Control of retinal isomerization in bacteriorhodopsin in the high-intensity regime
A learning algorithm was used to manipulate optical pulse shapes and optimize retinal isomerization in bacteriorhodopsin, for excitation levels up to 1.8 x 10¹⁶ photons per square centimeter. Below 1/3 the maximum excitation level, the yield was not sensitive to pulse shape. Above this level the lea...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2009-07, Vol.106 (27), p.10896-10900 |
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| container_title | Proceedings of the National Academy of Sciences - PNAS |
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| creator | Florean, Andrei C Cardoza, David White, James L Lanyi, J.K Sension, Roseanne J Bucksbaum, Philip H |
| description | A learning algorithm was used to manipulate optical pulse shapes and optimize retinal isomerization in bacteriorhodopsin, for excitation levels up to 1.8 x 10¹⁶ photons per square centimeter. Below 1/3 the maximum excitation level, the yield was not sensitive to pulse shape. Above this level the learning algorithm found that a Fourier-transform-limited (TL) pulse maximized the 13-cis population. For this optimal pulse the yield increases linearly with intensity well beyond the saturation of the first excited state. To understand these results we performed systematic searches varying the chirp and energy of the pump pulses while monitoring the isomerization yield. The results are interpreted including the influence of 1-photon and multiphoton transitions. The population dynamics in each intermediate conformation and the final branching ratio between the all-trans and 13-cis isomers are modified by changes in the pulse energy and duration. |
| doi_str_mv | 10.1073/pnas.0904589106 |
| format | Article |
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Below 1/3 the maximum excitation level, the yield was not sensitive to pulse shape. Above this level the learning algorithm found that a Fourier-transform-limited (TL) pulse maximized the 13-cis population. For this optimal pulse the yield increases linearly with intensity well beyond the saturation of the first excited state. To understand these results we performed systematic searches varying the chirp and energy of the pump pulses while monitoring the isomerization yield. The results are interpreted including the influence of 1-photon and multiphoton transitions. 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Below 1/3 the maximum excitation level, the yield was not sensitive to pulse shape. Above this level the learning algorithm found that a Fourier-transform-limited (TL) pulse maximized the 13-cis population. For this optimal pulse the yield increases linearly with intensity well beyond the saturation of the first excited state. To understand these results we performed systematic searches varying the chirp and energy of the pump pulses while monitoring the isomerization yield. The results are interpreted including the influence of 1-photon and multiphoton transitions. The population dynamics in each intermediate conformation and the final branching ratio between the all-trans and 13-cis isomers are modified by changes in the pulse energy and duration.</description><subject>Absorption</subject><subject>Absorption spectra</subject><subject>Algorithms</subject><subject>Atoms & subatomic particles</subject><subject>Bacteria</subject><subject>Bacteriorhodopsins</subject><subject>Bacteriorhodopsins - chemistry</subject><subject>Biological Sciences</subject><subject>Chirp</subject><subject>Fourier transforms</subject><subject>Halobacterium salinarum - chemistry</subject><subject>Isomerism</subject><subject>Isomerization</subject><subject>Light</subject><subject>Molecules</subject><subject>Photons</subject><subject>Physical Sciences</subject><subject>Pumps</subject><subject>Retina</subject><subject>Retinaldehyde - chemistry</subject><subject>Spectrum Analysis</subject><subject>Stimulated emission</subject><subject>Wave excitation</subject><subject>Wavelengths</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2009</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFkU1PGzEQhi1UVALtmRN0xa2HhfHHeu0LUhXRFgkJCcrZcnbtrKPNOrWdivTX10siQk-cRpp55p13ZhA6xXCJoaZXq0HHS5DAKiEx8AM0wSBxyZmED2gCQOpSMMKO0HGMCwCQlYCP6AjLijMOYoIepn5IwfeFt0UwyQ26L1z0SxPcX52cHwo3FDPdpJzwofOtX0X3kkydKTo370o3JDNElzZZYO6W5hM6tLqP5vMunqCn7ze_pj_Lu_sft9Nvd2WTzaZS1IKIBlMrGwoto9yStmWmopZrKaTFtGLWsFYYzjEmtWUCDGBKpeVkpmf0BF1vdVfr2dK0jcmL6F6tglvqsFFeO_V_ZXCdmvs_itQgal5lgYudQPC_1yYmtfDrkC8QFQHMCKUwQldbqAk-xmDs6wAMavyBGn-g9j_IHedvfe353dEz8HUHjJ17OZ6d5SAkV3bd98k8p8wW77AZOdsii5h8eGUYMEFrPI77sq1b7ZWeBxfV02NekALORwBe03_Y4K9z</recordid><startdate>20090707</startdate><enddate>20090707</enddate><creator>Florean, Andrei C</creator><creator>Cardoza, David</creator><creator>White, James L</creator><creator>Lanyi, J.K</creator><creator>Sension, Roseanne J</creator><creator>Bucksbaum, Philip H</creator><general>National Academy of Sciences</general><general>National Acad Sciences</general><scope>FBQ</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QR</scope><scope>7SN</scope><scope>7SS</scope><scope>7T5</scope><scope>7TK</scope><scope>7TM</scope><scope>7TO</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>5PM</scope></search><sort><creationdate>20090707</creationdate><title>Control of retinal isomerization in bacteriorhodopsin in the high-intensity regime</title><author>Florean, Andrei C ; 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| subjects | Absorption Absorption spectra Algorithms Atoms & subatomic particles Bacteria Bacteriorhodopsins Bacteriorhodopsins - chemistry Biological Sciences Chirp Fourier transforms Halobacterium salinarum - chemistry Isomerism Isomerization Light Molecules Photons Physical Sciences Pumps Retina Retinaldehyde - chemistry Spectrum Analysis Stimulated emission Wave excitation Wavelengths |
| title | Control of retinal isomerization in bacteriorhodopsin in the high-intensity regime |
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