Slow Cooling of High‐Energy C Excitons Is Limited by Intervalley‐Transfer in Monolayer MoS2

High‐energy C exciton in 2D transition metal dichalcogenides with strong photon absorption can be utilized prospectively in light‐harvesting and opto‐electric devices. Here, a detailed study on C exciton dynamics in monolayer MoS2 is presented by femtosecond transient absorption (TA) spectroscopy. I...

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Published in:Laser & photonics reviews 2019-04, Vol.13 (4), p.n/a
Main Authors: Li, Yuanzheng, Shi, Jia, Chen, Heyu, Mi, Yang, Du, Wenna, Sui, Xinyu, Jiang, Chuanxiu, Liu, Weizhen, Xu, Haiyang, Liu, Xinfeng
Format: Article
Language:English
Subjects:
C excitons
Cooling
Cooling rate
Electric devices
Excitons
Fluence
intervalley transfer
Molybdenum disulfide
Monolayers
MoS2
Photon absorption
Spectroscopy
Spectrum analysis
Temperature
transient absorption
Transition metal compounds
ultrafast cooling
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creator Li, Yuanzheng
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Chen, Heyu
Mi, Yang
Du, Wenna
Sui, Xinyu
Jiang, Chuanxiu
Liu, Weizhen
Xu, Haiyang
Liu, Xinfeng
description High‐energy C exciton in 2D transition metal dichalcogenides with strong photon absorption can be utilized prospectively in light‐harvesting and opto‐electric devices. Here, a detailed study on C exciton dynamics in monolayer MoS2 is presented by femtosecond transient absorption (TA) spectroscopy. In the experiment, the C exciton with unique parallel band structure exhibits a slow process within tens of picoseconds (≈10–50 ps) as well as a fast process within several picoseconds (≈1–6 ps) instead of previous reported ultrafast cooling (
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Here, a detailed study on C exciton dynamics in monolayer MoS2 is presented by femtosecond transient absorption (TA) spectroscopy. In the experiment, the C exciton with unique parallel band structure exhibits a slow process within tens of picoseconds (≈10–50 ps) as well as a fast process within several picoseconds (≈1–6 ps) instead of previous reported ultrafast cooling (&lt;500 fs) process. From TA spectroscopy, the experimental results confirmed that the relatively slow cooling of C exciton is mainly limited by the rates of intervalley transfer rather than Pauli blocking effect from band‐edge excitons. The timescale of intervalley transfer is longer than that of intraband relaxation of C exciton, therefore, leading to the slow cooling of C exciton. Moreover, intervalley transfer time are estimated with two processes of 5.1 ± 0.6 ps and 69.5 ± 8 ps when the pump fluence is ≈127 µJ cm−2. This work provides further understanding of the ultrafast dynamics of C exciton in monolayer MoS2 and opens new opportunities for opto‐electric related applications. Developing an insight into C exciton dynamics is important to effectively collect these high‐energy hot carriers in two‐dimensional transition metal dichalcogenides. Herein, the C exciton exhibits a slow cooling instead of a previous reported sub‐picosecond timescale. 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Here, a detailed study on C exciton dynamics in monolayer MoS2 is presented by femtosecond transient absorption (TA) spectroscopy. In the experiment, the C exciton with unique parallel band structure exhibits a slow process within tens of picoseconds (≈10–50 ps) as well as a fast process within several picoseconds (≈1–6 ps) instead of previous reported ultrafast cooling (&lt;500 fs) process. From TA spectroscopy, the experimental results confirmed that the relatively slow cooling of C exciton is mainly limited by the rates of intervalley transfer rather than Pauli blocking effect from band‐edge excitons. The timescale of intervalley transfer is longer than that of intraband relaxation of C exciton, therefore, leading to the slow cooling of C exciton. Moreover, intervalley transfer time are estimated with two processes of 5.1 ± 0.6 ps and 69.5 ± 8 ps when the pump fluence is ≈127 µJ cm−2. This work provides further understanding of the ultrafast dynamics of C exciton in monolayer MoS2 and opens new opportunities for opto‐electric related applications. Developing an insight into C exciton dynamics is important to effectively collect these high‐energy hot carriers in two‐dimensional transition metal dichalcogenides. Herein, the C exciton exhibits a slow cooling instead of a previous reported sub‐picosecond timescale. The experimental results based on transient absorption measurements confirm that the slow cooling of C exciton is mainly caused by intervalley transfer.</description><subject>C excitons</subject><subject>Cooling</subject><subject>Cooling rate</subject><subject>Electric devices</subject><subject>Excitons</subject><subject>Fluence</subject><subject>intervalley transfer</subject><subject>Molybdenum disulfide</subject><subject>Monolayers</subject><subject>MoS2</subject><subject>Photon absorption</subject><subject>Spectroscopy</subject><subject>Spectrum analysis</subject><subject>Temperature</subject><subject>transient absorption</subject><subject>Transition metal compounds</subject><subject>ultrafast cooling</subject><issn>1863-8880</issn><issn>1863-8899</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNo9kE1OwzAQhS0EEqWwZW2JdWDsNLGzRFGhlVIV0bK27NQprlI7OCklO47AGTkJroo6mzef9OZHD6FbAvcEgD7UjfP3FAgPwOAMDQhP44jzLDs_9Rwu0VXbbgCSUOkAiUXt9jh3rjZ2jV2FJ2b9_vv9M7bar3uc4_FXaTpnWzxtcWG2ptMrrHo8tZ32n7KudR_cSy9tW2mPjcUzZ10t-wAzt6DX6KKSdatv_nWI3p7Gy3wSFfPnaf5YRA1JY4hWFaOgV5pCmSQxU0mZUuCg1CgBmQFjo6wCpgjTDKjSmgeVOlFlRUgYrOIhujvubbz72Om2Exu38zacFJTCiKU8AQiu7Ojam_C4aLzZSt8LAuKQoDgkKE4JiuJl_nqi-A_6EmjG</recordid><startdate>201904</startdate><enddate>201904</enddate><creator>Li, Yuanzheng</creator><creator>Shi, Jia</creator><creator>Chen, Heyu</creator><creator>Mi, Yang</creator><creator>Du, Wenna</creator><creator>Sui, Xinyu</creator><creator>Jiang, Chuanxiu</creator><creator>Liu, Weizhen</creator><creator>Xu, Haiyang</creator><creator>Liu, Xinfeng</creator><general>Wiley Subscription Services, Inc</general><scope>7SP</scope><scope>7U5</scope><scope>8FD</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0002-7662-7171</orcidid></search><sort><creationdate>201904</creationdate><title>Slow Cooling of High‐Energy C Excitons Is Limited by Intervalley‐Transfer in Monolayer MoS2</title><author>Li, Yuanzheng ; Shi, Jia ; Chen, Heyu ; Mi, Yang ; Du, Wenna ; Sui, Xinyu ; Jiang, Chuanxiu ; Liu, Weizhen ; Xu, Haiyang ; Liu, Xinfeng</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p1630-df720ede20c5537b5c62080bb450a907749f07b17e702bee8e70ae5bcf1120ef3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>C excitons</topic><topic>Cooling</topic><topic>Cooling rate</topic><topic>Electric devices</topic><topic>Excitons</topic><topic>Fluence</topic><topic>intervalley transfer</topic><topic>Molybdenum disulfide</topic><topic>Monolayers</topic><topic>MoS2</topic><topic>Photon absorption</topic><topic>Spectroscopy</topic><topic>Spectrum analysis</topic><topic>Temperature</topic><topic>transient absorption</topic><topic>Transition metal compounds</topic><topic>ultrafast cooling</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Yuanzheng</creatorcontrib><creatorcontrib>Shi, Jia</creatorcontrib><creatorcontrib>Chen, Heyu</creatorcontrib><creatorcontrib>Mi, Yang</creatorcontrib><creatorcontrib>Du, Wenna</creatorcontrib><creatorcontrib>Sui, Xinyu</creatorcontrib><creatorcontrib>Jiang, Chuanxiu</creatorcontrib><creatorcontrib>Liu, Weizhen</creatorcontrib><creatorcontrib>Xu, Haiyang</creatorcontrib><creatorcontrib>Liu, Xinfeng</creatorcontrib><collection>Electronics &amp; Communications Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Laser &amp; photonics reviews</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Yuanzheng</au><au>Shi, Jia</au><au>Chen, Heyu</au><au>Mi, Yang</au><au>Du, Wenna</au><au>Sui, Xinyu</au><au>Jiang, Chuanxiu</au><au>Liu, Weizhen</au><au>Xu, Haiyang</au><au>Liu, Xinfeng</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Slow Cooling of High‐Energy C Excitons Is Limited by Intervalley‐Transfer in Monolayer MoS2</atitle><jtitle>Laser &amp; photonics reviews</jtitle><date>2019-04</date><risdate>2019</risdate><volume>13</volume><issue>4</issue><epage>n/a</epage><issn>1863-8880</issn><eissn>1863-8899</eissn><abstract>High‐energy C exciton in 2D transition metal dichalcogenides with strong photon absorption can be utilized prospectively in light‐harvesting and opto‐electric devices. 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This work provides further understanding of the ultrafast dynamics of C exciton in monolayer MoS2 and opens new opportunities for opto‐electric related applications. Developing an insight into C exciton dynamics is important to effectively collect these high‐energy hot carriers in two‐dimensional transition metal dichalcogenides. Herein, the C exciton exhibits a slow cooling instead of a previous reported sub‐picosecond timescale. The experimental results based on transient absorption measurements confirm that the slow cooling of C exciton is mainly caused by intervalley transfer.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/lpor.201800270</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0002-7662-7171</orcidid></addata></record>
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subjects C excitons
Cooling
Cooling rate
Electric devices
Excitons
Fluence
intervalley transfer
Molybdenum disulfide
Monolayers
MoS2
Photon absorption
Spectroscopy
Spectrum analysis
Temperature
transient absorption
Transition metal compounds
ultrafast cooling
title Slow Cooling of High‐Energy C Excitons Is Limited by Intervalley‐Transfer in Monolayer MoS2
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