡿ㛗ࡉᩘ cm ⛬ᗘࡢ㟁Ꮚࡢ㞟ᅋ㸦㟁Ꮚࣂࣥࢳ㸧ࡿࠋࡣ⵳✚ࣜࣥࢢෆࢆᏳᐃ࡟ᅇࡾ⥆ࡅࡿࡇ࡜ࡀ࡛ࡁ

3. ࣃࣝࢫ X ⥺ࢆ⏝࠸ࡓ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈ
ィ ἲ

ࡿࠋୖ㏙ࡢࡼ࠺࡟㟁Ꮚࣂࣥࢳࡀ☢ሙ࡟ࡼࡗ࡚ຍ㏿㐠ືࡍࡿ࡜ࠊࡑࡢ✵㛫ⓗᗈࡀࡾ࡟ᑐᛂࡋࡓ᫬㛫ᖜࢆᣢࡘ㟁☢Ἴ㸦ᨺᑕගࣃࣝࢫ㸧ࡀⓎ⏕ࡍࡿࠋᨺᑕ
ගࣃࣝࢫࡢ᫬㛫ⓗᛶ㉁ࡣ㧗࿘Ἴຍ㏿ࡢ࿘Ἴᩘࠊ⵳

3.1. ࣏ࣥࣉ࣭ࣉ
ࣉ࣮ࣟࣈィ ἲ࡜ࡣ✚ࣜࣥࢢ୰ࡢ㟁Ꮚࣅ࣮࣒ࢧ࢖ࢬࠊ㟁Ꮚࣂࣥࢳ࠶ࡓ

ࡇࡇ࡛ࡣගࢆࢺ࣮ࣜ࢞࡜ࡋࡓ㉸㧗㏿࡞ᵓ㐀ኚࡾ࡟⵳✚ࡉࢀࡓ㟁Ꮚᩘ࡞࡝ࡢ᮲௳࡟ࡼࡗ࡚␗࡞

໬ࢆ᫬㛫ศゎ X ⥺ᐇ㦂࡛ほࡍࡿᢏ⾡࡟ࡘ࠸࡚ゎࡿࡀࠊࣃࣝࢫ᫬㛫ᖜࡣ್༙ᖜ࡛ᴫࡡ 100 ps ⛬ᗘㄝࡍࡿࠋ᫬㛫ศゎ ᐃ࡛ほࡍࡿບ㉳≧ែࡀ㛗ᑑ࡛࠶ࡿࠋࡇࡢᨺᑕගࡢ᫬㛫ⓗᛶ㉁ࢆ฼⏝ࡍࡿࡇ࡜࿨࡛࠶ࢀࡤ㐃⥆ X ⥺࡜㧗㏿᳨ฟჾࢆ฼⏝ࡋࡓ᫬㛫࡟ࡼࡾࠊࣆࢥ⛊࣮࢜ࢲ࣮ࡢ᫬㛫ศゎ X ⥺ᐇ㦂ࡀྍศゎ X ⥺ ᐃࡣ༑ศ࡟ᐇ᪋ྍ⬟࡛࠶ࡿࡀࠊࡑࡢᑑ

⬟࡜࡞ࡿ[2]ࠋ

࿨ࡀ▷ࡃ࡞ࡿ࡯࡝㐣Ώⓗ࡞ࢩࢢࢼࣝ㔞ࡣῶᑡࡍࡿࡢ࡛ࠊ⌧ᐇⓗ࡟ࡣ࣐࢖ࢡࣟ⛊௨ୗࡢ᫬㛫ࢫࢣ࣮

3.3. SASE--XFEL ࡟࠾ࡅࡿࣇ࢙࣒ࢺ⛊ࣃࣝࢫ X⥺Ⓨ⏕

ࣝ࡟࠾ࡅࡿᵓ㐀ኚ໬ࡢ᝟ሗࢆᚓࡿࡓࡵ࡟ࡣࠊ㧗ᙉᗘࣃࣝࢫ X ⥺ࢆ⏝࠸ࡓ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲࡀᚲせ⌧ᅾࠊ᪥ᮏࠊ⡿ᅜ࡛✌ാ୰ࡢ XFEL ࡣࠊ⥺ᙧຍ࡜࡞ࡿࠋ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲ࡜ࡣ࣏ࣥࣉග࡟ࡼࡗ

㏿ჾ࡜ SASE ࡢཎ⌮ࢆ⏝࠸࡚࠸ࡿࠋග㟁ᨺฟࡸ㟁࡚సࡾฟࡋࡓບ㉳≧ែࢆࣉ࣮ࣟࣈග࡟ࡼࡗ࡚ほ⏺㟁Ꮚᨺฟࢆ⏝࠸࡚㟁Ꮚ㖠࠿ࡽⰋ㉁࡞ࣃࣝࢫ㟁ࡍࡿᡭἲ࡛࠶ࡿࠋ࣏ࣥࣉග࡜ࣉ࣮ࣟࣈගࡢ㐜ᘏᏊࣅ࣮࣒ࢆྲྀࡾฟࡋࠊ⥺ᙧຍ㏿ჾ࡟ࡼࡗ࡚࡯ࡰග

᫬㛫ࢆኚ࠼࡞ࡀࡽ ᐃࢆ⾜࠺ࡇ࡜࡛ࠊບ㉳≧ែࡢ㏿ᗘ࡟ຍ㏿ࡉࡏࠊ㛗㊥㞳࢔ࣥࢪ࣮ࣗࣞࢱ࣮࡟ධᑕ

᫬㛫ኚ໬ࢆࢫࢺࣟ࣎᧜ᙳࡢࡼ࠺࡟㏣㊧ࡍࡿࡇ࡜ࡉࡏࡿࠋ࢔ࣥࢪ࣮ࣗࣞࢱ࣮ࡢ୰ࢆ⺬⾜ࡍࡿ㟁Ꮚࡢ 㸫 

ືࡁࡣ࠾஫࠸࡟ᙉ࠸┦㛵ࢆᣢࡕࠊྛ㟁Ꮚࡢฟࡍග

ࣥࢳᅽ⦰࡟ࡼࡿ 100 fs ௨ୗࡢศゎ⬟ࡀཎ⌮ⓗ࡟ࡀᖸ΅ࡍࡿࡇ࡜࡟ࡼࡾ X ⥺㡿ᇦࡢ⮬⏤㟁Ꮚ࣮ࣞࢨࡣᚓࡽࢀࡿࠋ

࣮ࡀ SASE ࡜ࡋ࡚Ⓨගࡍࡿࠋᨺᑕගࡢࣜࣥࢢᆺຍ
㏿ჾ࡜ࡣ␗࡞ࡾࠊXFEL ࡛ࡣ㟁Ꮚࢆ⵳✚ࡉࡏࡿᚲせࡀ↓࠸ࡓࡵࠊຍ㏿ჾෆ࡟࠾ࡅࡿ㐍⾜᪉ྥࡢ㟁Ꮚࣂࣥࢳᅽ⦰ࡀᐜ᫆࡜࡞ࡿࠋ㐍⾜᪉ྥ఩⨨࡟┦㛵ࡋࡓ࢚ࢿࣝࢠ࣮ኚㄪࢆ㧗࿘Ἴ㟁ሙ࡟ࡼࡗ࡚௜ࡅࡿ

4. ࢫ ࣆࣥ㌿⛣࡟㉳ᅉࡋࡓ㉸㧗㏿ศᏊᵓ㐀ኚ໬
4.1. 㕲㘒య࡟࠾ࡅࡿࢫࣆࣥࢡࣟࢫ࣮࢜ࣂ࣮

ࡇ࡜࡛⥺ᙧຍ㏿ჾෆ࡟࠾࠸࡚ࣂࣥࢳᅽ⦰ࡀᐇ⌧㕲㸦஧౯㸧㘒యࡣ㟁Ꮚ≧ែࠊ☢ᛶࠊࡑࡋ࡚ศᏊ

ࡉࢀࠊ᭱⤊ⓗ࡟ࡣᩘ࣑ࢡࣟࣥ⛬ᗘࡲ࡛㟁Ꮚࣂࣥࢳᵓ㐀࡟࠾ࡅࡿࢲ࢖ࢼ࣑ࢡࢫࡀᙉࡃ⤖ࡧ௜࠸࡚࠾

ࡣᅽ⦰ࡉࢀࡿࠋࡋࡓࡀࡗ࡚ XFEL ࡛ࡣ 100 fs ௨ࡾࠊ㏆ᖺࠊእ㒊せᅉ࡟ࡼࡗ࡚పࢫࣆࣥ(LS)ᇶᗏ≧ୗࡢ㧗ᙉᗘࣃࣝࢫ X ⥺ࢆ⏝࠸ࡓ≀ᛶ◊✲ࢆ⾜࠺ࡇែ࠿ࡽ㧗ࢫࣆࣥ(HS)ບ㉳≧ែ࡬ࡢࢫࣆࣥ㌿⛣ࢆ࡜ࡀྍ⬟࡜࡞ࡿ[3]ࠋ

♧ࡍࢫࣆࣥࢡࣟࢫ࣮࢜ࣂ࣮⌧㇟࡟ࡘ࠸࡚ࠊ≉࡟⢭ຊⓗ࡟◊✲ࡀ⾜ࢃࢀ࡚࠸ࡿࠋHS ≧ែ࠿ࡽ LS ≧3.4. ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲࡢ᫬㛫ศゎ⬟ែ࡬ࡢ⦆࿴ࢲ࢖ࢼ࣑ࢡࢫࡢ◊✲ࡣᇶ♏≀ᛶࡢ⌮࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲࡢ᫬㛫ศゎ⬟ࡣ᳨ฟჾࡢ᫬

ゎࡢࡳ࡞ࡽࡎࠊ㛗ᑑ࿨ࡢ HS ≧ែࢆᣢࡘศᏊࡢタ㛫ᛂ⟅ᛶ࡛Ỵᐃࡉࢀࡿࡶࡢ࡛ࡣ↓ࡃࠊ2 ࡘࡢࣃࣝィ࡟࠾࠸࡚ࡶ㔜せ࡛࠶ࡾࠊ☢Ẽグ᠈⿦⨨ࡸ཮Ᏻᐃࢫࡢ㐜ᘏ᫬㛫ࡢࡳ࡟౫Ꮡࡍࡿࠋ࣏ࣥࣉග࡜ࡋ࡚ග

ࢹࣂ࢖ࢫࡢ㛤Ⓨ࡟㈉⊩ࡍࡿࡇ࡜ࡀᮇᚅࡉࢀࡿࠋࡲ

Ꮫࣃࣝࢫ࣮ࣞࢨ࣮ࠊࣉ࣮ࣟࣈග࡜ࡋ࡚ຍ㏿ჾ࠿ࡽࡓ㉸㧗㏿ࢫࣆࣥ㌿⛣⌧㇟ࢆ⏝࠸ࡓࢼࣀࢫࢣ࣮ࣝ

Ⓨࡏࡽࢀࡿ X ⥺ࢆ⏝࠸ࡿ᫬㛫ศゎ X ⥺ ᐃ࡛ࡣࠊ࡛ࡢᶵ⬟⣲Ꮚ࡜࠸ࡗࡓ᪂ࡋ࠸ᢏ⾡ࡶᥦ᱌ࡉࢀ࡚

ࡑࡢ᭱ᑡ᫬㛫ศゎ⬟ࡣࠊ୧ග※ࡢࣃࣝࢫᖜ࡛Ỵᐃ࠾ࡾࠊࡇࡢࡼ࠺࡞◊✲࡟࠾࠸࡚ࠊࡼࡾ▷࠸᫬㛫ࢫࡉࢀࡿࠋ࣏ࣥࣉග࡛࠶ࡿගᏛࣃࣝࢫ࣮ࣞࢨ࣮࡛ࡣ

ࢣ࣮࡛ࣝࡢᒁᡤⓗ࡞ᵓ㐀࣭㟁Ꮚ≧ែ࣭ࢫࣆࣥ≧ែ

100 fs ௨ୗࡢග※ࡣᗈࡃὶ㏻ࡋ࡚࠸ࡿࡓࡵࠊ᫬㛫ࡢ᝟ሗࢆᚓࡿࡇ࡜ࡣᚲせ୙ྍḞ࡛࠶ࡿࠋศゎ X ⥺ ᐃࡢ᫬㛫ศゎ⬟ࡣࣉ࣮ࣟࣈග࡛࠶ࡿ X⥺ࡢࣃࣝࢫᖜ࡟౫Ꮡࡋࠊᨺᑕග࡛ࡣ⮬↛ࣂࣥࢳ㛗

4.2. ᫬㛫ศゎ XAFS ἲ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲࢆ⏝࠸ࡓ᫬㛫ศゎ XAFS ࡢ࡟㉳ᅉࡋࡓ 100 ps ⛬ᗘࡢศゎ⬟ࠊXFEL ࡛ࡣࣂ⧞ࡾ㏉ࡋ࿘Ἴᩘࡣග※ࡢ࿘Ἴᩘࠊ᳨ฟჾ⣔ࡢືస

Fig. 2: ⵳✚ࣜࣥࢢᆺᨺᑕග࡟࠾ࡅࡿ࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲࢆ⏝࠸ࡓ᫬㛫ศゎ XAFS ࡢ ᐃࢩࢫࢸ࣒ᴫ␎ᅗ 㸫 

7125 eV

EXAFS
低スピン状態
差分スペクトル
励起後50ピコ秒

プリエッジ

7120

7130

7140

差分

0

7110

7125 eVにおける時間発展

強度 (相対値)

強度 (相対値)(b)

Fe K-edge XAFS

(a)

-200

7150

0

200

400

600

800

遅延時間 (ピコ秒)

X線エネルギー (eV)Fig. 3: (a)ᇶᗏ≧ែࡀపࢫࣆࣥ≧ែ࡛࠶ࡿ[FeII(phen)3]2+Ỉ⁐ᾮࡢ Fe K ྾཰➃࡟࠾ࡅࡿ XAFS ࢫ࣌ࢡࢺࣝ㸦ᐇ⥺㸧࡜ගບ㉳ᚋ 50 ps ࡟࠾ࡅࡿ㐣Ώ྾཰ᕪศࢫ࣌ࢡࢺࣝ㸦ⓑ୸㸧㸬(b)ᶓ㍈ࢆ X ⥺࡜࣮ࣞࢨ࣮ࡢ㐜ᘏ᫬㛫࡜ࡋ࡚ࣉࣟࢵࢺࡋࡓ 7125 eV ࡟࠾ࡅࡿᙉᗘࡢ᫬㛫Ⓨᒎ㸬࿘Ἴᩘࠊບ㉳≧ែᑑ࿨ࠊ➼ࢆ⪃៖ࡋ࡚Ỵᐃࡉࢀࡿ࡚࣮ࣞࢨ࣮ບ㉳ࡉࢀࡓ X ⥺ࢩࢢࢼࣝࡢࡳ᳨ฟࡍࡿ

ࡀࠊᨺᑕග࡟࠾ࡅࡿ ᐃ࡛ࡣ୍⯡ⓗ࡟㧗ᙉᗘࣃࣝ᪉ἲࠊࢳࣙࢵࣃ࣮ࢆ⏝࠸࡚ࢧࣥࣉࣝ࡟ධᑕࡍࡿ๓

ࢫ X ⥺ࡀᚓࡽࢀࡿ㧗㟁ⲴᐦᗘᏙ❧ࣂࣥࢳࢆྵࡴ㐠࡟࿘Ἴᩘࢆྜࢃࡏࡿ᪉ἲࠊࡲࡓࡣᮏࢩࢫࢸ࣒ࡢࡼ

㌿࣮ࣔࢻ᫬࡟ᐇ᪋ࡉࢀࡿࡓࡵࠊ᭱኱⧞ࡾ㏉ࡋ࿘Ἴ࠺࡟ࢩࢢࢼࣝࢆࣃࣝࢫ࡛ィᩘࡣ 1 MHz ⛬ᗘࡢᏙ❧ࣂࣥࢳ࿘Ἴᩘ࡜࡞ࡿࠋ

㑅ᢥࡍࡿ᪉ἲࠊ➼ࡀ⏝࠸ࡽࢀࡿࠋࡲࡓࠊࡇࡢᴫ␎

ࡋ㐺ᙜ࡞ࣃࣝࢫࢆ

Fig.2 ࡟ KEK PF-AR ࡟࠾ࡅࡿ᫬㛫ศゎ XAFSᅗ࡟࠾࠸࡚⁐ᾮࡢࢧࣥࣉࣝࡣ࣐ࢢࢿࢵࢺࢠ࢔࣏

ᐃࢩࢫࢸ࣒ࡢᴫ␎ᅗࢆ♧ࡍࠋ㏻ᖺࢩࣥࢢࣝࣂࣥ

ࣥࣉ࡟ࡼࡗ࡚ᚠ⎔ࡉࢀ࡚࠸ࡿࡀࠊ᫬㛫ศゎ XAFSࢳ࣮ࣔࢻ࡛㐠㌿ࡉࢀ࡚࠸ࡿ PF-AR ࡟࠾࠸࡚࿘ᅇ

࡛ࡣ X ⥺࡟ຍ࠼ࣃࣝࢫ࣮ࣞࢨ࣮ࡶࢧࣥࣉࣝ࡟ධᑕ

࿘Ἴᩘ 794 kHz ࡛ฟᑕࡉࢀࡿ㧗ᙉᗘࣃࣝࢫ X ⥺ࡍࡿࡓࡵࠊࡑࢀࡽ࡟ࡼࡿヨᩱࡢᦆയ≧ἣࢆ༑ศ࡟

ࡣࠊSi(111)⤖ᬗࢆ⏝࠸ࡓ஧⤖ᬗศගჾ࡟ࡼࡗ࡚༢

⟶⌮ࡋ࡚ ᐃࢆ⾜࠺ᚲせࡀ࠶ࡿࠋⰍ໬ࡉࢀࠊ‴᭤෇⟄࣑࣮ࣛ࡟ࡼࡗ࡚ࠊヨᩱ఩⨨࡟㞟ගࡉࢀࡿࠋᮏࢩࢫࢸ࣒࡛ࡣࠊ᪋タࡢ࣐ࢫࢱ࣮ࢡ

ほ
4.3. ࢫ ࣆࣥࢡࣟࢫ࣮࢜ࣂ࣮࡜ᵓ㐀ኚ໬ࡢ┤᥋ほࣟ ࢵ ࢡ ࡜ ྠ ᮇ ࡋ ࡓ 946 Hz ࡢ ࣇ ࢙ ࣒ ࢺ ⛊Ti:Sapphire ࣮ࣞࢨ࣮ࢆ࣏ࣥࣉග࡜ࡋ࡚⏝࠸࡚࠾ୖグࢩࢫࢸ࣒ࢆ⏝࠸࡚㕲஧౯పࢫࣆࣥ㘒య࡟ࡾࠊ࣮ࣞࢨ࣮ගࡣᚲせ࡟ᛂࡌ࡚Ἴ㛗ኚ᥮ࢆ⾜ࡗࡓ࠾ࡅࡿ㉸㧗㏿ගㄏ㉳ࢫࣆࣥ㌿⛣ࢆᚋࠊࢧࣥࣉࣝ࡟㞟ගࡉࢀࡿࠋࡇࡢ㝿ࠊ࣏ࣥࣉග࡜

♧ࡍ[4]ࠋᐃᖖ≧ែ࡛ ᐃࡉࢀࡓࠊᇶᗏ≧ែࡀపࢫࣉ࣮ࣟࣈගࡢᗄఱᏛⓗ࡞㔜ࡡྜࢃࡏࢆ༑ศ࡟⪃ࣆࣥ≧ែ࡛࠶ࡿ[FeII(phen)3]2+Ỉ⁐ᾮࡢ Fe K ➃៖ࡍࡿࡇ࡜኱ษ࡛࠶ࡿࠋᮏᴫ␎ᅗࡣ⺯ගἲ࡟࠾ࡅXAFS ࢫ࣌ࢡࢺࣝࢆࠊFig.3(a)ࡢୖ㒊࡟ᐇ⥺࡛ࠊࣞࡿࢭࢵࢺ࢔ࢵࣉࢆ♧ࡋ࡚࠶ࡿࡀࠊ᳨ฟჾࡣࣃࣝࢫ

࣮ࢨ࣮ບ㉳ᚋ 50 ps ᚋ࡜࣮ࣞࢨ࣮ບ㉳๓ࡢᕪศࢫ

ィࢆ⪃៖ࡋ࡚ࢼࣀ⛊ࢫࢣ࣮ࣝࡢᛂ⟅㏿ᗘࢆᣢ࣌ࢡࢺࣝࢆ Fig.3(a)ࡢୗ㒊࡟୸༳࡛♧ࡋࡓࠋࡇࡢ

ࡘࢩࣥࢳ࣮ࣞࢩࣙࣥࣉ࣮ࣟࣈࢆ⏝࠸࡚࠸ࡿࠋ࣏ࣥ

⣔࡟࠾ࡅࡿ Fe G 㟁Ꮚࡢࢫࣆࣥࢡࣟࢫ࣮࢜ࣂ࣮

ࣉග࡜ࣉ࣮ࣟࣈගࡢ࿘Ἴᩘࡀྜࡗ࡚࠸࡞࠸ሙྜ

ࡣࠊ㓄఩Ꮚሙ࡜ࣇࣥࢺ๎ࡢ➇ྜ࡟㉳ᅉࡋ࡚࠾ࡾࠊ

࡟ࡣࠊ㟁Ẽⓗࢤ࣮ࢺࢆ฼⏝ྍ⬟࡞᳨ฟჾ⣔ࢆ⏝࠸

Fe-N 㛫ࡢ⤖ྜ㊥㞳ࡢኚ໬࡜ࢫࣆࣥࢡࣟࢫ࣮࢜ࣂ 㸫 

ᐃࡋࡓ౛ࢆ࣮ࡣᐦ᥋࡟㛵ಀࡋ࡚࠸ࡿࠋ୸༳ࡢᕪศࢫ࣌ࢡࢺࣝ

⬟ࢆᯝࡓࡋ࡚࠸ࡿࠋࡋ࠿ࡋࠊᐇ㝿ࡢࢱࣥࣃࢡ㉁ࡀࠊ

࡟࠾࠸࡚ 7125 eV ࡟ぢࡽࢀࡿṇࡢࣆ࣮ࢡࡣ Fe V㧗㏿࡟ືࡁ࡞ࡀࡽᶵ⬟ࡋ࡚࠸ࡿጼࢆື⏬ⓗ࡟ࠊࡋS ཮ᴟᏊ㑄⛣ࡢቑ኱ࢆ⾲ࡋ࡚࠾ࡾࠊࡇࢀࡣ࣮ࣞ

࠿ࡶỈ୰࡛ᐊ

ࢨ࣮ບ㉳ᚋ 50 ps ࡢ㧗ࢫࣆࣥບ㉳≧ែ࡟࠾࠸࡚ࠊ

㏆࠸≧ែ࡛ほ ࡍࡿࡇ࡜ࡣᅔ㞴࡛࠶ࡗࡓࠋࡇࡇ࡛

Fe-N 㛫ࡢ⤖ྜ㊥㞳ࡀఙࡧࡓࡇ࡜࡟㉳ᅉࡍࡿࠋࡲ

ࡣࠊ࣏ࣥࣉ-ࣉ࣮ࣟࣈ X ⥺⁐ᾮᩓ஘ἲ࠿ࡽᚓࡽࢀ

ࡓ 7135 eV ௨ୖ࡛ほ ࡉࢀࡿ EXAFS ᣺ືࡢኚㄪ

ࡓࢹ࣮ࢱࢆ⏝࠸࡚ࠊ⁐ᾮ୰ࡢࢱࣥࣃࢡ㉁ࡀගࡢ่

ࡶࠊ୺࡟୰ᚰ㔠ᒓ࡛࠶ࡿ㕲࡜ࠊ➨୍㓄఩ඖ⣲࡛࠶⃭࡟ࡼࡗ࡚༠ྠⓗ࡟ᵓ㐀ࢆኚ࠼࡚࠸ࡃᵝᏊࢆ┤ࡿ❅⣲ࡢ㊥㞳ࡢኚ໬࡟⏤᮶ࡍࡿࠋຍ࠼࡚ࠊࡼࡾ┤᥋ほ ࡋࡓ◊✲౛ࢆ⤂௓ࡍࡿࠋ࡜࠸ࡗࡓ⏕యෆࡢ⎔ቃ࡜ᴟࡵ࡚

᥋ⓗ࡟ Fe 3d ࢫࣆࣥ≧ែࢆ♧ࡍ Fe VG ᅄᴟᏊ㑄⛣࡟㉳ᅉࡋࡓ྾཰➃๓ࡢࣉ࢚ࣜࢵࢪࣆ࣮ࢡ࡟

5.2. ࢞ ࢫศᏊࡢゎ㞳ࢆࢺ࣮ࣜ࢞࡜ࡋࡓ࣊ࣔࢢࣟ
ࣅࣥࡢᵓ㐀ኚ໬

࠾࠸࡚ࡶࠊࢫࣆࣥࢡࣟࢫ࣮࢜ࣂ࣮࡟㉳ᅉࡋࡓගㄏ
㉳ኚ໬ࢆほ ࡍࡿࡇ࡜ࡀ࡛ࡁࡿࠋ

ᮏ◊✲ࡢᑐ㇟࡜࡞ࡗࡓࢱࣥࣃࢡ㉁ࡣࠊ஧ᯛ㈅ࡀ

Fig.3(b)ࡣ[FeII(phen)3]2+ ࡢ XAFS ࢫ࣌ࢡࢺࣝ

ࡶࡘ࣊ࣔࢢࣟࣅ࡛ࣥࠊ⾑ᾮ୰࡛㓟⣲㐠ᦙࡢᶵ⬟ࢆ࡟࠾࠸࡚ࠊ࢚ࢿࣝࢠ࣮7125 eV ࡟࠾ࡅࡿᙉᗘࡢ᫬

ᢸࡗ࡚࠸ࡿࠋ஧ᯛ㈅ࡢ࣊ࣔࢢࣟࣅࣥࡣே㛫ࡢ⾑ᾮ㛫Ⓨᒎࢆࠊ⦪㍈ࢆᙉᗘࠊᶓ㍈ࢆ࣏ࣥࣉ࣮ࣞࢨ࣮࡜

୰࡟࠶ࡿᅄ㔞యࡢ࣊ࣔࢢࣟࣅࣥ࡜ࡣᑡࡋ␗࡞ࡾࠊ

ࣉ࣮ࣟࣈ X ⥺ࡢ㐜ᘏ᫬㛫࡜ࡋ࡚ࣉࣟࢵࢺࡋࡓࡶࡢ

஧ࡘࡢࢧࣈࣘࢽࢵࢺࡀỈ⣲⤖ྜࢆ௓ࡋ࡚ᙅࡃ⤖࡛࠶ࡿࠋ ᐃࡉࢀࡓྛ㐜ᘏ᫬㛫࡟࠾ࡅࡿᙉᗘࢆ୸

ྜࡋࡓ஧㔞యᵓ㐀ࢆྲྀࡗ࡚࠸ࡿࠋ஧ࡘࡢࣘࢽࢵࢺ

༳࡛♧ࡋࡓࠋࡑࡢ᣺ࡿ⯙࠸ࡣࠊࣃࣝࢫ࣮ࣞࢨ࣮ບ

࡟ࡣࡑࢀࡒࢀࠊ㕲㸫࣏ࣝࣇ࢕ࣜࣥ㘒య(࣒࣊)ࡀ཰

㉳࡟ࡼࡾᙉᗘࡀᛴ⃭࡟ቑຍࡋࠊࡑࡢᚋࠊ⦆ࡸ࠿࡟

ࡲࡗ࡚࠾ࡾࠊࡑࡢ㕲࡟㓟⣲ࡸ୍㓟໬Ⅳ⣲࡞࡝ࡢ࢞ῶᑡࡋ࡚࠸ࡃࠋࡇࡢᙉᗘኚ໬ࡣࠊࢫࢸࢵࣉ㛵ᩘࢆࢫศᏊࡀྍ㏫ⓗ࡟⤖ྜࡋ㐠ᦙࡉࢀࡿ[5-7]ࠋ

ᣢࡘ୍ḟῶ⾶㛵ᩘࢆ ǒ SV ࡢ X ⥺ࡢ᫬㛫ᖜ࡛஧㔞య࣊ࣔࢢࣟࣅࣥࡢ஧ࡘࡢࣘࢽࢵࢺ࡟⤖ྜ␚ࡳ㎸ࢇࡔ㛵ᩘ㸦ᐇ⥺㸧࡛ࣇ࢕ࢵࢺࡍࡿࡇ࡜ࡀฟ

ࡋࡓ࢞ࢫศᏊࡀࢱࣥࣃࢡ㉁࠿ࡽゎ㞳ࡍࡿ࡜ࠊࡑࡢ

᮶ࡿࠋࡍ࡞ࢃࡕගບ㉳┤ᚋ࡟ HS ≧ែ࡟࡞ࡗࡓ⣔༠ྠⓗຠᯝ࡟ࡼࡗ࡚ࠊ஧ࡘࡢࣘࢽࢵࢺࡢ఩⨨㛵ಀࡀࣆࢥ⛊ࡢࢫࢣ࣮࡛ࣝ LS ≧ែ࡟⦆࿴ࡋ࡚࠸ࡃᵝࡀ┦ᑐⓗ࡟ኚ໬ࡋࠊ࢞ࢫศᏊࡀ⤖ྜࡋࡸࡍ࠸ᵓ㐀Ꮚࢆほ ࡋ࡚࠸ࡿࠋ

(R ᆺ)࠿ࡽ⤖ྜࡋ࡟ࡃ࠸ᵓ㐀(T ᆺ)࡬࡜ኚ໬ࡍࡿ࡜

ࡇࡢࡼ࠺࡟᫬㛫ศゎ XAFS ࢆ⏝࠸ࡿ࡜ࠊᴟࡵ࡚

⪃࠼ࡽࢀ࡚࠸ࡓ[8-10]ࠋࡋ࠿ࡋ࡞ࡀࡽ R ᆺ࡜ T ᆺ▷࠸᫬㛫ࡢᶵ⬟ࡢኚ໬ࢆࠊࡑࡢᶵ⬟ኚ໬࡜⤖ࡧࡘࡢ㟼ⓗ࡞ᵓ㐀ࡢ᝟ሗࡔࡅ࡛ࡣࠊヲࡋ࠸ᵓ㐀ࡢືࡁ࠸ࡓཎᏊࢫࢣ࣮ࣝࡢศᏊᵓ㐀ኚ໬࡜ྜࢃࡏ࡚ྠ

ࡸ୰㛫ᵓ㐀࡟ࡘ࠸࡚ࡢ᝟ሗࢆᚓࡿࡇ࡜ࡣ࡛ࡁ࡞

᫬࡟┤᥋ほ ࡍࡿࡇ࡜ࡀ࡛ࡁࡿࡓࡵࠊࡑࡢ཯ᛂ㐣࠸ࠋ≉࡟࣊ࣔࢢࣟࣅࣥ࡟௦⾲ࡉࢀࡿ࢔ࣟࢫࢸࣜࢵ

⛬࡟࠾ࡅࡿ㟁Ẽⓗ࣭⛉Ꮫⓗᛶ㉁ࡢヲ⣽࡞▱ぢࢆᚓࢡࢱࣥࣃࢡ㉁࡛ࡣࠊᒁᡤⓗ࡞ᵓ㐀ኚ໬ࡀᶵ⬟Ⓨ⌧ࡿࡇ࡜ࡀྍ⬟࡜࡞ࡿࠋ࡟㔜せ࡞㧗ḟᵓ㐀ኚ໬ࢆㄏ㉳ࡍࡿࡓࡵ X ⥺ࢆ⏝࠸

5. ࢱࣥࣃࢡ㉁ࡢ༠ྠⓗᵓ㐀ࢲ࢖ࢼ࣑ࢡࢫ

ࡓ᫬㛫ศゎᐃ࡟ࡼࡗ࡚ືⓗᵓ㐀ኚ໬ࢆ㏣㊧ࡋ࡚࠸ࡃࡇ࡜ࡣ㔜せ࡛࠶ࡿࠋࡑࡇ࡛ᡃࠎࡢ◊✲ࢢ࣮ࣝࣉ࡛ࡣࠊKEK ࡢᨺᑕග⛉Ꮫ◊✲᪋タࡢࣅ࣮࣒ࣛ

5.1. ࢱࣥࣃࢡ㉁ࡢᵓ㐀ኚ໬࡜ᶵ⬟ฟ⌧࢖ࣥ NW14A ࢆ⏝࠸࡚ࠊ᫬㛫ศゎ㹖⥺⁐ᾮᩓ஘ἲ

ࢱࣥࣃࢡ㉁ࡣࠊ࢔࣑ࣀ㓟ࡀ࢔࣑ࢻ⤖ྜࢆ௓ࡋ࡚

ࢆ⏝࠸ࡓື⏬᧜ᙳ࡟ᣮᡓࡋࡓࠋ

㐃⤖ࡋ 1 ᮏࡢ㙐࡜࡞ࡗ࡚ᢡࡾ␚ࡲࢀࡓᵓ㐀ࢆྲྀࡾࠊࡑࡢᢡࡾ␚ࡲࢀࡓᵓ㐀ࡀࠊ㓝⣲άᛶ࡞࡝ࡢ⏕యෆࡢ⏕࿨άື࡟࡜ࡗ࡚㔜せ࡞ᶵ⬟࡟῝ࡃ㛵ࢃࡗ࡚࠸ࡿࠋ≉࡟ࠊᢡࡾ␚ࡲࢀࡓࢱࣥࣃࢡ㉁ࡀࠊ࠶
ࡿ≉ᐃࡢືࡁ(ᵓ㐀ኚ໬)ࢆࡍࡿࡇ࡜࡛ࠊᰤ㣴⣲ࢆศゎࡋࡓࡾࠊ➽⫗ࢆື࠿ࡋࡓࡾ࡜࠸ࡗࡓᵝࠎ࡞ᶵ 㸫 

࡟Ἴ㛗ኚ᥮ࡋࡓගࢆ⏝࠸ࡿࡀࠊࣆࢥ⛊㹼ࢼࣀ⛊ࠊ

5.3. ᫬㛫ศゎ X ⥺⁐ᾮᩓ஘ἲࡇࡢᐇ㦂࡛ࡣࠊ୍㓟໬Ⅳ⣲ศᏊࡀ⤖ྜࡋࡓ஧㔞య࣊ࣔࢢࣟࣅࣥࢆྵࡴ⁐ᾮ࡟࣮ࣞࢨ࣮ග࡜ X ⥺ࢆ࡯ࡰྠࡌࢱ࢖࣑ࣥࢢ࡛⧞ࡾ㏉ࡋ↷ᑕࡋ࡚ X ⥺ᩓ஘ࢹ࣮ࢱࢆ ᐃࡍࡿࡇ࡜࡟ࡼࡾࠊ᭱⤊ⓗ࡟ࢱࣥࣃࢡ㉁ ࡢ ᵓ 㐀ኚ ໬ ࡢ ᝟ሗ ࢆྲྀ ࡾ ฟ ࡍࡇ ࡜ ࡀ ࡛ࡁ ࡿ
(Fig. 4)ࠋNW14A ࡣ࿘ᮇ㛗ࡀ␗࡞ࡿ 2 ࡘࡢ࢔ࣥࢪ
࣮ࣗࣞࢱ㸫ࡀタ⨨ࡉࢀ࡚࠸ࡿࡀࠊ ᐃ࡟༑ศ࡞ X⥺ᙉᗘࢆಖࡘࡓࡵ࡟㸰ࡘࡢ࢔ࣥࢪ࣮ࣗࣞࢱ㸫ࡢࢠࣕࢵࣉࢆ㛢ࡌࡿࡇ࡜࡛ 15.7 keV (0.79 Å)ࡢ㧗ᙉᗘ X ⥺ࢆసࡾฟࡋࠊ࡞࠾࠿ࡘࠊ⁐ᾮᩓ஘᭤⥺ࡢ㧗ศゎ⬟࡞ ᐃࡀྍ⬟࡜࡞ࡿࡼ࠺࡟ࠊX ⥺ከᒙ⭷࣑࣮ࣛࢆ⏝࠸ࡿࡇ࡜࡛࢚ࢿࣝࢠ࣮ࢫ࣌ࢡࢺࣝࡀ 5 %࢚ࢿࣝࢠ࣮ᖜࡢᑐ⛠ᵓ㐀ࢆᣢࡘࡼ࠺࡟ࡋࡓࠋࡇࡢ
㝿ࠊ1 ࣃࣝࢫ࠶ࡓࡾࡢ X ⥺ࣇ࢛ࢺࣥᩘࡣ 3 × 108
photons/pulse ࡛࠶ࡿࠋPF-AR ࣜࣥࢢ࠿ࡽⓎࡏࡽࢀࡿ 100 ps ࣃࣝࢫ X ⥺ࡢ࿘Ἴᩘࡣ 794 kHz ࡛࠶ࡿࡀࠊ࣊ࣔࢢࣟࣅࣥ࡟࠾ࡅࡿගບ㉳≧ែࡀᇶᗏ≧ែ࡬⦆࿴ࡍࡿ᫬㛫ࢆ⪃៖ࡋࠊ࠿ࡘ࣮ࣞࢨ࣮ࡢ࿘Ἴ
ᩘ࡟ྜࢃࡏࡓ࣏ࣥࣉ-ࣉ࣮ࣟࣈ ᐃࢆ⾜࠺ࡓࡵࠊX⥺ࡣࢳࣙࢵࣃ࣮࡜㧗㏿ࢩࣕࢵࢱ࣮࡟ࡼࡗ࡚ 10 Hz࠾ࡼࡧࢼࣀ⛊㹼࣑ࣜ⛊ࡢ᫬㛫ࢫࢣ࣮ࣝࡢኚ໬ࢆ
㏣㊧ࡍࡿ㝿ࡣࠊࡑࢀࡒࢀ NW14A ࡟タ⨨ࡉࢀ࡚࠸ࡿ Ti:Sapphire ࣇ ࢙ ࣒ ࢺ ⛊ ࣞ ࣮ ࢨ ࣮ ࠊ ࠾ ࡼ ࡧ
Nd:YAG ࢼࣀ⛊࣮ࣞࢨ࣮ࢆ⏝࠸࡚᫬㛫ศゎ ᐃࢆ⾜ࡗ࡚࠸ࡿࠋࣇ࢙࣒ࢺ⛊࣮ࣞࢨ࣮ࢆ⏝࠸ࡿ᫬ࡣࡑ
ࡢ㧗࠸ᑤ㢌್ᙉᗘ࡟ࡼࡿࢧࣥࣉࣝ࡬ࡢࢲ࣓࣮ࢪ
ࢆ⪃៖ࡋࠊගᏛࢢ࣮ࣞࢸ࢕ࣥࢢ࡟ࡼࡗ࡚ᩘࣆࢥ⛊ࡢࣃࣝࢫᖜ࡟ఙࡤࡋ࡚࠿ࡽࢧࣥࣉࣝࢆບ㉳ࡋ࡚࠸ࡿࠋࡇࡇ࡛ࠊ࣮ࣞࢨ࣮ࡢ࢚ࢿࣝࢠ࣮ᐦᗘࡣ㹼0.5
mJ/mm2 ࡟ㄪᩚࡉࢀࠊ࣮ࣞࢨ࣮࡜ X ⥺ࡣࠊ࡯ࡰྠ
㍈࠿ࡽࢧࣥࣉࣝ࡟ධᑕࡋࠊࢧࣥࣉࣝ⾲㠃࡟࠾࠸࡚࣐࢖ࢡ࣓࣮ࣟࢺࣝࡢ఩⨨⢭ᗘ࡛୧⪅ࡀ㔜࡞ࡿࡼ࠺࡟ㄪ⠇ࡉࢀࡿࠋX ⥺ᩓ஘࢖࣓࣮ࢪࡣ 165 mm ᚄࢆ ᣢ ࡘ ஧ ḟ ඖ CCD ᳨ ฟ ჾ 㸦 MarCCD 165 ࠊ
MarUSA㸧ࢆ⏝࠸࡚ᐃࡉࢀࡓࠋHe ࣃࢫࢆ⏝࠸ࡿࡇ࡜࡛ࣂࢵࢡࢢࣛ࢘ࣥࢻ࡜࡞ࡿ✵Ẽᩓ஘ࢆᢚ࠼ࠊ࣓࢝ࣛ㛗ࢆ㹼300 mm ࡟ࡍࡿ࡜ q ್ࡀ 0.15㹼
2 Å-1 ࡢᩓ஘࢖࣓࣮ࢪࢆྲྀᚓ࡛ࡁࡿࡓࡵࠊ࣊ࣔࢢࣟ
ࣅࣥࡢග཯ᛂ࡟࠾ࡅࡿᵓ㐀ኚ໬ࢆ d = 0.1 Å ⛬ᗘࡢศゎ⬟࡛ᤊ࠼ࡿࡇ࡜ࡀྍ⬟࡜࡞ࡿ[11]ࠋ

࡟㛫ᘬ࠿ࢀ࡚ࢧࣥࣉࣝ࡟ධᑕࡍࡿࠋ࣊ࣔࢢࣟࣅࣥ
ࡢບ㉳࡟ࡣࠊගࣃ࣓ࣛࢺࣜࢵࢡቑᖜჾ࡛ 532 nm
Fig. 4: Time-resolved X-ray solution
scattering data were acquired using thepump–probe method at the beamline
NW14A. The sample, aqueous solutionof HbI ligated with CO ligands[HbI(CO)2] contained in a capillary of 1mm thickness were excited with 35 ps
laser pulses at 532 nm. Time-resolved
scattering curves were collected at 40–
70 pump–probe time delays between thelaser pump pulse and the X-ray probe
pulse in the range from 100 ps to 56.2 ms
DVZHOODVDWDUHIHUHQFHWLPHGHOD\RIïǍV7RDWWDLQDVLJQDO-to-noise ratio goodenough for data analysis, about 20
images were acquired and averaged ateach time delay.

 㸫 

5.4. ࡡࡌࢀ㐠ື࡟ࡼࡿ࢞ࢫศᏊࡢᨺฟ
ᮏ◊✲࡛ࡣࠊᖖ

࡛ヨᩱ࡟࣮ࣞࢨ࣮ගࢆ↷ᑕࡋࠊ஧㔞య࣊ࣔࢢࣟࣅࣥศᏊෆࡢ࣒࣊࡜୍㓟໬Ⅳ⣲ࡢ⤖ྜࢆษ᩿ࡋ࡚ࠊ▐㛫ⓗ࡟୍㓟໬Ⅳ⣲ࡀࢱࣥ
ࣃࢡ㉁࠿ࡽゎ㞳ࡋࡓ≧ែࢆసࡾฟࡋࡓࠋࡑࡋ࡚ࠊ
ࡇࡢ㐣Ώⓗ࡞≧ែ࠿ࡽጞࡲࡿࢱࣥࣃࢡ㉁ࡢᵓ㐀ኚ໬ࢆࠊ᫬㛫ศゎ㹖⥺⁐ᾮᩓ஘ἲࢆ⏝࠸࡚ࠊ࣮ࣞ
ࢨ࣮ග࡜ X ⥺ࡢ᫬㛫ࢆ⣔⤫ⓗ࡟ࡎࡽࡋ࡞ࡀࡽ㏲ḟ
ほࡋࡓࠋFig.5 ࡟࠾ࡅࡿࠊ࢚࣮ࣛࣂ࣮௜ࡁࡢࣉࣟ

ࢵࢺ࡛♧ࡋࡓྛ᫬㛫࡟࠾ࡅࡿᕪศࢫ࣌ࢡࢺࣝࡣࠊ
ගບ㉳๓ࡢࣜࣇ࢓ࣞࣥࢫ⁐ᾮᩓ஘᭤⥺࡜ࡢᕪศࢆྲྀࡗࡓࡶࡢ࡛࠶ࡾࠊ࢚࣮ࣛࣂ࣮↓ࡋࡢᐇ⥺ࡣゎᯒ࡟ࡼࡗ࡚ᚓࡽࢀࡓࣇ࢕ࢵࢺ⤖ᯝ࡛࠶ࡿࠋྛ᫬㛫Ⅼ࡟࠾ࡅࡿ“࣊ࣔࢢࣟࣅࣥࡢᵓ㐀”࡜“࣊ࣔࢢࣟࣅ
ࣥ࡜⁐፹࡜ࡢ┦஫స⏝”ࢆ ศᏊືຊᏛࢩ࣑࣮ࣗࣞ
ࢩࣙࣥࠊ࠾ࡼࡧ㔞Ꮚ໬Ꮫィ⟬࡟ࡼࡗ࡚ぢ✚ࡾࠊࡑࡇ࡛ᚓࡽࢀࡓ್ࢆඖ࡟ࢢ࣮ࣟࣂ࣭ࣝࣇ࢕ࢵࢸ࢕ࣥ
ࢢ࡟ࡼࡿᵓ㐀ゎᯒࢆ⾜࠺ࠋ཯ᛂ㐍⾜ᗘࡢ᫬㛫ኚ໬ࢆ≉␗್ศゎἲ࡟ࡼࡾヲࡋࡃゎᯒࡍࡿ࡜ࠊගບ㉳ᚋ 100 ps㹼10 ms ࡢ᫬㛫ࢫࢣ࣮ࣝ࡟࠾ࡅࡿບ㉳≧ែ࡟࠾࠸࡚ 3 ࡘࡢ⊂❧࡞୰㛫≧ែ㸦I1, I2, I3㸧ࡀᏑᅾࡋࠊࡑࢀࡒࢀࡢẚ⋡ࡀ้ࠎ࡜ኚ໬ࡋ࡚࠸ࡿᵝᏊࡀࠊࡉࡽ࡟ࡣ୍ࡘࡢࣘࢽࢵࢺ࠿ࡽ୍㓟໬Ⅳ⣲ࡀගゎ㞳ࡋࡓ≧ែ࡜ࠊ୧᪉ࡢࣘࢽࢵࢺ࠿ࡽゎ㞳ࡋࡓ≧ែࡀᏑᅾࡋࠊࡑࢀࡽࡢ≧ែࡣྠࡌᵓ㐀ኚ໬ࢆᘬࡁ㉳ࡇࡍࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓࠋFig.6 ࡣ୰㛫≧ែࡢᵓ㐀࡟࠾ࡅࡿ 2 ࡘࡢࣘࢽࢵࢺࡢ㊥㞳㸦ࡑࢀࡒࢀࡢ࣒࣊㛫ࡢ㊥㞳㸧ࠊ┦ᑐⓗ࡞ゅᗘࠊ࠾ࡼࡧࠊᵓ㐀ኚ໬࡟ࡼࡗ࡚ࣘࢽࢵࢺ㛫⏺㠃࡟࠾࠸࡚ฟࡋධࢀ
ࡉࢀࡿỈศᏊ㸦ࢧࣈࣘࢽࢵࢺ㛫ࡢ୸㸧ࡢᩘࢆ♧ࡋࡓࡶࡢ࡛࠶ࡿࠋἼ㛗 532 nm ࡢࣃࣝࢫ࣮ࣞࢨ࣮↷ᑕ࡟ࡼࡿ୍㓟໬Ⅳ⣲ࡢගゎ㞳ࢆࢺ࣮ࣜ࢞࡜ࡋ࡚ࠊ
R ᆺ࡟㢮ఝࡋࡓゎ㞳≧ែ࡛࠶ࡿ I1 ୰㛫≧ែࡀගບ㉳ᚋ 100 ps ௨ෆ࡟⏕ᡂࡉࢀࠊࡑࡢᚋ R ᆺ࡟㢮ఝࡋࡓูࡢゎ㞳≧ែ I2 ୰㛫≧ែ࡬࡜ 3.2 ± 0.2 nsࡢ᫬ᐃᩘࢆᣢࡗ࡚ኚᙧࡍࡿࠋ⥆࠸࡚ࠊࣘࢽࢵࢺࡢᅇ㌿࡜ࠊ࣒࣊㛫㊥㞳ࡢῶᑡࠊ࠾ࡼࡧࣘࢽࢵࢺ㛫⏺
㠃࡟࠾ࡅࡿỈศᏊࡢቑຍࢆ⤒࡚ T ᆺ࡟㢮ఝࡋࡓ
I3 ୰㛫≧ែࡀ⏕ᡂࡍࡿࠋI2 ୰㛫≧ែ࠿ࡽ I3 ୰㛫≧ែ࡬ࡢኚᙧࡀ㉳ࡇࡿ᫬ᐃᩘࡣࠊ୍㓟໬Ⅳ⣲ࡢゎ㞳ࡀ 1 ࡘࡢࢧࣈࣘࢽࢵࢺ࡛㉳ࡁࡓ࠿ࠊ୧᪉ࡢࢧࣈ

Fig. 5: Picosecond pump–probe X-ray solution
scattering for wild-type HbI(CO)2. Timeresolved difference X-ray solution scattering
FXUYHVƦ6 TW PHDVXUHGIRUVROXWLRQVDPSOHV
of wild-type HbI are shown. The time delay
after photoexcitation is indicated above eachcurve. For clarity, only data at selected timedelays are shown. Experimental curves arecompared with theoretical curves that weregenerated from linear combinations of three
time-independent
species-associatedscattering curves extracted from the kinetic
analysis.
ࣘࢽࢵࢺ࡛㉳ࡁࡓ࠿࡟౫Ꮡࡋ࡚␗࡞ࡿ್ࢆྲྀࡾࠊ
๓⪅࡛ࡣ 730 ± 120 ns ࡛࠶ࡾࠊ ᚋ⪅࡛ࡣ 5.6 ±
0.8 Ps ࡜࡞ࡿࡇ࡜ࡀ᫂ࡽ࠿࡜࡞ࡗࡓࠋࡑࡢᚋࠊ୍ 㸫 

Fig. 6: Structural dynamics of HbI extracted from the species-associated scattering curves
using structure refinement. The green and blue arrows are used to indicate the relative
magnitudes and directions of the changes in the heme–heme distance and subunit rotation angle
relative to HbI(CO)2. The structural transitions induce a change in the number of interfacial
water molecules (shown in red), well-organized at the interface of the two subunits.
㓟໬Ⅳ⣲ࡀ෌⤖ྜࡋ⣔ࡣᇶᗏ≧ែ࡬࡜ᡠࡿࠋࡇࡢ

ࢹࣂ࢖ࢫᮦᩱࢆ㛤Ⓨࡍࡿࡓࡵࡢ᪂᪉㔪࡜ࡋ࡚ᮇࡼ࠺࡟ࡋ࡚ࠊ୍㓟໬Ⅳ⣲ࡢගゎ㞳ࢆࢺ࣮ࣜ࢞࡜ࡋ

ᚅࡉࢀࡿࠋ࡚࣊ࣔࢢࣟࣅࣥศᏊࡀ 100 ൨ศࡢ 1 ⛊(100 ps)࠿ࡽ 100 ศࡢ 1 ⛊(10 ms)⛬ᗘࡢ᫬㛫ෆ࡟ᚎࠎ࡟ᵓ

6.2. ࣌ ࣟࣈࢫ࢝࢖ࢺᆺ࣐ࣥ࢞ࣥ㓟໬≀ࡢගㄏ㉳┦㌿⛣㐀ኚ໬ࡋࠊ஧ࡘࡢࣘࢽࢵࢺ㛫ࡢ㊥㞳ࡀ▷ࡃ࡞ࡿ࡜࡜ࡶ࡟ࠊ஧ࡘࡢࣘࢽࢵࢺࡀࡡࡌࢀ㐠ື࡛ᙧࢆኚ໬

㑄⛣㔠ᒓ㓟໬≀࡟௦⾲ࡉࢀࡿᙉ┦㛵㟁ᏊᮦᩱࡍࡿᵝᏊࡀࠊ100 ൨ศࡢ 1 ⛊⢭ᗘࡢ X ⥺ື⏬࡜ࡋࡣࠊ㏆ᖺࡢ≀ᛶ≀⌮Ꮫࡢ㔜せ࡞◊✲ㄢ㢟࡜ࡋ࡚⢭࡚┤᥋ほ ࡉࢀࡓ[12]ࠋ

ຊⓗ࡟◊✲ࡉࢀ࡚࠾ࡾࠊࡲࡓᕤᴗⓗ࡟ࡣ㧗㞟✚࣓
࣮ࣔࣜ㸦ReRAM㸧࡞࡝ࡢ㟁Ꮚࢹࣂ࢖ࢫ࡬ࡢᛂ⏝ࡀ

6. ㉸㧗㏿ගࢹࣂ࢖ࢫᮦᩱ㛤Ⓨᮇᚅࡉࢀ࡚࠸ࡿࠋ
୰࡛ࡶ࣌ࣟࣈࢫ࢝࢖ࢺᆺ࣐ࣥ࢞ࣥ㓟໬≀ࡣࠊ㈇6.1. ගࢆ⏝࠸ࡓ≧ែไᚚࡢᕧ኱☢Ẽ᢬ᢠຠᯝࡢⓎぢࢆዎᶵ࡟⢭ຊⓗ࡞◊ගࢆ⏝࠸ࡓ≀㉁ࡢ≧ែไᚚࡣࠊᚑ᮶ࡢ≀㉁⛉Ꮫ✲ࡀ࡞ࡉࢀ࡚ࡁࡓࠋ࣌ࣟࣈࢫ࢝࢖ࢺᆺ࣐ࣥ࢞ࣥ㓟ࡀᇶ┙࡜ࡍࡿࠕᏳᐃ࡛ࠖࠕ㟼ⓗࠖ࡞ᵓ㐀࡜ࡣ␗࡞໬≀ࡣప ࡛ࡣᏳᐃ࡛㟼ⓗ࡞ᵓ㐀࡜ࡋ࡚ࠊ㹢㟁Ꮚࡗࡓࠊࠕືⓗ࡛ࠖࠕኚ໬ࡍࡿࠖᵓ㐀࡟ᇶ࡙ࡃ᪂ࡋ࠸

㌶㐨ࡀつ๎ṇࡋࡃ⛛ᗎࡔࡗࡓࠕ㌶㐨⛛ᗎࠖ≧ែ

≀㉁⛉Ꮫࡢᵓ⠏࡜࠸࠺ᇶᮏၥ㢟࡜ࡋ࡚௒ࠊᖜᗈ࠸

㸦Fig. 7 ᕥୗ㸧ࢆ࡜ࡾࠊ⤯⦕య≧ែ࡟࡞ࡗ࡚࠸ࡿࠋ

⯆࿡ࢆ㞟ࡵ࡚࠸ࡿࠋࡇࢀ࡟ຍ࠼࡚ࠊḟୡ௦ࡢග᝟

࠸ࢃࡤ㑄⛣㔠ᒓ࡜࿘ᅖࡢ㓟⣲ཎᏊ࡜ࡢ㛫ࡢ໬Ꮫሗฎ⌮⣲Ꮚࡢ㛤Ⓨࡢࡓࡵࡢ࣮࢟ࢸࢡࣀࣟࢪ࣮࡜

⤖ྜ࡟㛵୚ࡍࡿ㟁Ꮚ㌶㐨ࡀࠊ࠾ࡢ࠾ࡢつ๎ṇࡋࡃࡋ࡚ࡶᮇᚅࡉࢀ࡚࠸ࡿࠋࡇࡇ࡛⤂௓ࡍࡿ◊✲ࡣࠊ␗᪉ⓗ࡞୪ࡧ᪉ࢆ࡜ࡿࡓࡵ㟁Ꮚࡣືࡁ࡙ࡽ࠸≧㑄⛣㔠ᒓ㓟໬≀࡟௦⾲ࡉࢀࡿᙉ┦㛵㟁Ꮚᮦᩱ࡟ែ࡟࡞ࡗ࡚࠸ࡿࡢ࡛࠶ࡿࠋࡇࢀ࡟ᑐࡋ࡚㧗 ࡛ࡣ࠾࠸࡚ࠊᏳᐃ࡞཯ᙉ☢ᛶ⤯⦕య┦ࢆගບ㉳ࡍࡿࡇࡇࡢ⛛ᗎࡀᾘ⁛ࡋࠊ㹢㟁Ꮚ㌶㐨ࡣⓙ➼᪉ⓗ࡞≧ែ࡜࡛ࠊഹ࠿ 100 ൨ศࡢ㸯⛊ࡔࡅฟ⌧ࡍࡿูࡢ㌶㐨

㸦Fig. 7 ᕥୖ㸧࡜࡞ࡾࠊ㟁Ꮚࡣືࡁࡸࡍࡃ࡞ࡿࡓࡵ

⛛ᗎ┦ࢆ㗦ᩄ࡟᳨ฟࡍࡿࡇ࡜ࢆᐇ⌧ࡋࡓࡶࡢ࡛

ᙉ☢ᛶ㔠ᒓ┦ࢆ♧ࡍࠋ࠶ࡿࠋࡲࡓほ ࡉࢀࡓ≀㉁┦ࡣࠊ ᗘ࡞࡝㏻ᖖࡢ

ࡇࢀࡲ࡛࡟࣌ࣟࣈࢫ࢝࢖ࢺᆺ࣐ࣥ࢞ࣥ㓟໬≀⇕ຊᏛⓗ᪉ἲ࡛ࡣᐇ⌧ࡉࢀ࡚࠸࡞࠿ࡗࡓගບ㉳ࡢప ᮲௳ୗ࡛ᐇ⌧ࡍࡿ⤯⦕య┦ࡣࠊ☢ሙࠊᅽຊࠊ

≧ែ≉᭷ࡢࡶࡢ࡛࠶ࡾࠊᚑ᮶ࡢ㟼ⓗ࡛Ᏻᐃ࡞≀㉁ග↷ᑕ࡞࡝ࡢእሙ࡟ࡼࡾ┦㌿⛣ࢆ㉳ࡇࡍࡇ࡜ࡀ

ୡ⏺࡜ࡣูୡ⏺ࡢཎᏊࣞ࣋ࣝࡢ⛛ᗎᵓ㐀ࡀࠊග࡟ሗ࿌ࡉࢀ࡚࠸ࡿࠋ≉࡟ࣃࣝࢫ࣮ࣞࢨ࣮ࢆ⏝࠸ࡓࡼࡗ࡚ᐇ⌧࡛ࡁࡿࡇ࡜ࢆึࡵ࡚♧ࡋࡓࠋࡇࡢⓎぢࡣࠊ⇕㞧㡢࡞࡝ࡢᙳ㡪ࢆཷࡅ࡞࠸᪂ࡓ࡞㉸㧗㏿ග 㸫 

Fig. 7: ගບ㉳๓ࡢ㟼ⓗᵓ㐀࡜ࠊ ᗘኚ໬࡟ࡼࡿ㟼ⓗ࡞ᵓ㐀ኚ໬ࠊ࡞ࡽࡧ࡟ගບ㉳࡟ࡼࡿືⓗᵓ㐀ኚ໬࡜ࡢẚ㍑ࠋࠕගᏛ≉ᛶࡢ ᗘୖ᪼࡜ගບ㉳࡟ࡼࡿኚ໬ࠖ
㸹ගບ㉳┤ᚋࠊ0.5 eV(ගࡢἼ㛗ኚ᥮࡛ࡣ⣙ 2480 nm)㎶ࡾ࡟ࣆ࣮ࢡࡀฟ⌧ࡍࡿࠋග㏻ಙ࡛ࡣ 1260 nm ࡼࡾ㛗࠸㡿ᇦࡢἼ㛗ࡀ฼⏝ࡉࢀ࡚࠾ࡾࠊ
ࡇࡢ㡿ᇦෆ࡛ࡢኚ໬ࡣ㉸㧗㏿ගࢹࣂ࢖ࢫ࡬ࡢྍ⬟ᛶࢆ♧ࡍࠋࠕ㹖⥺ᅇᢡࡢ ᗘㄏ㉳࡜ගບ㉳࡟ࡼࡿኚ໬ࠖ㸹㧗 ࡟ࡼࡿኚ໬࡛ࡣ୰ኸ࡟୍ࡘࡢࣆ࣮ࢡࡀ࡛ࡁࡿࠋࡇࢀࡣ⛛ᗎࡀ↓ࡃ࡞ࡗࡓࡇ࡜ࢆ♧ࡋࠊ㔠ᒓ┦࡟࡞ࡗࡓࡇ࡜ࢆ⾲ࡍࠋ୍᪉ࠊගບ㉳࡟ࡼࡿኚ໬࡛ࡣࠊ୧➃ࡢࣆ࣮ࢡ(⛛ᗎ┦)ࡀಖࡓࢀࡓࡲࡲࡎࢀ࡚
࠸ࡿࠋࡇࢀࡣ⇕࡟ࡼࡿኚ໬࡛ࡣ⌧ࢀ࡞࠸᪂ࡋ࠸⛛ᗎ┦࡛࠶ࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿࠋ
໬࡜ࡢ㢮᥎࠿ࡽࠊ㧗 ᮲௳ୗ࡛ᐇ⌧ࡍࡿᙉ☢ᛶ㔠ἲ㸦࣏ࣥࣉ࣭ࣉ࣮ࣟࣈἲ㸧࡟ࡼࡾࠊ࿘ᮇⓗ࡟㠀ᖖᒓ┦ࡢᵓ㐀࡜㢮ఝࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀ࡚ࡁࡓࠋග

࡟▷࠸㛫ࡔࡅฟ⌧ࡍࡿ≧ែࢆࠊࣃࣝࢫ X ⥺ࢆ⏝࠸࡟ࡼࡾ୍▐࡟ࡋ࡚⤯⦕య┦࠿ࡽ㔠ᒓ┦࡬㌿⛣ࡍ࡚ᤕࡽ࠼ࡿࡇ࡜ࢆᚲせ࡜ࡍࡿࠋࡿᛶ㉁ࡣࠊ㉸㧗㏿ࢫ࢖ࢵࢳࣥࢢ࡞࡝㉸㧗㏿ගࢹࣂ௚᪉ࠊヨᩱ㠃࡛ࡣ࣐ࣥ࢞ࣥ㓟໬≀࡬౵ධࡍࡿ῝࢖ࢫ࡬᭷⏝࡛࠶ࡿࡓࡵࠊࡑࡢᵓ㐀ࡢゎ᫂ࡀồࡵࡽࡉ㸦౵ධ㛗㸧ࡀ X ⥺࡜ບ㉳࣮ࣞࢨ࣮ග࡛ࡣࠊࡑࢀ

ࢀ࡚࠸ࡓࠋࡒࢀᩘ࣐࢖ࢡ࣓࣮ࣟࢺࣝ࡜ᩘ༑ࢼࣀ࣓࣮ࢺࣝ⛬ᗘ࡜ࠊ㸰᱆௨ୖࡶ␗࡞ࡿࡓࡵࠊ㏻ᖖࡢ࣐ࣥ࢞ࣥ㓟

6.3. ᫬㛫ศゎ X ⥺ᅇᢡἲ໬≀⤖ᬗヨᩱ࡛ࡣࠊ࣮ࣞࢨ࣮࡟ࡼࡗ࡚ບ㉳ࡉࢀ࡚ග࡟ࡼࡾ㐣Ώⓗ࡟ฟ⌧ࡍࡿ᪂≀㉁┦ࡢືⓗ⤖࠸࡞࠸ᡂศࡢ᝟ሗࡋ࠿ᚓࡿࡇ࡜ࡀ࡛ࡁ࡞࠿ࡗࡓࠋ

ᬗᵓ㐀ࢆཎᏊ࡛ࣞ࣋ࣝㄪ࡭ࡿ࡟ࡣࠊX ⥺ᅇᢡ ᐃࡑࡇ࡛౵ධ㛗ࡢၥ㢟ࢆᅇ㑊ࡍࡿࡓࡵ࡟ࠊ
ཌࡉ 80 ࢼࡀ᭷ຠ࡛࠶ࡿࡀࠊ㧗㏿⌧㇟ࡢ ᐃ࡟ࡣ࣮ࣞࢨ࣮ࣃ

ࣀ࣓࣮ࢺࣝࡢⷧ⭷ᙧ≧ࡢ⤖ᬗࢆ࣮ࣞࢨ࣮✚ᒙ࢚ࣝࢫ࡜ X ⥺ࣃࣝࢫࢆ஺஫࡟⧞ࡾ㏉ࡋධᑕࡍࡿ ᐃࣆࢱ࢟ࢩ࣮ᡂ㛗ἲ࡟ࡼࡾస〇ࡋࡓ㸦Fig. 8㸧ࠋࡇࡢ 㸫 

Fig. 8: ᮏ◊✲ࡢࡓࡵ࡟ࣃࣝࢫ࣮ࣞࢨ࣮ሁ✚ἲ࡟ࡼࡗ࡚‽ഛࡉࢀࡓࠊ࣐ࣥ࢞ࣥ㓟໬≀ࡢⷧ⭷(a)࡜ࡑࡢ⤖ᬗࠊ㟁Ꮚᵓ㐀ᶍᘧᅗ(b)ࠋFWHM ࡟ࣃࣝࢫࡢ್༙඲ᖜࢆ♧ࡍࠋࡼ࠺࡞ヨᩱ㛤Ⓨ࡟ࡼࡗ࡚ࠊࢃࡎ࠿࡞㔞ࡢ⤖ᬗ࡛ࡶ࡜ࢆ♧ࡋ࡚࠸ࡿࠋࡲࡓࠊࡇࢀࡣ ᗘ࡟ࡼࡿ┦㌿⛣᪂ཎ⌮࡟ᇶ࡙ࡃ≀㉁࣭ᮦᩱ㛤Ⓨࡀ⾜࠼ࡿࡇ࡜ࠊࡉ

࡛ࡣ฿㐩ࡍࡿࡇ࡜ࡢ࡛ࡁ࡞࠸ࠕ㞃ࢀࡓ≀㉁┦ࠖࢆࠊࡽ࡟ࡣගࢹࣂ࢖ࢫ࡞࡝࡟᭷⏝࡞㉸ⷧ⭷ᙧែࡑࡢග࡟ࡼࡗ࡚ᐇ⌧ྍ⬟࡛࠶ࡿࡇ࡜ࢆᐇドࡋ࡚࠸ࡿࠋ

ࡶࡢ࡛ගບ㉳≧ែࡢືⓗᵓ㐀◊✲ࡀྍ⬟࡛࠶ࡿ
6.5. ගᶵ⬟ᮦᩱ㛤Ⓨ࡬ࡢ㈉⊩ࡇ࡜ࡀᐇドࡉࢀࡓࠋ

ࡇࡢࡼ࠺࡞㞃ࢀࡓ≀㉁┦ࡢᐇᅾᛶࡣࠊ≀㉁ࡢᏑ

6.4. ග࡟ࡼࡗ࡚ບ㉳ࡉࢀࡿ㞃ࢀࡓ≀㉁┦ᅾᙧែ࡟㛵ࡍࡿᇶᮏၥ㢟࡜ࡋ࡚㛗ࡃ⥆࠸ࡓ㆟ㄽᮏ◊✲࡛ࡣ⵳✚ᆺᨺᑕගࡢࣃࣝࢫ X ⥺࡟ࡼࡗ࡚100 ൨ศࡢ㸯⛊ࡢ㛫ࡔࡅฟ⌧ࡍࡿ᪂ࡋ࠸≀㉁┦ࡢᵓ㐀ࢆほࡍࡿࡇ࡜࡟ᡂຌࡋࡓ[13]ࠋほ࡟ᑐࡋ୍ࡘࡢ⟅࠼ࢆ୚࠼ࠊ⇕ᨐ஘ࢆཷࡅ࡞࠸ࢹࣂ
࢖ࢫᮦᩱ㛤Ⓨࡢ᪂ࡓ࡞ࣇ࢕࣮ࣝࢻࢆᣅ࠸ࡓࠋ
ࡲࡓᮏ◊✲࡛㛤Ⓨࡉࢀࡓ᫬㛫ศゎ㹖⥺ᅇᢡἲࡉࢀࡓᵓ㐀 ࡣ Fig.7 ྑୗ࡟♧ࡍࡼ࠺࡟ ࠊᚑ᮶ࡢண

ࡣࠊཎᏊࢫࢣ࣮ࣝ࡟࠾ࡅࡿᴟࡵ࡚▷࠸᫬㛫㸦100 ൨㸦Fig.7 ᕥୖ㸧࡜ࡣ඲ࡃ␗࡞ࡗ࡚࠾ࡾࠊ⤖ᬗ୰࡛ගศࡢ㸯⛊㸧ࡢኚ໬ࢆࠊࡑࡢගᏛ≉ᛶ࡞࡝ࡢ≀ᛶኚບ㉳๓㸦Fig.7 ᕥୗ㸧࡜ࡶ␗࡞ࡿ᪂ࡓ࡞㌶㐨⛛ᗎ≧໬࡜⤖ࡧࡘࡅ࡞ࡀࡽࠊྠ᫬࡟┤᥋ほ ࡍࡿࡇ࡜ࢆ

ែࡀ⏕ࡌ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡗࡓࠋࡇࢀࡣගບ㉳࡛ྍ⬟࡟ࡍࡿࠋࡇࢀࡣ㉸㧗㏿࡞ග⌧㇟ࡢ࣓࢝ࢽࢬ࣒

⏕ࡳฟࡉࢀࡿືⓗᵓ㐀࡟ᇶ࡙ࡃ≀㉁┦ࡀࠊ㟼ⓗᏳࢆື⏬࡜ࡋ࡚ほᐃᵓ㐀࡟ᇶ࡙ࡃᚑ᮶ࡢ≀㉁⛉Ꮫࡢ⪃࠼᪉࠿ࡽࡣ

࡛ᴟࡵ࡚⏬ᮇⓗ࡞ࡶࡢ࡛࠶ࡿࠋࡇࡢࡼ࠺࡟ග࡟ࡼ

඲ࡃண᝿እࡢࠊ᪂ࡋ࠸⛛ᗎࢆࡶࡗࡓࡶࡢ࡛࠶ࡿࡇ

ࡗ࡚ගᏛ≉ᛶࠊఏᑟᛶࠊ☢ᛶ➼ࡢ≀ᛶࡀ㉸㧗㏿ኚࡍࡿࡇ࡜ࡀ࡛ࡁࡿ࡜࠸࠺ព࿡

Fig. 9: XFEL ࢆ฼⏝ࡋࡓࣇ࢙࣒ࢺ⛊᫬㛫ศゎ X ⥺ᩓ஘ ᐃࡢᴫ␎ᅗ 㸫 

໬ࡍࡿ⌧㇟ࢆヲࡋࡃ᥈ồࡍࡿࡇ࡜࡛ࠊ㉸㧗㏿࡞㉸

7.2. XFEL ࢆ⏝࠸ࡓࣇ࢙࣒ࢺ⛊ X ⥺᫬㛫ศゎᚤᑠ࣓ࣔࣜࡸ┦ࢫ࢖ࢵࢳࡢᮦᩱ㛤Ⓨࡸࢹࣂ࢖ࢫ

ᐃືసࡑࡢሙゎᯒࡀ᥎㐍ࡉࢀࡿࡇ࡜ࡀᮇᚅࡉࢀࡿࠋ

ࡽⓎ᣺ࡍࡿ X ⥺࡜㧗⢭ᗘ࡟ྠᮇࡋࡓࣃࣝࢫ࣮ࣞࢨ

7. ⁐ᾮ୰࡟࠾ࡅࡿ໬Ꮫ཯ᛂࡢྍど໬࣮ගࢆࢧࣥࣉࣝ࡟↷ᑕࡋ࡚཯ᛂࢆ㛤ጞࡉࡏࠊ୍ᐃ
ࡢ㐜ᘏ᫬㛫ᚋ࡟ X ⥺ࣃࣝࢫࢆ↷ᑕࡋ࡚཯ᛂ୰㛫య

7.1. ศᏊື⏬࡟ࡼࡿ໬Ꮫ཯ᛂࡢᐇ᫬㛫ほX ⥺⮬⏤࣮ࣞࢨ࣮㸦XFEL㸧ࢆ฼⏝ࡋࡓࣇ࢙࣒
ࢺ⛊᫬㛫ศゎ X ⥺ᩓ஘ ᐃࢆ⾜࠺ࡇ࡜࡛ࠊ໬Ꮫ཯
ᛂࡢ㐍⾜࡟క࠸ศᏊࡢᵓ㐀ࡀ᫬ࠎ้ࠎ࡜ኚ໬ࡍ
ࡿᵝᏊࢆࠊศᏊື⏬࡜ࡋ࡚ᐇ᫬㛫࡛ほ ࡍࡿࡇ࡜࡟ᡂຌࡋࡓ◊✲ࢆ⤂௓ࡍࡿ[14]ࠋỈ⣲⤖ྜࡸぶ࿴ᛶ➼ࡢᙅ࠸ศᏊ㛫ຊ࡛」ᩘࡢศᏊࡀ⤖ࡧࡘ࠸ࡓศᏊ఍ྜయࡣࠊ཯ᛂࡀᣑᩓᚊ㏿࡛ไ㝈ࡉࢀࡿ⁐ᾮ࡜ࡣ␗࡞ࡾࠊึᮇศᏊ㓄ྥࡸ཯ᛂ࡟㛵୚ࡍࡿศᏊ
ࡢᩘࢆᐃࡵࡿࡇ࡜ࡀ࡛ࡁࡿࡓࡵࠊ཯ᛂᶵᵓ◊✲࡟࠾ࡅࡿ⌮᝿ⓗ࡞ጞ≧ែ࡜࠸࠼ࡿࠋᚑࡗ࡚ࠊ㉸㧗㏿᫬㛫ศゎᐃࡢᴫ␎ᅗ㸦Fig. 9㸧࡟♧ࡍࡼ࠺࡟ XFEL ࠿ᐃ࡟ࡼࡗ࡚఍ྜయෆ཯ᛂࡢ㐍⾜ࢆ㏣㊧ࡍࡿࡇ࡜ࡣࠊ໬Ꮫ཯ᛂ◊✲ࡢ“✲ᴟ”ࢆ┠ᣦࡍヨࢆ X ⥺ᩓ஘ࢩࢢࢼࣝ࡜ࡋ࡚

ᐃࡍࡿࠋXFEL ࡟࠾ࡅࡿ X ⥺ࡢࣃࣝࢫᖜࡣ 10 fs ࡞ࡢ࡛ཎ⌮ⓗ࡟ࡣ 1
ࢥ࣐ 10 fs ࡢ᫬㛫ศゎ⬟ࢆᣢࡗࡓศᏊື⏬ࢆ᧜ᙳࡍࡿࡇ࡜ࡀྍ⬟࡜࡞ࡿ[3]ࠋX ⥺ᩓ஘ࢫ࣌ࢡࢺࣝࢆ
ࣇ࣮࢚ࣜኚ໬ࡋ࡚ᚓࡽࢀࡿືᚄศᕸ㛵ᩘࡣࠊཎᏊ
㛫ࡢ⤖ྜ㊥㞳ࢆ┤᥋୚࠼ࡿࡓࡵࠊ໬Ꮫ཯ᛂࢆศᏊ
ᵓ㐀ኚ໬࡜ࡋ࡚ᢕᥱ࡛ࡁࡿࠋࡑࡢࡓࡵࠊศᏊᵓ㐀ㄽ࡟ᇶ࡙࠸ࡓ཯ᛂㄽࢆ㆟ㄽࡍࡿࡇ࡜ࡀྍ⬟࡛࠶ࡾࠊ໬Ꮫ཯ᛂࡢᐇ᫬㛫ほ ࡀᐇ⌧ࡉࢀࡿࠋࡲࡉ࡟
ࡇࢀࡣ໬Ꮫ཯ᛂᘧ࡟࠾ࡅࡿ´ńµࡢࠕྍど໬࡛ࠖ࠶ࡾࠊ཯ᛂ࣓࢝ࢽࢬ࣒ࡢヲ⣽࡟ࡘ࠸࡚᪂ࡋ࠸ࣞ࣋ࣝ
ࡢ⌮ゎࢆࡶࡓࡽࡍࠋ

ࡳ࡛࠶ࡿ࡜࠸࠼ࡿࠋ

Fig. 10: ග໬Ꮫ཯ᛂࡢ㐍⾜࡟క࠺ศᏊᵓ㐀ኚ໬ࢆ♧ࡍ ᐃࢹ࣮ࢱࠋගບ㉳๓㸦S0㸧࡜ගບ㉳ᚋ㸦S1,T1,tetramer㸧࡟࠾ࡅࡿືᚄศᕸ㛵ᩘࠋᶓ㍈ࡣ㔠ཎᏊ࠿ࡽࡢ⤖ྜ㊥㞳࡛࠶ࡾࠊࣆ࣮ࢡࡣศᏊ୰ࡢ㔠-㔠㛫⤖ྜ㊥㞳ࢆ⾲ࡍࠋ 㸫 

ࡲ࡛ࡶ࡞࠸ࠋ≉࡟ᮏ◊✲࡛ࡣࠊග࡟ࡼࡗ࡚ᘬࡁ㉳

7.3. ศᏊື⏬࡟ࡼࡿศศᏊ⏕ᡂࡢ▐㛫ࡢࡢྍど໬ࢪࢩ࢔ࣀ㔠㘒య୰ࡢ㔠(I)࢖࢜ࣥࡣ㔠㸫㔠㛫ぶ࿴ᛶ࡟ࡼࡗ࡚Ỉ⣲⤖ྜ࡜ྠ⛬ᗘࡢᙉࡉ࡛఍ྜయ
ࢆᙧᡂࡍࡿࠋࡇࡢ఍ྜయࡢ᭱పບ㉳≧ែ࡟࠾࠸࡚ǔ ⤖ྜᛶ㌶㐨ࡀ༨᭷ࡉࢀࡿࡓࡵࠊගບ㉳࡟ࡼࡗ࡚఍ྜయ୰ࡢ㔠ཎᏊ㛫࡟ඹ᭷⤖ྜࡀ⏕ᡂࡉࢀࡿࠋࡋ
ࡓࡀࡗ࡚ࡇࡢග཯ᛂࢆ㏣㊧ࡍࢀࡤ໬Ꮫ⤖ྜᙧᡂ࡟ࡼࡗ࡚᪂ࡋ࠸ศᏊࡀ⏕ࡲࢀࡿ▐㛫ࡢྍど໬ࡀᐇ⌧ࡉࢀࡿࠋඛ⾜ࡉࢀ࡚⾜ࢃࢀࡓ㐣Ώ྾཰ ᐃ࡛ࡣࠊ㠀ᖖ࡟Ὑ⦎ࡉࢀࡓග཯ᛂࡢไᚚࡀᐇ⌧ࡉࢀ࡚࠾ࡾࠊᮏ◊✲࡟࠾࠸࡚ࡶࠊࡑࡢ᮲௳ࢆ⏝࠸࡚ບ㉳ࣂࣥࢻࢆ㑅ᢥࡍࡿࡇ࡜࡛≉ᐃࡢࢧ࢖ࢬࡢ఍ྜయ
ෆࡢ཯ᛂࢆㄏ㉳ࡉࡏ࡚ ᐃࢆ⾜ࡗࡓࠋࢪࢩ࢔ࣀ㔠㘒యࡀ 3 ࡘ㞟ྜࡋࡓ 3 㔞యࢆࢱ࣮ࢤࢵࢺ࡟ࡋ࡚ࠊ
ࡇࡢ఍ྜయ୰ࡢග໬Ꮫ཯ᛂࢆ XFEL ࠿ࡽᚓࡽࢀ
ࡿࣇ࢙࣒ࢺ⛊ X ⥺ࣃࣝࢫࢆ⏝࠸࡚ྍど໬ࡋࡓࠋࡑ
ࡢ⤖ᯝࠊගࢆ࠶࡚ࡿ๓ࡢ㔠㘒యࡢ㞟ྜయࡣࠊ㔠࢖࢜ࣥྠኈࡀᢡࢀ᭤ࡀࡗࡓᵓ㐀ࢆᣢࡕࠊᙅ࠸ᘬຊࡢ
ࡓࡵ㞟ྜయ࡜ࡋ࡚ࡢᵓ㐀ࡶ୙Ᏻᐃ࡟ᦂࢀ࡚࠸ࡿ

ࡇࡉࢀࡿࠊ㉸㧗㏿࡞໬Ꮫ཯ᛂ࡟㛵ࡍࡿヲ⣽࡞▱ぢࢆᚓࡿࡇ࡜࡟ᡂຌࡋ࡚࠸ࡿࠋ᳜≀ࡢගྜᡂ཯ᛂࢆ
ᶍೌࡋ࡚ග࢚ࢿࣝࢠ࣮ࢆ໬Ꮫ࢚ࢿࣝࢠ࣮࡟ኚ᥮
ࡍࡿேᕤගྜᡂᢏ⾡࡛ࡣࠕගࡢᤕ㞟࣭ࠖࠕཎᏊ㛫ࡢ
࢚ࢿࣝࢠ࣮ఏᦙ࣭ࠖࠕゐ፹㒊఩࡟࠾ࡅࡿ໬Ꮫ࢚ࢿࣝ
ࢠ࣮࡬ࡢኚ᥮ࠖࡀ㔜せ࡞㛤Ⓨせ⣲࡜࡞ࡗ࡚࠸ࡿࠋ
ேᕤගྜᡂࡢᐇ⏝໬ࡢࡓࡵ࡟ࡣࠊ⤖ྜ≧ែࡸศᏊᵓ㐀ࡀኚ໬ࡍࡿගບ㉳┤ᚋࡢ㧗࢚ࢿࣝࢠ࣮≧ែ࡟࠾࠸࡚ࡇࢀࡽࡢせ⣲ࢆ㧗ຠ⋡࡟㥑ືࡉࡏࡿᚲ
せࡀ࠶ࡿࠋ௒ᅇ㛤ⓎࡉࢀࡓศᏊື⏬᧜ᙳἲࡣග࢚
ࢿࣝࢠ࣮ኚ᥮㐣⛬ࢆᵓ㐀ⓗ࡞㠃࠿ࡽཎᏊࣞ࣋ࣝ
࡛ヲ⣽࡟㏣㊧ࡍࡿࡇ࡜ࡀྍ⬟࡞ࡓࡵࠊேᕤගྜᡂ
ࡢᢏ⾡㛤Ⓨ࡟࠾࠸࡚ᇶ┙ⓗほᢏ⾡࡜࡞ࡿᡭἲ

࡛࠶ࡿࠋ㧗ຠ⋡࡞ேᕤගྜᡂࢩࢫࢸ࣒ࡢ㛤Ⓨ࡟ྥࡅ࡚ࠊࡑࡢタィᣦ㔪ࢆ୚࠼ࡿࡓࡵ࡟ศᏊື⏬᧜ᙳἲࡀάⓎ࡟฼⏝ࡉࢀࡿࡇ࡜ࡀᮇᚅࡉࢀࡿࠋ

8. ࠾ࢃࡾ࡟

ࡀ㸦Fig. 10: S0 ≧ែ㸧ࠊගࢆ࠶࡚ࡓ▐㛫࡟㔠࢖࢜ࣥ ᮏࣀ࣮ࢺ࡛ࡣ▷ࣃࣝࢫ X ⥺ࢆ⏝࠸࡚⾜ࢃࢀࡿඛ㛫ࡢ㊥㞳ࡣᛴ⃭࡟⦰ࡲࡗ࡚ᙉᅛ࡞┤⥺ᵓ㐀ࢆྲྀ➃ⓗ࡞ືⓗᐇ㦂࡟㛵㐃ࡋࡓ◊✲౛ࢆ⤂௓ࡋࡓࠋㅮ

ࡿࡇ࡜ࡀࢃ࠿ࡗࡓ㸦Fig. 10: S1 ≧ែ㸧ࠋࡇࡢᵓ㐀ኚ

⩏࡛ࡣ✵㛫ࢥࣄ࣮ࣞࣥࢫࡸࢼࣀࣅ࣮࣒࡜࠸ࡗࡓ

໬࠿ࡽ㔠̿㔠࢖࢜ࣥ㛫࡟໬Ꮫ⤖ྜࡀᙧᡂࡉࢀ᪂

௚ࡢ≉ᚩࢆ㋃ࡲ࠼ࠊERL ࡛ࡣ᝿ᐃࡉࢀࡿඛ➃ⓗ࡞ࡋ࠸ศᏊࡀㄌ⏕ࡋࡓࡇ࡜ࡀ⌮ゎ࡛ࡁࡿࠋࡇࡢᚋࠊ

ᐇ㦂࡟ࡘ࠸࡚ࡉࡽ࡟ヲࡋࡃ㆟ㄽࢆ⾜࠺ࠋ
ࡲࡓࠊ2.7 ࡛ᑡࡋゐࢀࡓࡀࠊ㉸ఏᑟຍ㏿✵Ὕᢏ⾡ࡇࡢศᏊࡣࣆࢥ㹼ࢼࣀ⛊ࡢẚ㍑ⓗ㐜࠸᫬㛫ࢫࢣ࣮ࣝ࡟࠾࠸࡚ࠊᵓ㐀ኚ໬ࢆక࠸࡞ࡀࡽ㸦Fig. 10: T1ࢆ⏝࠸ࡓ ERL ࡜ẚ࡭ࠊᚑ᮶ࡢᖖఏᑟຍ㏿✵Ὕࢆ≧ែ㸧㔠㘒యࢆࡶ࠺୍ࡘྲྀࡾ㎸ࡳࠊࡉࡽ࡟᪂ࡋ࠸

⏝࠸࡚ࡿ SASE-XFEL ࡟࠾࠸࡚ࠊᐇ㦂ⓗᅔ㞴ࢆ⏕ศᏊ࡬࡜ኚ໬ࡍࡿ㸦Fig. 10: tetramer ≧ែ㸧㸧ࠋࡇࡳฟࡍせᅉࡣࠊప⧞ࡾ㏉ࡋ࡟㉳ᅉࡋࡓࢹ࣮ࢱ࣮཰

ࡢศᏊ࠿ࡽࡢⓎගࡢⰍࡣ㔠㘒యࢆྲྀࡾ㎸ࡴ๓࡜㞟ຠ⋡ࡢᝏࡉ࡜ࠊ㧗ࣃࣝࢫᙉᗘ࡟㉳ᅉࡋࡓࢼࣀࣅ

ẚ࡭࡚኱ࡁࡃኚ໬ࡍࡿࡓࡵࠊⓎගᮦᩱࡸศᏊࢭࣥ

࣮࣒㞟ගୗ࡛ࡢࢧࣥࣉࣝࡢ◚ቯᛶ࡛࠶ࡿࠋࡋ࠿ࡋ

ࢧ࣮࡜࠸ࡗࡓගᶵ⬟ᮦᩱ࡜ࡋ࡚ࡢ฼⏝ࡶᮇᚅࡉ࡞ࡀࡽ⡿ᅜ SLAC ◊✲ᡤ࡛ࡣ㉸ఏᑟຍ㏿✵Ὕࢆ⏝ࢀ࡚࠸ࡿࡀࠊࡇࡢᶵ⬟ᛶࡢฟ⌧ࡣ㔠࢖࢜ࣥࡢᩘࡀ

࠸ࡓ㧗⧞ࡾ㏉ࡋࡢ FEL ィ⏬ࡀ㐍⾜୰࡛࠶ࡾࠊ㧗ቑ࠼ࡓศᏊᵓ㐀ࡢኚ໬࡟㉳ᅉࡍࡿࡇ࡜ࡶᮏ◊✲⧞ࡾ㏉ࡋ࣭పࣃࣝࢫᙉᗘ࡜࠸࠺ ERL ࡢ㛗ᡤ࡜ࡋ⤖ᯝ࠿ࡽ⌮ゎ࡛ࡁࡿࠋ࡚⤂௓ࡋࡓ≉ᚩࢆවࡡഛ࠼ࡓ FEL ග※ࡀᩘᖺᚋ
࡟ࡣⓏሙࡍࡿࠋ௒ᚋࠊ㉸ఏᑟࣜࢽ࢔ࢵࢡຍ㏿✵Ὕ

7.4. ศ Ꮚື⏬᧜ᙳἲࢆ⏝࠸ࡓග࢚ࢿࣝࢠ࣮ኚ᥮

ࢆ⏝࠸ࡓ㧗⧞ࡾ㏉ࡋග※ࡣୡ⏺ⓗ࡟୺࡞₻ὶ࡟࡞ࡗ࡚ࡺࡃࡶࡢ࡜⪃࠼ࡽࢀࡿࠋ

ᮦᩱ࡟ᑐࡍࡿタィᣦ㔪ࡢᥦ᱌ᮏ◊✲࡛ࡣཎᏊ࡜ཎᏊ࡜ࡢ㛫࡟⤖ྜࡀᙧᡂࡉ
ࢀࠊ᪂ࡋ࠸ศᏊࡀ⏕ࡲࢀࡿ▐㛫ࢆ㹖⥺࡛ᤊ࠼ࡿࡇ
࡜࡟ึࡵ࡚ᡂຌࡋࡓࠋࡇࡢࡼ࠺࡞᪂ࡋ࠸ ᐃᢏ⾡ཧ ⪃ ᩥ ⊩
>@ (QHUJ\ 5HFRYHU\ /LQDF &RQFHSWXDO 'HVLJQ
5HSRUW.(.5HSRUW2FWREHU

ࡀᇶ♏໬ᏛࡢⓎᒎ࡟኱ࡁࡃᐤ୚ࡍࡿࡇ࡜ࡣゝ࠺ 㸫 

>@ 6 1R]DZD 6 $GDFKL HW DO - $P &KHP 6RF  >@ 7,VKLNDZDࠊ HWDO1DWXUH3KRWRQ  >@ 61R]DZD6$GDFKLHWDO-6\QFKURWURQ5DG
  >@ 0)3HUXW]1DWXUH  
>@ :$(DWRQHWDO1DW6WUXFW%LRO  >@ 6$GDFKLHWDO3URF1DWO$FDG6FL
 
>@ (&KLDQFRQHHWDO-0RO%LRO  >@ ( $QWRQLQL HW DO - %LRO &KHP  
 
>@$ 0R]]DUHOOL HW DO - %LRO &KHP  
 
>@.,FKL\DQDJLHWDO-6\QFKURWURQ5DG
 
>@. + .LP HW DO - $P &KHP 6RF  
 
>@+,FKLNDZD61R]DZDHWDO1DWXUH0DWHULDOV  >@. + .LP 6 1R]DZD HW DO 1DWXUH    㸫 