Suppression of Stimulated Raman Scattering via Photon Depletion in a Two-Color Three-Beam Setup

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(2) . ϭϴƚŚƵƌŽƉĞĂŶŽŶĨĞƌĞŶĐĞKŶEŽŶͲ>ŝŶĞĂƌKƉƚŝĐĂů^ƉĞĐƚƌŽƐĐŽƉǇ͕ƚŚĞĂŶŶƵĂů ŵĞĞƚŝŶŐĚĞǀŽƚĞĚƚŽĚŝǀĞƌƐĞƚŽƉŝĐƐŝŶƚŚĞĨŝĞůĚŽĨŶŽŶůŝŶĞĂƌŽƉƚŝĐĂů ƐƉĞĐƚƌŽƐĐŽƉǇ͕ŝŶĐůƵĚŝŶŐĐŽŚĞƌĞŶƚZĂŵĂŶƐĐĂƚƚĞƌŝŶŐ͕ŶŽǀĞůůĂƐĞƌƐŽƵƌĐĞƐ͕ ŵŝĐƌŽƐĐŽƉǇ͕ŝŵĂŐŝŶŐ͕ĐŽŵďƵƐƚŝŽŶ͕ƵůƚƌĂĨĂƐƚĂŶĚǀŝďƌĂƚŝŽŶĂůƐƉĞĐƚƌŽƐĐŽƉǇ͘ dŚĞĐŽŶĨĞƌĞŶĐĞŵĂŝŶƚŽƉŝĐƐŽĨƚŚŝƐĞĚŝƚŝŽŶǁŝůůďĞŚŝŐŚůŝŐŚƚĞĚďǇƌĞĐŽŐŶŝǌĞĚ ƐĐŝĞŶƚŝĨŝĐƐƉĞĂŬĞƌƐǁŚŽĂŐƌĞĞĚƚŽĚĞůŝǀĞƌƚŽKEK^ĂƚƚĞŶĚĂŶƚƐƉĞĚĂŐŽŐŝĐ ůĞĐƚƵƌĞƐ͘. /ŶƚŚĞƚƌĂĚŝƚŝŽŶŽĨƌĞĐĞŶƚǇĞĂƌƐ͕ĂƐƉĞĐŝĂůŝƐƐƵĞ͚KEK^ͬt͛ŽĨƚŚĞ:ŽƵƌŶĂůŽĨ ZĂŵĂŶƐƉĞĐƚƌŽƐĐŽƉǇĨŽƌƚŚĞWƌŽĐĞĞĚŝŶŐƐŽĨƚŚĞĐŽŶĨĞƌĞŶĐĞŝƐƉůĂŶŶĞĚ͘ƵƚŚŽƌ ŝŶĨŽƌŵĂƚŝŽŶƌĞŐĂƌĚŝŶŐƚŚĞƉƌĞƉĂƌĂƚŝŽŶŽĨŵĂŶƵƐĐƌŝƉƚƐĐĂŶďĞĨŽƵŶĚŽŶ:Z^ ǁĞďƉĂŐĞ .

(3) . . KDD/dd^ ^ƚĞĞƌŝŶŐĐŽŵŵŝƚƚĞĞ͗ x x x x x x x x x x x x x x x x x x x. ƌŝŐŝƚƚĞƚƚĂůͲdƌĞƚŽƵƚ;ŚĂŝƌͿʹKEZ;WĂůĂŝƐĞĂƵ͕&ƌĂŶĐĞͿ WĞƌͲƌŝŬĞŶŐƚƐƐŽŶʹ>ƵŶĚhŶŝǀĞƌƐŝƚǇ;^ǁĞĚĞŶͿ ŝŽŶŝƐŝŽĞƌŵĞũŽʹ/ŶƐƚŝƚƵƚŽĚĞƐƚƌƵĐƚƵƌĂĚĞůĂDĂƚĞƌŝĂ;DĂĚƌŝĚ͕^ƉĂŝŶͿ WŝĞƌƌĞ:ŽƵďĞƌƚʹ/ŶƐƚŝƚƵƚhƚŝŶĂŵ;ĞƐĂŶĕŽŶ͕&ƌĂŶĐĞͿ :ŽŚĂŶŶĞƐ<ŝĞĨĞƌʹhŶŝǀĞƌƐŝƚǇŽĨƌĞŵĞŶ;'ĞƌŵĂŶǇͿ ůĞǆĂŶĚĞƌ<ŽƵǌŽǀʹ^ĂŝŶƚWĞƚĞƌƐďƵƌŐ^ƚĂƚĞhŶŝǀĞƌƐŝƚǇ;ZƵƐƐŝĂͿ ŵŝƚƌǇ<ŽǌůŽǀʹZƵƐƐŝĂŶĐĂĚĞŵǇŽĨ^ĐŝĞŶĐĞƐ;DŽƐĐŽǁ͕ZƵƐƐŝĂͿ ƌƵŶŽ>ĂǀŽƌĞůʹ/ŶƐƚŝƚƵƚĂƌŶŽƚĚĞŽƵƌŐŽŐŶĞ;ŝũŽŶ͕&ƌĂŶĐĞͿ DŝĐŚĞůĞDĂƌƌŽĐĐŽʹE;ZŽŵĂ͕/ƚĂůŝĂͿ ƌŶƵůĨDĂƚĞƌŶǇʹhŶŝǀĞƌƐŝƚǇŽĨƌĞŵĞŶ;'ĞƌŵĂŶǇͿ :ƵůŝĂŶDŽŐĞƌʹhŶŝǀĞƌƐŝƚǇŽĨǆĞƚĞƌ;ŶŐůĂŶĚͿ ,ĞƌŵĂŶKĨĨĞƌŚĂƵƐʹhŶŝǀĞƌƐŝƚǇŽĨdǁĞŶƚĞ;ŶƐĐŚĞĚĞ͕EĞƚŚĞƌůĂŶĚƐͿ ĂƌŝŽWŽůůŝʹWŽůŝƚĞĐŶŝĐŽĚŝDŝůĂŶŽ;/ƚĂůǇͿ WĞƚĞƌZĂĚŝʹhŶŝǀĞƌƐŝƚǇŽĨĞƌŶĞ;^ǁŝƐƐͿ DŽŶŝŬĂZŝƚƐĐŚͲDĂƌƚĞʹDĞĚŝĐĂů&ĂĐƵůƚǇŽĨƚŚĞhŶŝǀĞƌƐŝƚǇŽĨ/ŶŶƐďƌƵĐŬ;ƵƐƚƌŝĂͿ DĂĂƌƚĞŶZŽĞĨĨĂĞƌƐʹhŶŝǀĞƌƐŝƚǇŽĨ>ĞƵǀĞŶ;ĞůŐŝƵŵͿ DŝĐŚĂĞů^ĐŚŵŝƚƚʹ&ƌŝĞĚƌŝĐŚͲ^ĐŚŝůůĞƌhŶŝǀĞƌƐŝƚǇ;:ĞŶĂ͕'ĞƌŵĂŶǇͿ dŚŽŵĂƐ^ĞĞŐĞƌʹhŶŝǀĞƌƐŝƚǇŽĨ^ŝĞŐĞŶ;'ĞƌŵĂŶǇͿ ůĞŬƐĞŝŚĞůƚŝŬŽǀʹDŽƐĐŽǁ^ƚĂƚĞhŶŝǀĞƌƐŝƚǇ;ZƵƐƐŝĂͿ. ϮϬϭϵKƌŐĂŶŝƐŝŶŐĐŽŵŵŝƚƚĞĞ ŽͲŚĂŝƌƐ͗WƌŽĨ͘&ƌĠĚĠƌŝĐ'Z/^,ΘƌĞŶŽŠƚZs/h͕KZ/ͲhDZϲϲϭϰ;ZŽƵĞŶ͕&ƌĂŶĐĞͿ͕ ƌŝŐŝƚƚĞdd>ͲdZdKhd͕KEZ;WĂůĂŝƐĞĂƵ͕&ƌĂŶĐĞͿ KƌŐĂŶŝƐĞƌ͗ŚƌŝƐƚŽƉŚĞ>d/>>hZ͕KZ/ͲhDZϲϲϭϰ;ZŽƵĞŶ͕&ƌĂŶĐĞͿ͘ ^ĞĐƌĞƚĂƌǇ͗&ůŽƌĞŶĐĞ&Zd͕KZ/ͲhDZϲϲϭϰ;ZŽƵĞŶ͕&ƌĂŶĐĞͿ͘ ^ƚĂĨĨ͗ĠĚƌŝĐ,DZ>E;/dŵĂŶĂŐĞƌͿ͕^ĂŢĚ/>,E͕^ǇůǀĂŝŶ>'ZK^͕ƌƵŶŽD/>>͕ WƌĂĚŝƉys/Z͕KZ/ͲhDZϲϲϭϰ;ZŽƵĞŶ͕&ƌĂŶĐĞͿ͘.

(4) . KEK^,ŝƐƚŽƌǇ͕ϯϳǇĞĂƌƐŽĨŚŝƐƚŽƌǇ &ŽƌŵĞƌϭϳĞĚŝƚŝŽŶƐŽĨƚŚĞKEK^DĞĞƚŝŶŐƐ͗ x x x x x x x x x x x x x x x x x. KEK^ϮϬϭϴ͕DŝůĂŶ͕/ƚĂůǇ͕ƉƌŝůϴͲϭϭ KEK^ϮϬϭϳ͕:ĞŶĂ͕'ĞƌŵĂŶǇ͕ƉƌŝůϮͲϱ KEK^ϮϬϭϲ͕'ƂƚĞďŽƌŐ͕^ǁĞĚĞŶ͕ƉƌŝůϮϰͲϮϳ KEK^ϮϬϭϱ͕>ĞƵǀĞŶ͕ĞůŐŝƵŵ͕ƉƌŝůϭϮͲϭϱ KEK^ϮϬϭϰ͕ŽůĞ͕&ƌĂŶĐĞ͕DĂǇϭϭͲϭϰ KEK^ϮϬϭϯ͕ǆĞƚĞƌ͕h<͕ƉƌŝůϮϮͲϮϰ KEK^ϮϬϭϮ͕ďĞƌĚĞĞŶ͕h<͕:ƵůǇϴͲϭϭ KEK^ϮϬϭϭ͕ŶƐĐŚĞĚĞ͕EĞƚŚĞƌůĂŶĚƐ͕DĂǇϮϯͲϮϱ KEK^ϮϬϭϬ͕ƌĞŵĞŶ͕'ĞƌŵĂŶǇ͕:ƵŶϮϭͲϮϯ KEK^ϮϬϬϵ͕&ƌĂƐĐĂƚŝ͕/ƚĂůǇ͕DĂǇϮϱͲϮϳ KEK^ϮϬϬϴ͕/ŐůƐ͕ƵƐƚƌŝĂ͕DĂǇϮϱͲϮϳ KEK^ϮϬϬϳ͕^ƚ͘WĞƚĞƌƐďƵƌŐ͕ZƵƐƐŝĂ͕DĂǇϭϮͲϭϱ KEK^ϮϬϬϲ͕^ŵŽůĞŶŝĐĞ͕^ůŽǀĂŬZĞƉƵďůŝŬ͕ƉƌŝůϵͲϭϭ KEK^ϮϬϬϱ͕KǆĨŽƌĚ͕hŶŝƚĞĚ<ŝŶŐĚŽŵ͕ƉƌŝůϭϬͲϭϮ KEK^ϮϬϬϰ͕ƌůĂŶŐĞŶ͕'ĞƌŵĂŶǇ͕ƉƌŝůϰͲϲ KEK^ϮϬϬϯ͕ĞƐĂŶĐŽŶ͕&ƌĂŶĐĞ͕DĂƌĐŚϯϬ͕ϯϭĂŶĚƉƌŝůϭ KEK^ϮϬϬϮ͕sŝůůŝŐĞŶ͕^ǁŝƚǌĞƌůĂŶĚ͕DĂƌĐŚϭϴͲϭϵ dŚĂƚŝƐŶŽƚĂůůƚŚĞƐƚŽƌǇ͕ŝŶĚĞĞĚ͕ƚŚĞĐŽŶĨĞƌĞŶĐĞŝƐŶĂŵĞĚKEK^ƐŝŶĐĞϮϬϬϮ͕ĂŶĚ ǁĂƐƉƌĞǀŝŽƵƐůǇĐĂůůĞĚƵƌŽƉĞĂŶZ^ǁŽƌŬƐŚŽƉ͕ƐƚĂƌƚŝŶŐŝŶϭϵϴϮ͊ ϮϬϬϭ͕>ƵŶĚ͕^ǁĞĚĞŶͲϮϬϬϬ͕DŽƐĐŽǁ͕ZƵƐƐŝĂͲϭϵϵϵ͕&ƌĂƐĐĂƚŝ͕/ƚĂůǇͲϭϵϵϴ͕ ĞƐĂŶĕŽŶ͕&ƌĂŶĐĞͲϭϵϵϳ͕,ĞŝĚĞůďĞƌŐ͕'ĞƌŵĂŶǇͲϭϵϵϲ͕^ŚĞĨĨŝĞůĚ͕hŶŝƚĞĚ<ŝŶŐĚŽŵͲ ϭϵϵϱ͕DĂĚƌŝĚ͕^ƉĂŝŶͲϭϵϵϰ͕'ŝĨƐƵƌzǀĞƚƚĞ͕&ƌĂŶĐĞͲϭϵϵϯ͕sŝůůŝŐĞŶ͕^ǁŝƐƐͲϭϵϵϮ͕ &ůŽƌĞŶĐĞ͕/ƚĂůǇͲϭϵϵϭ͕'ĂƌĐŚŝŶŐ͕'ĞƌŵĂŶǇͲϭϵϵϬ͕ŝũŽŶ͕&ƌĂŶĐĞͲϭϵϴϵ͕KǆĨŽƌĚ͕ hŶŝƚĞĚ<ŝŶŐĚŽŵͲϭϵϴϴ͕WŝƐĂ͕/ƚĂůǇͲϭϵϴϳ͕^ƚƵƚƚŐĂƌĚ͕'ĞƌŵĂŶǇͲϭϵϴϲ͕>ƵŶĚ͕ ^ǁĞĚĞŶͲϭϵϴϱ͕ZŽƵĞŶ͕&ƌĂŶĐĞͲϭϵϴϰ͕,ĂƌǁĞůů͕hŶŝƚĞĚ<ŝŶŐĚŽŵͲϭϵϴϯ͕ŚĂƚŝůůŽŶ͕ &ƌĂŶĐĞͲϭϵϴϮ͕,ĂƌǁĞůů͕hŶŝƚĞĚ<ŝŶŐĚŽŵ .

(5) . /ŶƐƚŝƚƵƚŝŽŶĂůƉĂƌƚŶĞƌƐ . . . . . . . . . . . . . . . . .

(6) /ŶĚƵƐƚƌŝĂůƉĂƌƚŶĞƌƐ . . . . . . .

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(8) ^ƵŶĚĂǇƉƌŝůϳƚŚ͕ϮϬϭϵ͘ ϭϲ͗ϬϬ ϭϲ͗ϰϬ ϭϳ͗ϬϬ. . tĞůĐŽŵĞŝŶƚŚĞƚŽƵƌŝƐƚŽĨĨŝĐĞŽĨZŽƵĞŶ KƉĞŶŝŶŐŽĨKEK^ϮϬϭϵďǇ͘ĂƌǀŝĂƵΘ&͘'ƌŝƐĐŚ. <ĞǇŶŽƚĞ ƌŝĐWŽƚŵĂ͕hŶŝǀĞƌƐŝƚǇŽĨĂůŝĨŽƌŶŝĂ/ƌǀŝŶĞ EŽŶůŝŶĞĂƌŽƉƚŝĐĂůŵŝĐƌŽƐĐŽƉǇŝŶƚŚĞŵŝĚͲŝŶĨƌĂƌĞĚ ϭϴ͗ϬϬ ŽĐŬƚĂŝůĚŝŶŶĞƌ ϭϵ͗ϬϬ ĂƚŚĞĚƌĂůĐĂƌŝůůŽŶƐĐŽŶĐĞƌƚďǇDƌ>ĂƚŽƵƌ . DŽŶĚĂǇƉƌŝůϴƚŚ͕ϮϬϭϵ͘ ϴ͗ϬϬ ϴ͗ϯϬ ϵ͗ϬϬ ϵ͗ϰϬ. ZĞŐŝƐƚƌĂƚŝŽŶ ^ƉĞĞĐŚĞƐďǇŝŶƐƚŝƚƵƚŝŽŶĂůƌĞƉƌĞƐĞŶƚĂƚŝǀĞƐ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ :ŽĂŬŝŵŽŽĚ͕>ƵŶĚhŶŝǀĞƌƐŝƚǇ ĂĐŬǁĂƌĚůĂƐŝŶŐĨŽƌƌĂŶŐĞͲƌĞƐŽůǀĞĚĚĞƚĞĐƚŝŽŶŽĨĂƚŽŵŝĐƐƉĞĐŝĞƐ. ůŝ,ŽƐƐĞŝŶŶŝĂ͕>ƵŶĚhŶŝǀĞƌƐŝƚǇ ^ŝŶŐůĞͲƐŚŽƚZĂŵĂŶůŝŶĞǁŝĚƚŚŵĞĂƐƵƌĞŵĞŶƚƐƵƐŝŶŐƚŝŵĞͲƌĞƐŽůǀĞĚŚǇďƌŝĚ ĨĞŵƚŽƐĞĐŽŶĚͬŶĂŶŽƐĞĐŽŶĚƌŽƚĂƚŝŽŶĂůZ^ ϭϬ͗ϬϬ DŝĐŚĂĞů^ĐŚĞƌŵĂŶ͕KEZWĂůĂŝƐĞĂƵ ŵƉůŝĨŝĞĚůĂƐĞƌĂƌĐŚŝƚĞĐƚƵƌĞĨŽƌƵůƚƌĂĨĂƐƚƌŽͲǀŝďƌĂƚŝŽŶĂůĨƐͬƉƐͲZ^ƚŚĞƌŵŽŵĞƚƌǇŝŶ ĨůĂŵĞƐ ϭϬ͗ϮϬ K&&Z<ΘWK^dZ^^^/KE .

(9) ϭϭ͗ϬϬ DŝĐŚĞůĞDĂƌƌŽĐĐŽ͕EZŽŵĞ ŚŝƌƉĞĨĨĞĐƚƐŝŶZ^ƐŝŐŶĂůƐŐĞŶĞƌĂƚĞĚďǇĨĞŵƚŽƐĞĐŽŶĚůĂƐĞƌƉƵůƐĞƐƵŶĚĞƌƐƚƌŽŶŐ ĐŚŝƌƉƌĞŐŝŵĞŽĨƚŚĞƉƌŽďĞ ϭϭ͗ϮϬ ^ǇůǀĂŝŶ>ĞŐƌŽƐ͕KZ/ZŽƵĞŶ ^ŝŶŐůĞͲ^ŚŽƚϭŬ,ǌWWĨƐZ^͗dĞŵƉĞƌĂƚƵƌĞDĞĂƐƵƌĞŵĞŶƚƐ&ƌŽŵƚŵŽƐƉŚĞƌŝĐƚŽ ,ŝŐŚͲWƌĞƐƐƵƌĞŶǀŝƌŽŶŵĞŶƚƐ ϭϭ͗ϰϬ zĂŶŐZĂŶ͕&ƌŝĞĚƌŝĐŚͲ^ĐŚŝůůĞƌͲhŶŝǀĞƌƐŝƚćƚ:ĞŶĂ ŽůůŝƐŝŽŶͲĨƌĞĞƚǁŽͲďĞĂŵƵůƚƌĂďƌŽĂĚďĂŶĚĐŽŚĞƌĞŶƚĂŶƚŝͲƐƚŽŬĞƐZĂŵĂŶƐĐĂƚƚĞƌŝŶŐ ƐƉĞĐƚƌŽƐĐŽƉǇĨŽƌŚŝŐŚƉƌĞƐƐƵƌĞƚŚĞƌŵŽŵĞƚƌǇ ϭϮ͗ϬϬ ůĞǆŝƐŽŚůŝŶ͕ĞůĨƚhŶŝǀĞƌƐŝƚǇŽĨdĞĐŚŶŽůŽŐǇ ^ŝŶŐůĞͲƐŚŽƚZ^ŝŵĂŐŝŶŐŽĨŶĞĂƌͲǁĂůůƚƵƌďƵůĞŶƚƌĞĂĐƚŝŶŐĨůŽǁƐ ϭϮ͗ϮϬ >hE, ϭϯ͗ϱϬ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ ŵŵĂŶƵĞůĞĂƵƌĞƉĂŝƌĞ͕>KWĂůĂŝƐĞĂƵ DƵůƚŝĐŽůŽƌŵƵůƚŝƉŚŽƚŽŶŵŝĐƌŽƐĐŽƉǇŽĨĚĞǀĞůŽƉŝŶŐĂŶĚŶĞƌǀŽƵƐƚŝƐƐƵĞƐ ϭϰ͗ϯϬ ^ĂŶĚƌŽ,ĞƵŬĞ͕/ŶƐƚŝƚƵƚ&ƌĞƐŶĞů͕DĂƌƐĞŝůůĞ ŽŚĞƌĞŶƚĂŶƚŝͲ^ƚŽŬĞƐZĂŵĂŶ&ŽƵƌŝĞƌWƚǇĐŚŽŐƌĂƉŚǇDŝĐƌŽƐĐŽƉǇ ϭϰ͗ϱϬ dŝĂŐŽƵĐŬƵƉ͕hŶŝǀĞƌƐŝƚćƚ,ĞŝĚĞůďĞƌŐ dŝŵĞͲZĞƐŽůǀĞĚŽŚĞƌĞŶƚZĂŵĂŶ^ƉĞĐƚƌŽƐĐŽƉǇŽĨtŝůĚdǇƉĞĂŶĚDƵƚĂƚĞĚŶĂďĂĞŶĂ ^ĞŶƐŽƌǇZŚŽĚŽƉƐŝŶ ϭϱ͗ϭϬ K&&Z<ΘWK^dZ^^^/KE ϭϱ͗ϱϬ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ ŚŵĞĚďĚĞůŵŽŶĞŵ͕<ĂƌůƐƌƵŚĞ/ŶƐƚŝƚƵƚĞŽĨdĞĐŚŶŽůŽŐǇ DŽůĞĐƵůĂƌůĞǀĞůĐŚĂƌĂĐƚĞƌŝǌĂƚŝŽŶŽĨĂƚŵŽƐƉŚĞƌŝĐĂĞƌŽƐŽůʹǁĂƚĞƌʹŝĐĞŝŶƚĞƌĂĐƚŝŽŶƐ ƵƐŝŶŐŶŽŶůŝŶĞĂƌŽƉƚŝĐĂůƐƉĞĐƚƌŽƐĐŽƉǇ͕ŵĂŝŶůǇ^,'ĂŶĚ^&' ϭϲ͗ϯϬ DĂǆŝŵŝůŝĂŶƌŝŶŬŵĂŶŶ͕hŶŝǀĞƌƐŝƚǇŽĨDƵĞŶƐƚĞƌ >ŝǀĞDƵůƚŝͲŽůŽƌŽŚĞƌĞŶƚZĂŵĂŶ/ŵĂŐŝŶŐŶĂďůĞĚďǇĂŽŵƉĂĐƚĂŶĚ ZŽďƵƐƚ>ŝŐŚƚ^ŽƵƌĐĞ . . ϭϲ͗ϱϬ ůĞũĂŶĚƌŽĞůĂĂĚĞŶĂ͕WŽůŝƚĞĐŶŝĐŽĚŝDŝůĂŶŽ ƌŽĂĚďĂŶĚ^ƚŝŵƵůĂƚĞĚZĂŵĂŶ^ĐĂƚƚĞƌŝŶŐDŝĐƌŽƐĐŽƉǇǁŝƚŚ/ŶͲ>ŝŶĞĂůĂŶĐĞĚͲĞƚĞĐƚŝŽŶ . . ϭϳ͗ϭϬ ĂƌŝŽWŽůůŝ͕WŽůŝƚĞĐŶŝĐŽĚŝDŝůĂŶŽ ZĞƚƌŝĞǀŝŶŐƚŚĞĐŽŵƉůĞǆǀŝďƌĂƚŝŽŶĂůƐƵƐĐĞƉƚŝďŝůŝƚǇǁŝƚŚŝŶƚĞƌĨĞƌŽŵĞƚƌŝĐƐƚŝŵƵůĂƚĞĚ ZĂŵĂŶƐĐĂƚƚĞƌŝŶŐ;ŝ^Z^Ϳ ϭϴ͗ϯϬ ,ŝƐƚŽƌŝĂů:ĞĂŶŶĞĚΖƌĐ ŽĐŬƚĂŝůĚŝŶŶĞƌĂŶĚĞŶũŽǇĂƉůĂĐĞƐƚĞĞƉĞĚŝŶŚŝƐƚŽƌǇ. .

(10) dƵĞƐĚĂǇƉƌŝůϵƚŚ͕ϮϬϭϵ͘ ϴ͗ϯϬ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ tĂƌƵŶĂ<ƵůĂƚŝůĂŬĂ͕dĞǆĂƐΘDhŶŝǀĞƌƐŝƚǇ hůƚƌĂƐŚŽƌƚͲWƵůƐĞDƵůƚŝͲWŚŽƚŽŶDƵůƚŝͲ^ƉĞĐŝĞƐ/ŵĂŐŝŶŐdĞĐŚŶŝƋƵĞƐĨŽƌ ŽŵďƵƐƚŝŽŶŝĂŐŶŽƐƚŝĐƐ ϵ͗ϭϬ WĞŶŐũŝŝŶŐ͕>ƵŶĚhŶŝǀĞƌƐŝƚǇ &ĞŵƚŽƐĞĐŽŶĚdǁŽͲWŚŽƚŽŶďƐŽƌƉƚŝŽŶ>ĂƐĞƌͲ/ŶĚƵĐĞĚ&ůƵŽƌĞƐĐĞŶĐĞ/ŵĂŐŝŶŐŽĨ ƚŽŵŝĐ,ǇĚƌŽŐĞŶĂŶĚKǆǇŐĞŶŝŶĂWůĂƐŵĂͲƐƐŝƐƚĞĚDĞƚŚĂŶĞͬŝƌ&ůĂŵĞ ϵ͗ϯϬ <ŽŶƐƚĂŶƚŝŶ͘sĞƌĞƐŚĐŚĂŐŝŶ͕&ĞĚĞƌĂů^ƚĂƚĞ/ŶƐƚŝƚƵƚŝŽŶŽĨ^ĐŝĞŶĐĞ͘D͘WƌŽŬŚŽƌŽǀ 'ĞŶĞƌĂůWŚǇƐŝĐƐ/ŶƐƚŝƚƵƚĞ 'ĞŶĞƌĂƚŝŽŶŽĨWĂƌĂŵĞƚƌŝĐ^ƵƉĞƌĨůƵŽƌĞƐĐĞŶĐĞďǇWŝĐŽƐĞĐŽŶĚWƵůƐĞƐƵŶĚĞƌ>Žǁ &ƌĞƋƵĞŶĐǇWƵŵƉŝŶ<dWƌǇƐƚĂů ϵ͗ϱϬ K&&Z<ΘWK^dZ^^^/KE ϭϬ͗ϯϬ ůŝ,ŽƐƐĞŝŶŶŝĂ͕>ƵŶĚhŶŝǀĞƌƐŝƚǇ WƵƌĞƌŽƚĂƚŝŽŶĂůĐŽŚĞƌĞŶƚĂŶƚŝͲ^ƚŽŬĞƐZĂŵĂŶƐƉĞĐƚƌŽƐĐŽƉǇŽĨĞƚŚǇůĞŶĞͲŶŝƚƌŽŐĞŶ ŵŝǆƚƵƌĞƐ͕ǆƉĞƌŝŵĞŶƚƐĂŶĚŵŽĚĞůůŝŶŐ ϭϬ͗ϱϬ dŚŽŵĂƐtƺƌƚŚǁĞŝŶ͕hŶŝǀĞƌƐŝƚǇŽĨDƺŶƐƚĞƌ ^ƵƉƉƌĞƐƐŝŽŶŽĨ^ƚŝŵƵůĂƚĞĚZĂŵĂŶ^ĐĂƚƚĞƌŝŶŐǀŝĂWŚŽƚŽŶĞƉůĞƚŝŽŶŝŶĂdǁŽͲŽůŽƌ dŚƌĞĞͲĞĂŵ^ĞƚƵƉ ϭϭ͗ϭϬ DĂůŝŬEĂĨĂ͕EZͬ/EKΘ>E^ d,ǌͲY>ƐŽƵƌĐĞƐĨŽƌƉƌĞĐŝƐŝŽŶƐƉĞĐƚƌŽƐĐŽƉǇ ϭϭ͗ϯϬ ĂǀŝĚ^ĞĚĂƌƐŬǇ͕ŚĂůŵĞƌƐhŶŝǀĞƌƐŝƚǇŽĨdĞĐŚŶŽůŽŐǇ dŝŵĞͲŐĂƚĞĚďĂĐŬͲƐĐĂƚƚĞƌŝŵĂŐŝŶŐŝŶƚƵƌďŝĚŵĞĚŝĂ ϭϭ͗ϱϬ >hE,. . . .

(11) ϭϯ͗ϮϬ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ ůĞŶĂKďƌĂǌƚƐŽǀĂ͕/ŶƐƚŝƚƵƚĞŽĨZƵƐƐŝĂŶĂĐĂĚĞŵǇŽĨ^ĐŝĞŶĐĞƐ͕DŽƐĐŽǁ DŽĚŝĨŝĞĚƐŝŶŐůĞͲǁĂůůĐĂƌďŽŶŶĂŶŽƚƵďĞƐĂŶĚŐƌĂƉŚĞŶĞĨŽƌƐĂƚƵƌĂďůĞĂďƐŽƌďĞƌƐ ŝŶƐŽůŝĚƐƚĂƚĞůĂƐĞƌƐ ϭϰ͗ϬϬ ŶŐĞůĂsĞůůĂ͕'WDZŽƵĞŶ ^ƚƵĚǇŽĨƐƚƌĂŝŶƐĞŶƐŝƚŝǀŝƚǇĂŶĚƐǇŵŵĞƚƌǇŽĨĐŽůŽƌĐĞŶƚĞƌŝŶĚŝĂŵŽŶĚŶĂŶŽƐĐĂůĞŶĞĞĚůĞƐ ďǇĐŽŶƚĂĐƚůĞƐƐŽƉƚŝĐĂůƉŝĞǌŽͲƐƉĞĐƚƌŽƐĐŽƉǇ ϭϰ͗ϮϬ DŝĐŚĞůĞDĂƌƌŽĐĐŽ͕EZŽŵĞ ůĂƐƐŝĐĂůZĞƉƌĞƐĞŶƚĂƚŝŽŶŽĨEŽŶͲ>ŝŶĞĂƌZĞƐƉŽŶƐĞ&ƵŶĐƚŝŽŶƐĂŶĚƚŚĞŝƌŽŶŶĞĐƚŝŽŶƐƚŽ YƵĂŶƚƵŵͲDĞĐŚĂŶŝĐĂů'ƌĂƉŚŝĐZĞƉƌĞƐĞŶƚĂƚŝŽŶƐĂƐĞĚŽŶŽƵďůĞͲ^ŝĚĞĚ&ĞǇŶŵĂŶ ŝĂŐƌĂŵƐĂŶĚ>ŝŽƵǀŝůůĞ^ƉĂĐĞŽƵƉůŝŶŐ^ĐŚĞŵĞ ϭϰ͗ϰϬ /ŶĚƵƐƚƌŝĂůƐĞƐƐŝŽŶ >&/͕DW>/dh͕͘W͕͘͘K,ZEd͕&DdK^z͕,KZ/͕D<^EtWKZd͕ EKs͕KWdKE>^Z͕d>zEWZ/EdKE͕d,KZ>^͘ ϭϱ͗ϰϬ K&&Z<ΘWK^dZ^^^/KE ϭϲ͗ϬϬ WĞƚĞƌZĂĚŝ͕WĂƵů^ĐŚĞƌƌĞƌ/ŶƐƚŝƚƵƚĞ ǆƉĞƌŝŵĞŶƚĂůĞƚĞƌŵŝŶĂƚŝŽŶŽĨƚŚĞWŽƚĞŶƚŝĂůŶĞƌŐǇ&ƵŶĐƚŝŽŶŽĨƚŚĞ ŽƉƉĞƌŝŵĞƌ'ƌŽƵŶĚ^ƚĂƚĞ ϭϲ͗ϮϬ ,ĂŝƐƵŚĂŶŐ͕hŶŝǀĞƌƐŝƚĠĚĞŽƵƌŐŽŐŶĞ&ƌĂŶĐŚĞŽŵƚĠ ZŽƚĂƚŝŽŶĂůĞĐŚŽĞƐ͗ĂǀĞƌƐĂƚŝůĞƚŽŽůĨŽƌŝŶǀĞƐƚŝŐĂƚŝŶŐƵůƚƌĂĨĂƐƚĚŝƐƐŝƉĂƚŝŽŶ ϭϲ͗ϰϬ /ƌǇŶĂ'ŽǌŚǇŬ͕hDZϭϮϱEZ^ͬ^ĂŝŶƚͲ'ŽďĂŝŶ ŽƌƌĞĐƚŝŽŶŽĨƉůĂƐŵĂĞŵŝƐƐŝŽŶŝŶƌĞĨůĞĐƚŝǀŝƚǇƐƉĞĐƚƌŽƐĐŽƉǇĚƵƌŝŶŐ ƐƉƵƚƚĞƌŝŶŐĚĞƉŽƐŝƚŝŽŶ ϭϳ͗ϯϬ ZŽƵĞŶƉĞĚĞƐƚƌŝĂŶŐƵŝĚĞĚƚŽƵƌ ϭϵ͗ϬϬ ŽŶĨĞƌĞŶĐĞĚŝŶŶĞƌŝŶΗ>ĂŚĂůůĞĂƵǆƚŽŝůĞƐΗŽĨZŽƵĞŶ . . . . .

(12) tĞĚŶĞƐĚĂǇƉƌŝůϭϬƚŚ͕ϮϬϭϵ͘ ϵ͗ϬϬ /ŶǀŝƚĞĚƐƉĞĂŬĞƌ ĂƚĞƌŝŶĂDĞƌůĂ͕EZŽŵĂ tŝĚĞĨŝĞůĚZ^ŵŝĐƌŽƐƉĞĐƚƌŽƐĐŽƉǇĂŶĚƌĞĂůͲƚŝŵĞĨŽůůŽǁͲƵƉŽĨŚǇĚƌĂƚŝŽŶĐŚĂŶŐĞƐ ŝŶĚƵĐĞĚďǇĞůĞĐƚƌŽƉƵůƐĂƚŝŽŶŽĨůŝƉŽƐŽŵĞƐ ϵ͗ϰϬ >ƵŝƐDŝƌ͕EZ^sŝůůĞũƵŝĨ ŽŶĨŽĐĂůZĂŵĂŶDŝĐƌŽƐƉĞĐƚƌŽƐĐŽƉǇƚŽ/ŶǀĞƐƚŝŐĂƚĞƚŚĞŽŶƐĞƋƵĞŶĐĞƐŽĨƚŚĞĞůŝǀĞƌǇ ŽĨůĞĐƚƌŝĐWƵůƐĞƐƚŽ>ŝǀĞĞůůƐ ϭϬ͗ϬϬ sŝŬĂƐ<hDZ͕hŶŝǀĞƌƐŝƚǇŽĨƵŝƐďƵƌŐƐƐĞŶ dŝŵĞʹĂŶĚƉŽůĂƌŝǌĂƚŝŽŶͲƌĞƐŽůǀĞĚZ^ƐƉĞĐƚƌŽƐĐŽƉǇŽĨ ɲͲEW;ϮͲ;Ϯ͕ϰͲĚŝŶŝƚƌŽďĞŶǌǇůͿƉǇƌŝĚŝŶĞͿŝŶƚŚĞĞůĞĐƚƌŽŶŝĐŐƌŽƵŶĚƐƚĂƚĞ ϭϬ͗ϮϬ K&&Z< ϭϭ͗ϬϬ WŝĞƌƌĞ'ŝůůŝŽƚ͕WD^^ƚƌĂƐďŽƵƌŐ ^ƚƌƵĐƚƵƌĞĚŝůůƵŵŝŶĂƚŝŽŶĞǆƉĞƌŝŵĞŶƚƐǁŝƚŚǀŽƌƚĞǆďĞĂŵƐ ϭϭ͗ϮϬ dŚŽŵĂƐ'ŽĚŝŶ͕KZ/ZŽƵĞŶ WŚŽƚŽŶŝĐƚŝŵĞͲƐƚƌĞƚĐŚ͗ĂƉƉůŝĐĂƚŝŽŶƐƚŽƵůƚƌĂĨĂƐƚƐƉĞĐƚƌŽƐĐŽƉǇĂŶĚƌĞĂůͲƚŝŵĞŝŵĂŐŝŶŐ ϭϭ͗ϰϬ ůŽƐŝŶŐΘŝŶƚƌŽ͘ƚŽKEK^ϮϬϮϬ ϭϮ͗ϬϬ >hE, ϭϰ͗ϬϬ KZ/>ĂďƚŽƵƌ͕^ĂŝŶƚƚŝĞŶŶĞĚƵZŽƵǀƌĂǇ͕^ƵďƐĐƌŝƉƚŝŽŶŶĞĞĚĞĚ.

(13)

(14) . ^ŽĐŝĂůǀĞŶƚƐ ^ƵŶĚĂǇ͕ĂƉƌŝůϳƚŚĨƌŽŵϰƉŵͲtĞůĐŽŵĞƌĞĐĞƉƚŝŽŶŝŶƚŚĞƚŽƵƌŝƐƚŽĨĨŝĐĞ;ŝŶĨƌŽŶƚŽĨ ƚŚĞĐĂƚŚĞĚƌĂůͿ. ^ĞƚƚůĞĚŝŶƚŚŝƐZĞŶĂŝƐƐĂŶĐĞŵĂŶƐŝŽŶ͕ĨƌŽŵ&ĞďƌƵĂƌǇƚŽŵŝĚͲƉƌŝůϭϴϵϮĂŶĚϭϴϵϯŝƚǁĂƐŚĞƌĞ ƚŚĂƚůĂƵĚĞDŽŶĞƚƉĂŝŶƚĞĚŚŝƐĨĂŵŽƵƐƐĞƌŝĞƐŽĨƚŚŝƌƚǇƉĂŝŶƚŝŶŐƐŽĨƚŚĞǁĞƐƚĞƌŶĨĂĐĂĚĞŽĨ EŽƚƌĞĂŵĞĂƚŚĞĚƌĂů͘ůĂƵĚĞDŽŶĞƚ͛ƐƐƚƵĚŝŽ͕ĂƉƌĞƐƚŝŐŝŽƵƐƌŽŽŵĂƚƚŚĞŚĞĂƌƚŽĨZŽƵĞŶ͙. ϳƉŵ͗ĂƌŝůůŽŶĐŽŶĐĞƌƚŽĨƚŚĞĐĂƚŚĞĚƌĂů. .

(15) DŽŶĚĂǇ͕ĂƉƌŝůϴƚŚ͕ϲ͗ϯϬƉŵ ŽĐŬƚĂŝůŝŶƚŚĞ͞:ĞĂŶŶĞĚ͛ƌĐŚŝƐƚŽƌŝĂů͟. . dƵĞƐĚĂǇ͕ĂƉƌŝůϵƚŚ ϱ͗ϯϬƉŵ͗ZŽƵĞŶŐƵŝĚĞĚƚŽƵƌ. ϳ͗ϬϬƉŵ͗KEK^ŝŶŶĞƌŝŶƚŚĞ͞,ĂůůĞĂƵǆƚŽŝůĞƐ͟ŽĨZŽƵĞŶ͘. .

(16)

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(140) Broadband Stimulated Raman Scattering Microscopy with In-Line Balanced-Detection Alejandro De la Cadena, Andrea Ragni, Giuseppe Sciortino, Giorgio Ferrari, Marco Sampietro, Giulio Cerullo and Dario Polli Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milano (Italy). Stimulated Raman scattering (SRS) is an increasingly employed technique in optical nonlinear microscopy, as it is capable of identifying different chemical species and their concentration in a sample. It exploits the third-order nonlinear optical response of the specimen to ultrashort pump and Stokes pulses, by setting up and detecting a vibrational coherence within the ensemble of molecules inside the laser focus. In its broadband modality, SRS excites a manifold of molecular vibrational bands, thus providing more information about the chemical composition of the sample compared to the narrowband version. It therefore opens up the possibility to discriminate chemical species with overlapping Raman signatures. We report here on an innovative broadband SRS setup capable of high-speed imaging in the C-H stretching region (2800-3050 cm-1). It is based on a homemade optical parametric oscillator at 80-MHz repetition rate [1]. It delivers broadband pump pulses in the 780-810 QPUHJLRQDQGQDUURZEDQG §FP-1) Stokes pulses at 1040-nm, PRGXODWHGDW§0+]IUHTXHQF\LQRUGHUWRGHWHFWWKHVWLPXODWHG5DPDQORVV 65/

(141) RIWKHSXPS. To increase the signal-to-noise ratio, which is typically limited by the relative intensity noise fluctuations of the laser source, we take advantage of the in-line balanced detection scheme [2] (see Fig. 1(a)). A birefringent plate is placed before the sample in the broadband pump branch, to generate two replicas with orthogonal polarization, one serving as the pump pulse for SRS and the second as a reference for balancing purposes. Both replicas interact with the sample, although only one temporally coincides with the narrowband Stokes beam DQGXQGHUJRHV65/. In this way, the reference pulse experiences the same local attenuation, due to spatially varying sample transmission, but it does not bear any modulation transfer due to SRS. After the sample, a spectral filter rejects the Stokes while the pump/reference pulses are dispersed with a transmissiRQ JUDWLQJ LQ /LWWURZ FRQILJXUDWLRQ, separated with a polarizing beam splitter and sent to different photodiodes for the pump and the reference beams. Their intensities are electronically subtracted before demodulation, thus reaching close to shot-noise-limited detection. SRS detection can be performed in two modalities. In the first (IBD-G, see left inset of Fig. 1(a)), an off-theshelf balanced photodiode with two single-pixel detectors is employed, whose output is connected to a standard single-channel lock-in amplifier, employed at maximum speed (1.8-ȝV LQWHJUDWLRQ WLPH

(142) . Retrieval of the vibrational spectrum is performed by varying the detected pump wavelength after the sample by means of a singleaxis galvanometric scanning mirror. Figures 1(b-c) report imaging results on a test sample made of dispersed PMMA (6-ȝP GLDPHWHU VHH UHG VSKHUHV LQ SDQHO F

(143) DW 2956 cm-1) and polystyrene (3-ȝP GLDPHWHU VHH EOXH spheres in panel (d) at 3066 cm-1) beads. Panel (d) shows the image collected at 3005 cm-1, in which both specimens are visible due to overlapping vibrational features. Fig. 1(e) reports exemplary SRS spectra of PS and PMMA. In the second detection modality, a home-made multi-channel lock-in amplifier (M-/,$, see right inset of Fig. 1(a)) [3] is employed with 4 parallel channels and 10-ȝVLQWHJUDWLRQWLPH constant, thus allowing very fast SRS imaging at 4 distinct frequencies. In the future, the system will be upgraded to a 32-channel M-/,$. Fig. 1 (a) Scheme of the experimental set-up, showing the two possible detection schemes employing either a galvanometric scanner (IBD-G, on the left) or a multi-channel lock-in amplifier (M-/,$RQWKHULJKW

(144) (b-c-d) SRS imaging of PMMA and PS beads at 2956 (c), 3066 (d) and 3005 cm-1 (e) Raman shift. 6FDOHEDUȝP (e) Raman spectra of the two components. >1@ N. Coluccelli, D. Viola, V. Kumar, A. Perri, M. Marangoni, G. Cerullo, and D. Polli, “Tunable 30 fs light pulses at 1 W power level from a Yb-pumped optical parametric oscillator´2SW/HWW42, 4545 (2017). >2@ F. Crisafi, V. Kumar, T. Scopigno, M. Marangoni, G. Cerullo, and D. Polli, “In-line balanced detection stimulated Raman scattering microscopy”, Sci. Rep. 7, 10745 (2017). [3] A. Ragni, G. Sciortino, M. Sampietro, G. Ferrari, and D. Polli, “/RFN-In Based Differential Front-End for Raman Spectroscopy Applications”, 14th Conference on Ph.D. Research in Microelectronics and Electronics (PRIME) 1, 221–224 (2018)..

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