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Half-wave nanolasers and intracellular plasmonic lasing particles

Nature Nanotechnology volume 20, pages 404–410 (2025)Cite this article

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Abstract

The ultimate limit for laser miniaturization would be achieving lasing action in the lowest-order cavity mode within a device volume of ≤(λ/2n)3, where λ is the free-space wavelength and n is the refractive index. Here we highlight the equivalence of localized surface plasmons and surface plasmon polaritons within resonant systems, introducing nanolasers that oscillate in the lowest-order localized surface plasmon or, equivalently, half-cycle surface plasmon polariton. These diffraction-limited single-mode emitters, ranging in size from 170 to 280 nm, harness strong coupling between gold and InxGa1−xAs1−yPy in the near-infrared (λ = 1,000–1,460 nm), away from the surface plasmon frequency. This configuration supports only the lowest-order dipolar mode within the semiconductor’s broad gain bandwidth. A quasi-continuous-level semiconductor laser model explains the lasing dynamics under optical pumping. In addition, we fabricate isolated gold-coated semiconductor discs and demonstrate higher-order lasing within live biological cells. These plasmonic nanolasers hold promise for multi-colour imaging and optical barcoding in cellular applications.

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Fig. 1: Strong coupling of plasmonic and semiconductor dipolar modes.
Fig. 2: Characteristics of semiconductor-on-gold nanodevices.
Fig. 3: A semiconductor laser ‘waterfall’ model.
Fig. 4: Dependence of lasing threshold and far-field emission on particle size.
Fig. 5: Plasmonic laser particles and intracellular lasing.

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Data availability

The laser experiment data used within this paper are available via the Harvard Dataverse at https://doi.org/10.7910/DVN/AOWZN8. Additional data that support the findings of this study are available from the corresponding author upon reasonable request.

Code availability

The code used for the semiconductor laser modelling and analysis of the laser experiment data is available via Code Ocean and the Harvard Dataverse at https://doi.org/10.7910/DVN/AOWZN8. The code associated with the FDTD calculations is available from the corresponding author upon reasonable request.

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Acknowledgements

K. Kim, Y. Wu and D. Sarkar are acknowledged for helpful discussions. This study was supported by National Institutes of Health research grants (R01-EB033155 and R01-EB034687). S.C. acknowledges the MGH Fund for Medical Discovery fundamental research fellowship award. This research used the resources of the Center for Nanoscale Systems, part of Harvard University, a member of the National Nanotechnology Coordinated Infrastructure, supported by the National Science Foundation under award number 1541959.

Author information

Authors and Affiliations

  1. Wellman Center for Photomedicine, Massachusetts General Hospital, Cambridge, MA, USA

    Sangyeon Cho, Nicola Martino & Seok-Hyun Yun

  2. Harvard Medical School, Boston, MA, USA

    Sangyeon Cho, Nicola Martino & Seok-Hyun Yun

  3. Harvard–MIT Health Sciences and Technology, Cambridge, MA, USA

    Seok-Hyun Yun

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  1. Sangyeon Cho
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  2. Nicola Martino
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Contributions

S.C. and S.-H.Y. designed the study. S.C. performed the experiments and FDTD simulations. N.M. contributed to the optical set-ups. S.-H.Y. conducted the semiconductor laser modelling. S.C. and S.-H.Y. analysed the data and wrote the paper.

Corresponding author

Correspondence to Seok-Hyun Yun.

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Competing interests

N.M. and S.-H.Y. have financial interests in LASE Innovation Inc., a company focused on commercializing technologies that are based on laser particles. The financial interests of N.M. and S.-H.Y. were reviewed and are managed by Mass General Brigham in accordance with their conflict-of-interest policies. S.C. declares no competing interests.

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Extended data

Extended Data Fig. 1 Mode properties of metal-semiconductor nanoparticles.

a-b, Mie scattering spectra of gold nano-spheres (a) and gold nano-discs (b) in air for planar incident waves. While the excitation of higher order modes is evident for spheres, only the fundamental electrical dipole mode clearly appears for discs owing to the symmetry; the higher modes in discs are not efficiently excited by the uniform driving field. In nano-lasers, however, higher-order plasmonic modes are driven by local emitters and can be efficiently excited via near-field interactions. c, Schematic depicting mode coupling between plasmonic and semiconductor disc modes for three representative cases: (i) Non-lasing metallic luminescence when a semiconductor disc is too thin. Because of the large differences of the modes in energy, mode coupling is weak, and the lowest order modes are largely plasmonic. Because of the mode proximity, it is difficult to selectively amplify only the ED mode; (ii) Higher-order hybrid laser, where multiple dielectric-like modes are present within a gain bandwidth; (iii) A hybrid dipole laser — which may be regarded a ‘spaser’ — where the individual modes in the metal and semiconductor discs have similar energies. Strong coupling occurs between ED modes, separating the hybrid plasmon-like mode from the other hybrid modes. This mode shift may be considered as the effect of the refractive index of the semiconductor on the plasmonic mode. However, mode coupling is a more accurate explanation as the effective index experienced by the plasmonic ED mode matches the index of the ED mode in the dielectric medium. Note that the MD modes, the lowest order modes in dielectric discs, are not efficiently coupled with the plasmonic ED mode because of the field symmetry. d, FDTD simulation of metal-semiconductor discs with different diameters, as depicted in the inset. The resonance wavelength, quality factor, and mode confinement factor in the semiconductor vary as a function of the diameter ratio from 0 (III-V only) to infinity (on a gold substrate). The resonance wavelength of the hybrid ED mode increases dramatically from 600 nm to 1300 nm at size matching and then 1220 nm for oversized gold. The quality factor reaches its maximum at a diameter ratio of 0.5, partly due to optimal mode energy matching and partly due to reduced metallic absorption at 800–900 nm. The Q factor approaches slightly over 10 at infinite gold, with a quarter of electromagnetic energy residing in the semiconductor while the remaining three quarters are stored in the metal. See Supplementary Fig. 2 for more examples of Mie scattering spectra. e, Simulated Mie scattering spectra of a complex of semiconductor (n = 3.5) and gold rhombus-like particles, each with a side length of 250 nm and heights of 130 nm and 100 nm, respectively, for various gap distances. The arrow indicates the lowest-order mode at contact. f, Electric field amplitude profiles of the semiconductor-gold particles in contact (dashed outline). g, Simulated Mie scattering spectra of a semiconductor on infinite substrates for different gap distances. The arrow indicates the lowest mode at contact. h, Electric field amplitude profiles of the semiconductor-on-gold structure. i, Simulated Mie scattering spectra of a rhombus-shaped semiconductor on an infinite substrate for different rhombus interior angles.

Extended Data Fig. 2 Size and thickness tuning of semiconductor particles.

a, SEM images of a semiconductor wafer after RIE, showing pillars with a diameter of 1.21 µm ± 45 nm. b, (Left) A high-resolution transmission electron micrograph (HRTEM) of a silica-coated microdisc; (Right) an electron diffraction (SAED) pattern from a selected area (dashed square). The zone axis is labeled as 001, and two lattice plane directions, 100 and 110, marked for clarity. c, Two-dimensional etching for reducing the diameters of InGaAsP layers while preserving their thickness using piranha acid solution. The InP layer remains the same size while InGaAsP is etched away. The bottom layer with a composition of In0.53Ga0.47As0.92P0.08 was primarily used in most experiments (unless specified). d, Three-dimensional etching of InGaAsP layers, performed after a full (typically) or partial (for this dataset) etching of InP layers between InGaAsP layers. This process reduces both the thickness and lateral sizes. The 2D and 3D etching techniques were judiciously used to obtain desired thicknesses and sizes for InGaAsP particles. e, SEM images of six particles obtained from a single batch targeting a thickness of 130 nm and a mean side length of 250 nm. This batch was used to produce the experimental data in Fig. 2c. The variation in size and shape was largely introduced during the size reduction process via wet etching. More uniform discs could be produced from reduced pillar diameters. f, SEM image of an isolated semiconductor nanodisc placed on top of a gold-coated substrate. The polycrystalline domains of the gold layer are visualized.

Extended Data Fig. 3 Half-wave dipolar lasers.

a, Schematic of a microscope setup used for optical characterizations. b, Measured lasing linewidth Q factors of 40 devices with different sizes and shapes. Representative spectra are displayed in Fig. 2c. c, Emission spectra of two devices at a room temperature of 298 K. d, Emission spectra of two devices at a Peltier cooled temperature of ~ 230 K (nominal). Compared to the room temperature spectra, the falling edges at the high energy side, or near the quasi-Fermi levels, are steeper, presumably due to slightly reduced thermal excitations at the lower temperature. Note that the simulated spectra exhibit ever steeper spectral falloff at the quasi-Fermi level (see Fig. 3b and Extended Data Fig. 6), because no thermal excitations have been considered in the model, which corresponds to zero-degree temperature (0 K). e, Output spectra through a polarizer at different angles. The stimulated emission peak at 0.94 eV (1321 nm) is linear polarized while the broad lower-energy background above the peak (0.75 to 0.9 eV) is approximately unpolarized.

Extended Data Fig. 4 Semiconductor gain and a ‘waterfall’ laser model.

a, Energy level diagram and various transitions paths in a semiconductor laser. This essentially forms a four-level laser system (or a quasi-three-level including valence band absorption of intracavity light). The blue shade represents free electrons (or the electron-hole plasma) that fill the electronic states in the conduction band. The simplified ‘waterfall’ model depicted in Fig. 3a is based on this diagram. b, Analysis of charge carrier loss due to Auger recombination for bulk (blue) and Purcell-enhanced (yellow) radiative decays. See Supplementary Note 2. c, Gain profiles at room temperature at three different carrier density levels, calculated using standard semiconductor theory considering the Fermi-Dirac distribution of the carriers at room temperature. Thermodynamic excitation was neglected in our numerical modeling, resulting a sharp gain cliff beyond the quasi-Fermi level. d, Calculated total carrier density versus transparency (zero-gain) wavelength. e, Simulated output spectra of a device with a size of 240 nm for the cases of different Purcell factors, from 1 to 30, as the pump fluence is varied from 0.021 to 2.1 mJ/cm2. The output saturates. The dashed curve illustrates the cold-cavity mode profile with a Q factor of 10. At \({F}_{p}=1\), the lasing threshold is never reached even at extreme pumping levels. At \({F}_{p}=10\), the lasing threshold is barely reached with a stimulated-to-spontaneous ratio of 1.07. Compared to \({F}_{p}=20\), \({F}_{p}=30\) results in reduced linewidths. Best correspondence to experimental data was obtained with \({F}_{p}=18\) (Device 1) and \({F}_{p}=19\) (Device 2). f, (Left) The emitter population and stimulated-to-spontaneous ratio at a threshold pump fluence, where the quasi-Fermi level is just below the modal resonant frequency. (Right) At a pump level 7.3 times above the threshold when all the entire excited states are almost filled.

Extended Data Fig. 5 Laser simulation and experimental results.

a, Half-wave device (semiconductor volume: 183 × 183 × 130 nm3). b, Half-wave device (225 × 225 × 130 nm3). c, One-wave device (400 × 400 × 130 nm3).

Extended Data Fig. 6 Higher-order mode devices.

a-b, Representative devices from different batches of varying sizes (same thickness of 290 nm) for plasmonic (a) and dielectric cavities (b). Dielectric devices with less than 880 nm sizes did not reach lasing threshold even at the highest pump power levels. c, Emission linewidths measured from six different size batches, with a total of 120 devices and 15 samples per batch. The threshold pump fluences of these devices are shown in Fig. 2. The box in the error bar represents the mean value, while the whiskers show the standard deviation. d, The ratio between the peak threshold powers for picosecond and nanosecond pumping of the devices batches, as shown in Fig. 2 and Extended Data Fig. 6c. Again, the box in the error bar represents the mean value, while the whiskers show the standard deviation. e, FDTD results of a 350-nm rhombus-shape showing a second order mode at 1206 nm (top) and a rectangular-shape 500-nm device showing a whispering gallery mode (Q = 94) at 1164 nm (bottom).

Extended Data Fig. 7 Temporal responses of picosecond-pumped devices.

a-e, Output intensity (left) and temporal (right) curves at varying pump powers from four representative devices: a, a pristine semiconductor wafer; b, a photonic microlaser with a diameter of approximately 2 µm placed on a glass substrate; c, a plasmonic nanodisc device with a diameter of approximately 350 nm on a gold substrate; and d-e, two different nanodisc devices with a diameter of approximately 230 nm on a gold substrate. Colors represent measurements at different pump powers. All laser devices exhibit kink behaviors indicative of the lasing threshold and accelerated lifetime. f, Superimposition of three representative temporal curves obtained from the devices in a, b, and d, above their respective lasing thresholds. The temporal profiles in the vicinity of the peak are nearly identical, indicating they are limited by the finite temporal resolution of the measurement instrument.

Extended Data Fig. 8 Structure of metal-semiconductor particles.

a, Schematic and SEM images of disc-on-pillar array following SiO2 coating and gold deposition. b, Bright-field and SEM images of plasmonic laser particles drop-cast onto a silica-coated silicon substrate, presenting both the III/V side (left) and the Au side (right). c, Transmission Electron Microscopy (TEM) image of a cross-section of a sample, prepared using focused ion-beam (FIB) etching. The image reveals the InGaAsP layer with a thickness of ~290 nm, 5–7 nm thick SiO2 layer, and ~ 80-nm thick gold layer. d, Higher magnification view of the cross section. e-f, Scanning transmission electron microscopy (STEM) images and elemental maps. The samples in c-f were prepared by placing the InGaAsP side on a silica-coated silicon substrate and depositing Ga on top of the Au side of the particles. The samples were then placed upside down on a TEM grid.

Extended Data Fig. 9 Emission spectra of isolated plasmonic LPs.

a, SEM image of a semiconductor particle after electron-beam gold deposition. The deposited gold layer appears noticeably rougher that the ‘ultra-flat’ gold substrate shown in Extended Data Fig. 2f. b, SEM images of samples with a gold thickness of 100 nm and a side length of 580 nm. c, Emission spectra at varying pump fluences. d, Light-in-light-out curves measured (circles) along with a theoretical fit (red curve). e, Output spectra of 4 LPs. f, Evolution of output spectra of two LPs at pump fluences varying from 0.1 to 4 mJ/cm2. The Q factor of the fourth-order longitudinal mode in these devices is estimated to be 42. g, SEM images of two samples after gold deposition with a thickness of 15 nm. h, Output spectra of two thin-gold-coated samples. The Q factor of the fourth-order mode in these devices is estimated to be approximately 30.

Extended Data Fig. 10 Device volume and mode order comparison.

Device volume (a) and the mode order (b) of single particle and micro- and nano-lasers operating at room temperature (cyan circles) and cryogenic temperature (pink circles). Each data point is labeled with the device name used in Supplementary Tables 1 and 2. Numerous non-metallic lasers based on periodic distributed feedback, photonic crystal reflection, and lattice structures, which operate in their lowest photonic modes, are not included in this tables since their device sizes exceed multiple wavelengths. Metal-coated lasers in C1 and C5 demonstrate photonic-like modes but do not represent the overall lowest-order plasmonic modes.

Supplementary information

Supplementary Information

Supplementary Notes 1–5, Figs. 1–4, Data Tables 1–3 and refs. 1–33 in Data Tables 1–3.

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Cho, S., Martino, N. & Yun, SH. Half-wave nanolasers and intracellular plasmonic lasing particles. Nat. Nanotechnol. 20, 404–410 (2025). https://doi.org/10.1038/s41565-024-01843-7

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