Approaching the intrinsic exciton physics limit in two-dimensional semiconductor diodes
Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality 1 – 5 . Despite considerable efforts, a disconnect persists between the fu...
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| Published in | Nature (London) Vol. 599; no. 7885; pp. 404 - 410 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
18.11.2021
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality
1
–
5
. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor–contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley–Read–Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton–charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton–charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices.
Two-dimensional transition metal dichalcogenide diodes with defect-free van der Waals contacts allows minimization of the extrinsic interfacial disorder-dominated recombination and access to the intrinsic excitonic behaviour in two-dimensional semiconductor devices. |
|---|---|
| AbstractList | Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality.sup.1-5. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality.sup.1-5. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. Two-dimensional transition metal dichalcogenide diodes with defect-free van der Waals contacts allows minimization of the extrinsic interfacial disorder-dominated recombination and access to the intrinsic excitonic behaviour in two-dimensional semiconductor devices. Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality 1 – 5 . Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor–contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley–Read–Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton–charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton–charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. Two-dimensional transition metal dichalcogenide diodes with defect-free van der Waals contacts allows minimization of the extrinsic interfacial disorder-dominated recombination and access to the intrinsic excitonic behaviour in two-dimensional semiconductor devices. Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality . Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality1-5. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices.Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality1-5. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and strong gate tunability, which arise from their reduced dimensionality1-5. Despite considerable efforts, a disconnect persists between the fundamental photophysics in pristine 2D semiconductors and the practical device performances, which are often plagued by many extrinsic factors, including chemical disorder at the semiconductor-contact interface. Here, by using van der Waals contacts with minimal interfacial disorder, we suppress contact-induced Shockley-Read-Hall recombination and realize nearly intrinsic photophysics-dictated device performance in 2D semiconductor diodes. Using an electrostatic field in a split-gate geometry to independently modulate electron and hole doping in tungsten diselenide diodes, we discover an unusual peak in the short-circuit photocurrent at low charge densities. Time-resolved photoluminescence reveals a substantial decrease of the exciton lifetime from around 800 picoseconds in the charge-neutral regime to around 50 picoseconds at high doping densities owing to increased exciton-charge Auger recombination. Taken together, we show that an exciton-diffusion-limited model well explains the charge-density-dependent short-circuit photocurrent, a result further confirmed by scanning photocurrent microscopy. We thus demonstrate the fundamental role of exciton diffusion and two-body exciton-charge Auger recombination in 2D devices and highlight that the intrinsic photophysics of 2D semiconductors can be used to create more efficient optoelectronic devices. |
| Audience | Academic |
| Author | Lee, Sung-Joon Lin, Zhaoyang Caram, Justin R. Atallah, Timothy L. Wang, Peiqi Duan, Xiangfeng Ping, Yuan Chen, Peng Huang, Zhihong Huang, Yu Duan, Xidong Xu, Junqing |
| Author_xml | – sequence: 1 givenname: Peng orcidid: 0000-0001-8527-1210 surname: Chen fullname: Chen, Peng organization: Department of Chemistry and Biochemistry, University of California, Los Angeles – sequence: 2 givenname: Timothy L. surname: Atallah fullname: Atallah, Timothy L. organization: Department of Chemistry and Biochemistry, University of California, Los Angeles – sequence: 3 givenname: Zhaoyang orcidid: 0000-0002-6474-7184 surname: Lin fullname: Lin, Zhaoyang organization: Department of Chemistry and Biochemistry, University of California, Los Angeles – sequence: 4 givenname: Peiqi surname: Wang fullname: Wang, Peiqi organization: Department of Chemistry and Biochemistry, University of California, Los Angeles – sequence: 5 givenname: Sung-Joon surname: Lee fullname: Lee, Sung-Joon organization: Department of Materials Science and Engineering, University of California, Los Angeles – sequence: 6 givenname: Junqing surname: Xu fullname: Xu, Junqing organization: Department of Chemistry and Biochemistry, University of California Santa Cruz – sequence: 7 givenname: Zhihong orcidid: 0000-0002-5927-5995 surname: Huang fullname: Huang, Zhihong organization: Department of Materials Science and Engineering, University of California, Los Angeles – sequence: 8 givenname: Xidong orcidid: 0000-0002-4951-901X surname: Duan fullname: Duan, Xidong organization: State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University – sequence: 9 givenname: Yuan surname: Ping fullname: Ping, Yuan organization: Department of Chemistry and Biochemistry, University of California Santa Cruz – sequence: 10 givenname: Yu orcidid: 0000-0003-1793-0741 surname: Huang fullname: Huang, Yu organization: Department of Materials Science and Engineering, University of California, Los Angeles, California NanoSystems Institute, University of California, Los Angeles – sequence: 11 givenname: Justin R. orcidid: 0000-0001-5126-3829 surname: Caram fullname: Caram, Justin R. email: xduan@chem.ucla.edu organization: Department of Chemistry and Biochemistry, University of California, Los Angeles, California NanoSystems Institute, University of California, Los Angeles – sequence: 12 givenname: Xiangfeng orcidid: 0000-0002-4321-6288 surname: Duan fullname: Duan, Xiangfeng email: jcaram@chem.ucla.edu organization: Department of Chemistry and Biochemistry, University of California, Los Angeles, California NanoSystems Institute, University of California, Los Angeles |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/34789906$$D View this record in MEDLINE/PubMed |
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| ContentType | Journal Article |
| Copyright | The Author(s), under exclusive licence to Springer Nature Limited 2021 2021. The Author(s), under exclusive licence to Springer Nature Limited. COPYRIGHT 2021 Nature Publishing Group Copyright Nature Publishing Group Nov 18, 2021 |
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| DOI | 10.1038/s41586-021-03949-7 |
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| Snippet | Two-dimensional (2D) semiconductors have attracted intense interest for their unique photophysical properties, including large exciton binding energies and... |
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| SubjectTerms | 140/125 142/126 639/766/1130/2799 639/925/357/1018 639/925/927/1007 Augers Charge density Diffusion Diodes Diodes, Semiconductor Doping Electric fields Electrostatic properties Exciton theory Excitons Humanities and Social Sciences Interfaces multidisciplinary Optical properties Optoelectronic devices Photoelectric effect Photoelectric emission Photoluminescence Photons Recombination Science Science (multidisciplinary) Semiconductor diodes Semiconductors Short circuits Tungsten |
| Title | Approaching the intrinsic exciton physics limit in two-dimensional semiconductor diodes |
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