1 Mid- and far-infrared localized surface plasmon resonance s in chalcogen -hyperdoped silicon

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Mid- and far-infrared localized surface plasmon resonances in

chalcogen-hyperdoped silicon

Mao Wang1,*, Ye Yu2,‡, Slawomir Prucnal1, Yonder Berencén1, Mohd Saif Shaikh1, Lars Rebohle1,

Muhammad Bilal Khan1, Vitaly Zviagin3, René Hübner1, Alexej Pashkin1, Artur Erbe1,4, Yordan M.

Georgiev1,5, Marius Grundmann3, Manfred Helm1,6, Robert Kirchner2,4 and Shengqiang Zhou1

1Helmholtz-Zentrum Dresden-Rossendorf, Institute of Ion Beam Physics and Materials Research, Bautzner

Landstraße 400, 01328 Dresden, Germany

2Institute of Semiconductors and Microsystems, Technische Universität Dresden, 01062 Dresden, Germany

3Felix-Bloch-Institut für Festkörperphysik, Universität Leipzig, Linnéstraße 5, 04103 Leipzig, Germany

4Centre for Advancing Electronics Dresden (CfAED), Technische Universität Dresden, 01062 Dresden, Germany

5Institute of Electronics at the Bulgarian Academy of Sciences, 1784 Sofia, Bulgaria

6Institut für Angewandte Physik (IAP), Technische Universität Dresden, 01062 Dresden, Germany

Abstract

Plasmonic sensing in the infrared region employs the direct interaction of the vibrational

fingerprints of molecules with the plasmonic resonances, creating surface-enhanced sensing

platforms that are superior than the traditional spectroscopy. However, the standard noble

metals used for plasmonic resonances suffer from high radiative losses as well as fabrication

challenges, such as tuning the spectral resonance positions into mid- to far-infrared regions, and

the compatibility issue with the existing complementary metal-oxide-semiconductor (CMOS)

manufacturing platform. Here, we demonstrate the occurrence of mid-infrared localized surface

plasmon resonances (LSPR) in thin Si films hyperdoped with the known deep-level impurity

tellurium. We show that the mid-infrared LSPR can be further enhanced and spectrally extended

to the far-infrared range by fabricating two-dimensional arrays of micrometer-sized antennas

in a Te-hyperdoped Si chip. Since Te-hyperdoped Si can also work as an infrared photodetector,

we believe that our results will unlock the route toward the direct integration of plasmonic

sensors with the one-chip CMOS platform, greatly advancing the possibility of mass

manufacturing of high-performance plasmonic sensing systems.

Corresponding authors, email: *m.wang@hzdr.de; ‡ye.yu@tu-dresden.de.

I. Introduction

The field of plasmonics has elicited great attention and research efforts for potential

applications as varied as enhanced sensing, waveguides for integrated optical interconnects,

and nanoscale optoelectronic devices [1-3]. Surface plasmons generated by the coupling of

collective charge oscillations with electromagnetic radiation at a conducting surface [4] offer

effective light-matter interactions in nanoscale structures with sub-wavelength light

confinement and large enhancement of the local electromagnetic field intensity [5,6]. In this

framework, materials with a good crystalline quality and a small amount of plasmon losses are

proposed for plasmonic applications that span a wide range of electromagnetic frequencies

[5,7,8]. Particularly, the mid-infrared (MIR) spectral range that covers the frequency band from

3000 to 300 cm-1 is of high interest for chemical and biological molecular sensing [9-11], since

many molecules display unique spectral vibrational fingerprints in this range. Therefore, a

plasmonic material platform that can be tailored to the frequency range of interest with strong

subwavelength confinement is desired [12].

It has been recently shown that hyperdoped semiconductors [10,13-18] provide a

promising material system for the development of a plasmonic platform with inherent

advantages in the mid-infrared (MIR) region [19,20]. Here, hyperdoping means a doping

concentration well above the impurity solid solubility limit. Contrary to metals (Au, Ag, and

Al), in which the density of free electrons is fixed and the resulting resonance frequencies are

mainly located in the visible and near-infrared (VIS-NIR) spectral range [11], the plasmon

resonance in doped semiconductors can be tuned over a broad spectral window, ranging from

NIR to far-infrared (FIR) by controlling the carrier concentration [12,15,21-26]. Among

hyperdoped semiconductor materials, Si is the most desired material for plasmonic applications

in the MIR spectral range, owing to its compatibility with the complementary metal-oxide-

semiconductor (CMOS) technology [21,22,27-32]. Moreover, a plasmonic material based on

doped Si has certain advantages over other doped semiconductors, such as cost-effectiveness,

environmental friendliness and the well-developed and versatile fabrication process.

Importantly, compared to III-V semiconductors, the absence of optical phonon absorption in

the FIR spectral range in Si will naturally reduce the plasmon losses since Si is a non-polar

semiconductor [15,33-35]. Recently, Si hyperdoped with the chalcogen dopant Te has gained

increasing attention in the development of room-temperature MIR photodetectors [36]. Also,

Te-hyperdoped Si exhibits a high free-electron concentration with a reasonably high mobility

[37], as well as a better thermal stability as compared to other deep-level impurities [33]. This

boosts the potential of Te-hyperdoped Si serving as a nanoscale MIR plasmonics platform with

a broadly tunable plasma frequency. Such a platform could allow an easy integration with the

current chip technology, providing room-temperature enhanced IR sensing.

In this work, we explore the potential of using Si hyperdoped with the deep-level dopant

Te as an alternative for MIR-FIR plasmonic materials. A plasma frequency



p of around 1880

~1630 cm-1 is obtained in the Te-hyperdoped Si material. In addition, micrometer-sized antenna

arrays, which are fabricated from the Te hyperdoped-Si layer via electron-beam lithography

and reactive ion etching, exhibit an enhanced localized plasmon resonance in the spectral range

of 100 to 700 cm-1 compared to the non-patterned Te-hyperdoped Si material. This work points

out the potential of Si hyperdoped with Te for plasmon-enhanced sensing applications such as

the detection of the vibrational fingerprints of thin molecular films.

II. Methods

A. Experimental methods

A non-equilibrium approach combining ion implantation and flash lamp annealing (FLA)

is used to achieve solid-phase epitaxial regrowth of hyperdoped-Si layers with a Te doping

concentration several orders of magnitude above the equilibrium solid solubility limit. The

electrical and optical properties of Si hyperdoped with Te have been systematically investigated

previously [36,37]. It was found that the hyperdoped-Si layer with a Te concentration of 1.5%

exhibits below-bandgap infrared absorption and yields high electron concentrations. In this

work, we used (100)-oriented double-side polished Si wafers (p-type, boron-doped, ρ ≈ 1-10

Ωcm) with a thickness of around 380 μm. A triple implantation with energies of 350 keV, 150

keV and 50 keV with a fluence ratio of 5.3:2.3:1 was applied to compensate the Gaussian

distribution of Te dopants during the implantation process [31]. The dopant concentration and

the doping depth can be increased by increasing implantation fluence and energy, respectively.

The parameters can be simulated by using the software of the Stopping and Range of Ions in

Matter (SRIM) [38-40]. Note that, in our previous works [36,37], we used pulsed laser melting

to recrystallize Te-implanted Si with a thickness of about 100 nm. Here, millisecond-range FLA

is applied to recrystallize the implanted layer [41,42]. The FLA was performed in nitrogen

ambient with a pulse length of 3 ms along with an energy density of around 58 J/cm2. This

corresponds to a temperature in the range of around 1200 ± 50 °C at the sample surface. Further

details on the FLA system employed in our experiments can be found in the supplementary

information (SI). The optimal FLA parameters were obtained by inspecting the crystalline

quality of the implanted layers using micro-Raman spectroscopy.

The antenna patterning was achieved by electron-beam lithography and reactive ion

etching (see SI for more details). The geometrical details of the two-dimensional Te-

hyperdoped Si antenna arrays are schematically depicted in Fig. 1. The rectangular antenna

arms have a size of 2 µm (length) × 0.8 µm (width), and two equal arms featuring different gap

sizes varied between 0.2 and 1 µm.

FIG. 1. A sketch of the geometry of the Te-hyperdoped Si antenna arrays. The geometrical details are indicated in

the figure.

Structural characterization of the Te-hyperdoped Si layers and antenna arrays were

performed by micro-Raman spectroscopy using a linearly polarized continuous 532 nm

Nd:YAG laser for excitation and by scanning electron microscopy (SEM, S-4800, Hitachi). In

addition, the micro-structural properties of FLA-treated Te-hyperdoped Si layer with a Te

doping concentration of 1.5% were carried out by high-angle annular dark-field scanning

transmission electron microscopy (HAADF-STEM) with energy-dispersive x-ray spectroscopy

(EDXS) element distributions, further details concerning the TEM techniques employed in our

experiments can be found elsewhere [40]. The electrical properties were characterized using a

Lake Shore Hall measurement system in a van der Pauw configuration. IR measurements were

carried out at room temperature by Fourier-transform infrared spectroscopy (FTIR, Bruker

Vertex 80v). A Deuterated L-Alanine doped Triglycine Sulphate (DLaTGS) detector was used

for the detection of MIR (from 10000 to 400 cm-1) radiation, while a deuterated triglycine

sulfate (DTGS) detector was used for FIR (from 700 to 10 cm-1). FTIR measurements were

performed in vacuum to eliminate the infrared absorption lines of the atmosphere. A reflection

geometry was employed to quantify the absolute reflectivity of FLA-performed Te-hyperdoped

Si layers and the antenna arrays. The reflectance of a gold mirror was measured as a 100%

reflectance standard for the FTIR data.

B. Theoretical methods

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1Mid-andfar-infraredlocalizedsurfaceplasmonresonancesinchalcogen-hyperdopedsiliconMaoWang1,*,YeYu2,‡,SlawomirPrucnal1,YonderBerencén1,MohdSaifShaikh1,LarsRebohle1,MuhammadBilalKhan1,VitalyZviagin3,RenéHübner1,AlexejPashkin1,ArturErbe1,4,YordanM.Georgiev1,5,MariusGrundmann3,ManfredHelm1,6,RobertKirch...

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