1 Localized Nitrogen -Vacancy centers generated by low-repetition rate fs -laser pulses Charlie Oncebay12 Juliana M. P. Almeida13 Gustavo F. B. Almeida14

2025-04-24 1 0 705.31KB 15 页 10玖币

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Localized Nitrogen-Vacancy centers generated by

low-repetition rate fs-laser pulses

Charlie Oncebay1,2 ∥, Juliana M. P. Almeida1,3, ∥, Gustavo F. B. Almeida1,4,

Sérgio R. Muniz1*, Cleber R. Mendonça1*

1 São Carlos Institute of Physics, University of São Paulo, 13560-970, São Carlos, SP, Brazil

2 National University of Engineering, Science Departament, Peru.

3 Department of Materials Engineering - Federal University of São Carlos, 13565-905, São

Carlos-SP, Brazil

4 Federal University of Uberlândia, Institute of Physics

∥ C.O. and J.M.P.A. contributed equally to this work.

*corresponding authors: crmendon@ifsc.usp.br; srmuniz@ifsc.usp.br

( 14/10/2022 )

Abstract

Among hundreds of impurities and defects in diamond, the nitrogen-vacancy (NV)

center is one of the most interesting to be used as a platform for quantum

technologies and nanosensing. Traditionally, synthetic diamond is irradiated with

high-energy electrons or nitrogen ions to generate these color-centers. For

precise positioning of the NV centers, fs-laser irradiation has been proposed as

an alternative approach to produce spatially localized NV centers in diamond.

However, most of the studies reported so far used high-repetition rate fs-laser

systems. Here, we studied the influence of the irradiation conditions on the

generation of NV−. Specifically, we varied pulse fluence, laser focusing, and the

number of pulses upon irradiation with 150 fs pulses at 775 nm from a Ti:sapphire

laser amplifier operating at 1 kHz repetition rate. Optically Detected Magnetic

Resonance (ODMR) was used to investigate the produced NV centers, revealing

a sizeable zero-field splitting in the spectra and indicating the conditions in which

the lattice strain produced in the ablation process may be deleterious for quantum

information applications.

Keywords: Localized Nitrogen-Vacancy centers, fs-laser pulses, NV color-centers production,

irradiation conditions for NV center creation, fs-laser microfabrication, NV center produced by fs-

laser pulses, ODMR study of fs-laser ablation, fs-laser production of color-centers

1. Introduction

There is much interest in developing methods allowing the precise

placement of engineered solid-state quantum systems, such as manufactured

artificial atoms (like spin color-centers and quantum dots), in different materials,

for quantum technology applications. One of the most promising solid-state

optically active spin systems currently studied is the nitrogen-vacancy (NV) center

in diamond, which is usually produced by irradiating ultrapure synthetic diamond

with beams of electrons or nitrogen ions. Recently, optical microfabrication using

fs-lasers has been studied as an alternative method to create such defects, but

most studies investigated systems with high-repetition rates, and few do a

detailed study of the irritation conditions.

The NV center is one of the several hundred naturally occurring defects in

the diamond lattice [1-3]. It is a point-defect created by a missing carbon next to

a substitutional nitrogen impurity in the lattice, and it has attracted a lot of interest

recently because of its distinct physical properties and many potential

applications. For example, NV centers can be optically initialized in a well-defined

quantum state, presenting long coherence times at room temperature (ranging

up to a few ms in single NV) and allowing creating protocols to manipulate its

spin-state using a combination of optical and magnetic resonance techniques.

Finally, the system’s quantum state can easily be read out by its [4-7], allowing

to control and detect a single NV center with high efficiency. Such aspects have

opened the possibility of exploring ideas and applications of quantum information

and quantum computing at room temperature [7-11].

NV centers can also be used as quantum sensors to detect physical

parameters, such as temperature, magnetic and electric fields [12-15], which

have been explored even in studies of biomolecules and cell structures [16].

Furthermore, NV centers in diamonds have emerged as a promising platform for

integrated photonic circuits [17-19], combining their nonlinear optical properties

with excellent thermal properties. The nonlinearity of diamond [20-22] has be

demonstrated to be useful for frequency conversion in the wavelength range of

telecommunication, for example [23].

In this context, the controlled production of single NV centers, or a

controlled set (ensemble) of them [24, 25], is of utmost importance to developing

semiconductor-based quantum devices because the ability to engineer such

devices can be widely used in quantum optics, magnetometry, thermometry, and

other applications. Therefore, such controlled production has prompted the

development of new methods that can be potentially used for the precise

positioning of an individual NV center, or a small set of them, in particular regions

of a diamond structure.

To generate the color-centers, the synthetic diamonds are typically

irradiated with high-energy particles, from a few keV to MeV, usually with

electrons or nitrogen ions. In addition to the particle energy, another tunable

parameter is the irradiation dose, which determines the density of vacancies

generated in the sample [26-28]. Alternatively, ultrashort-pulse laser irradiation

has also been proposed as a potential method for generating color centers,

vacancies and NV centers in diamonds [29-33]. In this approach, intense laser

pulses propagating in air ionizes molecules, like O2 and N2, generating free

electrons that are accelerated by the subsequent pulses to produce a beam of

electrons that collide with carbon atoms at the diamond’s surface, taking them

out of the crystal lattice, thus generating the vacancies. These vacancies can

move during annealing (at high temperatures), creating the possibility of binding

to some nitrogen impurity in the crystal, resulting in the NV center [29]. Direct

generation of vacancies by fs-laser followed by annealing to promote NV- centers

have also been reported [31].

Preliminary investigations on the subject demonstrated diamond

transformation to amorphous carbon, graphitic phases and 3H center formation

when using picosecond-laser irradiation [33]. Later, the same team reported the

enhancement of NV luminescence in diamond due to sp3 carbon allotropic

structures induced by picosecond laser exposure [30]. When using fs-laser, it was

demonstrated the formation NV centers in high nitrogen content-diamond through

photoluminescence (PL) measurements [29]. More recently, similar

achievements was reported in diamond with nitrogen concentration < 5ppb by

using a statistical approach and single fs-laser pulses [31] or using UV fs-laser

pulses at nanoablation regime, in which laser fluence was kept below a certain

threshold [32].

Although ultrashort-laser has been demonstrated to be useful for NV

center generation in diamonds, further investigations are essential to determine

the formation of such centers by femtosecond pulses at low-repetition,

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1LocalizedNitrogen-Vacancycentersgeneratedbylow-repetitionratefs-laserpulsesCharlieOncebay1,2∥,JulianaM.P.Almeida1,3,∥,GustavoF.B.Almeida1,4,SérgioR.Muniz1*,CleberR.Mendonça1*1SãoCarlosInstituteofPhysics,UniversityofSãoPaulo,13560-970,SãoCarlos,SP,Brazil2NationalUniversityofEngineering,ScienceDepart...

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1 Localized Nitrogen -Vacancy centers generated by low-repetition rate fs -laser pulses Charlie Oncebay12 Juliana M. P. Almeida13 Gustavo F. B. Almeida14

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