On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection

Yunxuan Zhu; Sai C. Yelishala; Shusen Liao; Jackson Shropshire; Douglas Natelson; Longji Cui

doi:10.1038/s41377-025-02030-6

Your Location：

Home >

Browse articles >

On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection

Original Articles

- On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection
- On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection
- Light: Science & Applications 2025年14卷第11期页码：3506-3516
- Affiliations：
  
  1.Paul M. Rady Department of Mechanical Engineering, University of Colorado Boulder, Boulder, CO, USA
  2.Department of Physics and Astronomy, Rice University, Houston, TX, USA
  3.Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, CO, USA
  4.Department of Electrical and Computer Engineering, Rice University, Houston, TX, USA
  5.Department of Materials Science and Nanoengineering, Rice University, Houston, TX, USA
  6.Materials Science and Engineering Program and Center for Experiments on Quantum Materials, University of Colorado Boulder, Boulder, CO, USA
- Author bio：
  
  Yunxuan Zhu (yunxuan.zhu@colorado.edu)
  Douglas Natelson (natelson@rice.edu)
  Longji Cui (longji.cui@colorado.edu)
- Funds：
- DOI：10.1038/s41377-025-02030-6
  中图分类号：
- 收稿：2025-04-11，
  
  修回：2025-08-15，
  
  录用：2025-08-31，
  
  网络出版：2025-09-16，
  
  纸质出版：2025-11-30
- Accepted：
Scan QR Code
Yunxuan Zhu, Sai C. Yelishala, Shusen Liao, 等. On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection[J]. Light: Science & Applications, 2025,14(11):3506-3516.

Zhu, Y. X. et al. On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection. Light: Science & Applications, 14, 3506-3516 (2025).
Yunxuan Zhu, Sai C. Yelishala, Shusen Liao, 等. On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection[J]. Light: Science & Applications, 2025,14(11):3506-3516. DOI： 10.1038/s41377-025-02030-6.

Zhu, Y. X. et al. On-chip single-crystal plasmonic optoelectronics for efficient hot carrier collection and photovoltage detection. Light: Science & Applications, 14, 3506-3516 (2025). DOI： 10.1038/s41377-025-02030-6.

摘要

Abstract

Large-area chemically synthesized single-crystal metals with nanometer-scale thickness have emerged as promising materials for on-chip nanophotonic applications

owing to their superior plasmonic properties compared to nanofabricated polycrystalline counterparts. While much recent attention has focused on their optical properties

the combined optimal electrical and optical characteristics

which hold great potential for high-performance optoelectronic functionalities

remain largely unexplored. Here

we present a single-crystal plasmonic optoelectronic platform based on nanowires fabricated from synthesized gold flakes and demonstrate its capabilities for highly enhanced hot carrier collection

electroluminescence

and photovoltage detection. Notably

single-crystal gold nanogap devices exhibit an order of magnitude higher open-circuit photovoltage compared to polycrystalline devices

representing one of the highest reported photovoltage sensing performances in terms of on-chip device density and responsivity per area. Our analysis revealed that this enhancement is attributed mostly to the suppression of electron-phonon scattering and improved hot carrier tunneling efficiency in single-crystal devices. These results highlight the potential of large-scale single-crystal nanostructures for both fundamental studies of nanoscale hot carrier transport and scalable electrically driven nanophotonic applications.

关键词

Keywords

references

Zhu, Y. X. et al. Molecular scale nanophotonics: hot carriers, strong coupling, and electrically driven plasmonic processes. Nanophotonics 13 , 2281–2322 (2024)..

Brongersma, M. L., Halas, N. J. & Nordlander, P. Plasmon-induced hot carrier science and technology. Nat. Nanotechnol. 10 , 25–34 (2015)..

Anker, J. N. et al. Biosensing with plasmonic nanosensors. Nat. Mater. 7 , 442–453 (2008)..

Mejía-Salazar, J. R. & Oliveira, O. N. Plasmonic biosensing. Chem. Rev. 118 , 10617–10625 (2018)..

Lee, C. et al. Q uantum plasmonic sensors. Chem. Rev. 121 , 4743–4804 (2021)..

Cortés, E. et al. Experimental characterization techniques for plasmon-assisted chemistry. Nat. Rev. Chem. 6 , 259–274 (2022)..

Lin, J. S. et al. Advanced plasmonic technologies for multi-scale biomedical imaging. Chem. Soc. Rev. 51 , 9445–9468 (2022)..

Wang, M. N. et al. Plasmonic phenomena in molecular junctions: principles and applications. Nat. Rev. Chem. 6 , 681–704 (2022)..

Sharifi, M. et al. Plasmonic gold nanoparticles, optical manipulation, imaging, drug delivery and therapy. J. Control. Release 311-312 , 170–189 (2019)..

Zhan, C. et al. From plasmon-enhanced molecular spectroscopy to plasmon-mediated chemical reactions. Nat. Rev. Chem. 2 , 216–230 (2018)..

Karabchevsky, A. et al. On-chip nanophotonics and future challenges. Nanophotonics 9 , 3733–3753 (2020)..

Liang, Y. et al. Plasmo nic nanolasers in on-chip light sources: prospects and challenges. ACS Nano 14 , 14375–14390 (2020)..

Niu, X. X. et al. Plasmon-induced transparency effect for ultracompact on-chip devices. Nanophotonics 8 , 1125–1149 (2019)..

Zhu, Y. X. et al. Electroluminescence as a probe of strong exciton-plasmon coupling in few-layer WSe 2 . Nano Lett. 24 , 525–532 (2024)..

Huang, J. S. et al. Atomically flat single-crystalline gold nanostructures for plasmonic nanocircuitry. Nat. Commun. 1 , 150 (2010)..

Méjard, R. et al. Advanced engineering of single-crystal gold nanoantennas. Opt. Mater. Express 7 , 1157–1168 (2017)..

Horák, M. et al. Comparative study of plasmonic antennas fabricated by electron beam and focused ion beam lithography. Sci. Rep. 8 , 9640 (2018)..

Kaltenecker, K. J. et al. Mono-crystalline gold platelets: a high-quality platform for surface plasmon polaritons. Nanophotonics 9 , 509–522 (2020)..

Frank, B. et al. Short-range surface plasmonics: localized electron emission dynamics from a 60-nm spot on an atomically flat single-crystalline gold surface. Sci. Adv. 3 , e1700721(2017)..

Spektor, G. et al. Revealing the subfemtosecond dynamics of orbital angular momentum in nanoplasmonic vortices. Science 355 , 1187–1191 (2017)..

Cuche, A. et al. Modal engineering of surface plasmons in apertured Au nanoprisms. Sci. Rep. 5 , 16635 (2015)..

Kejík, L. et al. Structural and optical properties of monocrystalline and polycrystalline gold plasmonic nanorods. Opt. Express 28 , 34960–34972 (2020)..

Staechelin, Y. U. et al. Size-dependent electron-phonon coupling in monocrystalline gold nanoparticles. ACS Photonics 8 , 752–757 (2021)..

Chow, T. H. et al. Gold nanobipyramids: an emerging and versatile type of plasmonic nanoparticles. Acc. Chem. Res. 52 , 2136–2146 (2019)..

Lee, Y. J. et al. Ultrasmooth, highly spherical monocrystalline gold particles for precision plasmonics. ACS Nano 7 , 11064–11070 (2013)..

Li, Z. H. et al. Synthesis of single-crystal gold nanosheets of large size in ionic liquids. J. Phys. Chem. B 109 , 14445–14448 (2005)..

Li, C. C. et al. Mass synthesis of large, single-crystal Au nanosheets based on a polyol process. Adv. Funct. Mater. 16 , 83–90 (2006)..

Ye, S. J. et al. Sub-nanometer thick gold nanosheets as highly efficient catalysts. Adv. Sci. 6 , 1900911 (2019)..

Krauss, E. et al. Controlled growth of high-aspect-ratio single-crystalline gold platelets. Cryst. Growth Des. 18 , 1297–1302 (2018)..

Pan, C. X. Y. et al. Large area single crystal gold of single-nanometer thickness for nanophotonics. Nat. Commun. 15 , 2840 (2024)..

Karaman, C. O. et al. Ultrafast hot-carrier dynamics in ultrathin monocrystalline gold. Nat. Commun. 15 , 703 (2024)..

Knittel, V. et al. Nonline ar photoluminescence spectrum of single gold nanostructures. ACS Nano 9 , 894–900 (2015)..

Li, Q. et al. A mono-cuboctahedral series of gold nanoclusters: photoluminescence origin, large enhancement, wide tunability, and structure-property correlation. J. Am. Chem. Soc. 141 , 5314–5325 (2019)..

Bowman, A. R. et al. Quantum-mechanical effects in photoluminescence from thin crystalline gold films. Light Sci. Appl. 13 , 91 (2024)..

Siampour, H. et al. Ultrabright single-photon emission from germanium-vacancy zero-phonon lines: deterministic emitter-waveguide interfacing at plasmonic hot spots. Nanophotonics 9 , 953–962 (2020)..

Kowalska, E. et al. Mono- and bi-metallic plasmonic photocatalysts for degradation of organic compounds under UV and visible light irradiation. Catal. Today 230 , 131–137 (2014)..

Wang, L. et al. Two-dimensional gold nanostructures with high activity for selective oxidation of carbon–hydrogen bonds. Nat. Commun. 6 , 6957 (2015)..

Kern, J. et al. Electrically driven optical antennas. Nat. Photonics 9 , 582–586 (2015)..

Teng, F. et al. Photoelectric detectors based on inorganic p-type semiconductor materials. Adv. Mater. 30 , 1706262 (2018)..

Shi, L. L. et al. Status and outlook of metal–inorganic semiconductor–metal photodetectors. Laser Photonics Rev. 15 , 2000401 (2021)..

Liang, F. X. et al. Near-infrared-light photodetectors based on one-dimensional inorganic semiconductor nanostructures. Adv. Opt. Mater. 5 , 1700081 (2017)..

Liu, R. et al.Band alignment engineering in two-dimensional transition metal dichalcogenide-based heterostructures for photodetectors. Small Struct. 2 , 2000136 (2021)..

Lu, X. W. et al. Progress of photodetectors based on the photothermoelectric effect. Adv. Mater. 31 , 1902044 (2019)..

Zwicker, H. R. Photoemissive detectors. in Optical and Infrared Detectors 2nd edn, (ed. Keyes, R. J.). (New York: Springer), 149-196 (1977).

Dorodnyy, A. et al. Plasmonic photodetectors. IEEE J. Sel. Top. Quantum Electron. 24 , 4600313, https://doi.org/10.1109/JSTQE.2018.2840339 (2018)..

Zhu, Y. X., Cui, L. J. & Natelson, D. Hot-carrier enhanced light emission: the origin of above-threshold photons from electrically driven plasmonic tunnel junctions. J. Appl. Phys. 128 , 233105 (2020)..

Zhu, Y. X. et al. Tuning light emission crossovers in atomic-scale aluminum plasmonic tunnel junctions. Nano Lett. 22 , 8068–8075 (2022)..

Cui, L. J. et al. Thousand-fold increase in plasmonic light emission via combined electronic and optical excitations. Nano Lett. 21 , 2658–2665 (2021)..

Cui, L. J. et al. Electrically driven hot-carrier generation and above-threshold light emission in plasmonic tunnel junctions. Nano Lett. 20 , 6067–6075 (2020)..

Zolotavin, P., Evans, C. I. & Natelson, D. Substantial local variation of the Seebeck coefficient in gold nanowires. Nanoscale 9 , 9160–9166 (2017)..

Evans, C. I. et al. Thermoelectric response from grain boundaries and lattice d istortions in crystalline gold devices. Proc. Natl. Acad. Sci. USA 117 , 23350–23355 (2020)..

Zolotavin, P., Evans, C. & Natelson, D. Photothermoelectric effects and large photovoltages in plasmonic Au nanowires with nanogaps. J. Phys. Chem. Lett. 8 , 1739–1744 (2017)..

Natelson, D., Evans, C. I.&Zolotavin, P. Photovoltages and hot electrons in plasmonic nanogaps. Proceedings of SPIE 10540, Quantum Sensing and Nano Electronics and Photonics XV. San Francisco, California, USA: SPIE, 105400S (2018).

Herzog, J. B. et al. Dark plasmons in hot spot generation and polarization in interelectrode nanoscale junctions. Nano Lett. 13 , 1359–1364 (2013)..

Olmon, R. L. et al. Optical dielectric function of gold. Phys. Rev. B 86 , 235147 (2012)..

Jermyn, A. S. et al. Transport of hot carriers in plasmonic nanostructures. Phys. Rev. Mater. 3 , 075201 (2019)..

Lei, D. Y., Su, D. & Maier, S. A. New insights into plasmonic hot-electron dynamics. Light Sci. Appl. 13 , 243 (2024)..

Wang, J. Time-dependent quantum transport theory from non-equilibrium Green’s function approach. J. Comput. Electron. 12 , 343–355 (2013)..

Buret, M. et al. Spontaneous hot-electron light emission from electron-fed optical antennas. Nano Lett. 15 , 5811–5818 (2015)..

Huang, W. Y. et al. Effect of the lattice crystallinity on the electron-phonon relaxation rates in gold nanoparticles. J. Phys. Chem. C. 111 , 10751–10757 (2007)..

Guo, Z. R. et al. Facile synthesis of micrometer-sized gold nanoplates through an aniline-assisted route in ethylene glycol solution. Colloids Surf. A: Physicochem. Eng. Asp. 278 , 33–38 (2006)..

Dai, W. et al. Giant photothermoelectric effect in silicon nanoribbon photodetectors. Light Sci. Appl. 9 , 120 (2020)..

Desiatov, B. et al. Plasmonic enhanced silicon pyramids for internal photoemission Schottky detectors in the near-infrared regime. Optica 2 , 335–338 (2015)..

Wu, D. et al. Plasmo n-enhanced photothermoelectric conversion in chemical vapor deposited graphene p-n junctions. J. Am. Chem. Soc. 135 , 10926–10929 (2013)..

Chalabi, H., Schoen, D. & Brongersma, M. L. Hot-electron photodetection with a plasmonic nanostripe antenna. Nano Lett. 14 , 1374–1380 (2014)..

Briones, E. et al. Seebeck nanoantennas for the detection and characterization of infrared radiation. Opt. Express 22 , A1538–A1546 (2014)..

Mauser, K. W. et al. Resonant thermoelectric nanophotonics. Nat. Nanotechnol. 12 , 770–775 (2017)..

Groenendijk, D. J. et al. Photovoltaic and photothermoelectric effect in a double-gated WSe 2 device. Nano Lett. 14 , 5846–5852 (2014)..

Buscema, M. et al. Large and tunable photothermoelectric effect in single-layer MoS. Nano Lett. 13 (2), 358–363 (2013)..

Viti, L. et al. Thermoelectric terahertz photodetectors based on selenium-doped black phosphorus flakes. Nanoscale 11 , 1995–2002 (2019)..

Cai, X. et al. Sensitive room-temperature terahertz detection via the photothermoelectric effect in graphene. Nat. Nanotechnol. 9 , 814–819 (2014)..

Freitag, M., Low, T. & Avouris, P. Increased responsivity of suspended graphene photodetectors. Nano Lett. 13 , 1644–1648 (2013)..

Limpert, S. et al. Bipolar photothermoelectric effect across energy filters in single nanowires. Nano Lett. 17 , 4055–4060 (2017)..

Deborde, T. et al. Photothermoelectric effect in suspended semiconducting carbon nanotubes. ACS Nano 8 , 216–221 (2014)..

Szakmany, G. P. et al. Antenna-coupled nanowire thermocouples for infrared detection. IEEE Trans. Nanotechnol. 12 , 163–167 (2013)..

Szakmany, G. P. et al. Novel nanoscale single-metal polarization-sensitive infrared detectors. IEEE Trans. Nanotechnol. 14 , 379–383 (2015)..

Zhang, X. W. et al. Construction of ZnSe–ZnO axial p–n junctions via regioselective oxidation process and their photo-detection applications. Appl. Surf. Sci. 357 , 1939–1943 (2015)..

Bie, Y. Q. et al. Self-powered, ultrafast, visible-blind UV detection and optical logical operation based on ZnO/GaN nanoscale p-n junctions. Adv. Mater. 23 , 649–653 (2011)..

浏览量

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

暂无数据